TMP DCCD

Atmos. Chem. Phys.
, 14, 1001310060, 2014

www.atmos-chem-phys.net/14/10013/2014/
doi:10.5194/acp-14-10013-2014
Author(s) 2014. CC Attribution 3.0 License.
Modeling regional aerosol and aerosol precursor variability over
California and its sensitivity to emissions and long-range transport
during the 2010 CalNex and CARES campaigns
J. D. Fast
1
, J. Allan
2
, R. Bahreini
3,4
, J. Craven
5
, L. Emmons
6
, R. Ferrare
7
, P. L. Hayes
3,****
, A. Hodzic
6
,
J. Holloway
3,4
, C. Hostetler
7
, J. L. Jimenez
3
, H. Jonsson
8
, S. Liu
9
, Y. Liu
1
, A. Metcalf
5,**
, A. Middlebrook
4
,
J. Nowak
10
, M. Pekour
1
, A. Perring
3,4
, L. Russell
11
, A. Sedlacek
12
, J. Seinfeld
5
, A. Setyan
14,*
, J. Shilling
1
,
M. Shrivastava
1
, S. Springston
12
, C. Song
1
, R. Subramanian
13
, J. W. Taylor
2
, V. Vinoj
1,***
, Q. Yang
1
, R. A. Zaveri
1
,
and Q. Zhang
14
1
Pacic Northwest National Laboratory, Richland, Washington, USA
2
School of Atmospheric and Environmental Sciences, University of Manchester, Manchester, UK
3
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, Colorado, USA
4
Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, Colorado, USA
5
California Institute of Technology, Pasadena, California, USA
6
National Center for Atmospheric Research, Boulder, Colorado, USA
7
NASA Langley Research Center, Hampton, Virginia, USA
8
Center for Interdisciplinary Remotely Piloted Aerosol Studies, Marina, California, USA
9
Los Alamos National Laboratory, Los Alamos, New Mexico, USA
10
Aerodyne, Inc. Billerica, Massachusetts, USA
11
Scripps Institute of Oceanography, University of California San Diego, San Diego, California, USA
12
Brookhaven National Laboratory, Upton, New York, USA
13
Department of Mechanical Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania, USA
14
Department of Environmental Toxicology, University of California Davis, Davis, California, USA
*
now at: Empa, Swiss Federal Laboratories for Materials Science and Technology, 8600 Dbendorf, Switzerland
**
now at: Department of Mechanical Engineering, University of Minnesota Twin Cities, Minneapolis, Minnesota, USA
***
now at: Indian Institute of Technology, Bhubaneswar, India
****
now at: Department of Chemistry, University of Montreal, Montreal, Quebec, Canada
Correspondence to: J. D. Fast (jerome.fast@pnnl.gov)
Received: 20 February 2014 Published in Atmos. Chem. Phys. Discuss.: 18 March 2014
Revised: 13 August 2014 Accepted: 21 August 2014 Published: 22 September 2014
Abstract. The performance of the Weather Research and
Forecasting regional model with chemistry (WRF-Chem)
in simulating the spatial and temporal variations in aerosol
mass, composition, and size over California is quantied us-
ing the extensive meteorological, trace gas, and aerosol mea-
surements collected during the California Nexus of Air Qual-
ity and Climate Experiment (CalNex) and the Carbonaceous
Aerosol and Radiative Effects Study (CARES) conducted
during May and June of 2010. The overall objective of the
eld campaigns was to obtain data needed to better under-
stand processes that affect both climate and air quality, in-
cluding emission assessments, transport and chemical aging
of aerosols, aerosol radiative effects. Simulations were per-
formed that examined the sensitivity of aerosol concentra-
tions to anthropogenic emissions and to long-range trans-
port of aerosols into the domain obtained from a global
model. The conguration of WRF-Chem used in this study
is shown to reproduce the overall synoptic conditions, ther-
mally driven circulations, and boundary layer structure ob-
served in region that controls the transport and mixing of
Published by Copernicus Publications on behalf of the European Geosciences Union.
10014 J. D. Fast et al.: Modeling regional aerosol and aerosol precursor variability over California
trace gases and aerosols. Reducing the default emissions in-
ventory by 50 % led to an overall improvement in many sim-
ulated trace gases and black carbon aerosol at most sites and
along most aircraft ight paths; however, simulated organic
aerosol was closer to observed when there were no adjust-
ments to the primary organic aerosol emissions. We found
that sulfate was better simulated over northern California
whereas nitrate was better simulated over southern Califor-
nia. While the overall spatial and temporal variability of
aerosols and their precursors were simulated reasonably well,
we show cases where the local transport of some aerosol
plumes were either too slow or too fast, which adversely af-
fects the statistics quantifying the differences between ob-
served and simulated quantities. Comparisons with lidar and
in situ measurements indicate that long-range transport of
aerosols from the global model was likely too high in the
free troposphere even though their concentrations were rela-
tively low. This bias led to an over-prediction in aerosol op-
tical depth by as much as a factor of 2 that offset the under-
predictions of boundary-layer extinction resulting primarily
from local emissions. Lowering the boundary conditions of
aerosol concentrations by 50 % greatly reduced the bias in
simulated aerosol optical depth for all regions of California.
This study shows that quantifying regional-scale variations
in aerosol radiative forcing and determining the relative role
of emissions from local and distant sources is challenging
during clean conditions and that a wide array of measure-
ments are needed to ensure model predictions are correct for
the right reasons. In this regard, the combined CalNex and
CARES data sets are an ideal test bed that can be used to
evaluate aerosol models in great detail and develop improved
treatments for aerosol processes.
1 Introduction
Accurately simulating aerosol number, mass, composition,
size distribution, and hygroscopicity continues to be a major
challenge for air quality and climate models. There are sev-
eral factors that contribute to errors in regional-scale model
predictions of aerosol properties. First, it is well known that
the complex spatial and temporal variability in human ac-
tivities (e.g., fossil fuel uses, biomass burning) and natu-
ral sources (e.g., biological emissions, dust, sea-salt) con-
tribute to uncertainties in trace gas precursor and primary
aerosol emission estimates. Emission inventories suitable for
regional models have been developed by many organizations
for specic cities, regions, or countries, but they are often
rely on different assumptions and apply only for specic
time periods (e.g., Granier et al., 2011). Second, errors aris-
ing from meteorological parameterizations in regional mod-
els directly affect the simulated aerosol life cycle. Meteoro-
logical processes that have large uncertainties include, tur-
bulent vertical mixing that affects the dilution and chemi-
cal processing of aerosols and their precursors (e.g., Aan de
Brugh et al., 2012; Nilsson et al., 2001), vertical motions as-
sociated with sub-grid scale clouds that affect the vertical
transport of aerosols (e.g., Gustafson et al., 2008), the spa-
tial extent and lifetime of clouds that affects aerosol chemi-
cal and size transformation within clouds (e.g., Ervens et al.,
2011; Fahey and Pandis, 2001) and photochemistry above
and below clouds (e.g., Feng et al., 2004; Tang et al., 2003),
and precipitation that controls wet removal of aerosols and
their trace gas precursors (e.g., Wang et al., 2013; Yang et
al., 2012; Barth et al., 2007). Third, the level of complexity
in the treatment of aerosol chemistry (equilibrium versus dy-
namic approach for gas-to-particle partitioning, the number
of aerosol species and gas-phase precursors) (e.g., Baklanov
et al., 2014) and size distribution (bulk, modal, and sectional
approaches) varies among models. A fourth factor is the in-
complete understanding of secondary organic aerosol (SOA)
formation, aging, and removal based on laboratory and eld
studies, which leads to large uncertainties in simulated SOA
(e.g., Heald et al., 2011; Spracklen et al., 2011; Hodzic et al.,
2013). The spatial resolution of regional models contributes
to all four of these factors, but the implications of ignor-
ing the sub-grid scale variability of aerosol properties (Qian
et al., 2010; Gustafson et al., 2011) is largely unexplored.
Therefore, inadequate resolution of the large observed spatial
and temporal variability of aerosols is a fth factor. Finally,
regional model predictions are often inuenced by bound-
ary conditions that are either specied by prescribed clima-
tological values or obtained from coarser global models that
can represent long-range transport of trace gases and aerosols
that affect local concentrations. Therefore a sixth factor con-
sists of errors from global model predictions that are propa-
gated into the regional model domains. It is likely that one
or more of these six factors are more signicant for some
regions than others.
Previous chemical transport modeling studies over the
continental US have shown geographical variations in model
performance. For example, Kang et al. (2010) used the
CMAQ model with a horizontal grid spacing of 12 km over
the continental US for a 1-year period and showed that PM
2.5
concentrations were generally too low over the eastern US
during the summer of 2007 and too high during the win-
ter months of 2007. The model performance was more vari-
able in California, a region with large topographic, land
use, and population variations, with positive biases at some
stations and negative biases at other stations. A simulation
over the continental US for 2009 using the GEOS-Chem
model (Walker et al., 2012) with a horizontal grid spacing
of 0.5
0.67
showed that while predicted annual mean

sulfate concentrations over the continental US were similar
to observations, nitrate and ammonium were too high over
the eastern and mid-western US and too low over California,
where the observed concentrations were the highest. They in-
dicated that the bias in nitrate over California was likely due
to both ammonia emission estimates that were too low and
Atmos. Chem. Phys., 14, 1001310060, 2014 www.atmos-chem-phys.net/14/10013/2014/
J. D. Fast et al.: Modeling regional aerosol and aerosol precursor variability over California 10015
simulated boundary-layer depths that were too high. Heald et
al. (2012) reported similar spatial variations in the biases in
sulfate and nitrate over the US during 2004, 2009, and 2010
from their GEOS-Chem simulations over North America.
Huang et al. (2012) used the STEM model with a 60 km grid
spacing to show that the performance in simulating surface
black carbon over a 2-week period during June, 2008 varied
over the US, with the largest negative biases in the southeast-
ern US and the highest positive biases over the northeastern
US. They also noted that black carbon was also 30 % too
low on average for surface sites in the southwestern US and
that the differences in simulated vertical proles of black car-
bon compared with NASA DC-8 aircraft data over California
could be attributed to the coarse spatial grid spacing that does
not permit the model to resolve the variability in meteorology
associated with topographic variations in the vicinity of Los
Angeles and the San Joaquin Valley.
Several eld campaigns have been conducted in Califor-
nia to collect data needed to better understand and char-
acterize ozone and particulates in the region and to ad-
dress modeling challenges using higher spatial resolution
that better represents the terrain inhomogeneity in Califor-
nia. These campaigns include the Southern California Air
Quality Study (SCAQS) conducted in August 1987 (Law-
son, 1990), the South Coast Air Basin of California (So-
CAB) study during September 1993 (Frasier et al., 1996),
the Southern California Ozone Study (SCOS) conducted be-
tween June and October of 1997 (Croes and Fujita, 2003),
the 19992001 California Regional Particulate Air Qual-
ity Study (CRPAQS) conducted between December 1999 to
February 2001 (Chow et al., 2006), the 2000 Central Cali-
fornia Ozone Study (CCOS) (Fujita et al., 2005), the Study
of Organic Aerosols at Riverside (SOAR) conducted be-
tween July and August 2005 (Docherty et al., 2011), the Bio-
sphere Effects on AeRosols and Photochemistry Experiment
(BEARPEX) conducted between August and October 2007
(Bouvier-Brown et al., 2009), and the Arctic Research of the
Composition of the Troposphere from Aircraft and Satellites
California Air Resources Board (ARCTAS-CARB) exper-
iment conducted in June 2008 (Jacob et al., 2010). Many
modeling studies that employ these eld campaign data have
focused on the performance of simulated meteorology (e.g.,
Bao et al., 2008) and ozone (e.g., Jacobson, 2001; Jin et al.,
2010; Lu et al., 1997). Modeling studies of aerosol mass,
composition, and size distribution using these eld campaign
data have focused on the performance in regions where con-
centrations are usually the highest, either in the vicinity of
Los Angeles (e.g., Grifn et al., 2002; Held et al., 2005;
Jacobson, 1997; Meng et al., 1998; Vutukuru et al., 2006;
Zhang et al., 2004) or over the San Joaquin Valley (e.g., Pun
et al., 2009; Ying and Kleeman, 2009; Zhang et al., 2010).
Since regional-scale models depend on boundary conditions
provided by other models, Huang et al. (2010) and Pster
et al. (2011) use large-scale chemical transport models and
ARCTAS-CARB measurements to show that uncertainties in
long-range transport of pollution from Asia can lead to errors
in simulated regional-scale trace gas and aerosol concentra-
tions over California.
While air quality issues associated with PM
2.5
concen-
trations have been the driving factor for previous measure-
ments and modeling studies in California, improving the un-
derstanding of regional-scale climate-chemistry interactions
and aerosol radiative forcing has received increasing atten-
tion in recent years (e.g., Xu et al., 2013; C. Zhao et al.,
2013). National and local agencies are interested in knowing
the relative contributions of local and upwind anthropogenic
pollution and their impact on current and future climate. Un-
derstanding the climate impact of aerosols rst requires that
the aerosol life cycle be represented reasonably well, which
requires that models accurately simulate aerosol composi-
tion, size distribution, hygroscopicity, and optical properties
in addition to total mass. This is a challenging task. To ad-
dress model uncertainties associated with climate and air-
quality relevant atmospheric processes, two campaigns were
conducted in California during the spring and early summer
of 2010 that collected extensive meteorological, trace gas,
and aerosol data: California Nexus (CalNex): Research at
the Nexus of Air Quality and Climate (Ryerson et al., 2013)
and the Carbonaceous Aerosol and Radiative Effects Study
(CARES) (Zaveri et al., 2012). A few meteorological and
aerosol model evaluation studies for this period have been
completed. The Weather Research and Forecasting (WRF)
model with a 4 km horizontal grid spacing was used to evalu-
ate the simulated boundary layer and thermally driven circu-
lations over central California using CARES measurements
(Fast et al., 2012) and the simulated boundary layer and
land/sea breezes over the southern California coastal zone
using CalNex measurements (Angevine et al., 2012). Ens-
berg et al. (2013) used CalNex ground and aircraft mea-
surements to evaluate predictions of trace gases, inorganic
aerosols, and black carbon made by the CMAQ model with
a 4 km grid spacing over southern California, while Knote et
al. (2014) used the CARES and CalNex data and the WRF-
Chem model to evaluate the effect of various glyoxal treat-
ments on the formation of SOA.
The combined CalNex and CARES eld campaigns pro-
vide an unprecedented data set in terms of the number of pa-
rameters measured and their spatial and temporal resolution
that can be used to evaluate predictions of aerosol concen-
tration, composition, hygroscopicity, and size needed to un-
derstand the sources of uncertainties in estimates of aerosol
radiative forcing. We have combined the data from these two
eld campaigns with other operational monitoring data set
into the Aerosol Model Testbed (AMT) framework as de-
scribed by Fast et al. (2011). The rst objective of this study
is to evaluate regional-scale predictions of aerosols, aerosol
precursors, and meteorological processes affecting aerosols
using as much of the measurements collected over California
during the eld campaign period. While several factors are
known to contribute to errors in aerosol predictions, it is not
www.atmos-chem-phys.net/14/10013/2014/ Atmos. Chem. Phys., 14, 1001310060, 2014
feasible to investigate all of them in a single study. Therefore,
our second objective is using the AMT and the CalNex and
CARES data set to investigate two sources of uncertainties,
emissions estimates and long-range transport, and their effect
on the predictions of aerosols and their precursor over Cal-
ifornia. In contrast to most previous modeling studies that
focus on either the Los Angeles Basin or San Joaquin Val-
ley, the combined CalNex and CARES data set enables the
model to be evaluated over a larger region where aerosols
are inuenced by a wider range of meteorological conditions.
Not surprisingly, we nd that model performance varies over
the region and some trace gases and aerosol species are sim-
ulated better than others. The sensitivity simulations show
many trace gases and black carbon emissions in the latest
emissions inventory are likely too high in the entire region.
We also show that while errors in long-range transport do
not signicantly affect simulated aerosol properties close to
the surface near emissions sources, small errors in free tropo-
spheric aerosol concentrations led to a large positive bias in
simulated aerosol optical depth. This indicates that regional-
scale climate simulations can easily produce erroneous re-
sults regarding the relative role of local emissions and long-
range transport on local aerosol radiative forcing, even over
regions with substantial overall emissions such as California.
A brief description of the eld campaign measurements
and how they are incorporated into the AMT is included in
Sect. 2. The conguration of the regional aerosol model is
described in Sect. 3. The comparison of the model simula-
tion with the measurements is presented in Sect. 4, starting
with discussion of model performance associated with me-
teorological and trace gas quantities in Sects. 4.1 and 4.2,
respectively. Most of our analysis will focuses on model per-
formance in simulating aerosol properties, divided into car-
bonaceous aerosols in Sect. 4.3 and inorganic aerosols in
Sect. 4.4. Section 4.5 presents the model performance on
aerosol volume and number distributions. The impact of sim-
ulated aerosols on aerosol optical depth and extinction is pre-
sented in Sect. 5 since comparisons with observations is way
of evaluating simulated aerosol concentrations throughout a
vertical column where in situ measurements may not exist.
Section 6 is a discussion that compares the present simu-
lations with those conducted by other CalNex investigators
and describes how various model uncertainties contribute to
model performance, while Sect. 7 summarizes our primary
ndings.
2 Measurements
Measurements collected in California during May and June
of 2010 as part of the CalNex and CARES campaigns
are used to evaluate mesoscale predictions of aerosols and
aerosol precursors. CalNex was designed to address sci-
ence issues relevant to emission inventory assessment, dis-
persion of trace gases and aerosols, atmospheric chemistry,
and the interactions of aerosols clouds, and radiation (Ryer-
son et al., 2013). Ground-based instruments were deployed
at two sites in southern California as shown in Fig. 1a: one in
Pasadena (34.141
N, 118.112
W, 240 mm.s.l.) (Chan

et al., 2013; Hayes et al., 2013; Pennington et al., 2012;
Thompson et al., 2012; Veres et al., 2011) and one in Bakers-
eld (35.346
N, 118.965
W, 123 mm.s.l.) (Alm et al.,

2012; Liu et al., 2012; Rollins et al., 2012, 2013; Y. Zhao
et al., 2013). Four research aircraft, the NOAA WP-3D, the
National Oceanic and Atmospheric Administration (NOAA)
Twin Otter, the Center for Interdisciplinary Remotely Piloted
Aerosol Studies (CIRPAS) Twin Otter and the NASA B-
200, sampled atmospheric conditions aloft and the NOAAre-
search vessel (R/V) Atlantis sampled atmospheric conditions
along the coast of California. In situ measurements of meteo-
rological, trace gas, and aerosol quantities were collected by
the WP-3D (Bahreini et al., 2012; Ryerson et al., 2013; Lan-
gridge et al., 2012; Moore et al., 2012; Pollack et al., 2012;
Warneke et al., 2011; Peischl et al., 2012), CIRPAS Twin Ot-
ter (Duong et al., 2011; Metcalf et al., 2012; Craven et al.,
2013; Hersey et al., 2013), and the R/V Atlantis. The Tun-
able Optical Proler for Aerosols and oZone (TOPAZ) differ-
ential absorption lidar (DIAL) was deployed on the NOAA
Twin Otter (Langford et al., 2012) and the High Spectral Res-
olution Lidar (HSRL-1) (Hair et al., 2008) was deployed on
the B-200 (Scarino et al., 2014). As shown in Fig. 1a, most
of the CalNex aircraft and research vessel sampling was con-
ducted in southern California in the vicinity of the Los An-
geles basin. Ozonesondes were launched at six sites to ob-
tain proles of meteorological quantities along with ozone
mixing ratio in the region (Cooper et al., 2011). A detailed
description of the instrumentation for each of the CalNex
surface sites and mobile platforms is given by Ryerson et
al. (2013).
CARES was designed to address science issues associ-
ated with the interactions of biogenic and anthropogenic
precursors on secondary organic aerosol (SOA), black car-
bon mixing state, and the effects of organic species and
aerosol mixing state on optical properties and the activation
of cloud condensation nuclei (CCN) (Zaveri et al., 2012).
As shown in Fig. 1b, ground-based instruments were de-
ployed at two sites in northern California: one in Sacramento
(38.649
N, 121.349
W, 30 mm.s.l.) and the other in

Cool (38.889
N, 120.974
W, 450 mm.s.l.), a small

town located about 40 km northeast of Sacramento. The
Sacramento and Cool sites are also referred to as T0 and
T1, respectively, to denote transport time intervals associ-
ated with the predominately southwesterly daytime winds.
This sampling strategy was based on the known transport
pathways of the Sacramento plume that was also observed
during BEARPEX (Bouvier-Brown et al., 2009). Three re-
search aircraft, the DOE G-1, the NASA B-200, and the
NOAA Twin Otter sampled atmospheric conditions aloft in
the vicinity of the T0 and T1 sites. In situ measurements
of meteorological, trace gas, and aerosol quantities were
Figure 1. Geographic distributions of xed and mobile sampling during the (a) CalNex and (b) CARES campaigns along with operational
(c) meteorological and (d) air quality sampling sites. Yellow circle in (a) and (b) denote measurement supersites while blue lines in (c) denote
geographic regions to compute statistics. Gray shading denotes model topography using x =4 km. The modeling domain extends 150 km
west of the western boundary shown above. BBY = Bodega Bay, BKF = Bakerseld, CCL = Chowchilla, CCO = Chico, GRM= Gorman,
IRV = Irvine, LHS = Lost Hills, LVR = Livermore, ONT = Ontario, SAC = Sacramento, USC = University of Southern California, VIS
= Visalia, WAP = Whiteman Airport Pacomia, TRK = Truckee.
collected by the G-1 while the NOAA Twin Otter and the
B-200 had the same remote sensing instrumentation as dur-
ing CalNex. Zaveri et al. (2012) describe the instrumentation
for each of the surface sites and mobile platforms. Most of
the sampling during CalNex occurred between 15 May and
16 June, while sampling during CARES occurred between 2
and 28 June.
In addition to the extensive measurements collected from
the two campaigns, a wide range of meteorological and air-
quality data are routinely collected over California as shown
in Fig. 1c and d, respectively. Meteorological data collected
by several agencies were available from several hundred sur-
face sites, hourly proles of wind speed and direction were
available from 14 radar wind prolers, and proles of tem-
perature, humidity, pressure, wind speed, and wind direction
from radiosondes were launched up to twice a day at four
sites in California. An air-quality monitoring network op-
erated by the California Air Resources Board (CARB) pro-
vides hourly data on ozone (O
3
), nitrogen oxides (NO
x
), sul-
fur dioxide (SO
2
), carbon monoxide (CO), PM
2.5
, and PM
10
at sites throughout California (http://www.arb.ca.gov/aqd/
aqmoninca.htm). The Interagency Monitoring of Protected
Visual Environment (IMPROVE) network (Malm et al.,
1994) provides 24 h average aerosol composition at 20 sites
in California. Additionally, there were 10 sites during 2010
that provided measurements of column integrated aerosol op-
tical properties (e.g., aerosol optical depth) as part of the
NASAs AErosol RObotic NETwork (AERONET) (Holben
et al., 1998; Dubovik et al., 2002).
A discussion on how the CARES, CalNex, and operational
measurements have been merged into a single data set (Fast
et al., 2011) is included in the Supplement in Fig. S1.
3 Model description
Version 3.3.1 of the WRF-Chem community model (Grell et
al., 2005) is used in this study to simulate the evolution of
aerosols over California. The model conguration is similar
to that used for operational meteorological and tracer fore-
casting during CARES as described by Fast et al. (2012), ex-
cept that trace gas and aerosol chemistry are now included.
The specic physical parameterizations used in this study,
also available in the public release of the model, are listed in
Table 1. We use the SAPRC-99 photochemical mechanism
(Carter, 2000a, b) to simulate gas-phase chemistry, and the
MOSAIC module (Zaveri et al., 2008) with eight size bins
to simulate aerosol chemistry, thermodynamics, kinetic gas-
particle partitioning for inorganic species, and aerosol dy-
namics. The simplied two-product volatility basis set (VBS)
parameterization is used to simulate equilibrium SOA parti-
tioning as described in Shrivastava et al. (2011), except that
the factor of 2 used to increase primary organic aerosol emis-
sions in that study to obtain better agreement between sim-
ulated primary organic aerosol (POA) and estimates of POA
derived from aerosol mass spectrometer (AMS) data is not
employed here.
The model domain encompasses all of California, Nevada,
and the adjacent Pacic Ocean using a horizontal grid spac-
ing of 4 km. The domain is identical to the domain used in
Fast et al. (2012), and extends 150 km further over the
ocean than is shown in Fig. 1. A stretched vertical coordi-
nate that uses 65 grid levels extends up to 1620 kma.g.l.,
with a 30 m grid spacing adjacent to the surface and 43 lev-
els located within 2 km of the ground. The simulation pe-
riod is from 1 May to 30 June 2010. Initial and boundary
conditions for the meteorological variables were based on
analyses from the National Center for Environmental Pre-
dictions North American Mesoscale (NAM) model, while
initial and boundary conditions for trace gases and aerosols
were obtained from the global MOZART model (Emmons et
al., 2010). Boundary conditions were updated at 6 h intervals
from both models and then interpolated linearly in time by
WRF (Skamarock et al., 2005). Instead of performing a series
of short forecasts, a single simulation was performed over the
2-month period in which four-dimensional meteorological
data assimilation was applied above 1.5 kma.g.l. using anal-
Table 1. Selected WRF-Chem conguration options used for this
study.
Atmospheric process Option
Advection monotonic
Long wave radiation RRTMG
Shortwave radiation RRTMG
Surface layer MoninObukhov (Janic)
similarity theory
Land surface Noah
Boundary layer MellorYamadaJanic
Cumulus convection KainFritsch
Cloud microphysics Morrison
Gas-phase chemistry SAPRC-99
Photolysis FTUV
Aerosol chemistry MOSAIC with volatility
basis set (VBS)
Direct effect on
Indirect effect off
yses from the NAM model so that the simulated large-scale
ows did not diverge from observed synoptic conditions. A
test simulation without data assimilation (not shown) pro-
duced similar results, suggesting that the free tropospheric
meteorological conditions were largely governed by the lat-
eral boundary conditions.
Anthropogenic emissions were obtained from the CARB
2008 ARCTAS emission inventory developed for the NASA
Arctic Research of the Composition of the Troposphere from
Aircraft and Satellite (ARCTAS) mission over California
(Pster et al., 2011). The CARB inventory contains hourly
emissions for a 13-day period using a 4 km grid spacing over
California. We created diurnally averaged emissions from 5
of the weekdays and 2 of the weekend days and used those
averages for all weekdays and weekends in the entire 2-
month simulation period. Anthropogenic emissions from the
2005 National Emissions Inventory (NEI) were used for re-
gions outside of California. Emissions of semi-volatile and
intermediate volatility SOA trace gas precursors were as-
sumed to be 6.5 times the mass of primary organic aerosol
emissions from anthropogenic and biomass burning sources
as in Shrivastava et al. (2011) and Tsimpidi et al. (2010).
Biogenic emissions were computed on-line using the Model
of Emissions of Gases and Aerosols from Nature (MEGAN)
model (Guenther et al., 2006) and lumped into isoprene, ter-
penes, and sesquiterpenes for the SAPRC-99 photochem-
ical mechanism. Sea-salt emissions (sodium and chloride)
from the ocean were computed online using uxes based
on predicted surface winds and boundary layer quantities
as described by Gong et al. (2002). While biomass burning
and dust emissions are not considered in the present study,
long-range transport of smoke and dust from Asia as rep-
resented by MOZART were included through the boundary
Figure 2. Spatial distribution of anthropogenic volatile organic compounds (VOC) (top) and biogenic isoprene (bottom) emission rates for
a representative day at 10:00 LST over California and in the vicinity of the Pasadena, T0, and T1 supersites (white dots). The middle panels
depict the Los Angeles Basin and the right panels depict a portion of the Sacramento Valley. Contours denote model topography (m) and
regions that are not shaded denote low emission rates.
conditions. Satellite detection methods indicated that there
were very few res in California during this 2-month period.
Anthropogenic VOC and biogenic isoprene emission rates
over California and in the vicinity of the Los Angeles and
Sacramento supersites at 10 Local Standard Time (LST) on a
representative day are shown in Fig. 2. As expected, the high-
est anthropogenic volatile organic compound (VOC) emis-
sion rates are proportional to population density. A portion
of the interstate highway system is also evident in the g-
ure, especially in the sparsely populated regions of Nevada
and southeastern California. While biogenic emissions occur
in most non-desert regions of California, the emission rates
are highest along the foothills of the Sierra Nevada that are
dominated by oak trees.
Two preliminary simulations (not shown here) were per-
formed that used either the merged CARB 2008 and NEI
2005 inventories or only the NEI 2005 inventory over the
entire model domain. While both simulations usually over-
predicted CO, NO
x
, and black carbon (that largely originate
from trafc emissions), concentrations from the simulation
that used the CARB 2008 inventory were closer to observa-
tions in both southern and northern California (not shown).
This is consistent with the decrease in anthropogenic emis-
sions over the past decade in California reported by Bahadur
et al. (2011) and ARB (2009). Table 2 lists the total daily
trace gas and aerosol emissions over the modeling domain
for weekday and weekend periods. It is reasonable to as-
sume anthropogenic emissions during 2010 would be less
than during 2008, but the exact amount is still under inves-
tigation using a variety of methods. A few recent modeling
studies have examined how reasonable the 2008 emission in-
ventory is for this region. Using inverse modeling, Brioude et
al. (2013) developed an improved CO and NO
x
emission in-
ventory for the Los Angeles basin to correct for inconsisten-
cies in amounts and spatial distributions found in the CARB
emission inventory. To reduce uncertainties in VOC emis-
sions and their speciation, Knote et al. (2014) applied mea-
sured VOC/CO emission ratios obtained from the Los An-
geles basin during CalNex. They found considerable differ-
ences (up to a factor of 10 for some VOCspecies) in the es-
timates of VOC emissions as well as OH concentrations be-
tween the CARB inventory and the amounts estimated from
the measured VOC/CO emission ratios in the Los Angeles
basin. These updates have not yet been incorporated in the
publicly released inventory, and have not been considered in
our study.
Until a more rened inventory for 2010 is available,
we performed a default simulation, called DEF_ANT,
that employed the merged CARB 2008 and NEI 2005 in-
ventories (Table 2) and two sensitivity simulations, called
50 %_ANT and 0 %_ANT as indicated in Table 3. The
two sensitivity simulations reduce the anthropogenic emis-
sions by 50 % (except for SO
2
and NH
3
) in the former
and eliminate them in the latter. Reducing anthropogenic
Table 2. Total daily emissions (metric tons) of trace gases and ne particulates (PM
2.5
) over the modeling domain for weekday and week-
end periods derived from the 2008 CARB emission inventory (over California) and the 2005 National Emissions Inventory (elsewhere) as
described in the text. VOC are the sum of all non-methane volatile organic compounds and other inorganic (OIN) are other inorganic aerosol
of unspecied composition.
CO NO
x
SO
2
NH
3
VOC BC OA SO
4
NO
3
OIN
weekday 13 669.0 3409.3 509.9 803.6 3302.2 56.9 156.1 43.1 1.4 242.4
weekend 14 430.9 2031.0 499.7 803.3 3238.5 54.8 123.6 47.2 1.4 237.3
Table 3. Description of simulations performed for this study.
Simulation
Name
Description
DEF_ANT Default conguration that employs the
merged CARB 2008 emissions inven-
tory over California and NEI 2005
emissions inventory elsewhere. Bio-
genic and sea-salt emissions are com-
puted on-line.
50 %_ANT 50 % reduction of anthropogenic emis-
sions, with the exception of SO
2
and
NH
3
that are left unchanged; otherwise
identical to DEF_ANT
0 %_ANT no anthropogenic emissions, otherwise
identical to DEF_ANT
50 %_LBC 50 % reduction of aerosols for the ini-
tial and boundary conditions, otherwise
identical to 50 %_ANT
emissions by 50 % is a rather large adjustment considering
a 2-year trend, but this factor also assumes the CARB 2008
emission estimates may be too high for that time period.
Kozawa et al. (2014) recently reported similar reductions in
NO
x
and BC emission estimates based on truck-dominated
freeways in Los Angeles from 2009 to 2010. All three simu-
lations include on-line biogenic and sea-salt emissions. The
simulation with no anthropogenic emissions is performed to
estimate the relative contribution of local emission sources
and long-range transport on aerosol concentrations through-
out California. One additional sensitivity simulation is per-
formed, called 50 %_LBC in which aerosols for the ini-
tial and boundary conditions obtained from MOZART are
reduced by half in addition to reducing the anthropogenic
emissions by 50 %. As will be shown later, total aerosol mass
near the surface is usually not signicantly affected by long-
range transport, but small aerosol concentrations in the free
troposphere transported from Asia are the primary contribu-
tor to aerosol optical depth outside of major urban areas.
The four simulations all employ aerosol direct effects (Fast
et al., 2006), primarily to obtain aerosol optical properties to
compare with measurements. The impact of different aerosol
loading and distributions among the simulations on radiation
and subsequently meteorology is small (not shown); there-
fore, evaluation of the simulated meteorological quantities
is presented only for the DEF_ANT simulation. Aerosol in-
direct effects, cloud chemistry, and wet scavenging are cur-
rently neglected since there were relatively few clouds and
little rain over land during the 2-month period.
4 Model evaluation
The AMT software is used to extract variables related to me-
teorological, trace gas, aerosol, and aerosol optical properties
from the four WRF-Chem simulations compatible with most
of the measurements collected during CARES and CalNex
and perform most of the statistics shown in this section. Bias
is expressed in terms of simulated minus observed values.
In addition to root mean square error (RMSE) and correla-
tion coefcient (R), we also use the index of agreement (IA)
developed by Willmott (1981) that varies between 0 and 1
where 1 indicates a perfect match. While the AMT was orig-
inally conceived to test aerosol process modules while all
other processes remain the same, the same methodology is
used here to assess model sensitivity to emissions and bound-
ary conditions.
Meteorological predictions during CalNex and CARES
using the WRF model have been discussed previously by
Angevine et al. (2012) and Fast et al. (2012), respectively.
An evaluation of the simulated meteorological quantities not
described previously is included in the Supplement and in
Tables 47. In summary, the overall simulated diurnal and
multi-day variations in meteorological quantities (temper-
ature, humidity, wind speed and direction, boundary layer
depth) that affect the evolution of trace gases and aerosols are
consistent with a wide range of CARES and CalNex mea-
surements and the models statistical performance is simi-
lar to those from other chemical transport modeling studies.
While the near-surface wind speeds are too high, the over-
all bias in simulated winds aloft is closer to zero and trans-
port processes throughout the troposphere controls the move-
ment of trace gas and aerosol plumes. Nevertheless, rela-
tively small errors in the simulated meteorological quanti-
ties can still impact the timing and spatial variability of these
plumes as will be shown later.
Table 4. Performance of simulated temperature (T), relative humidity (RH), wind speed (WS), and wind direction (WD) in terms of bias,
root-mean-square error (RMSE), correlation coefcient (R), and index of agreement (IA) for the surface stations depicted in Fig. 1c. Statistics
given for all of California (CA) and by region (Fig. 1c).
Variable Region Observed Bias RMSE R IA
Mean
T (K)
CA 289.9 0.5 3.4 0.90 0.94
Southern_CA 292.0 0.3 3.5 0.87 0.93
San Joaquin valley 293.1 0.2 3.1 0.90 0.95
Sacramento Valley 292.3 0.7 3.2 0.89 0.94
Coastal 287.4 0.2 3.2 0.86 0.92
Interior Mountains 288.9 0.9 3.6 0.92 0.95
RH ( %)
CA 55.6 2.7 17.5 0.76 0.87
Southern CA 57.7 7.0 19.2 0.76 0.86
San Joaquin Valley 49.2 5.5 14.6 0.79 0.87
Coastal 65.9 0.2 17.1 0.72 0.85
WS (ms
1
)
CA 3.0 1.3 2.7 0.57 0.70
Southern_CA 2.6 1.2 2.6 0.58 0.68
Coastal 3.0 1.7 3.0 0.56 0.66
WD (
)
CA 285.0 12.7 99.9 0.27 0.77
Southern CA 15.0 22.5 121.0 0.23 0.67
Coastal 285.0 3.1 75.3 0.27 0.82
4.1 Trace gases
As mentioned previously, it is likely that the CARB emission
inventory developed for the 2008 ARCTAS eld campaign
may not be representative for the CalNex and CARES eld
campaign period in 2010. To demonstrate the sensitivity of
the model results to trace gas emission rates, the observed
and simulated diurnally averaged mixing ratios of CO, NO,
NO
2
, NH
3
, SO
2
, ve volatile organic compounds (VOCs),
and ozone at the four supersites are shown in Figs. 3, 4 and
5. Since CO reacts slowly, its spatial and temporal variations
can be used to evaluate how well transport and mixing pro-
cesses are represented by models. Nitrate evolution is con-
trolled by temperature and concentrations of NO, NO
2
, and
NH
3
, while sulfate is produced by oxidation of SO
2
. VOCs
will inuence oxidant chemistry and play a role in SOA for-
mation. Finally, ozone is a useful quantity to examine since it
is the byproduct of photochemistry that also impacts aerosol
chemistry and high concentrations can adversely affect hu-
man health. Ozone has also been shown to be correlated with
SOA (Herndon et al., 2008; Wood et al., 2010) and the SOA
treatment used by the model depends on simulated hydroxyl
radical (OH) concentrations (Shrivastava et al., 2011).
As seen in Fig. 3a, simulated CO from the 50 %_ANT
simulation performs better than DEF_ANT at all the super-
sites. The diurnal and multi-day variations from 50 %_ANT
at the urban supersites agree reasonably well with obser-
vations as shown in Fig. S5 in the Supplement. Errors in
the simulated boundary layer depth cannot account for the
large CO mixing ratios simulated by DEF_ANT. At the ru-
ral T1 site, the simulated CO from 50 %_ANT is still too
high. The 0 %_ANT simulation shows that there are periods
when the background mixing ratios from long-range trans-
port lead to higher than observed CO mixing ratios (1216
and 2024 June in Fig. S5d in the Supplement), suggesting
that the global MOZART simulation contributes to these er-
rors over California. In general, the CO from the boundaries
may be 2030 ppb too high on many days. Therefore, errors
in simulated CO are due to both uncertainties in the emis-
sions rates and boundary conditions, with the errors associ-
ated from boundary conditions relatively more important at
rural locations, such as T1, where emission rates are much
smaller than in the urban areas.
Uncertainties in the boundary conditions do not likely
contribute to the over-predictions of NO and NO
2
in
the DEF_ANT simulation, since the mixing ratios from
Table 5. Performance of simulated temperature (T), relative humidity (RH), wind speed (WS), and wind direction (WD) in terms of bias,
root-mean-square error (RMSE), correlation coefcient (R), and index of agreement (IA) for all of the aircraft ight paths and ship track.
Platform Number of Observed Bias RMSE R IA
Data Points Mean
T (K)
G-1 24 213 294.7 2.3 3.53 0.89 0.90
WP-3D 442 273 287.4 2.9 5.11 0.90 0.92
CIRPAS Twin Otter 3415 289.3 3.0 4.21 0.86 0.86
R/V Atlantis 35 489 287.7 1.1 2.68 0.69 0.79
RH ( %)
G-1 24 041 39.3 0.1 12.90 0.65 0.80
WP-3D 442 273 37.5 4.0 17.55 0.70 0.82
CIRPAS Twin Otter 3413 49.2 5.8 19.88 0.60 0.76
R/V Atlantis 35 489 84.8 6.6 15.30 0.49 0.66
WS (ms
1
)
G-1 23 988 5.4 0.2 3.80 0.45 0.65
WP-3D 440 073 6.2 0.1 3.98 0.71 0.83
R/V Atlantis 35 488 4.9 2.0 4.38 0.33 0.58
WD (
) G-1 23 988 195.0 9.6 57.60 0.36 0.84

WP-3D 440 073 315.0 3.7 68.24 0.27 0.79
R/V Atlantis 35 488 255.0 12.4 72.40 0.23 0.60
0 %_ANT are very low compared to the observations as
shown in Figs. 3b, 3c, S6, and S7 in the Supplement. As
with CO, NO and NO
2
are in better agreement with obser-
vations from the 50 %_ANT simulation; however, the simu-
lated mixing ratios are still too high in Pasadena. As shown
in Figs. 3d and S8 in the Supplement, the observed and sim-
ulated diurnal variation in ammonia (NH
3
) at Bakerseld are
very similar, although simulated mixing ratios are somewhat
lower than observed. At the Pasadena site, simulated NH
3
is too high, with peak mixing ratios occurring just before
sunrise when the observations have a minimum value. The
simulated diurnal variation in NH
3
at Pasadena and Bakers-
eld are very similar, but the observations at Pasadena ex-
hibit much less diurnal variability. While the observed diur-
nal variation in HNO
3
is reproduced by the model and the
mixing ratios from the 50 %_ANT simulation are similar to
observed at Bakerseld (Figs. 3e and S9 in the Supplement),
HNO
3
from all the simulations is too low at the Pasadena
site.
Model results also indicate that the amount of SO
2
trans-
ported from Asia is also very small, as shown by comparison
of the observations with the 0 %_ANT simulation in Figs. 3f
and S10 in the Supplement. The diurnal and multi-day vari-
ation of SO
2
is simulated reasonably well at the T0 site, al-
though the magnitude is higher than observed at night. The
episodic nature of the SO
2
mixing ratios associated with the
interacting synoptic and thermally driven ows (Fast et al.,
2012) and their impact on sulfate (SO
2
4
) in the vicinity of
Sacramento will be discussed in Sect. 4.4. In Bakerseld, the
overall magnitude of SO
2
simulated is similar to observed,
but the diurnal variation is not represented well by the model.
While the model often has the highest concentration at night
after midnight that decreases rapidly with daytime vertical
mixing in the boundary layer, the observations indicate an
increase in SO
2
mixing ratios around sunrise that do not de-
crease dramatically during the day. In contrast, the observed
and simulated average diurnal variation in SO
2
at Pasadena
is similar, but the simulated mixing ratios are far too high
suggesting that emissions in this region are likely too high.
VOCs, including isoprene, terpene, and methyl-vinyl-
ketone +methacrolein (MVK+MACR), toluene and
formaldehyde were measured by proton transfer reaction
mass spectrometer (PTR-MS) instruments (Lindinger et al.,
1998) deployed at Pasadena, T0, and T1 and a gas chro-
matography instrument (Gentner et al., 2012) at Bakerseld.
Isoprene, terpene, and MVK+MACR originate primarily
from biogenic emissions, while toluene and formaldehyde
are associated with anthropogenic emissions. We note
that Liu et al. (2013) recently found that isoprene-derived
peroxyl radicals were measured by the PTR-MS at the same
mass-to-charge (m/z) ratio as MVK and MACR; therefore,
the measurements are likely to be higher than reality.
The model reproduces the observed diurnal and multi-day
variations in isoprene (Figs. 4a and S11 in the Supplement) as
well as the trend in peak mixing ratios, with the highest mix-
ing ratios at the T1 site, followed by T0, Pasadena, and Bak-
erseld. However, daytime mixing ratios from DEF_ANT
and 50 %_ANT are usually a factor of 2 too low. Simulated
terpene at the T0 site is also a factor of 2 too low as shown
in Figs. 4b and S12 in the Supplement, but the mixing ratios
are closer to observed at night. Conversely, simulated terpene
mixing ratios are similar to observations during the day but a
factor of 3 too high at night at the T1 site. Figures 4c and S13
in the Supplement show that simulated MVK+MACR is too
low at Pasadena, T0, and the T1 sites throughout the day.
These results suggest that there are likely uncertainties in
Table 6. Performance in simulated wind speed (ms
1
) in terms of bias, root-mean-square error (RMSE), correlation coefcient (R), and
index of agreement (IA) for the radar wind prolers shown in Fig. 1c. Statistics given for range gates (measurements at discrete altitudes)
close to 250, 1000, and 2000 ma.g.l.. Statistics at TRK are not given because relatively little data were available May and June of
2010.
Station Height Number of Observed Bias RMSE R IA
(ma.g.l.) Observations mean
BBY 245 1359 9.4 0.5 3.3 0.79 0.88
BKF 239 1265 2.2 2.3 3.6 0.08 0.34
CCL 253 1294 7.1 1.7 3.5 0.69 0.80
CCO 239 1347 7.3 0.3 4.0 0.54 0.74
GMN 253 622 5.5 6.3 6.0 0.34 0.51
IRV 290 1160 1.4 2.2 2.8 0.36 0.44
LHS 239 1206 5.6 0.1 3.0 0.60 0.77
LVR 271 1379 4.4 2.1 3.4 0.56 0.66
ONT 266 395 2.1 2.1 1.7 0.34 0.52
SAC 220 1370 7.0 0.6 3.0 0.64 0.79
USC 271 1193 3.1 1.2 2.5 0.58 0.71
VIS 271 1381 5.8 1.2 3.4 0.73 0.83
WAP 245 1024 2.7 1.6 2.7 0.52 0.64
BBY 994 630 7.0 0.8 2.3 0.67 0.81
BKF 992 1278 5.0 0.3 2.9 0.43 0.67
CCL 1006 1067 6.5 0.5 2.8 0.56 0.75
CCO 992 753 7.3 2.4 3.3 0.34 0.57
GMN 1006 660 8.1 1.1 4.0 0.29 0.57
IRV 977 1074 3.0 1.2 2.8 0.14 0.44
LHS 992 1160 6.7 0.5 3.1 0.51 0.71
LVR 1021 1237 6.6 0.3 2.8 0.59 0.77
ONT 1010 402 2.8 0.6 1.4 0.16 0.46
SAC 1021 1059 5.7 0.2 2.4 0.61 0.78
USC 1021 702 3.6 1.6 2.8 0.33 0.51
VIS 1021 1014 4.8 0.4 2.2 0.58 0.76
WAP 989 908 5.4 1.0 2.9 0.59 0.75
BBY 1983 352 7.9 0.5 1.5 0.78 0.88
BKF 1954 1302 7.4 1.0 3.2 0.51 0.70
CCL 1969 946 6.3 1.6 3.1 0.35 0.59
CCO 1954 702 7.9 2.5 3.5 0.51 0.66
GMN 1969 475 9.1 2.4 2.8 0.47 0.66
IRV 2014 629 6.9 1.0 2.2 0.65 0.80
LHS 1954 1130 7.2 1.2 2.9 0.56 0.73
LVR 1986 841 7.6 0.4 2.3 0.67 0.81
ONT 2014 370 6.0 0.8 1.7 0.55 0.74
SAC 1957 957 7.0 0.8 2.5 0.61 0.77
USC 2014 367 6.5 0.3 1.6 0.50 0.72
VIS 2003 962 5.2 1.0 2.3 0.43 0.65
WAP 2027 821 8.2 1.4 2.8 0.57 0.74
biogenic emission rates obtained from MEGAN. As shown
in Guenther et al. (2006) a 1 degree error in simulated tem-
perature could lead to a 15 % error in isoprene emission
rate, but the relatively small errors in simulated tempera-
ture do not fully explain the under-prediction in isoprene.
While MEGAN computes 138 biogenic species, SAPRC-
99 (as with any photochemical model) has a limited num-
ber of VOC species and consequently many of the biogenic
species computed by MEGAN are lumped together. Knote et
al. (2014) suggest that there is a decient description of vege-
tation in urban areas in the MEGAN land use database, lead-
ing to too low biogenic emissions over Los Angeles. In their
work with WRF-Chem, they increased emissions of all bio-
genic VOCs as determined in MEGANby a factor of 2.5 over
grid points with an urban land use type in WRF-Chem.
Thus, uncertainties in the biogenic trace gases can arise from
Pasadena
0 6 12 18 0
0
300
600
900
C
O

(
p
p
b
V
)
(a)
0 6 12 18 0
0
300
600
900
C
O

(
p
p
b
V
)
0 6 12 18 0
50
150
250
350
Bakersfield
0 6 12 18 0
50
150
250
350
0 6 12 18 0
50
150
250
350
Sacramento (T0)
0 6 12 18 0
50
150
250
350
0 6 12 18 0
50
150
250
350
Cool (T1)
0 6 12 18 0
50
150
250
350
0 6 12 18 0
0
20
40
N
O

(
p
p
b
V
)
(b)
0 6 12 18 0
0
20
40
N
O

(
p
p
b
V
)
0 6 12 18 0
0
10
20
0 6 12 18 0
0
10
20
0 6 12 18 0
0
5
10
0 6 12 18 0
0
5
10
0 6 12 18 0
0
1
2
0 6 12 18 0
0
1
2
0 6 12 18 0
0
30
60
N
O
2

(
p
p
b
V
)
(c)
0 6 12 18 0
0
30
60
N
O
2

(
p
p
b
V
)
0 6 12 18 0
0
20
40
0 6 12 18 0
0
20
40
0 6 12 18 0
0
10
20
0 6 12 18 0
0
10
20
0 6 12 18 0
0
10
20
0 6 12 18 0
0
10
20
0 6 12 18 0
0
10
20
N
H
3

(
p
p
b
V
)
(d)
0 6 12 18 0
0
10
20
N
H
3

(
p
p
b
V
)
0 6 12 18 0
0
15
30
0 6 12 18 0
0
15
30
0 6 12 18 0
0
4
8
0 6 12 18 0
0
4
8
0 6 12 18 0
0
2
4
0 6 12 18 0
0
2
4
0 6 12 18 0
time (LST)
0
2
4
S
O
2

(
p
p
b
v
)
(f)
0 6 12 18 0
time (LST)
0
2
4
S
O
2

(
p
p
b
v
)
0 6 12 18 0
time (LST)
0
1
2
0 6 12 18 0
time (LST)
0
1
2
0 6 12 18 0
time (LST)
0
1
2
0 6 12 18 0
time (LST)
0
1
2
0 6 12 18 0
time (LST)
0.0
0.2
0.4
0 6 12 18 0
time (LST)
0.0
0.2
0.4
0 6 12 18 0 time (LST)
0
3
6
H
N
O
3

(
p
p
b
V
)
(e)
0 6 12 18 0 time (LST)
0
3
6
H
N
O
3

(
p
p
b
V
)
0 6 12 18 0 time (LST)
0
2
4
0 6 12 18 0 time (LST)
0
2
4
0 6 12 18 0 time (LST)
0
2
4
0 6 12 18 0 time (LST)
0
2
4
0 6 12 18 0 time (LST)
0
2
4
0 6 12 18 0 time (LST)
0
2
4
observed DEF_ANT 50%_ANT 0%_ANT
Figure 3. Observed and simulated diurnally averaged (a) carbon monoxide (CO), (b) nitrogen oxide (NO), (c) nitrogen dioxide (NO
2
),
(d) ammonia (NH
3
), (e) nitric acid (HNO
3
), and (f) sulfur dioxide (SO
2
) over the 2-month period at the Pasadena, Bakerseld, T0, and
T1 supersites. Gray shading denotes night. Missing observations indicate measurements were not collected at a particular site. 50 %_LBC
simulation results not shown since they are nearly identical to those from the 50 %_ANT simulation.
the species-lumping in SAPRC-99 and from how well vege-
tation is represented in the model, particularly in the vicinity
of the sampling sites. For example, Fig. 2 shows that simu-
lated biogenic emissions vary by a factor of 2 within 8 km of
the T1 site. The 0 %_ANT simulation also demonstrates that
isoprene and terpene mixing ratios are sensitive to anthro-
pogenic emissions rates while MVK+MACR are not very
sensitive; therefore, uncertainties in some biogenic species
are also affected by uncertainties in anthropogenic emissions.
Toluene is emitted by anthropogenic sources, and as with
the other primary anthropogenic emissions the 50 %_ANT
simulation is closer to observed at all four sites as shown
in Figs. 4d and S14 in the Supplement, except during the
night at Bakerseld. As shown in Figs. 4e and S15 in the
Supplement, afternoon formaldehyde mixing ratios from the
DEF_ANT simulation are closer to observations at the four
supersites, while the 50 %_ANT simulation better represents
the mixing ratios at night and several hours after sunrise.
As seen in Figs. 5a and S16 in the Supplement, the model
captures the diurnal and multi-day variability of ozone. Day-
time peak values are well simulated at the T0 and T1 sites,
but are too low at the Bakerseld and Pasadena sites. Re-
ducing ozone precursor emissions in the 50 %_ANT simu-
lation, increased peak ozone mixing ratios at Pasadena, but
reduced daytime ozone concentration at Bakerseld. Statis-
tics describing the performance of the model in simulating
ozone at all the surface monitoring sites are given in Ta-
bles S15S17 in the Supplement. Ozone from the DEF_ANT
simulation is too low overall by 3.9 ppbv in contrast with the
results at the Bakerseld and Pasadena sites that are 13 to
15 ppbv too low on average. The overall bias over California
from the 50 %_ANT simulation is nearly identical to the bias
from the DEF_ANT simulation; however, the bias in ozone is
improved for the southern California and Sacramento Valley
regions. A similar difference between the two simulations is
also produced for the sum of NO and NO
2
.
Table 7. Performance in simulated wind direction (degrees) in terms of bias, root-mean-square error (RMSE), correlation coefcient (R),
and index of agreement (IA) for the radar wind prolers shown in Fig. 1c. Statistics given for range gates close to 250, 1000, and
2000 ma.g.l. Statistics at TRK are not given because relatively little data were available May and June of 2010.
Station Height Number of Observed Bias RMSE R IA
(ma.g.l.) observations mean
BBY 245 1359 315.0 3.7 44.4 0.37 0.84
BKF 239 1265 285.0 16.3 66.0 0.33 0.81
CCL 253 1294 315.0 1.2 39.6 0.43 0.78
CCO 239 1347 135.0 2.1 67.0 0.52 0.87
GMN 253 622 345.0 14.6 71.3 0.07 0.93
IRV 290 1160 165.0 11.5 70.1 0.33 0.73
LHS 239 1206 345.0 2.6 66.3 0.05 0.88
LVR 271 1379 255.0 17.2 55.3 0.32 0.69
ONT 266 395 255.0 7.9 71.2 0.25 0.61
SAC 220 1370 255.0 14.4 36.5 0.45 0.84
USC 271 1193 255.0 21.5 67.5 0.43 0.81
VIS 271 1381 345.0 0.1 53.2 0.29 0.79
WAP 245 1024 165.0 5.5 65.8 0.43 0.82
BBY 994 630 345.0 4.1 40.6 0.32 0.93
BKF 992 1278 345.0 1.5 58.5 0.26 0.86
CCL 1006 1067 315.0 7.2 50.2 0.41 0.85
CCO 992 753 165.0 1.4 75.6 0.30 0.83
GMN 1006 660 315.0 0.9 58.8 0.40 0.91
IRV 977 1074 165.0 16.6 89.0 0.31 0.76
LHS 992 1160 345.0 0.7 45.6 0.20 0.96
LVR 1021 1237 285.0 7.2 43.0 0.32 0.94
ONT 1010 402 225.0 9.5 81.2 0.46 0.81
SAC 1021 1059 345.0 5.6 56.2 0.31 0.89
USC 1021 702 345.0 6.1 71.8 0.14 0.89
VIS 1021 1014 345.0 3.2 52.8 0.28 0.86
WAP 989 908 345.0 4.6 60.3 0.38 0.90
BBY 1983 352 15.0 6.0 34.8 0.48 0.98
BKF 1954 1302 315.0 0.8 44.3 0.49 0.91
CCL 1969 946 165.0 16.1 65.6 0.34 0.82
CCO 1954 702 165.0 2.9 63.3 0.16 0.85
GMN 1969 475 285.0 2.5 60.9 0.38 0.87
IRV 2014 629 285.0 8.3 50.3 0.44 0.91
LHS 1954 1130 345.0 3.0 43.9 0.39 0.93
LVR 1986 841 255.0 3.4 40.0 0.56 0.96
ONT 2014 370 285.0 8.9 52.2 0.44 0.92
SAC 1957 957 195.0 4.6 43.2 0.60 0.95
USC 2014 367 315.0 0.8 40.7 0.62 0.95
VIS 2003 962 345.0 7.0 47.9 0.30 0.91
WAP 2027 821 315.0 3.1 43.9 0.50 0.92
Observed and simulated O
x
, the sum of O
3
and NO
2
, is
shown in Fig. 5b because it is often used as an indicator of
photochemistry that removes the effect of titration by NO. O
x
from the 50 %_ANT simulation is in much better agreement
with observations at the Pasadena site during much of the
day, but is still too low during the afternoon. While O
x
from
the DEF_ANT simulation is in better agreement with the ob-
servations at Bakerseld and Sacramento, we have shown
that NO, NO
2
, and some of the VOCs in that simulation are
too high. Observed and simulated OH is shown in Fig. 5c for
the Pasadena site. OH is a useful indicator of daytime pho-
tochemistry; however, OH measurements have large uncer-
tainties and the observed nighttime mixing ratios in Fig. 5c
were removed since there are much fewer measurements con-
tributing to the diurnal average. Decreasing anthropogenic
emissions in the 50 % ANT simulation results in higher OH
mixing ratios than in DEF_ANT and somewhat higher than
Pasadena
0 6 12 18 0
0.0
0.5
1.0
i
s
o
p
r
e
n
e

(
p
p
b
V
) (a)
0 6 12 18 0
0.0
0.5
1.0
i
s
o
p
r
e
n
e

(
p
p
b
V
)
0 6 12 18 0
0.0
0.3
0.6
Bakersfield
0 6 12 18 0
0.0
0.3
0.6
0 6 12 18 0
0
1
2
Sacramento (T0)
0 6 12 18 0
0
1
2
0 6 12 18 0
0
1
2
Cool (T1)
0 6 12 18 0
0
1
2
0 6 12 18 0
0.0
0.1
0.2
t
e
r
p
e
n
e

(
p
p
b
V
)
(b)
0 6 12 18 0
0.0
0.1
0.2
t
e
r
p
e
n
e

(
p
p
b
V
)
0 6 12 18 0
0.0
0.2
0.4
0 6 12 18 0
0.0
0.2
0.4
0 6 12 18 0
0.0
0.2
0.4
0 6 12 18 0
0.0
0.2
0.4
0 6 12 18 0
0
1
2
0 6 12 18 0
0
1
2
0 6 12 18 0
0.0
0.5
1.0
M
V
K
+
M
A
C
R

(
p
p
b
V
)
(c)
0 6 12 18 0
0.0
0.5
1.0
M
V
K
+
M
A
C
R

(
p
p
b
V
)
0 6 12 18 0
0.0
0.2
0.4
0 6 12 18 0
0.0
0.2
0.4
0 6 12 18 0
0
1
2
0 6 12 18 0
0
1
2
0 6 12 18 0
0
1
2
0 6 12 18 0
0
1
2
0 6 12 18 0
0
1
2
3
t
o
l
u
e
n
e

(
p
p
b
V
)
(d)
0 6 12 18 0
0
1
2
3
t
o
l
u
e
n
e

(
p
p
b
V
)
0 6 12 18 0
0.0
0.3
0.6
0.9
0 6 12 18 0
0.0
0.3
0.6
0.9
0 6 12 18 0
0.0
0.3
0.6
0.9
0 6 12 18 0
0.0
0.3
0.6
0.9
0 6 12 18 0 time (LST)
0.0
0.3
0.6
0.9
0 6 12 18 0
0.0
0.3
0.6
0.9
0 6 12 18 0
time (LST)
0
2
4
C
H
2
O

(
p
p
b
V
)
(e)
0 6 12 18 0
time (LST)
0
2
4
C
H
2
O

(
p
p
b
V
)
0 6 12 18 0
time (LST)
0
2
4
0 6 12 18 0
time (LST)
0
2
4
0 6 12 18 0
time (LST)
0
2
4
0 6 12 18 0
time (LST)
0
2
4
0 6 12 18 0
time (LST)
0
2
4
0 6 12 18 0
time (LST)
0
2
4
Figure 4. Observed and simulated diurnally averaged (a) isoprene, (b) terpene, (c) methyl-vinyl-ketone +methacrolein (MVK+MACR),
(d) toluene, and (e) formaldehyde (CH
2
O) over the 2-month period at the Pasadena, Bakerseld, T0, and T1 supersites. Gray shading denotes
night. Missing observations indicate measurements were not collected at a particular site. 50 %_LBC simulation results not shown since they
are nearly identical to those from the 50 %_ANT simulation.
observed on average. The impact of OH mixing ratios on
simulated SOA formation will be discussed in Sect. 4.3.
Figure 6 shows the comparison of observed and simu-
lated CO, NO, NO
2
, NH
3
, HNO
3
, SO
2
, and O
3
distribu-
tions in terms of percentiles for all the G-1 ights (as high
as 3.2 kmm.s.l.), all the WP-3D ights north of 35
N
(as high as 6.8 kmm.s.l.), all the WP-3D ights south of
35
N (as high as 5.6 kmm.s.l.), and the entire RV-Atlantis

transect in the marine boundary layer. The statistics for the
WP-3D aircraft are divided in this way so that the northern
transects are more comparable to the G-1 in the vicinity of
the Sacramento while the southern transects are expected to
have higher mixing ratios associated with the large emissions
in the Los Angeles Basin. As with CO, NO, and NO
2
at the
supersites, the results from the 50 %_ANT simulation are in
better agreement with the observations than the DEF_ANT
simulation. However, the 50 %_ANT simulation still has sig-
nicantly higher than observed mixing ratios along the RV-
Atlantis transects in the marine boundary layer. These over-
predictions are likely related to the simulated marine bound-
ary layer depth near the coast of southern California that
was often too shallow (as low as 30 m one vertical model
level). In contrast, radiosondes launched from San Nicolas
Island indicated that the average depth of the marine bound-
ary layer was 250 m(Angevine et al., 2012). Off-shore pro-
les made by the WP-3D ight on 16 May indicated a well
mixed layer that was 550 m deep (Angevine et al., 2012);
however, the simulated boundary layer depth in that region
varied from 300 to 500 m. The largest over-predictions of
CO, NO, and NO
2
over the ocean occurred when the ship
is in the vicinity of Los Angeles (not shown), suggesting
that emissions may also be too high along the coast or that
the simulated local circulations transport too much material
from the land to the ocean. As with the rural T1 site, back-
ground mixing ratios from the global MOZART model may
affect CO mixing ratios over the ocean but uncertainties in
the boundary conditions are not likely to affect simulated
NO and NO
2
. The median simulated NH
3
mixing ratios of
1 ppb over northern California are about 2.5 ppb lower than
observed (Fig. 6b), which is similar to the average differ-
ence between average observed and simulated mixing ratios
at the Bakerseld site (Fig. 3d) during most of the day. In
contrast with the over-prediction in NH
3
at the Pasadena site
(Fig. 3d), the simulated NH
3
aloft over southern California
is close to observed (Fig. 6c). HNO
3
mixing ratios from the
DEF_ANT and 50 %_ANT simulations are somewhat higher
and lower, respectively, than observed over both northern and
southern California. In addition, the simulated HNO
3
mixing
Pasadena (a)
0 6 12 18 0

0
40
80
O
3

(
p
p
b
V
)
0 6 12 18 0

0
40
80
O
3

(
p
p
b
V
)
0 6 12 18 0

0
40
80
Bakersfield
0 6 12 18 0

0
40
80
0 6 12 18 0

0
40
80
Sacramento (T0)
0 6 12 18 0

0
40
80
0 6 12 18 0

0
40
80
Cool (T1)
0 6 12 18 0

0
40
80
(b)
0 6 12 18 0

0
40
80
O
x

(
p
p
b
V
)
0 6 12 18 0

0
40
80
O
x

(
p
p
b
V
)
0 6 12 18 0

0
40
80
0 6 12 18 0

0
40
80
0 6 12 18 0

0
40
80
0 6 12 18 0

0
40
80
0 6 12 18 0

0
40
80
0 6 12 18 0

0
40
80
(c)
0 6 12 18 0
time (LST)
0.0
0.1
0.2
0.3
O
H

(
p
p
t
V
)
0 6 12 18 0
time (LST)
0.0
0.1
0.2
0.3
O
H

(
p
p
t
V
)
0 6 12 18 0
time (LST)
0.0
0.3
0.6
0 6 12 18 0
time (LST)
0.0
0.3
0.6
0 6 12 18 0
time (LST)
0.0
0.3
0.6
0 6 12 18 0
time (LST)
0.0
0.3
0.6
0 6 12 18 0
time (LST)
0.0
0.3
0.6
0 6 12 18 0
time (LST)
0.0
0.3
0.6
Figure 5. Observed and simulated diurnally averaged (a) ozone (O
3
), (b) O
x
(O
3
+NO
2
), and (c) OH over the 2-month period at the
(a) Pasadena, Bakerseld, T0, and T1 supersites. Gray shading denotes night. 50 %_LBC simulation results not shown since they are nearly
identical to those from the 50 %_ANT simulation. NO
2
not measured at T1, OH not yet available at Bakerseld, and OH not measured at T0
and T1.
0 1 2 3 4 5 6 80
160
240
320
p
p
b
V
(a) all G-1 flights
0 1 2 3 4 5 6 0.001
0.010
0.100
1.000
10.000
0 1 2 3 4 5 6 0.01
0.10
1.00
10.00
100.00
0 1 2 3 4 5 6 0.0
0.5
1.0
1.5
2.0
0 1 2 3 4 5 6 0
30
60
90
0 1 2 3 4 5 6 0
5
10
15
0 1 2 3 4 5 6 0
2
4
6
0 1 2 3 4 5 6 80
160
240
320
p
p
b
V
(b) all WP-3D flights north of 35
o
N
0 1 2 3 4 5 6 0.001
0.010
0.100
1.000
10.000
0 1 2 3 4 5 6 0.01
0.10
1.00
10.00
100.00
0 1 2 3 4 5 6 0.0
0.5
1.0
1.5
2.0
0 1 2 3 4 5 6 0
30
60
90
0 1 2 3 4 5 6 0
5
10
15
0 1 2 3 4 5 6 0
2
4
6
0 1 2 3 4 5 6 80
160
240
320
p
p
b
V
(c) all WP-3D flights south of 35
o
N
0 1 2 3 4 5 6 0.001
0.010
0.100
1.000
10.000
0 1 2 3 4 5 6 0.01
0.10
1.00
10.00
100.00
0 1 2 3 4 5 6 0.0
0.5
1.0
1.5
2.0
0 1 2 3 4 5 6 0
30
60
90
0 1 2 3 4 5 6 0
5
10
15
0 1 2 3 4 5 6 0
2
4
6
0 1 2 3 4 5 6 80
160
240
320
p
p
b
V
(d) entire RV-Atlantis sampling period
CO
0 1 2 3 4 5 6 0.01
0.10
1.00
10.00
100.00
NO
0 1 2 3 4 5 6 0.01
0.10
1.00
10.00
100.00
NO
2
0 1 2 3 4 5 6 0
2
4
6
8
SO
2
0 1 2 3 4 5 6 0
30
60
90
O
3
0 1 2 3 4 5 6 0
5
10
15
NH
3
0 1 2 3 4 5 6 0
2
4
6
HNO
3
observed DEF_ANT 50%_ANT 0%_ANT 50%_LBC
Figure 6. Percentiles for carbon dioxide (CO), nitrogen oxide (NO), nitrogen dioxide (NO
2
), ammonia (NH
3
), nitric acid (HNO
3
), sulfur
dioxide (SO
2
), and ozone (O
3
) for all (a) G-1 ights, (b) WP-3D ights north of 35
N, (c) WP-3D ight ights south of 35
N, and (d) the

entire RV-Atlantis sampling period. Vertical lines denote 5th and 95th percentiles, boxes denote 25th and 75th percentiles, and the white
dots denote the 50th percentiles. Note that NH
3
was not measured on the G-1 or the RV-Atlantis, but the model results are included for
completeness.
0 1 2 3 4 5 6 0
1
2
3
p
p
b
V
(a) all G-1 flights
0 1 2 3 4 5 6 0.0
0.1
0.2
0.3
0.4
0 1 2 3 4 5 6 0
1
2
3
0 1 2 3 4 5 6 0.0
0.2
0.4
0.6
0 1 2 3 4 5 6 0
2
4
6
0 1 2 3 4 5 6 0.0
0.1
0.2
0.3
0.4
p
p
b
V
(b) all WP-3D flights north of 35
o
N
0 1 2 3 4 5 6 0.00
0.03
0.06
0.09
0 1 2 3 4 5 6 0.0
0.1
0.2
0.3
0 1 2 3 4 5 6 0.0
0.2
0.4
0.6
0 1 2 3 4 5 6 0
2
4
6
0 1 2 3 4 5 6 0.0
0.1
0.2
0.3
0.4
p
p
b
V
(c) all WP-3D flights south of 35
o
N
isoprene
0 1 2 3 4 5 6 0.00
0.03
0.06
0.09
terpene
0 1 2 3 4 5 6 0.0
0.1
0.2
0.3
MVK+MACR
0 1 2 3 4 5 6 0.0
0.2
0.4
0.6
toluene
0 1 2 3 4 5 6 0
2
4
6
formaldehyde
Figure 7. Percentiles as a function of height for isoprene, monoterpenes, methyl-vinyl-ketone +methacrolein (MVK+MACR), toluene, and
formaldehyde for all (a) G-1 ights (b) WP-3D ights north of 35
N, and (c) WP-3D ight ights south of 35
N. Vertical lines denote 5th

and 95th percentiles, boxes denote 25th and 75th percentiles, and the white dots denote the 50th percentiles. Note that formaldehyde was not
measured on the G-1, but the model results are included for completeness.
ratios are usually closer to observed than at the Pasadena site
(Fig. 3e). Simulated SO
2
is generally too low aloft along all
the G-1 and WP-3D ights, even though the overall simu-
lated magnitude was similar to that observed at the T0 and
Bakerseld sites. Observed median SO
2
values are between
0.4 and 0.7 ppb, while the simulated values are between 0.05
and 0.2 ppb. In contrast, the model signicantly over pre-
dicts SO
2
in the marine boundary layer along the RV-Atlantis
transects. The simulated 75th percentiles are 5 ppb, but the
observed values are 0.5 ppb. The factors that contribute to
the over-prediction in marine boundary layer SO
2
are likely
the same as those for NO and NO
2
. As with the supersites,
the DEF_ANT simulation produces ozone aloft in the vicin-
ity of Sacramento that is similar to observed, but is too low
everywhere else. The 50 %_ANT simulation decreases ozone
aloft, but improves the simulation over the ocean somewhat.
The high simulated NO mixing ratios lead to too much ozone
titration in the marine boundary layer.
PTR-MS instruments were also deployed on the G-1
(Shilling et al., 2013) and WP-3D (Warneke et al., 2011) air-
craft; therefore, we also compare the observed and simulated
isoprene, terpene, MVK+MACR, toluene, and formalde-
hyde distributions in Fig. 7. Observed biogenic trace gas
mixing ratios from the G-1 are about an order of magnitude
higher than those from the WP-3D north of 35
N because a
large fraction of the G-1 samples occurred over the forested
foothills of the Sierra Nevada (Fig. 1a and b). As with the su-
persites, simulated mixing ratios of biogenic species aloft are
too low, although the simulated isoprene along the WP-3D
transects in northern California are only somewhat lower
than observed. While toluene along the G-1 ights from
the DEF_ANT simulation are similar to observed, simulated
toluene is somewhat higher than observed along the WP-3D
ights over both southern and northern California. Simulated
toluene from the 50 %_ANT simulation is in better agree-
ment with the WP-3D data, but lower than observed for the
G-1 data. As with ozone, formaldehyde from the 50 %_ANT
simulation is too low and somewhat lower than from the
DEF_ANT simulation.
Additional statistics for the same trace gases as in Figs. 6
and 7 are given in Tables 8 and 9 for the G-1 and WP-3D
ights, respectively. The biases are similar to the per-
centile shown previously. As expected, the statistics from the
0 %_ANT simulation are usually poor because it neglects an-
thropogenic emissions. For the simulations that include an-
thropogenic emissions, the temporal and spatial variations in
ozone, CO, and formaldehyde are similar to observed along
the ight paths as indicated by correlation coefcients be-
tween 0.6 and 0.8. Somewhat lower correlation coefcients
between 0.4 and 0.6 were produced for NO, NO
2
, isoprene,
and toluene. The lowest correlation coefcients were pro-
duced for SO
2
, MVK+MACR, and terpene. Statistics quan-
tifying the performance in select trace gases averaged over all
the surface monitoring sites in California by region (Fig. 1c)
and for the individual supersites are given in Tables S15, S16,
and S17 in the Supplement for the DEF_ANT, 50 %_ANT,
and 0 %_ANT simulations, respectively. Model performance
varies from day to day based on the simulated meteorolog-
ical conditions and how well emissions are represented for
a particular day. Therefore, additional statistics on the trace
gases from the DEF_ANT simulation for the individual G-1
ights are given in Tables S18S26 in the Supplement and
for the individual WP-3D ights in Tables S26S36 in the
Supplement.
In summary, the simulated anthropogenic trace gases from
the 50 %_ANT and 50 %_LBC simulations that reduced the
emission rates in the 2008 CARB inventory were usually
closer to the surface and aircraft measurements collected dur-
ing the CARES and CalNex campaigns. Simulated isoprene
and terpene mixing ratios were usually too low at the surface
and aloft, except that simulated terpene was too high at night
at two surface sites. A number of factors probably contribute
to the errors in simulated biogenic species, such as meteo-
rological uncertainties, specication of vegetation types and
lumping of VOC species in MEGAN, and errors in simu-
lated anthropogenic emissions that interact biogenic sources
as shown by simulation 0 %_ANT.
4.2 Carbonaceous aerosols
Single Particle Soot Photometers (SP2) were used to mea-
sure black carbon (BC) concentrations at three of the super-
sites and on three research aircraft. The SP2 measures single-
particle refractory BC mass for particles for a discrete size
range. Metcalf et al. (2012) report a detection range of 80 to
696 nm volume equivalent diameter for the SP2 on the CIR-
PAS Twin Otter. Therefore, we use the rst four size-bins in
the model (0.625 m) to compare BC simulated mass with
the SP2 measurements. Both Metcalf et al. (2012) and Lan-
gridge et al. (2012) note that the overall uncertainties on SP2
reported BC mass due to calibration and other factors could
be as much as 40 %. Laborde et al. (2012) report that uncer-
tainty in BC mass of 10 % can be achieved when the SP2 is
carefully tuned and calibrated. The detection limits and un-
certainty in mass may vary somewhat among the CalNex and
CARES SP2 instruments and as a function of time, depend-
ing on the size of the peak BC mass distribution, and are not
accounted for here.
The time series and diurnal averages of observed and sim-
ulated BC at the supersites are shown in Fig. 8. As with
CO and NO that are emitted predominately by transporta-
tion sources, BC concentrations in the 50 %_ANT simulation
are closer to observations than in the DEF_ANT simulation
where simulated values are usually too high. The model also
reproduces much of the diurnal variability of BC, except at
the T1 site. While some of the multi-day variations in BC
that are associated with the changing meteorological condi-
tions are also reproduced, there are days in which the model
performs better than others. Simulated BC from 50 %_ANT
can be twice as high as observed on some days and it did
not produce the occasional peak concentrations that were
observed to exceed 1 g m
3
at the Pasadena site. BC con-
centrations from the 0 %_ANT simulation are occasionally
higher than the observations and during the same time pe-
riods when background CO concentrations were higher than
observed. The background BC concentrations are small, usu-
ally less than 0.03 g m
3
; however, this is 43 % of the av-
erage observed concentration of 0.07 g m
3
at the rural T1
site. Reducing background BC concentrations improves sim-
ulated BC at the T1 site (not shown), but does not have as
large an impact at the Pasadena and T0 sites since the overall
concentrations are higher. These results suggest that long-
range transport of BC as simulated by MOZART may be too
large. While the uncertainties in background BC will have
negligible impact on total PM
2.5
mass, it does have a signi-
cant impact on computed aerosol radiative forcing over most
of California as will be discussed in Sect. 5.
Simulated BC aloft was also compared with SP2 measure-
ments collected along the entire G-1, WP-3D, and CIRPAS
Twin Otter aircraft ight paths in terms of percentiles over
the sampling period as shown in Fig. 9a. Similar to the sur-
face BC concentrations in Fig. 8 and to simulated CO and
NO aloft (Fig. 6), BC concentrations from the 50 %_ANT
simulation were closer to observations although they are still
somewhat higher than observed. Observed and simulated
concentrations along the G-1 ight paths and the WP-3D
ight paths north of 35
N have similar medians and range of

values. Higher concentrations were observed and simulated
by the WP-3D and CIRPAS Twin Otter aircraft in the vicinity
of the Los Angeles Basin; therefore, the model was able to
reproduce the overall characteristics of higher and lower BC
concentrations over southern and northern California. The
observed and simulated percentiles along the CIRPAS Twin
Otter ight paths are also higher than those from the WP-3D
since the Twin Otter usually ew in the immediate vicinity
of the Los Angeles Basin, while the WP-3D also often ew
over the ocean and desert farther from the Los Angeles Basin
where BC concentrations were lower. The 50 %_LBC simu-
lation produced the best results for all locations. Statistics on
BC for individual aircraft ights from the DEF_ANT simu-
lation are given in Table S37 in the Supplement.
To demonstrate how well the model represents the spa-
tial and temporal variability of BC, observed and simulated
BC for two ights on 21 May in the vicinity of Los Angeles
are shown in Fig. 10. On this day, the CIRPAS Twin Otter
ew over the urban area and through Cajon Pass northeast
of Los Angeles, and the WP-3D sampled primarily over the
ocean. While observed BC concentrations from the WP-3D
close to the ocean surface in the marine boundary layer were
usually around 0.02 g m
3
, somewhat higher concentrations
Table 8. Performance of simulated carbon monoxide (CO), nitrogen oxide (NO), nitrogen dioxide (NO
2
), sulfur dioxide (SO
2
), ozone (O
3
),
isoprene, methyl-vinyl-ketone +methacrolein (MVK+MACR), toluene, terpene, and formaldehyde over all the G-1 ights in terms of bias,
root-mean-square error (RMSE), correlation coefcient (R), and index of agreement (IA).
Trace Simulation Number of Observed Bias RMSE R IA
gas data points mean (ppbg) (ppbv)
CO
DEF_ANT
22 675 140.2
13.9 34.0 0.60 0.71
50 %_ANT 5.0 22.7 0.62 0.76
0 %_ANT 24.5 34.7 0.45 0.49
50 %_LBC 5.1 22.8 0.62 0.76
NO
DEF_ANT
21 491 0.42
0.32 1.24 0.54 0.61
50 %_ANT 0.13 0.66 0.56 0.69
0 %_ANT 0.40 0.86 0.26 0.33
50 %_LBC 0.13 0.66 0.56 0.69
NO
2
DEF_ANT
20 361 1.05
0.63 2.11 0.57 0.64
50 %_ANT 0.30 1.17 0.58 0.72
0 %_ANT 0.99 1.67 0.28 0.39
50 %_LBC 0.31 1.16 0.59 0.72
SO
2
DEF_ANT
0.59
0.28 0.77 0.25 0.51
50 %_ANT 0.28 0.77 0.26 0.51
0 %_ANT 0.59 0.92 0.12 0.42
50 %_LBC 0.28 0.77 0.26 0.51
O
3
DEF_ANT
22 378 48.1
3.4 12.4 0.77 0.85
50 %_ANT 2.6 9.9 0.77 0.87
0 %_ANT 18.9 23.4 0.40 0.51
50 %_LBC 2.7 10.0 0.77 0.87
isoprene
DEF_ANT
21 617 0.53
0.40 0.94 0.65 0.49
50 %_ANT 0.36 0.87 0.70 0.61
0 %_ANT 0.10 0.72 0.72 0.84
50 %_LBC 0.36 0.87 0.70 0.61
MVK+MACR
DEF_ANT
21 636 0.58
0.37 0.81 0.65 0.53
50 %_ANT 0.34 0.78 0.68 0.57
0 %_ANT 0.16 0.68 0.67 0.68
50 %_LBC 0.34 0.78 0.67 0.57
toluene
DEF_ANT
20 470 0.09
0.04 0.15 0.40 0.55
50 %_ANT 0.03 0.09 0.42 0.64
0 %_ANT 0.08 0.11 0.35 0.42
50 %_LBC 0.03 0.09 0.42 0.64
terpene
DEF_ANT
21 606 0.07
0.06 0.09 0.25 0.46
50 %_ANT 0.05 0.09 0.27 0.48
0 %_ANT 0.02 0.10 0.32 0.55
50 %_LBC 0.05 0.09 0.26 0.48
between 0.02 and 0.05 g m
3
were observed 1 kmm.s.l.
above the ocean. The model suggests that the higher BC
concentrations at 1 kmm.s.l. were inuenced by local emis-
sions that were transported over the ocean. BC concentra-
tions from the DEF_ANT and 50 %_ANT simulations are
higher than observed at both altitudes. As with the rural sur-
face sites, the BC concentrations from the 0 %_ANT simula-
tion are frequently higher than observed over the ocean. Con-
sequently, simulated BC from 50 %_LBC is usually closer
to observations than the other simulations. As expected,
BC concentrations were an order of magnitude or more
higher over the urban areas. BC concentrations measured
on the CIRPAS Twin Otter were as high as 0.3 g m
3
. BC
from the DEF_ANT simulation was too high except above
2 kmm.s.l., and the 50 %_ANT and 50 %_LBC simulations
were in much better agreement with observed BC. The lo-
cation and magnitude of the simulated peak BC concen-
trations were sometimes consistent with the measurements,
Table 9. Performance of simulated ozone (O
3
), carbon monoxide (CO), nitrogen oxide (NO), nitrogen dioxide (NO
2
), ammonia (NH
3
), sul-
fur dioxide (SO
2
), isoprene, methyl-vinyl-ketone +methacrolein (MVK+MACR), toluene, terpene, and formaldehyde over all the WP-3D
ights in terms of bias, root-mean-square error (RMSE), correlation coefcient (R), and index of agreement (IA).
Trace Simulation Number of Observed Bias RMSE R IA
gas data points mean (ppbv) (ppbv)
CO
DEF_ANT
401 896 155.2
17.0 45.6 0.80 0.86
50 %_ANT 6.3 34.2 0.80 0.86
0 %_ANT 29.6 60.7 0.27 0.43
50 %_LBC 6.5 34.3 0.80 0.86
NO
DEF_ANT
370 374 0.47
0.36 2.22 0.57 0.67
50 %_ANT 0.14 1.35 0.59 0.69
0 %_ANT 0.45 1.73 0.07 0.17
50 %_LBC 0.14 1.35 0.59 0.69
NO
2
DEF_ANT
356 465 1.53
1.28 4.34 0.65 0.72
50 %_ANT 0.25 2.48 0.65 0.78
0 %_ANT 1.48 3.52 0.06 0.30
50 %_LBC 0.25 2.47 0.66 0.78
NH
3
DEF_ANT
301 891 5.80
3.68 15.23 0.47 0.28
50 %_ANT 3.45 15.10 0.46 0.29
0 %_ANT 5.82 16.82 0.04 0.21
50 %_LBC 3.38 15.09 0.46 0.29
SO
2
DEF_ANT
385 293 0.46
0.14 0.91 0.30 0.51
50 %_ANT 0.28 0.77 0.26 0.51
0 %_ANT 0.45 0.91 0.06 0.34
50 %_LBC 0.15 0.89 0.32 0.52
O
3
DEF_ANT
387 766 59.0
5.6 13.2 0.64 0.77
50 %_ANT 8.8 14.0 0.67 0.73
0 %_ANT 19.6 24.4 0.40 0.51
50 %_LBC 8.9 14.0 0.67 0.73
isoprene
DEF_ANT
20 380 0.05
0.01 0.09 0.62 0.78
50 %_ANT 0.01 0.09 0.57 0.74
0 %_ANT 0.12 0.27 0.43 0.43
50 %_LBC 0.01 0.09 0.57 0.74
MVK+MACR
DEF_ANT
1227 0.11
0.05 0.14 0.23 0.44
50 %_ANT 0.04 0.13 0.24 0.44
0 %_ANT 0.05 0.14 0.26 0.49
50 %_LBC 0.04 0.13 0.24 0.45
toluene
DEF_ANT
22 350 0.07
0.10 0.25 0.76 0.66
50 %_ANT 0.01 0.10 0.76 0.86
0 %_ANT 0.06 0.14 0.04 0.34
50 %_LBC 0.01 0.10 0.76 0.86
terpene
DEF_ANT
21 654 0.01
0.01 0.02 0.41 0.47
50 %_ANT 0.01 0.02 0.26 0.39
0 %_ANT 0.00 0.02 0.28 0.51
50 %_LBC 0.01 0.02 0.26 0.39
formaldehyde
DEF_ANT
22 833 1.92
0.69 1.04 0.77 0.76
50 %_ANT 0.88 1.19 0.77 0.69
0 %_ANT 1.36 1.71 0.62 0.50
50 %_LBC 0.88 1.19 0.77 0.69
B
C

(
u
g

m
-
3
)
15 17 19 21 23 25 27 29 31 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30
0
1
2
15 17 19 21 23 25 27 29 31 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30
0
1
2
Pasadena
diurnal average
0 6 12 18 0
0.0
0.5
1.0
1.5
15 17 19 21 23 25 27 29 31 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30
0
1
2
15 17 19 21 23 25 27 29 31 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30
0
1
2
Bakersfield
0 6 12 18 0
0.0
0.4
0.8
15 17 19 21 23 25 27 29 31 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30
0.0
0.5
1.0
15 17 19 21 23 25 27 29 31 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30
0.0
0.5
1.0
T0
0 6 12 18 0
0.0
0.2
0.4
May June
15 17 19 21 23 25 27 29 31 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30
0.0
0.2
0.4
15 17 19 21 23 25 27 29 31 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30
date (LST)
0.0
0.2
0.4
T1
time (LST)
0 6 12 18 0
0.0
0.2
0.4
Figure 8. Observed and simulated time series (left panels) and average diurnal variation (right panels) of BC at the four supersites. Simulated
BC is the total of the rst four model size bins (i.e., aerosol diameters up to 0.625 m). Gray shading denotes night and vertical lines in right
panels denote measurement uncertainty range. Results from 50 %_LBC simulation not shown since it is nearly the same as the 50 %_ANT
simulation. Bakerseld results shown for completeness even though no BC measurements were made at that site.
0 1 2 3 4 5 6 0.00
0.25
0.50
0.75
u
g

m
-
3
(a) BC percentiles for all aircraft flights
0 1 2 3 4 5 6 0
2
4
6
8
u
g

m
-
3
(b) OA percentiles for all aircraft flights
G-1
0 1 2 3 4 5 6 0.00
0.25
0.50
0.75
0 1 2 3 4 5 6 0
2
4
6
8
WP-3D > 35
o
N
0 1 2 3 4 5 6 0.00
0.25
0.50
0.75
0 1 2 3 4 5 6 0
2
4
6
8
WP-3D < 35
o
N
0 1 2 3 4 5 6 0.00
0.25
0.50
0.75
0 1 2 3 4 5 6 0
2
4
6
8
CIRPAS Twin Otter
Figure 9. Percentiles for (a) black carbon (BC) and (b) organic mat-
ter (OA) for all G-1, WP-3D, and CIRPAS Twin Otter ights. Ver-
tical lines denote 5th and 95th percentiles, boxes denote 25th and
75th percentiles, and the white dots denote the 50th percentiles.
but the simulated BC concentrations from 50 %_ANT and
50 %_LBC were still too high between 10:15 and 10:45 and
12:30 and 13:00 LST. This indicates that there are still uncer-
tainties in simulated thermally driven circulations, boundary
layer turbulent mixing, and/or emissions over the Los Ange-
les Basin that affect local variations in BC.
24 May is another day in which both the WP-3D and CIR-
PAS Twin Otter ew over southern California; however, the
WP-3D sampled primarily over the southern San Joaquin
Valley as shown in Fig. 11. These ights enable the model
to be evaluated over a larger geographic area. As the WP-3D
ew across the San Joaquin Valley, higher BC concentrations
were observed over the eastern side of the valley that con-
tribute to peak concentrations of 0.04 g m
3
between 16:30
and 20:30 LST. The model does not produce the strong gradi-
ent across the valley during the aircraft sampling period. The
simulated BC at 1 kma.g.l. in the right panel of Fig. 11
shows that at 14:00 LST, just prior to the WP-3D ight,
higher concentrations are simulated along the eastern side of
the valley consistent with measurements. Higher concentra-
tions of BC originating from the Bay Area are transported
into the San Joaquin Valley, reducing the simulated variabil-
ity of BC in the valley after 16:00 LST. Thus, transport er-
rors in the model contributed to the differences between the
observed and simulated variability in BC along the WP-3D
ight path. The agreement between the observed and simu-
lated BC concentrations is much better in the vicinity of Los
Angeles at all altitudes. The simulated variability in BC con-
centrations from the 50 %_ANT and 50 %_LBC simulation
are nearly identical to observations, although the simulated
concentration are somewhat higher than observed.
In contrast to the CARES and CalNex data, somewhat
different statistics are obtained when comparing the simu-
lations to the daily averaged BC measurements at the re-
mote IMPROVE site as shown in Table 10. For this data
set, correlation coefcients that were greater than 0.64 rep-
resent the models ability to replicate the multi-day varia-
tions rather than the diurnal variations. The bias in BC from
7.5 8.0 8.5 9.0 9.5 10.0 10.5
0.0
0.1
0.2
B
C

(
u
g

m
-
3
)
7.5 8.0 8.5 9.0 9.5 10.0 10.5
0.0
0.1
0.2
B
C

(
u
g

m
-
3
)
WP-3D
7.5 8.0 8.5 9.0 9.5 10.0 10.5
0
1
2
3
altitude (km MSL)
10.0 10.5 11.0 11.5 12.0 12.5 13.0 13.5 14.0
0.0
0.2
0.4
0.6
0.8
B
C

(
u
g

m
-
3
)
10.0 10.5 11.0 11.5 12.0 12.5 13.0 13.5 14.0
0.0
0.2
0.4
0.6
0.8
B
C

(
u
g

m
-
3
)
CIRPAS Twin Otter
10.0 10.5 11.0 11.5 12.0 12.5 13.0 13.5 14.0
time (LST)
0
1
2
3
altitude (km MSL)
0.000 0.167 0.333 0.500 0.667 0.833 1.000 0.00
0.25
0.50
0.75
1.00
color contours =
50%_LBC simulation ~0.5 km AGL at 12 LST
0.000 0.167 0.333 0.500 0.667 0.833 1.000 0.00
0.25
0.50
0.75
1.00
0.0 0.2 0.4 0.6 0.8 1.0
0.15
0.36
0.58
0.79
1.00
0.025
0.050
0.075
0.100
0.150
0.200
0.250
0.300

BC (ug m
-3
)
WP-3D
CIRPAS
Twin Otter
Figure 10. Observed and simulated BC on 21 May 2010 along the WP-3D and CIRPAS Twin Otter ight paths (left panels) and spatial
variations in observed BC (right panel). Gray contour lines in right panel denote model topography.
23 24 25 26 27 28 29
0.0
0.1
0.2
B
C

(
u
g

m
-
3
)
23 24 25 26 27 28 29
0.0
0.1
0.2
B
C

(
u
g

m
-
3
)
WP-3D
15.0 16.0 17.0 18.0 19.0 20.0 21.0
0
2
4
altitude (km MSL)
18.0 18.5 19.0 19.5 20.0 20.5 21.0 21.5 22.0
0.0
0.2
0.4
B
C

(
u
g

m
-
3
)
18.0 18.5 19.0 19.5 20.0 20.5 21.0 21.5 22.0
0.0
0.2
0.4
B
C

(
u
g

m
-
3
)
CIRPAS Twin Otter
10.0 10.5 11.0 11.5 12.0 12.5 13.0 13.5 14.0
time (LST)
0
2
4
altitude (km MSL)
0.000 0.167 0.333 0.500 0.667 0.833 1.000 0.00
0.25
0.50
0.75
1.00
color contours =
50%_LBC simulation ~1 km AGL at 14 LST
0.000 0.167 0.333 0.500 0.667 0.833 1.000 0.00
0.25
0.50
0.75
1.00
0.0 0.2 0.4 0.6 0.8 1.0
0.15
0.36
0.58
0.79
1.00
0.010
0.025
0.050
0.075
0.100
0.125
0.150
0.200

BC (ug m
-3
)
WP-3D
CIRPAS
Twin Otter
Figure 11. Same as Fig. 10, except for 24 May 2010.
the DEF_ANT and 50 %_ANT simulations was 0.02 and
0.02 g m
3
, respectively. When the boundary conditions
of BC are reduced in the 50 %_LBC simulation, the biases
increased to 0.04 g m
3
. Based on this data set, the bias
could be due to local anthropogenic emissions, boundary
conditions, or a combination of both. In contrast with the
evaluations using CARES and CalNex data, the 50 %_LBC
simulation performed worse. If the eld campaign obser-
vations were unavailable, it is possible to conclude that
reducing the CARB emissions by 25 % would produce BC
concentrations closer to the observations. Part of the reason
for the different BC statistics between IMPROVE and SP2
data sets are likely due to measurement technique; the IM-
PROVE method could have interference from organic car-
bon (e.g., Lack et al., 2014) that erroneously increases re-
ported BC concentrations. The differences in statistics stress
the importance of modeling studies to not rely solely on rou-
tine monitoring measurements.
As shown by Hayes et al. (2013), Hersey et al. (2013), Liu
et al. (2012), Setyan et al. (2012), and Shilling et al. (2013),
organic aerosol (OA) is the largest fraction of total non-
refractory aerosols observed during CARES and CalNex.
The time series and diurnally averaged OA obtained from
High-Resolution Time-of-Flight Aerosol Mass Spectrome-
ters (AMS) deployed at each of the supersites are shown
in Fig. 12 along with simulated OA. Since the AMS mea-
sures submicron aerosol mass (Canagaratna et al., 2007), OA
from the rst four model aerosol size bins up to 0.625 m
diameter are used to compute OA comparable to the mea-
surements. While there will be some uncertainty in the com-
parison due to the exact cut-off of the AMS measurements
(which may vary among the four instruments), simulated OA
in the fth size bin (0.6251.25 m) is usually small and
Table 10. Performance of simulated PM
2.5
at the IMPROVE monitoring sites in terms of bias, root-mean-square error (RMSE), correlation
coefcient (R), and index of agreement (IA).
Aerosol Simulation Observed Bias RMSE R IA
composition mean (g m
3
) (g m
3
)
SO
4
DEF_ANT
0.70
0.27 0.43 0.63 0.66
50 %_ANT 0.31 0.47 0.59 0.62
0 %_ANT 0.42 0.58 0.35 0.50
50 %_LBC 0.44 0.55 0.65 0.55
NO
3
DEF_ANT
0.48
0.14 0.56 0.58 0.75
50 %_ANT 0.33 0.58 0.57 0.65
0 %_ANT 0.48 0.75 0.04 0.41
50 %_LBC 0.32 0.57 0.57 0.66
BC
DEF_ANT
0.10
0.02 0.07 0.69 0.81
50 %_ANT 0.02 0.07 0.64 0.70
0 %_ANT 0.07 0.11 0.24 0.47
50 %_LBC 0.04 0.08 0.69 0.66
OC
DEF_ANT
0.68
0.41 0.73 0.74 0.74
50 %_ANT 0.05 0.38 0.74 0.85
0 %_ANT 0.51 0.71 0.52 0.48
50 %_LBC 0.09 0.38 0.74 0.85
sea salt
DEF_ANT
0.34
0.29 0.99 0.81 0.26
50 %_ANT 0.29 0.99 0.84 0.27
0 %_ANT 0.30 0.99 0.88 0.27
50 %_LBC 0.30 0.98 0.86 0.29
Cl
DEF_ANT
0.19
0.18 0.58 0.47 0.24
50 %_ANT 0.18 0.57 0.60 0.24
0 %_ANT 0.18 0.57 0.79 0.25
50 %_LBC 0.18 0.56 0.79 0.27
PM
2.5
DEF_ANT
3.90
0.27 2.23 0.50 0.71
50 %_ANT 0.83 2.20 0.46 0.62
0 %_ANT 2.00 3.03 0.08 0.45
50 %_LBC 1.68 2.58 0.51 0.59
PM
10
DEF_ANT
10.19
1.26 7.18 0.37 0.58
50 %_ANT 0.05 7.40 0.31 0.54
0 %_ANT 1.37 8.02 0.22 0.50
50 %_LBC 3.26 7.87 0.35 0.59
does not contribute signicant mass, as will be shown later
(Fig. 22a). Uncertainties in the aerosol mass from the AMS
instruments vary but typical errors have been reported to be
up to about 30 % (Bahreini et al., 2009; Canagaratna et al.,
2007; Middlebrook et al., 2012). Detection limits depend on
the averaging time period. For the AMS at the T1 site, the
2.5 min detection limits were reported to be 0.075, 0.011,
0.018, and 0.01 g m
3
for OA, SO
2
4
, nitrate (NO
3
), and
ammonium (NH
+
4
), respectively (Setyan et al., 2012). For
the AMS on the G-1 aircraft, the 13 s detection limits of 0.3,
0.07, 0.05, and 0.15 g m
3
for OA, SO
2
4
, NO
3
, and NH
+
4
,
respectively (Shilling et al., 2013), were higher because of
the much shorter sampling period needed for aircraft opera-
tions. The detection limit for OA from the AMS on the CIR-
PAS Twin Otter aircraft was reported to vary between 0.141
to 0.382 g m
3
, depending on the ight (Craven et al., 2013)
and is similar to the G-1. Observed and simulated composi-
tion concentrations are usually well above AMS detection
limits, and thus the limits do not affect the model evaluation
signicantly.
At the Pasadena site, observed peak concentrations of OA
exceeded 10 g m
3
on several days; however, simulated
OA concentration in from all the simulations were too low
and usually less than 5 g m
3
(Fig. 12). OA concentrations
from the DEF_ANT simulation are closer to observations
at the Bakerseld, T0, and T1 sites, with the model repro-
ducing much of the observed multi-day and diurnal variabil-
ity. At these sites, OA from the 50 %_ANT and 50 %_LBC
Figure 12. Observed (AMS instrument) and simulated time series (left panels) and average diurnal variation (right panels) of OA at the four
supersites. Simulated OA is the total of the rst four model size bins up to 0.625 m diameter. Gray shading denotes night and vertical lines
in right panels denote measurement uncertainty range. 50 %_LBC simulation results not shown since they are nearly identical to those from
the 50 %_ANT simulation.
simulations are lower than observed and 11.5 g m
3
lower
than those from the DEF_ANT simulation. The 0 %_ANT
simulation shows that boundary condition OA is a small frac-
tion of the total OA at the Pasadena site, so that OA is domi-
nated by local sources. While OA from the 0 %_ANT simu-
lation is still small at the other sites, it is not an insignicant
fraction of the total OA. The relatively higher OA from this
simulation is not from long-range transport, but associated
with biogenic SOA since the biogenic precursor emissions
are larger at these sites and particularly for T1. As described
in Fast et al. (2012) and Setyan et al. (2012), the meteoro-
logical conditions after 20 June are more favorable for SOA
formation, which is consistent with the increase in biogenic
SOA from the 0 %_ANT simulation during this time period.
Since OA is composed of primary and secondary mate-
rial, we use the results of positive matrix factorization (PMF)
analyses that have been applied to the AMS data from the
Pasadena (Hayes et al., 2013), Bakerseld (Liu et al., 2012),
T0, and T1 (Setyan et al., 2012) data sets to provide es-
timates of observed POA and SOA. To assess the model
sensitivity to emissions, a direct comparison of observed
and simulated POA is more appropriate than relying on OA
alone. Figure 13 compares the diurnally averaged simulated
POA and SOA with estimates derived from PMF. At the
Pasadena site (Fig. 13a), the overall magnitude of POA from
the DEF_ANT simulation is similar to the PMF estimate, ex-
cept that the model is up to 1 g m
3
too high at midnight and
up to 1 g m
3
too low during the afternoon. The DEF_ANT
simulation also produces a diurnal average that is similar to
the PMF estimate at the T0 site (Fig. 13b), except that simu-
lated POA is up to 0.5 g m
3
too low during the afternoon.
For both Pasadena and the T0 site, POA from 50 %_ANT
is lower as expected and is lower than the PMF estimate.
At the Bakerseld and T1 sites (Fig. 13c and d), however,
the 50 %_ANT simulation produces a diurnal average that
is nearly identical to the PMF estimate while the POA from
the DEF_ANT simulation is too high all day. These results
suggest that POA emission rates from the CARB emission
may be reasonable, at least in the highly populated areas.
The over-prediction in POA from the DEF_ANT simulation
at the rural T1 site could be due to the horizontal resolution.
As seen in Fig. 2, the city of Auburn is located just northwest
of T1 and the 4 km grid spacing, which is the same resolu-
tion as the 2008 CARB emission inventory, likely results in
numerical smoothing of anthropogenic plumes to the adja-
cent model grid cell over the T1 site. The spatial resolution
of the emission inventory could also be an issue at the Bak-
erseld site since it is located at the edge of the city (Alm et
al., 2012).
Figure 13a shows that the large under-prediction in OA
at Pasadena for both the DEF_ANT and 50 %_ANT simu-
lations is due primarily to simulated SOA that is too low.
The model does produce more SOA during the day sim-
ilar to the observed increase during the late morning and
afternoon, but the formation rate is far too low. The uncer-
tainties in POA emissions are far less than those associated
with SOA, so that changing the POA emissions is unlikely to
solve the under-prediction in SOA for the current volatility
(a) Pasadena
0 6 12 18 0
0
2
4
P
O
A

(
u
g

m
-
3
)
0 6 12 18 0

0
5
10
S
O
A

(
u
g

m
-
3
)
(b) Sacramento (T0)
0 6 12 18 0
0
1
2
0 6 12 18 0

0
2
4
(d) Cool (T1)
0 6 12 18 0
0.0
0.5
1.0
0 6 12 18 0
hour (LST)
0
2
4
(c) Bakersfield
0 6 12 18 0
0
2
4
P
O
A

(
u
g

m
-
3
)
0 6 12 18 0
time (LST)
0
2
4
S
O
A

(
u
g

m
-
3
)
PMF DEF_ANT 50%_ANT 0%_ANT
Figure 13. Diurnal averages of primary and secondary organic
aerosol components at the (a) Pasadena, (b) T0, (c) Bakerseld,
(d) T1 sites. Blue dots denote values derived from AMS measure-
ments using positive matrix factorization (PMF) techniques. Simu-
lated POA and SOA are the total of the rst four model size bins up
to 0.625 mdiameters. Gray shading denotes night and vertical lines
in right panels denote measurement uncertainty range. 50 %_LBC
simulation results not shown since they are nearly identical to those
from the 50 %_ANT simulation.
basis set approach to SOA unless POA is increased to un-
realistic levels compared with PMF estimates. As shown in
Fig. 5c, simulated OH is too high in the DEF_ANT simu-
lation. Since SOA formation rate in the VBS approach de-
pends on OH, the over-prediction in OH would suggest that
simulated SOA should be too high. The results indicate that
SOA formation processes from anthropogenic sources are
missing or not represented adequately at this urban site. In
contrast, simulated SOA is closer to the PMF estimates at
the other sites (Fig. 13bd). Setyan et al. (2012) show that
a large fraction of SOA at the T1 site originates from bio-
genic sources. However, the 0 %_ANT simulation that in-
cludes only biogenic SOA produces less than 0.5 g m
3
on
average at T1, suggesting that most of the simulated SOA is
from anthropogenic sources. Since POA in the DEF_ANT
simulation is too high and biogenic SOA is a small fraction
of the total SOA, the model is likely producing the correct
magnitude in SOA for the wrong reasons at the T1 site. It ap-
pears that uncertainties associated with anthropogenic semi-
volatile and intermediate volatility precursor emissions that
are poorly constrained and yields of multigenerational bio-
genic chemistry are canceling each other out to some extent.
In addition, semi-volatile and intermediate VOCs form SOA
rapidly in the current VBS approach, whereas light aromat-
ics (e.g., toluene) will make SOA continuously over several
days. Multi-generational chemistry for aromatics is currently
ignored; however, Hodzic et al. (2013) use an explicit model
to showthat this process could be important at regional scales
over several days of chemical processing.
Simulated OA aloft was also compared with AMS mea-
surements collected by the G-1, WP-3D, and CIRPAS Twin
Otter aircraft in terms of percentiles over the sampling pe-
riod as shown in Fig. 9b. The observed OA concentrations
from the G-1 are higher than those from the WP-3D since
the highest OA concentrations occurred during the last few
days of June and the last WP-3D ight north of 35
N was
on the 18 June. As with the T0 and T1 sites, OA concentra-
tions from the DEF_ANT simulation were closer to obser-
vations over northern California than the other simulations.
While OA from the DEF_ANT simulation was very similar
to observations from the WP-3D south of 35
N, that sim-
ulation produced higher than observed concentrations along
the CIRPAS Twin Otter paths. The variations in OA concen-
trations from the 50 %_ANT simulation were also closer to
Twin Otter observations. Note that the ight days and sam-
pling period for the WP-3D (4 May22 June) and Twin Otter
ights (628 May) are not identical, so that observed and
simulated percentiles for these two data sets are likely to be
different. Nevertheless, these results aloft are substantially
different than the under-predictions of OA at the Pasadena
site. Statistics on OA for individual aircraft ights from the
DEF_ANT simulation are given in Table S38 in the Supple-
ment.
To further illustrate the uncertainties in OA predictions,
Fig. 14 compares the observed and simulated OA and CO
from the G-1 ights on 12 and 28 June. The afternoon
G-1 ight on 28 June had the highest OA observed during
CARES, while 12 June had low OA concentrations as a re-
sult of strong northwesterly winds associated with an upper-
level trough (Fast et al., 2012). The simulated CO along the
ight path on 28 June is similar to observations downwind
of Sacramento, except that the peak concentrations in cen-
ter of the plume (points A and B in Fig. 14a) are too low.
While the simulated southwesterly up-slope winds are sim-
ulated reasonably well as described in Fast et al. (2012), the
simulated boundary layer (BL) depth during the afternoon
of 28 June was 61 % higher than observed at 13:00 LST and
25 % higher than observed at 16:00 LST, leading to excessive
dilution within the model. The spatial variation in simulated
OA is similar to CO, indicating that simulated SOA is in-
uenced or controlled by anthropogenic sources; however,
the concentrations from both DEF_ANT and 50 %_ANT are
much lower than the AMS measurements. Peak values from
DEF_ANT are 7 g m
3
, while observations are as high as
25 g m
3
. In addition to too much dilution, two other fac-
tors likely account for the under-prediction in OA. First, the
(a) G-1 flight during afternoon of June 28
22.0 22.5 23.0 23.5 24.0 24.5 25.0
0
8
16
24
O
M

(
u
g

m
-
3
)
DEF_ANT
50%_ANT
0%_ANT
22.0 22.5 23.0 23.5 24.0 24.5 25.0
0
8
16
24
O
M

(
u
g

m
-
3
)
A B C D E B A F
22.0 22.5 23.0 23.5 24.0 24.5 25.0
100
150
200
250
C
O

(
p
p
b
V
)
22.0 22.5 23.0 23.5 24.0 24.5 25.0
100
150
200
250
C
O

(
p
p
b
V
)
22.0 22.5 23.0 23.5 0.0 0.5 1.0
time (UTC)
0
1
2
altitude (km MSL)
0.000 0.167 0.333 0.500 0.667 0.833 1.000 0.00
0.25
0.50
0.75
1.00
color_contours = DEF_ANT simulation ~1 km AGL at 22 UTC
A
B
C
D
E
F
T0
T1
0.000 0.167 0.333 0.500 0.667 0.833 1.000 0.00
0.25
0.50
0.75
1.00
0.0 0.2 0.4 0.6 0.8 1.0
0.15
0.36
0.58
0.79
1.00
3
4
5
6
7
9
11
15
19

ug m
-3
(b) G-1 flight during afternoon of June 12
22.5 23.0 23.5 24.0 24.5 25.0 25.5
0
2
4
O
M

(
u
g

m
-
3
)
A B C D E F G H G
22.5 23.0 23.5 24.0 24.5 25.0 25.5
0
2
4
O
M

(
u
g

m
-
3
)
22.5 23.0 23.5 24.0 24.5 25.0 25.5
100
120
140
160
C
O

(
p
p
b
V
)
22.5 23.0 23.5 24.0 24.5 25.0 25.5
100
120
140
160
C
O

(
p
p
b
V
)
22.5 23.0 23.5 0.0 0.5 1.0 1.5
time (UTC)
0
1
2
altitude (km MSL)
0.000 0.167 0.333 0.500 0.667 0.833 1.000 0.00
0.25
0.50
0.75
1.00
color_contours = DEF_ANT simulation ~1 km AGL at 23 UTC
A
B
C
D E
F
G
H
T0
T1
0.000 0.167 0.333 0.500 0.667 0.833 1.000 0.00
0.25
0.50
0.75
1.00
0.0 0.2 0.4 0.6 0.8 1.0
0.15
0.36
0.58
0.79
1.00
0.4
0.6
0.8
1.0
1.2
1.4
1.8
2.2
2.6

ug m
-3
Figure 14. Observed and simulated OA during CARES in the vicinity of Sacramento for the afternoon of (a) 28 June and (b) 12 June. (a) and
(b) represent days with high and low observed OA, respectively. Simulated OA is the total of the rst four model size bins up to 0.625 m
diameter.
regional OA background concentrations transported into the
Sacramento region are too low, even though background con-
centrations of CO are close to observed. Second, the model
likely under-estimates enhanced SOA production resulting
from anthropogenic emissions mixing with biogenic SOA
precursors as described in Setyan et al. (2012) and Shilling
et al. (2013).
Similar to the G-1 measurements, lower OA concentra-
tions are simulated during the afternoon of 12 June than
on other days. The simulated concentrations are usually less
than 1 g m
3
while the observed concentrations are between
2 and 3 g m
3
(Fig. 14b). The model also fails to capture
the spatial variability in OA and CO on this day. The bot-
tom panel of Fig. 14b shows that highest concentrations of
observed OA are located on the eastern side of the valley,
but the model produced peak concentrations over the western
side of the valley. The spatial pattern in simulated CO is sim-
ilar to OA (not shown). While the simulated wind speed and
direction at the Sacramento radar wind proler 1 kma.g.l.
was very similar to the observations (Fig. S4a in the Supple-
ment), the simulated winds along the G-1 ight path were
northerly along the foothills of the Sierra Nevada and the ob-
servations were northwesterly. Tables S3 and S4 in the Sup-
plement show that the performance in simulated winds along
the G-1 ight path was reasonable during the morning of 12
June but decreased signicantly during the afternoon. While
transport errors likely accounts for all of the errors in simu-
lated CO, they cannot explain the bias in simulated OA. The
production of SOA is likely too low on this day as well.
In contrast, the spatial distributions of OA were usually
simulated better in the vicinity of the Los Angeles Basin.
Examples are shown in Fig. 15 for WP-3D ights on 20
and 3 June that had relatively higher and lower peak OA
concentrations, respectively. On both days, the model repro-
duced the spatial variability in both CO and OA reasonably
well. The correlation coefcients for OA on 20 and 3 June
were 0.83 and 0.7, respectively. The peak concentrations in
OA from the DEF_ANT and 50 %_LBC simulations were 5
and 3 g m
3
, respectively, for both days while the observed
peak values were between 7 and 10 g m
3
. OA concentra-
tions from both simulations were much closer to observed
on 3 June, with the DEF_ANT simulated OA somewhat
higher than observed and 50 %_ANT simulated OA some-
what lower than observed.
In general, BC from the 50 %_ANT simulation was much
closer to most surface and aircraft measurements than the
simulation that used the default emission inventory. Sim-
ulated BC was also somewhat further improved in the
50 %_LBC simulation in remote regions where a relatively
higher fraction to the total aerosol mass is inuenced by
boundary conditions provided by the global model. In con-
trast, organic matter (OM) simulated by the DEF_ANT simu-
lation was usually closer to observations than the other simu-
lations but the statistics show that performance varies signif-
icantly over California. Simulated POA from the DEF_ANT
Figure 15. Observed and simulated OA during CalNex in the vicinity of Los Angeles during (a) the afternoon of 20 June and (b) the
morning of 3 June. (a) and (b) represent days with high and low observed OA, respectively. The white dot denotes the location of the
Pasadena supersite. Simulated OA is the total of the rst four model size bins up to 0.625 m diameter.
simulation was also closer to POA derived from AMS mea-
surements at the Pasadena and T0 site, but the 50 %_ANT
simulation POA was closer to the derived POA at the Bak-
erseld and T1 sites. While uncertainties in POA emissions
contribute to errors in simulated OM, the largest source of
uncertainty in simulated OM is the treatment of SOA.
4.3 Inorganic aerosols
The time series and average diurnal variation of SO
2
4
ob-
tained from the AMS instruments at the four supersites
along with the simulated values are shown in Fig. 16. SO
4
concentrations from the DEF_ANT and 50 %_ANT simu-
lations at the Pasadena site are about a factor of 2 too low
on average, and the simulated diurnal variability is weaker
than observed. The simulated multi-day variations are qual-
itatively similar to observed with higher concentrations be-
tween 15 and 20 May and between 31 May and 8 June.
While the average SO
2
4
concentrations from the DEF_ANT
and 50 %_ANT simulations are similar to observations at the
Bakerseld site, the model fails to capture peak concentra-
tions frequently observed during the late afternoon. In con-
trast, the simulated diurnal and multi-day variability is pre-
dicted reasonably well by the model at the T0 and T1 sites,
but the concentrations from the DEF_ANT and 50 %_ANT
simulation are up to 50 % too high. While SO
2
emissions
were the same in the DEF_ANT and 50 %_ANT simula-
tions, differences in photochemistry altered the formation
rate of SO
2
4
. SO
2
4
concentrations of 0.5 g m
3
were
produced by the 0 %_ANT simulation at all four sites. Con-
centrations as high as 3 g m
3
were produced in Pasadena
between 31 May and 8 June, suggesting that that the over-
all increase in SO
2
4
during that period was associated with
sources outside of the domain. In fact, the magnitude and
multi-day variability of SO
4
from the 0 %_ANT simulation
were close to observed, suggesting that local emissions of
SO
2
do not signicantly contribute to SO
2
4
production in
the vicinity of Sacramento during June. However, this does
not seem plausible since there are large emissions of SO
2
upwind of Sacramento in the Carqueniz Strait and intrusions
of marine air transports SO
2
4
produced by these emissions
towards Sacramento (Fast et al., 2012; Setyan et al., 2012;
Zaveri et al., 2012). Decreasing the boundary conditions of
aerosols from MOZART for the 50 %_LBC simulation re-
sults in SO
2
4
concentrations that are close to observed most
times of the day.
An example of the impact of the marine intrusions on the
formation and transport of SO
2
4
from the Bay Area to the T1
site on 26 June is shown in Fig. 17. On this day, the observed
and simulated near-surface winds are southwesterly (up-
slope) throughout the late morning and afternoon (10:00
18:00 LST), although the observations are more variable than
simulated. Simulated SO
2
4
from the 50 %_LBC simulation
is very similar to observed, with concentrations increas-
ing from 0.4 to 1.0 g m
3
between 08:00 and 14:00 LST.
The contour plots of simulated SO
2
4
distributions over cen-
tral California at 05:00, 09:00, and 14:00 LST also show a
Figure 16. Observed and simulated time series (left panels) and average diurnal variation (right panels) of SO
2
4
at the four supersites.
Simulated SO
2
4
is the total of the rst four model size bins up to 0.625 m diameter. Gray shading denotes night and vertical lines in right
panels denote measurement uncertainty range.
trajectory of the mean winds originating at the oil renery
source at 05:00 LST. By 09:00 LST, a plume of SO
2
4
is pro-
duced downwind of the oil renery that has been transported
more than halfway towards the T1 site. The model also in-
dicates that SO
2
4
is formed locally in the vicinity of the T1
site as a result of photochemistry acting on previous days
emissions. By 14:00 LST, the air mass from the oil ren-
ery reached the T1 site at the same time as the observed
peak concentrations. The highest SO
2
4
concentrations, up
to 1.5 g m
3
, are produced south of Sacramento because of
the spatial and temporal variations in the thermally driven
winds during the day that spread the plume along the foothills
of the Sierra Nevada. A time series of simulated SO
2
and
SO
2
4
along the air mass trajectory indicates that as SO
2
4
is gradually produced along the trajectory. SO
2
decreases as
a result of both photochemistry and mixing in the growing
convective boundary layer. Peak concentrations of SO
2
4
are
actually produced at 12:00 LST over Sacramento as vertical
mixing rates after that time exceed photochemical production
during the late afternoon. The model therefore suggests that
the increase in SO
2
4
at the T1 site is due to both local pho-
tochemistry of aged emissions and same-day transport from
the Bay Area superimposed on a background concentration
that decreases slightly during the day (not shown).
The observed and simulated NO
3
at the four supersites is
shown in Fig. 18. Pasadena had the highest observed NO
3
,
with concentrations up to 20 g m
3
on 2 days and concen-
trations exceeding 5 g m
3
on many days. Daily peak con-
centrations were usually less than 3 g m
3
at Bakerseld,
although concentrations were as high as 7.5 g m
3
on 1
day. At the T0 and T1 sites, NO
3
concentrations were much
lower, usually less than 0.3 g m
3
so that it comprised only
a minor fraction of the total aerosol mass. In contrast with the
poor simulation of SO
2
4
, the magnitude and temporal vari-
ability in NO
3
is predicted reasonably well at the Pasadena
site. Decreasing anthropogenic precursor emissions in the
50 %_ANT simulation increases the concentration of NO
3
somewhat to be closer to observed, but both the DEF_ANT
and 50 %_ANT underestimate the daily peak concentrations
on many days. The performance in simulated NO
3
at the
Bakerseld site is not as good as at the Pasadena site. While
the observed and simulated peak concentrations both occur
around sunrise, the simulated NO
3
falls to near zero by the
late afternoon and the rate of increase at night is lower than
observed. The AMS measurements at the T0 and T1 sites in-
dicate the presence of low concentrations at all times; how-
ever, the simulated NO
3
is nearly zero except for short pe-
riods of time in June in which NO
3
concentrations are as
high as 1 g m
3
. The low observed NO
3
concentrations that
do not exhibit signicant diurnal variations coupled with the
known transport patterns suggest a regional background of
NO
3
that the model does not reproduce. Given the lack of
HNO
3
or NH
3
measurements at these sites, it is difcult
to determine the reason for the under-predictions; however,
04 10 16 22
0
90
180
270
360
w
i
n
d

d
i
r
e
c
t
i
o
n

(
d
e
g
)
observed at T1
simulated at T1
04 10 16 22
time (LST)
0.0
0.3
0.6
0.9
1.2
S
O
4
2
-

(
u
g

m
-
3
)
observed at T1
simulated at T1
57.50 57.75 58.00 58.25
0.0
0.3
0.6
0.9
1.2
S
O
4
2
-

(
u
g

m
-
3
)
0.000 0.167 0.333 0.500 0.667 0.833 1.000 0.00
0.25
0.50
0.75
1.00
Simulated SO
4
2-
at 05 LST June 26
T0
T1
0.000 0.167 0.333 0.500 0.667 0.833 1.000 0.00
0.25
0.50
0.75
1.00
0.000 0.167 0.333 0.500 0.667 0.833 1.000 0.00
0.25
0.50
0.75
1.00
Simulated SO
4
2-
at 09 LST June 26
T0
T1
0.000 0.167 0.333 0.500 0.667 0.833 1.000 0.00
0.25
0.50
0.75
1.00
0.000 0.167 0.333 0.500 0.667 0.833 1.000 0.00
0.25
0.50
0.75
1.00
Simulated SO
4
2-
at 14 LST June 26
T0
T1
0.000 0.167 0.333 0.500 0.667 0.833 1.000 0.00
0.25
0.50
0.75
1.00
0.0 0.2 0.4 0.6 0.8 1.0
0.00
0.25
0.50
0.75
1.00
0.2

0.4

0.6

0.8

1.0

1.2

1.4

1.6

ug m
-3
05 06 07 08 09 10 11 12 13 14
time (LST)
0.0
0.3
0.6
0.9
1.2
S
O
4
2
-

(
u
g

m
-
3
)
,

B
L

d
e
p
t
h

(
k
m
)
0.0
0.6
1.2
1.8
2.4
S
O
2

(
p
p
b
)
Figure 17. Observed and simulated time series of wind direction and SO
2
4
(left panels), near-surface SO
2
4
distributions between the San
Francisco Bay area and the T1 site at 05:00, 09:00, and 14:00 LST and one air mass trajectory that arrives at the T1 site at 14:00 LST
during the peak afternoon SO
2
4
concentration (upper right panels), and evolution of SO
2
4
, SO
2
, and boundary layer (BL) height along the
trajectory (lower right panel).
comparisons with the WP-3D measurements (Fig. 6b) sug-
gest that NH
3
emissions over northern California are likely
too low that could also impact NO
3
production.
Figure 19 depicts the performance in simulated NH
+
4
at
the four supersites. While the instantaneous data from the
T0 AMS is noisy, the average values are similar to those at
the T1 site; therefore, the data are included for complete-
ness. As with SO
2
4
, reducing anthropogenic emissions in
the 50 %_ANT simulation leads to lower NH
+
4
at all sites.
The overall performance in simulated NH
+
4
at the Pasadena
site is very similar to NO
3
in that much of the diurnal and
multi-day variability is captured by the model, although the
concentrations are a factor of 2 too low on average. At the
Bakerseld site, the model produces an average diurnal vari-
ation similar to observed with the peak concentration of
NH
+
4
around sunrise as observed, but the daily peak con-
centrations are better simulated in May than during June.
The performance of the model is best at the T1 site; how-
ever, the simulated NH
+
4
concentrations from the DEF_ANT
and 50 %_ANT simulations are somewhat too high. Simi-
lar to SO
2
4
at this site, reducing the boundary conditions of
aerosols also lower NH
+
4
. The average reduction in NH
+
4
is
0.08 g m
3
even though the background concentrations
from the 0 %_ANT simulation are 0.03 g m
3
or less. This
indicates that reduction in NH
+
4
is due primarily to the re-
duction of pre-existing aerosols that ammonia can condense
upon, rather than reducing NH
+
4
from the boundaries.
As with OA, we also compared the simulated SO
2
4
, NO
3
,
and NH
+
4
with the AMS measurements collected on the G-1,
WP-3D, and CIRPAS Twin Otter aircraft in terms of per-
centiles as shown in Fig. 20. In contrast with over-predictions
in SO
2
4
from DEF_ANT and 50 %_ANT simulation at the
T0 and T1 sites, the overall median and range of SO
2
4
sim-
ulated aloft is similar to the G-1 measurements. Even though
the average concentrations from the 50 %_LBC simulation
were very similar to observed at the T0 and T1 sites, reducing
the boundary conditions of aerosols leads to simulated SO
2
4
aloft that is 50 % lower than observed. A similar trend in the
SO
2
4
percentiles among the simulations was produced along
the WP-3D ights north of 35
N, except that the overall con-

centrations from the DEF_ANT and 50 %_ANT simulations
concentrations are lower than observed. The simulated SO
2
4
from the DEF_ANT, 50 %_ANT and 50 %_LBC simulations
are higher over southern California than over northern Cal-
ifornia, similar to the aircraft observations. While the simu-
lated SO
2
4
is lower than observed along the WP-3D ight
paths, the DEF_ANT and 50 %_ANT simulation are higher
than observed along the CIRPAS Twin Otter ight paths.
The overall concentrations from the 50 %_LBC simulation
are closest to the CIRPAS Twin Otter measurements. As
with the AMS measurements, the simulated NO
3
and NH
+
4
are much lower over northern California than over southern
California. The DEF_ANT simulation produced NO
3
con-
centrations closer to observed over southern California and
NH
+
4
concentrations were comparable to the CIRPAS Twin
Otter measurements. In contrast, the simulated NH
+
4
from
the 50 %_LBC simulation is closest to the WP-3D measure-
ments. Additional statistics for all of the aircraft ights are
shown in Tables 1113 and statistics from the DEF_ANT
simulation for individual ights are given in Tables S39S41
in the Supplement. The spatial and temporal variations as re-
ected by the correlation coefcient and index of agreement
are in general the best for OA, followed by BC, SO
2
4
, NH
+
4
,
and NO
3
.
In summary, the model is able to simulate much of the di-
urnal and multi-day variability of the inorganic aerosol con-
centrations. Simulated SO
2
4
concentrations were too low at
Figure 18. Observed and simulated time series (left panels) and average diurnal variation (right panels) of NO
3
at the four supersites.
Simulated NO
3
is the total of the rst four model size bins up to 0.625 m diameter. Gray shading denotes night and vertical lines in right
panels denote measurement uncertainty range. Results from 50 %_LBC simulation not shown since it is nearly the same as the 50 %_ANT
simulation.
Figure 19. Observed (AMS instrument) and simulated time series (left panels) and average diurnal variation (right panels) of NH
+
4
at the
four supersites. Gray shading denote night and vertical lines in right panels denote measurement uncertainty range. Simulated NH
+
4
is the
total of the rst four model size bins up to 0.625 m diameter.
Table 11. Performance of simulated aerosol composition over all the G-1 ights in terms of bias, root-mean-square error (RMSE), correlation
coefcient (R), and index of agreement (IA).
3
) (g m
3
)
SO
2
4
DEF_ANT
0.53
0.03 0.32 0.45 0.65
50 %_ANT 0.09 0.34 0.41 0.62
0 %_ANT 0.28 0.44 0.06 0.44
50 %_LBC 0.21 0.38 0.43 0.59
NO
3
DEF_ANT
0.31
0.14 0.35 0.30 0.41
50 %_ANT 0.17 0.37 0.16 0.39
0 %_ANT 0.29 0.45 0.14 0.37
50 %_LBC 0.21 0.39 0.18 0.40
NH
+
4
DEF_ANT
0.16
0.11 0.23 0.15 0.40
50 %_ANT 0.14 0.19 0.06 0.42
0 %_ANT 0.16 0.19 0.09 0.42
50 %_LBC 0.14 0.19 0.06 0.42
BC
DEF_ANT
0.07
0.09 0.11 0.54 0.53
50 %_ANT 0.03 0.06 0.55 0.67
0 %_ANT 0.03 0.07 0.18 0.38
50 %_LBC 0.01 0.05 0.54 0.69
OA
DEF_ANT
4.16
1.70 3.32 0.76 0.70
50 %_ANT 2.73 4.23 0.78 0.54
0 %_ANT 3.75 5.34 0.78 0.44
50 %_LBC 2.77 4.25 0.78 0.54
Cl
DEF_ANT
0.01
0.01 0.04 0.07 0.15
50 %_ANT 0.01 0.04 0.02 0.14
0 %_ANT 0.01 0.04 0.07 0.18
50 %_LBC 0.01 0.04 0.03 0.14
Pasadena and Bakerseld, but much closer to observations
at the northern California surface sites and along most of
the CARES and CalNex aircraft ight paths. NO
3
concen-
trations from all the simulations were generally too low, ex-
cept along the CIRPAS Twin Otter ight paths. In general,
SO
2
4
is better simulated in northern California and NO
3
is
better simulated in southern California. While the statistical
performance for all the simulations is similar at most loca-
tions, the DEF_ANT simulation produced inorganic aerosol
concentrations that were somewhat closer to observations.
4.4 Aerosol mass, volume, and size distribution
Table 14 presents statistics that quantify the performance in
simulated total PM
2.5
mass at all the available operational
monitoring sites shown in Fig. 1d. The simulated PM
2.5
mass from the DEF_ANT simulation is too low in gen-
eral except over the Sacramento Valley, with the largest av-
erage bias of 4.5 g m
3
over southern California which
is 38 % lower than the observed mean concentration of
11.8 g m
3
. Reducing the primary emissions by 50 % leads
to larger biases in the 50 %_ANT simulation, with biases
ranging from 1.3 g m
3
(27 % lower than observed) over
the Sacramento Valley to 6.8 (58 % lower than observed)
over southern California. The temporal variability in PM
2.5
is
also better simulated in some regions of California than oth-
ers. For example, relatively higher correlation coefcients of
0.48 and 0.44 were obtained for southern California stations
where the biases were the greatest for both the DEF_ANT
and 50 %_ANT simulations, respectively. The lowest corre-
lation coefcients of 0.09 and 0.16 from the DEF_ANT sim-
ulation were produced for the Coastal and Interior mountain
regions, respectively that are the stations that are least inu-
enced by local anthropogenic emissions.
In addition to total aerosol mass, it is also important to ad-
equately simulate the aerosol size distribution to show that
the model represents the total aerosol mass for the right
reasons. Accurately representing the aerosol size distribu-
tion also affects aerosol radiative forcing and the ability of
aerosols to serve as CCN. The T0 and T1 sites had mea-
surements from Scanning Mobility Particle Sizer (SMPS)
and Aerodynamic Particle Sizer (APS) instruments that were
used to evaluate the simulated number and volume size dis-
tributions in terms of percentiles as shown in Fig. 21. The
SMPS measures number as a function of mobility diameter
Table 12. Performance of simulated aerosol composition over all the WP-3D ights in terms of bias, root-mean-square error (RMSE),
correlation coefcient (R), and index of agreement (IA).
3
) (g m
3
)
SO
2
4
DEF_ANT
0.75
0.20 0.47 0.66 0.74
50 %_ANT 0.24 0.50 0.64 0.71
0 %_ANT 0.42 0.68 0.39 0.50
50 %_LBC 0.37 0.57 0.64 0.66
NO
3
DEF_ANT
0.71
0.03 1.64 0.57 0.74
50 %_ANT 0.41 1.53 0.56 0.64
0 %_ANT 0.69 1.92 0.07 0.28
50 %_LBC 0.40 1.52 0.57 0.66
NH
+
4
DEF_ANT
0.48
0.10 0.56 0.66 0.79
50 %_ANT 0.24 0.59 0.64 0.68
0 %_ANT 0.44 0.82 0.08 0.38
50 %_LBC 0.27 0.60 0.65 0.68
BC
DEF_ANT
0.08
0.08 0.15 0.64 0.70
50 %_ANT 0.02 0.09 0.64 0.75
0 %_ANT 0.03 0.12 0.19 0.37
50 %_LBC 0.00 0.09 0.64 0.76
OA
DEF_ANT
1.74
0.23 1.35 0.71 0.83
50 %_ANT 0.58 1.47 0.71 0.72
0 %_ANT 1.31 2.19 0.33 0.48
50 %_LBC 0.64 1.49 0.72 0.72
Cl
DEF_ANT
0.02
0.02 0.11 0.17 0.30
50 %_ANT 0.02 0.11 0.12 0.23
0 %_ANT 0.02 0.11 0.04 0.16
50 %_LBC 0.01 0.12 0.08 0.22
that is similar to geometric diameter used by the model. The
APS measures number as a function of aerodynamic diame-
ter; therefore, the observed values have been adjusted to ge-
ometric diameter (Baron and Willeke, 2001) using a density
of 2.36 g m
3
based on 20 % SO
2
4
(1.8 g cm
3
), 20 % sea
salt (2.2 g cm
3
), and 60 % other inorganics (2.6 g cm
3
).
Note that some uncertainty is introduced here since the actual
composition of aerosols >1 m was not measured and com-
position will likely vary in time (DeCarlo et al., 2004). The
results fromthe 50 %_LBCsimulation are shown since it bet-
ter represented the observed composition, except for organic
aerosol (OA), than the other simulations. The gray shading
in Fig. 21 denotes the size range of the eight size bins em-
ployed by the MOSAIC aerosol model. The average number
distributions (Fig. 21a, b) at both sites are lower than ob-
served for bin 1 (0.0390.078 m), higher than observed for
bins 2 and 3 (0.0780.313 m), similar to observed for bins
46 (0.3132.5 m), and lower than observed for bin 7 (2.5
5 m). The corresponding volume distributions have similar
biases as expected (Fig. 21c, d).
The simulated aerosol composition distribution is also
compared with the AMS distribution at the T1 site (Setyan et
al., 2012) and is shown in Fig. 22. While the largest OA mass
is observed and simulated in the size range of bin 3 (0.156
0.313 m) in the model (Fig. 22a), the simulated distribution
is narrower than observed so that the mass is too low in bins
12 (0.0390.156 m) and 4 (0.3130.625 m). As described
in Setyan et al. (2012), SO
2
4
had a bimodal mass distribu-
tion with peak values around 0.4 m. Although the simulated
SO
2
4
in bin 4 (0.3130.625 m) was close to the observed
mean value, peak concentrations from the model (Fig. 22b)
occurred in bin 3 (0.1560.313 m). Simulated concentra-
tions were also too low in bins 12 (0.0390.156 m), and
5 (0.6251.25 m). As shown previously in Fig. 18 the simu-
lated NO
3
(<1.25 m) is usually too low at the T1 site; how-
ever, the model does produce more NO
3
mass in bins 57
(0.6255 m) as shown in Fig. 22c. The shape of the simu-
lated SO
2
4
and NH
+
4
mass distributions are similar to one
another, as are the shape of the observed SO
2
4
and NH
+
4
dis-
tributions (Fig. 22d). In contrast with simulated SO
2
4
, the
simulated NH
+
4
concentrations in bins 3 (0.1560.313 m)
and 5 (0.6251.25 m) are similar to observed while con-
centrations in bins 12 (0.0390.156 m) and 4 are too low
(0.3130.625 m).
Table 13. Performance of simulated aerosol composition over all the CIRPAS Twin Otter ights in terms of bias, root-mean-square error
(RMSE), correlation coefcient (R), and index of agreement (IA).
Composition Simulation Observed Bias RMSE R IA
mean (g m
3
) (g m
3
)
SO
2
4
DEF_ANT
0.60
0.05 0.54 0.16 0.43
50 %_ANT 0.31 0.57 0.27 0.42
0 %_ANT 0.10 0.54 0.16 0.43
50 %_LBC 0.22 0.58 0.11 0.44
NO
3
DEF_ANT
1.77
0.57 2.02 0.49 0.68
50 %_ANT 1.76 2.76 0.16 0.41
0 %_ANT 1.14 2.24 0.43 0.56
50 %_LBC 1.10 2.20 0.44 0.58
NH
+
4
DEF_ANT
0.96
0.45 0.85 0.51 0.64
50 %_ANT 0.96 1.27 0.15 0.43
0 %_ANT 0.64 0.97 0.47 0.54
50 %_LBC 0.66 0.98 0.47 0.54
BC
DEF_ANT
0.05
0.19 0.26 0.41 0.36
50 %_ANT 0.02 0.09 0.15 0.24
0 %_ANT 0.08 0.13 0.39 0.51
50 %_LBC 0.07 0.12 0.41 0.54
OA
DEF_ANT
1.81
0.21 0.99 0.70 0.83
50 %_ANT 1.65 2.02 0.53 0.45
0 %_ANT 0.52 1.00 0.70 0.78
50 %_LBC 0.54 1.02 0.70 0.78
Cl
DEF_ANT
0.12
0.10 0.16 0.02 0.38
50 %_ANT 0.09 0.15 0.12 0.41
0 %_ANT 0.11 0.16 0.01 0.38
50 %_LBC 0.11 0.16 0.01 0.39
Composition distributions are also shown in Fig. 22e, f as a
percent of the total mass for the observed and simulated dis-
tributions, respectively. For the simulated composition dis-
tribution, BC, sea-salt (NaCl), and other inorganic material
(OIN) are shown since they comprise a signicant fraction
of the total mass. While the T1 site is located 200 km from
the ocean, Laskin et al. (2012) provided evidence of chlo-
ride depletion in aged sea salt particles sampled along the
G-1 ight paths using scanning electron microscopy, scan-
ning transmission X-ray microscopy, and near edge X-ray
absorption ne structure spectroscopy techniques. Moffet et
al. (2013) employ similar microscopy techniques using par-
ticles collected at the T0 and T1 sites to show that dust and
sea-salt particles were more prevalent at coarser sizes on 27
and 28 June. Comparing Fig. 22f with Fig. 21d suggests that
simulated coarse mode NaCl and OIN concentrations are too
high. Some of the simulated OIN results from long-range
transport of dust in the MOZART model, as will be shown in
the next section. Simulated sub-micron NaCl and OIN com-
prise 2040 % (depending on size) of the total mass at the
T1 site. This fraction is much higher than observed at the
Pasadena site (Hayes et al., 2013), but measurements from
the PALMS instrument at the T1 site are not yet available for
comparison.
An evaluation of both the ne and coarse aerosol compo-
nents at the Pasadena site using the available measurements
is shown in Fig. 23. The observations suggest that the sim-
ulated PM
2.5
OIN is roughly twice as high as observed dur-
ing CalNex. In contrast, simulated sea-salt concentrations are
similar to observed for PM
2.5
PM
1
, and are also a much
larger fraction of the total mass compared to PM
1
. The large
amount of simulated sum of OA+SO
2
4
+NO
3
for PM
2.5
PM
1
is due mostly to NO
3
. The average simulated PM
1
NO3
is too low while the simulated PM

2.5
PM
1.25
is too
high, suggesting that the size distribution is skewed towards
the coarser sizes, similar to the T1 site (Fig. 22c).
Additional analyses of the SP2 and single particle mea-
surements are needed to provide more quantitative informa-
tion to assess the simulated mass and size distributions asso-
ciated with BC, NaCl, and OIN. Size distribution measure-
ments using different instruments were also collected at other
surface sites and on two research aircraft, but additional eval-
uation of simulated size distributions will be performed later
Table 14. Performance of simulated PM
2.5
for all the surface operational monitoring sites in terms of bias, root-mean-square error (RMSE),
correlation coefcient (R), and index of agreement (IA).
Region Simulation Observed Bias RMSE R IA
Mean (g m
3
) (g m
3
)
CA
DEF_ANT
8.4
2.8 7.0 0.45 0.58
50 %_ANT 4.4 7.9 0.44 0.48
0 %_ANT 6.3 9.5 0.13 0.42
Southern CA
DEF_ANT
11.8
4.5 8.1 0.48 0.60
50 %_ANT 6.8 9.7 0.44 0.50
0 %_ANT 9.51 12.2 0.04 0.43
San Joaquin
DEF_ANT
7.7
1.5 5.1 0.46 0.63
50 %_ANT 3.6 6.0 0.43 0.51
0 %_ANT 5.6 7.7 0.08 0.44
Sacramento Valley
DEF_ANT
4.8
0.1 3.7 0.32 0.52
50 %_ANT 1.3 3.8 0.30 0.43
0 %_ANT 2.7 4.7 0.08 0.42
Coastal
DEF_ANT
6.5
3.0 7.2 0.09 0.34
50 %_ANT 3.7 7.5 0.11 0.36
0 %_ANT 4.6 8.0 0.23 0.37
Interior Mountains
DEF_ANT
6.3
2.2 8.2 0.16 0.31
50 %_ANT 3.2 8.5 0.15 0.30
0 %_ANT 4.1 8.9 0.07 0.31
0 1 2 3 4 5 6 0.0
0.5
1.0
1.5
2.0
u
g

m
-
3
(a) SO
4
2-
percentiles for all aircraft flights
0 1 2 3 4 5 6 0.0
0.5
1.0
1.5
2.0
u
g

m
-
3
(b) NO
3
-
0 1 2 3 4 5 6 0.0
0.5
1.0
u
g

m
-
3
(c) NH
4
+
G-1
0 1 2 3 4 5 6 0.0
0.5
1.0
1.5
2.0
0 1 2 3 4 5 6 0.0
0.5
1.0
1.5
2.0
0 1 2 3 4 5 6 0.0
0.5
1.0
WP-3D > 35
o
N
0 1 2 3 4 5 6 0.0
0.5
1.0
1.5
2.0
0 1 2 3 4 5 6 0
2
4
6
0 1 2 3 4 5 6 0
1
2
3
WP-3D < 35
o
N
0 1 2 3 4 5 6 0.0
0.5
1.0
1.5
2.0
0 1 2 3 4 5 6 0
2
4
6
0 1 2 3 4 5 6 0
1
2
3
CIRPAS Twin Otter
Figure 20. Percentiles for (a) sulfate (SO
2
4
), and (b) nitrate
(NO
3
), and ammonium (NH
+
4
) for all G-1, WP-3D, and CIRPAS
Twin Otter ights. Vertical lines denote 5th and 95th percentiles,
boxes denote 25th and 75th percentiles, and the white dots denote
the 50th percentiles. Note the scale differs for the northern and
southern ights for NO
3
and NH
+
4
.
after information from all the SP2 and single particle instru-
ments are available.
5 Extinction proles, AOT, and AOD
We have also compared the simulated extinction proles
with the observed proles obtained from the HSRL-1 on
the B-200 aircraft during the CARES and CalNex cam-
paigns to infer how well the model represents proles of
aerosol mass that are not necessarily sampled by the in situ
measurements on the other research aircraft. The aerosol
optical depth (AOD) is the vertically integrated extinction
throughout the entire atmospheric column usually obtained
from AERONET and satellite measurements. In contrast, the
aerosol optical thickness (AOT) is the vertically integrated
extinction over a discrete layer. For CARES and CalNex,
AOT from the HSRL was obtained from the ground to the
aircraft sampling altitude which was 9 kmm.s.l.
As an example, the observed and simulated extinction for
the B-200 ight on 25 May over southern California is shown
in Fig. 24. The highest extinction was observed in the con-
vective boundary layer (below 1.4 kmm.s.l. in Fig. 24a, d)
over the Los Angeles basin where the emissions are the high-
est. Extinction from the DEF_ANT simulation is also highest
in the convective boundary layer, but the magnitude is 1.5
2 times lower than observed on average. This is consistent
with the underprediction in aerosol mass at the Pasadena site
(a) T0 number distribution
0.01 0.10 1.00 10.00
geometric diameter (um)
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
d
N
/
d
l
o
g
D

(
c
m
-
3
)
SMPS
APS
WRF, 50%_LBC
(b) T1 number distribution
0.01 0.10 1.00 10.00
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
(c) T0 volume distribution
0.01 0.10 1.00 10.00
0.1
1.0
10.0
100.0
d
V
/
d
l
o
g
D

(
u
m
3

c
m
-
3
)
(d) T1 volume distribution
0.01 0.10 1.00 10.00
0.1
1.0
10.0
100.0
Figure 21. Overall observed aerosol number distribution from the SMPS (red) and APS (blue) instruments at the (a) T0 and (b) T1 sites
during June 2010 along with the simulated aerosol number distribution (gray). (c) and (d) same as (a) and (b), except for aerosol volume
distribution. Thick red and blue lines denote 50th percentile and thin vertical red and blue lines denote the 5th and 95th percentiles for the
observations. Gray vertical lines denote simulated 5th and 95th percentiles, boxes denote 25th and 75th percentiles, and the white dots denote
the 50th percentiles.
(e.g., Fig. 23); nevertheless, simulated aerosol mass aloft was
closer to observed along the WP-3D and CIRPAS Twin Ot-
ter ight paths. When the effect of long-range transport is
reduced in the 50 %_LBC simulation, the simulated extinc-
tion in the free troposphere is much closer to observed but
the aerosol mass and extinction in the convective boundary
layer is further reduced as well (Fig. 24b, d). Even though
the boundary layer extinction is under-estimated, the simu-
lated AOT from DEF_ANT is higher than observed by about
a factor of 2 (Fig. 24e) because of over-predictions in the
vertically integrated extinction in the free troposphere. Sim-
ilarly, the AOT from the 0 %_ANT simulation is higher than
observed which does not seem reasonable and also suggests
the background aerosol concentrations from MOZART are
too high. The AOT from the 50 %_LBC simulation is the
closest to observed outside of the Los Angeles Basin where
the emission rates are relatively low.
Another example in the vicinity of Sacramento during
CARES on 27 June is shown in Fig. 25. As expected, the
highest extinction was observed in the convective boundary
layer within 1kmm.s.l.; however, the lidar also detected a
layer of aerosols between 1.5 and 3.5 kmm.s.l. above the
boundary layer (Fig. 25a). Extinction from the DEF_ANT
simulation was similar to observed in the free troposphere
and somewhat lower than observed in the convective bound-
ary layer (Fig. 25b, d). This is consistent with predictions
of aerosol mass, particularly OA, that are too low along the
G-1 ight paths. The model qualitatively captured the ver-
tical structure of aerosols in the convective boundary layer
and the layer aloft. Similar to the layer described in Fast
et al. (2012), daytime upslope ows transport trace gases
and aerosols from the valley over the Sierra Nevada that are
subsequently transported back over the valley at night. The
0 %_ANT simulation produced no such layer aloft (Fig. 25d),
indicating that the layer is produced by local emissions and
not long-range transport. As with the previous case in south-
ern California, simulated extinction above 3.5 km was higher
than observed. Reducing aerosols from long-range transport
in the 50 %_LBC simulation improved the extinction above
3.5 kmm.s.l., but also led to extinctions being lower than
(a) OA
0.01 0.10 1.00 10.00
0
2
4
6
8
d
M
/
d
l
o
g
D

(
u
g

m
-
3
)
(b) SO
4
2-
0.01 0.10 1.00 10.00
0.0
0.2
0.4
0.6
0.8
1.0
d
M
/
d
l
o
g
D

(
u
g

m
-
3
)
(c) NO
3
-
0.01 0.10 1.00 10.00
0.0
0.2
0.4
0.6
0.8
1.0
d
M
/
d
l
o
g
D

(
u
g

m
-
3
)
(d) NH
4
+
0.01 0.10 1.00 10.00
0.0
0.1
0.2
0.3
0.4
d
M
/
d
l
o
g
D

(
u
g

m
-
3
)
0.01 0.10 1.00 10.00
vacuum aerodynamic diameter (um)
0.0
0.2
0.4
0.6
0.8
1.0
%

o
f

A
M
S

t
o
t
a
l

(
c
o
l
o
r
)
(e)
A
M
S

t
o
t
a
l
,

d
M
/
d
l
o
g
D

(
u
g

m
-
3
)
0
1
2
3
4
5
OA
SO
4
2-
NO
3
-
NH
4
+
0.01 0.10 1.00 10.00
0.0
0.2
0.4
0.6
0.8
1.0
%

s
i
m
u
l
a
t
e
d

t
o
t
a
l

(
c
o
l
o
r
)
s
i
m
u
l
a
t
e
d

t
o
t
a
l
,

d
M
/
d
l
o
g
D

(
u
g

m
-
3
)
0
1
2
3
4
5
BC
OA
SO
4
2-
NO
3
-
NH
4
+
NaCl
OIN
(f)
Figure 22. Observed size distribution of (a) OA, (b) SO
2
4
, (c) NO
3
, and (d) NH
+
4
(thick colored lines) at the T1 site along with the
percentiles for each size bin from the 50 %_LBC simulation (gray). Vertical lines denote 5th and 95th percentiles, boxes denote 25th and
75th percentiles, and the white dots denote the 50th percentiles. (e) and (f) depict % of total mass by composition as well as total mass.
Dashed lines in (e) and (f) are for the total of OA, SO
2
4
, NO
3
, and NH
+
4
, while the solid line in (f) is for all aerosol components in the
model.
BC
OA
SO
4
NO
3
NH
4
Cl
Na
OIN
0.51 0.45
7.00 1.95
2.90 1.22
3.60 2.03
2.10 0.93
0.12 0.20
0.24 0.27
0.49 0.97
observed
g m
-3
50%_LBC
g m
-3
observed PM
1

16.96 g m
-3
simulated PM
1.25

8.02 g m
-3
observed PM
2.5
PM
1

2.49 g m
-3
simulated PM
2.5
- PM
1.25

4.15 g m
-3
0.03 0.01
0.31 1.92
0.06 -
0.16 -
0.30 0.87
1.53 1.35
0.10 -
BC
OA+SO
4
+NO
3
biomass burning
oil combustion
dust
seasalt
unidentified
observed
g m
-3
50%_LBC
g m
-3
Figure 23. Average aerosol composition observed (left) and simu-
lated (right) at the Pasadena site. Observations adapted from Hayes
et al. (2013) where PM
1
observations obtained from AMS, ele-
mental carbon / organic carbon EC/ OC Sunset Analyzer, and X-ray
uorescence analysis and PM
2.5
PM
1
observations obtained from
PALMS particle types.
observed below 3.5 kmm.s.l. (Fig. 25c, d). As with Fig. 24,
AOT from the DEF_ANT simulation is too high compared to
the lidar AOT. The 50 %_LBC simulation produces AOT that
is closer to observed outside of the anthropogenic plumes,
but is too low where extinction in the convective boundary
layer was observed to be the highest.
Simulated aerosol water could also play a role in the bi-
ases in extinction; however, the observed relative humidity
over land was usually low and consequently water uptake
on aerosols would likely be small. As shown in Table 5,
the mean observed relative humidity aloft ranged between
37 and 49 % among the three aircraft. The simulated relative
humidity was close to observed for the G-1 ights, but the
relative humidity was usually 6 % too low for the WP-3D
and CIRPAS Twin Otter ights. For the G-1 ight on 27
June (Fig. 25), observed relative humidity ranged from 20 to
55 % and the model was 5 % too low over a portion of the
ight path. The low relative humidity also implies that errors
in simulated relative humidity do not adversely affect simu-
lated water uptake. Nevertheless, the aircraft did not sample
the entire vertical column as measured by the HSRL on the
B-200 aircraft so there could be locations and times when
the relative humidity is sufciently high and permits conden-
sation of water on aerosols. In addition to errors in aerosol
composition mass, errors in the simulated size distribution
(as shown in Sect. 4.4) could also affect the predicted optical
properties.
We have also compared the simulated AOD with the
AERONET measurements (Fig. 1d) made during the 2-
month simulation period as well as the measurements from
the moving R/V Atlantis platform as shown in Fig. 26. Con-
sistent with the lidar analyses, AOD is usually too high
from the two simulations that employ the MOZART bound-
ary conditions of aerosols (DEF_ANT and 50 %_ANT). The
50 %_LBC simulation produces the AOD that is most con-
sistent with the measurements. Much of the observed tem-
poral variability is reproduced by the model at all the sites,
except at Caltech. It is likely the bias in AOD at the Caltech
site results from the large under-prediction of OA (Fig. 12)
(a) HSRL Extinction 532 nm
1130 1200 1230 1300 1330 1400
0
1
2
3
4
h
e
i
g
h
t

(
k
m

M
S
L
)
(b) DEF_ANT Simulation
1130 1200 1230 1300 1330 1400
0
1
2
3
4
h
e
i
g
h
t

(
k
m

M
S
L
)
(c) 50%_LBC Simulation
1130 1200 1230 1300 1330 1400
0
1
2
3
4
h
e
i
g
h
t

(
k
m

M
S
L
)
(e) AOT,
1130 1200 1230 1300 1330 1400
time (LST)
0.00
0.04
0.08
0.12
0.16
A
O
T
km
-1
0.0 0.2 0.4 0.6 0.8 1.0
0.15
0.36
0.58
0.79
1.00
0.005
0.007
0.009
0.011
0.013
0.015
0.020
0.030
0.050
0.070
0.090
0.110
(d) Extinction Percentiles
0.00 0.03 0.06 0.09
km
-1
0
1
2
3
4
h
e
i
g
h
t

(
k
m

M
S
L
)
observed
DEF_ANT
50%_ANT
0%_ANT
50%_LBC
(f) observed AOT from HSRL
1130 1200 1230 1300 1330 0.0
0.5
1.0
1.5
2.0
1130 1200 1230 1300 1330 0.0
0.5
1.0
1.5
2.0
km
-1
0.0 0.2 0.4 0.6 0.8 1.0
0.15
0.36
0.58
0.79
1.00
0.030
0.040
0.050
0.060
0.070
0.080
0.090
0.100
0.110
0.120
0.130
0.140
Figure 24. (a) Observed extinction along the B-200 aircraft ight on 25 May over southern California and the corresponding simulated
proles from (b) DEF_ANT and (c) 50 %_LBC. (d) Percentiles of extinction as a function of altitude over the entire ight binned for
the observations and DEF_ANT simulation, where vertical lines denote 50th percentiles from the 50 %_ANT, 0 %_ANT, and 50 %_LBC
simulation. (e) Observed and simulated column integrated AOT obtained from the extinction proles along the ight path shown in (f).
and SO
2
4
(Fig. 16) as well as sub-grid scale variability in
emissions and meteorology. While the mean AOD from the
50 %_ANT simulation (0.171) is closer to observed (0.160)
at Caltech, that result is not consistent with the large under-
prediction in surface aerosol concentrations. C. Zhao et
al. (2013) use the WRF-Chem model, the 2008 CARB emis-
sion inventory, and MOZART boundary conditions to simu-
late AOD and aerosol radiative forcing over California dur-
ing 2005. While the model conguration is different than in
this study (i.e., coarser spatial resolution, different trace gas
chemistry, and simpler aerosol model), their simulated AOD
at four AERONET sites were similar to or lower than ob-
served. It is not clear why the performance in simulated AOD
is so different, since both modeling studies use MOZART
to represent long-range transport of aerosols. It is possible
that both global emission inventories (2005 versus 2010)
and long-range transport (different synoptic conditions) con-
tribute to different performance in MOZART over California.
As described by Yu et al. (2012), aerosols (mostly dust)
originating from Asia likely contribute a signicant fraction
of the AOD over the western US and the mass of dust im-
ported from Asia is similar in magnitude to the total primary
particulate emissions over North America. In the 0 %_ANT
simulation, dust from MOZART contributes on average to
5085 % of the total PM
2.5
in the free troposphere over Cal-
ifornia. This study clearly demonstrates that regional-scale
AOD simulations depend on how well global chemical trans-
port models represent the long-range transport of aerosols
from Asia to North America. While there were no large dust
events during our simulation period that might be represented
reasonably well by global models, simulating relatively clean
conditions is important when interpreting the simulated AOD
during CalNex and CARES period. In addition to the treat-
ment of dust emissions, uncertainties in anthropogenic emis-
sions over Asia and how well MOZART represents processes
that affect aerosol lifetime (e.g., chemical aging, wet re-
moval) subsequently affects the boundary conditions used by
the present regional-scale simulation.
(a) HSRL Extinction 532 nm
0830 0900 0930 1000 1030 1100 1130
0
1
2
3
4
h
e
i
g
h
t

(
k
m

M
S
L
)
(b) DEF_ANT Simulation
0830 0900 0930 1000 1030 1100 1130
0
1
2
3
4
h
e
i
g
h
t

(
k
m

M
S
L
)
(c) 50%_LBC Simulation
0830 0900 0930 1000 1030 1100 1130
0
1
2
3
4
h
e
i
g
h
t

(
k
m

M
S
L
)
(e) AOT,
0830 0900 0930 1000 1030 1100 1130
time (LST)
0.00
0.02
0.04
0.06
0.08
0.10
A
O
T
km
-1
0.0 0.2 0.4 0.6 0.8 1.0
0.15
0.36
0.58
0.79
1.00
0.005
0.007
0.009
0.011
0.013
0.015
0.020
0.030
0.050
0.070
0.090
0.110
(d) Extinction Percentiles
0.00 0.02 0.04 0.06
km
-1
0
1
2
3
4
h
e
i
g
h
t

(
k
m

M
S
L
)
observed
DEF_ANT
50%_ANT
0%_ANT
50%_LBC
(f) observed AOT from HSRL
0830 0900 0930 1000 1030 0.0
0.5
1.0
1.5
2.0
0830 0900 0930 1000 1030 0.0
0.5
1.0
1.5
2.0
km
-1
0.0 0.2 0.4 0.6 0.8 1.0
0.15
0.36
0.58
0.79
1.00
0.030
0.035
0.040
0.045
0.050
0.055
0.060
0.065
0.070
0.075
0.080
0.085
Figure 25. (a) Observed extinction along the B-200 aircraft ight in the vicinity of Sacramento on 27 June and the corresponding simulated
proles from (b) DEF_ANT and (c) 50 %_LBC. (d) Percentiles of extinction as a function of altitude over the entire ight binned for
the observations and DEF_ANT simulation, where vertical lines denote 50th percentiles from the 50 %_ANT, 0 %_ANT, and 50 %_LBC
simulation. (e) Observed and simulated column integrated AOT obtained from the extinction proles along the ight path shown in (f).
6 Discussion
To investigate aerosol radiative forcing over California, as
well as other regions, requires that temporal and spatial vari-
ations in aerosol mass, composition, and size be simulated
reasonably well. While the overall performance of the model
in simulating these quantities during the CalNex and CARES
is similar to other studies, there is certainly room for im-
provement. We have presented differences between observed
and simulated quantities that can be attributed to either lo-
cal emissions, sub-grid scale meteorology (particularly at the
Pasadena site), secondary formation processes (mostly from
SOA), long-range transport (mostly dust, but some anthro-
pogenic species as well), or a combination of these uncer-
tainties. To date, only a few aerosol modeling studies have
been conducted using the CalNex and CARES data and brief
comparison of the model performance with those studies is
described next.
Ensberg et al. (2013) evaluated simulated inorganic and
black carbon aerosols from the CMAQ model that used a do-
main encompassing southern California with a grid spacing
of 4 km. Since that study also uses the CARB 2008 emis-
sion inventory, their CMAQ simulation should be most com-
parable to the DEF_ANT simulation. They also found that
simulated BC concentrations were usually higher than ob-
served, with biases between 0.09 to 0.19 g m
3
for ve CIR-
PAS Twin Otter ights and between 0.03 and 0.07 g m
3
for ve WP-3D ights. In this study, biases in BC are be-
tween 0.08 and 0.20 g m
3
for the same ve Twin Otter
ights and between 0.06 and 0.13 g m
3
for the same ve
WP-3D ights (Table S37 in the Supplement). So the model
performance is similar for the Twin Otter ights, but the
present WRF-Chem simulation has a somewhat higher bias
than CMAQ for the WP-3D ights. For inorganics, Ensberg
et al. (2013) report biases in SO
2
4
, NO
3
, and NH
+
4
that
vary between 0.0 to 1.30 g m
3
, 1.47 to 0.31 g m
3
,
and 0.77 to 0.11 g m
3
, respectively among the 10 air-
craft ights. In this study, we obtain biases that vary be-
tween 0.19 to 0.32 g m
3
, 2.22 to 0.75 g m
3
, and
1.03 to 0.12 g m
3
for SO
2
4
, NO
3
, and NH
+
4
, respec-
tively (Tables S39S41 in the Supplement). Biases in SO
2
4
Figure 26. Observed and simulated AOD at 500 nm at the (a) Trinidad Head, (b) Monterey, (c) Caltech, (d) La Jolla, (e) McClellan,
(f) Goldstone, and (g) Table Mountain AERONET sites depicted in Fig. 1d and (h) along the R/V Atlantis transect depicted in Fig. 1a.
Average values over the 2-month period are given to the right of each panel.
from CMAQ were consistently positive, while biases in NO
3
and NH
+
4
were negative. In contrast, the biases in the present
study were both higher and lower than observed for the inor-
ganic aerosols depending on the ight. The different statistics
between the CMAQ and WRF-Chem simulations likely arise
from a number of factors. While the emissions are almost
the same, the models use different treatments for meteorol-
ogy, trace gas chemistry, and aerosols and employ boundary
conditions from different global chemical transport models.
Differences in SO
2
4
are likely due to the lack of aqueous
chemistry and cloudaerosol interactions in this study that
might be important at times in the Los Angeles Basin and
over the adjacent ocean where most of the CIRPAS Twin Ot-
ter measurements were collected.
Knote et al. (2014) also use the WRF-Chem model, with
a similar domain size and resolution as in this study, the
2008 CARB emission inventory, the MOSAIC aerosol model
(but with four size bins), and the same global models for
boundary conditions. Differences in their model congura-
tion with the present study include some of the meteoro-
logical parameterizations, the use of the MOZART photo-
chemical mechanism, SOA treatment, and a shorter simula-
tion period. The simulated diurnal variations in SO
2
4
, NO
3
,
and NH
+
4
concentrations at the four supersites reported in
Knote et al. (2014) are similar to those shown in this study.
There are some differences in simulated NO
3
at the Bak-
erseld and Pasadena sites, and the simulated overall mean
NH
+
4
is higher in Knote et al. (2014) and closer to observed.
These differences are likely due to differences in the trace
gas chemistry between MOZART and SAPRC-99 that will
inuence gas-to-particle partitioning. Not surprisingly, the
largest difference between the two studies is associated with
OA, with consistent over-predictions at the four supersites in
Knote et al. (2014) and consistent under-predictions in this
study. However, simulated average OA in this study is simi-
lar in magnitude to many of the aircraft measurements. Knote
et al. (2014) employ an anthropogenic SOA formation based
on a tracer co-emitted with CO as described by Hodzic and
Jimenez (2011), while the present study uses a VBS approach
described in Shrivastava et al. (2011). Interestingly, simu-
lated OH at the Pasadena site is higher than observed in our
DEF_ANT simulation and is too low in Knote et al. (2014),
showing that different photochemical mechanisms will lead
to different biases in OH that will affect SOA concentrations
to some extent. Since SOA is the largest fraction of OA at
most sites and most times, differences in the treatment of
SOA will have a large impact on simulated PM
2.5
.
It would be useful to compare the different treatments used
in Ensberg et al. (2013) and Knote et al. (2014), as well as
other studies with those used in this investigation to more
fairly compare the performance of trace gas and aerosol treat-
ments when all other processes such as domain congura-
tion, meteorology, emissions, and boundary conditions are
the same. This would also be useful to better identify the ar-
eas of improvement needed in specic processes that affect
the aerosol life cycle. Such a process-oriented methodology
was proposed by Fast et al. (2011) and is worth considering
in the future which can be achieved by merging code into a
single version of WRF-Chem.
It was also useful to examine model performance over all
of California because of the terrain complexity and land-
ocean contrasts that inuences boundary-layer properties and
circulations in the vicinity of major anthropogenic sources.
In general, the magnitude and diurnal and multi-day vari-
ations in OA, SO
2
4
and NH
+
4
were better simulated over
northern California, while NO
3
was better simulated over
southern California. While the temporal and spatial varia-
tions in BC were similar to observed, the simulated concen-
trations were usually too high everywhere using the CARB
2008 emissions. The magnitude was better represented in the
model when BC emissions were reduced by half, suggest-
ing a bias in the emissions inventory. Conversely, compar-
ison of the POA factor determined from PMF analyses of
AMS measurements with the simulated POA suggests that
the CARB 2008 emissions inventory of POA was reason-
able for this period. PMF analyses from the AMS measure-
ments obtained on the G-1, WP-3D, and CIRPAS Twin Otter
(Craven et al., 2013) aircraft are needed to further evaluate
the emissions inventory. Over southern California, the largest
errors in aerosol composition concentrations occurred at the
Pasadena sampling site; however, these errors were smaller
aloft along the aircraft transects in the vicinity of Los An-
geles. The near-surface wind speed bias and the inability of
the model to represent the large wind direction variations at
the Pasadena site (Fig. S2d and e in the Supplement) sug-
gests that sub-grid scale effects associated with the terrain are
inuencing model performance at this site. The model per-
forms better aloft because the aircraft sampled a signicant
portion of the urban plume affected by the larger-scale land-
sea breezes and thermally driven circulations in the basin.
Differences in performance along the aircraft ight paths
(predominately during the day) and at the Pasadena site may
be due to a simulated nighttime boundary layer that is too
shallow, leading to near-surface concentrations of most trace
gases that are too high at night. The model performance is
also better at the other three primary sampling sites because
the local terrain is simpler and the 4 km grid spacing is likely
sufcient to represent the local slope and valley thermally
driven circulations. However, sub-grid scale effects due to
variations in emissions in the vicinity of the T1 site likely
contribute to errors in the relative contribution of anthro-
pogenic and biogenic sources of trace gases and aerosols.
Errors in simulated secondary aerosol formation and aging
processes result from uncertainties in precursor emissions,
missing multigenerational oxidative chemistry for organics,
and model treatments of gas-to-particle partitioning. For ex-
ample, there may be missing sources of SO
2
2
in a portion
of the Los Angeles basin that could contribute to the under-
prediction in SO
2
4
at the Pasadena site. However, we show
that errors in SO
2
4
predictions over northern California are
likely due to relatively small transport errors in space and
time. It is not clear what processes are contributing to the
under-prediction in NO
3
. At the Pasadena site, simulated
NH
3
was too high during most of the day on average sug-
gesting that simulated NO
3
should be too high. Therefore,
the entire nitrogen cycle needs to be examined to determine
whether emissions of other precursor species, such as NO
and NO
2
, are contributing to errors in NO
3
. Unfortunately,
there were no NH
3
and HNO
3
observations over northern
California during CARES (other than a few WP-3D ights
over northern California) to help evaluate the under predic-
tions of NO
3
at the surface and aloft in that region.
It is not surprising that there are errors in simulated
OA concentrations, given that the theoretical understand-
ing of SOA formation and chemical processing is incom-
plete. When the model does simulate reasonable OA con-
centrations, it may be for the wrong reasons. OA under-
predictions in the current model may be due to missing
important interactions associated with anthropogenic emis-
sions inuencing biogenic SOA (e.g., Carlton et al., 2010)
or using lower yields that neglect multigenerational biogenic
chemistry (Shrivastava et al., 2011) which were shown to
be important on some days during CARES (Shilling et al.,
2013; Setyan et al., 2012). In addition, the current model
does not include contributions of glyoxal chemistry that was
shown by Knote et al. (2014) to potentially produce up to
15 % more SOA in the vicinity of the Los Angeles basin.
Biomass burning was a source of trace gases and aerosols
neglected in this study. While relatively few res were ob-
served in California by satellite detection methods during
the 2-month period, biomass-burning aerosols from a large
number of small, undetectable res could contribute to the
background concentrations of OA and BC. Analyses of the
mass spectra fromsingle particle measurements (Cahill et al.,
2012) indicate that a substantial fraction of aerosols could
be associated with biomass burning; however, the analyses
cannot determine whether they are due to local or distant
sources and there can be confounding factors that lead to
overestimation of biomass burning particles with single par-
ticle measurements (Hayes et al., 2013; Aiken et al., 2010).
In our study, biomass burning from long-rang transport is
included through the boundary conditions, but the current
MOZART conguration does not differentiate OA anthro-
pogenic, biomass burning, or biogenic sources. Another issue
is that MOZART likely underestimates SOA severely (Dun-
lea et al., 2009; Emmons et al., 2010), which inuences the
WRF-Chem boundary conditions of OA. We acknowledge
that reducing the anthropogenic emission rates by 50 % is ar-
bitrary, but some adjustment is needed to account for likely
reductions in emissions over time in California.
Considering that the current theoretical understanding of
SOA formation and transformation processes is highly un-
certain (e.g., Jimenez et al., 2009), errors in the treatment
of organic aerosol processes in models are expected (e.g.,
Volkamer et al., 2006; Hodzic et al., 2010). New insights
from recent laboratory and eld data (e.g., Perraud et al.,
2012; Vaden et al. 2011; Virtanen et al. 2010) as well as
explicit modeling studies (e.g., Lee-Taylor et al., 2011) that
identify important organic chemical reactions, examine the
role of semi- and intermediate volatile organic compounds,
and quantify phase and volatility of SOA will likely provide
improved modeling frameworks. Still unaccounted removal
processes of organic vapors that are in equilibrium with SOA
may also signicantly affect SOA concentrations (Hodzic et
al., 2013). The results of simulated OA using a revised VBS
framework that includes new ndings on volatility and frag-
mentation (Shrivastava et al., 2013) will be presented in a
subsequent study.
We demonstrated that evaluating predictions with only sur-
face aerosol concentrations is insufcient in terms of under-
standing uncertainties contributing to column optical prop-
erties that affect aerosol radiative forcing. It would have
been difcult, if not impossible, to ascertain errors associ-
ated with simulated aerosols originating outside of the Cali-
fornia region without the extensive aircraft and remote sens-
ing measurements available during CalNex and CARES. The
regional sampling from the HSRL-1 on the B-200 aircraft
was the most valuable measurement to quantify the over-
prediction in aerosols in the free troposphere. Even though
the simulated concentrations were relatively small in the free
troposphere compared to boundary layer concentrations, the
vertically integrated effect was large enough to affect predic-
tions of AOD that will affect shortwave radiation reaching
the surface. The in situ measurements also provided some
evidence of over-predictions in the free troposphere for tran-
sects upwind of urban emission sources; however, the lidar
provides more complete information on aerosol loading and
extinction in the vertical column than could possibly be ob-
tained from in situ sampling. In addition, the in situ measure-
ments do not provide information for all aerosol components
or coarse aerosols (>1 m). Kassianov et al. (2012) showed
that coarse particles often contributed more than 50 % of the
total observed aerosol volume during CARES and that even
during clean conditions those coarse particles contribute sig-
nicantly to direct aerosol radiative forcing. Yu et al. (2012)
used satellite measurements averaged over multiple years to
show that dust contributes a large fraction of the AOD over
the northern Pacic Ocean. Additional analyses of single par-
ticle measurements (e.g., Laskin et al., 2012; Moffet et al.,
2013; Vaden et al., 2011) coupled with size distribution in-
formation are needed to fully evaluate the simulated dust and
sea-salt aerosol.
While no eld campaign can provide measurements to
evaluate every aspect of an aerosol model, the extensive me-
teorological, trace gas, and aerosol measurements collected
during CalNex and CARES is the most comprehensive data
set currently available for the western US. It is particularly
useful to assess the strengths and weaknesses of current and
new treatments of SOA because of the proximity of both an-
thropogenic and biogenic precursors, the complexity of me-
teorology that will inuence aerosol formation, growth, and
removal, and the use of state-of-the-science instrumentation
to provide data on organic gases and aerosols.
7 Summary and conclusion
This study integrated the wide range of meteorological,
chemistry, and aerosol data collected during the CARES and
CalNex eld campaigns and by operational monitoring net-
works into a single publicly available data set for the Aerosol
Modeling Testbed. The AMT was used to comprehensively
evaluate the performance of one conguration of the WRF-
Chem model to simulate aerosols and their precursors over
California between May and June of 2010. We also assessed
the sensitivity of the aerosol predictions to uncertainties as-
sociated with the emission inventories and boundary con-
ditions. Independent measurements showed that the model
captured the overall meteorological conditions as reected
in simulated temperature, humidity, cloudiness, circulations,
and boundary layer depth. Any errors in the meteorological
quantities are consistent with those typically seen in other
other mesoscale modeling studies.
The main ndings of this modeling study are the follow-
ing.
Reducing the 2008 CARB emissions inventory by 50 %
improved simulated CO, NO
x
, and anthropogenic hy-
drocarbons such as toluene and formaldehyde at most
sites and along most aircraft ight paths.
Reducing anthropogenic emission rates led to reduc-
tions in mixing ratios of isoprene and terpene when
biogenic emissions rates remained the same. It is pos-
sible that there are uncertainties in biogenic emissions
from the on-line MEGAN model used in WRF-Chem,
but uncertainties in these emissions are also coupled
to interactions with anthropogenic sources that affect
the oxidation capacity of the atmosphere, as shown by
comparing the simulations with and without anthro-
pogenic emissions. Isoprene mixing ratios were usually
too low in the simulations that employed anthropogenic
emissions, except at the Bakerseld site and along the
WP-3D ights north of 35
N where the simulated val-

ues were similar to observations.
Simulated spatial and temporal variability in BC was
qualitatively similar to surface and aircraft measure-
ments when emissions of BC are reduced by 50 %.
While the spatial and temporal variability of OA is sim-
ulated reasonably well, the magnitude is generally too
low, particularly at the Pasadena site. In contrast with
other adjustments to the emissions, comparisons with
PMF results suggest that the original POA emission es-
timates may be reasonable.
Simulated SO
2
4
was too low in southern California, but
the magnitude as well as the diurnal and multi-day vari-
ability was better represented over northern California.
Simulated NO
3
was too low everywhere, but the mag-
nitude as well as the diurnal and multi-day variability
was better represented over southern California.
Long-range transport of aerosols simulated by the
global model was likely too high in the free troposphere
even though their concentrations were relatively low.
In addition, the sensitivity simulation that removed an-
thropogenic emissions suggest that CO from long-range
transport might be up to 20 ppb too high.
The bias in aerosols in the free troposphere leads to
over-predictions in AOD by about a factor of 2, and
offsets the effect of the under-predictions of boundary-
layer aerosols resulting primarily from local emissions.
Reducing aerosol concentrations by half from long-
range transport greatly improves the simulated AOD in
all regions of California.
Our long-term objectives are to use WRF-Chem to quan-
tify regional-scale variations in aerosol radiative forcing over
California and determine the relative role of emissions from
local and distant sources. This study was a necessary rst
step that rigorously evaluates simulated aerosol mass, com-
position, and size distribution. These properties inuence
the models treatment of optical properties and consequently
aerosol radiative forcing. While this study does not exten-
sively examine all simulated aerosol optical properties, we
evaluated simulated AOD and extinction proles to check for
consistency with simulated aerosol concentrations. Our eval-
uation using measurements from in situ and remote instru-
mentation deployed on the surface, aircraft, and ship plat-
forms shows that simulated mass and composition both at
the surface and aloft needs improvement to better represent
AOD and extinction proles and to have condence in cal-
culations of aerosol radiative forcing during the CalNex and
CARES periods as well as other time periods. In addition, an
evaluation of the simulated single scattering albedo and other
optical properties is needed.
The extensive data collected during CalNEX and CARES
provide a valuable opportunity to make sure that aerosol op-
tical properties are simulated adequately for the correct rea-
sons. The combined eld campaign and operational data pro-
vide an ideal test bed to evaluate aerosol models in more de-
tail and develop improved treatments for aerosol processes.
Simulating SOA is particularly important since it is often the
largest fraction of observed ne mode aerosol mass. New
particle formation events were observed during CARES (Za-
veri et al., 2012; Setyan et al., 2014) and CalNex (Alm et al.,
2012; Pennington et al., 2012) and better representing the
growth of aerosols could affect the overall mass and num-
ber in the region. Some studies are beginning to explore the
role of mixing state on aerosol optical properties and cloud
condensation nuclei (e.g., Zhang et al., 2014; Matsui et al.,
2013), which could be important at regional spatial scales.
These challenging issues will be explored in forthcoming
studies using the CalNex and CARES test bed.
The Supplement related to this article is available online
at doi:10.5194/acp-14-10013-2014-supplement.
Acknowledgements. We thank the numerous scientists (including
R. Cohen, A. Goldstein, J. de Gouw, T. Ryerson, I. Pollack, and
C. Warneke), pilots, and other staff that contributed to the data
collection during CalNex and CARES. CalNex was sponsored
by the National Oceanographic and Atmospheric Administration
(NOAA) Climate Change and Air Quality programs, the National
Aeronautics and Space Administration (NASA) Radiation Sciences
and Tropospheric Chemistry program, and the California Air
Resources Board. CARES was supported by the US Department
of Energys (DOE) Atmospheric Radiation Measurement (ARM)
and Atmospheric System Research (ASR) programs. Patrick
Hayes and Jose Jimenez were partially supported by CARB
11-305 and DOE (BER/ASR) DE-SC0006035 and Patrick Hayes
was also partially supported by a CIRES Visiting Postdoctoral
Fellowship. We thank Elaine Chapman for providing comments on
this manuscript. Funding for this research has been provided by
the US NOAAs Atmospheric Composition and Climate Program
(NA11OAR4310160) and DOEs ASR program and utilized
resources provided by the Pacic Northwest National Laboratory
(PNNL) Institutional Computing program. PNNL is operated
for the US DOE by Battelle Memorial Institute under contract
DE-AC05-76RL01830.
Edited by: G. McFiggans
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Author(s) 2014. CC Attribution 3.0 License.
Supplement of
Modeling regional aerosol and aerosol precursor variability over
California and its sensitivity to emissions and long-range transport
during the 2010 CalNex and CARES campaigns
J. D. Fast et al.
Correspondence to: J. D. Fast (jerome.fast@pnnl.gov)

This supplement contains additional tables and figures that summarize model
performance at surface sampling sites and along aircraft flight paths and ship tracks. Statistical
metrics in the tables include the bias, root-mean-square error (RMSE), correlation coefficient (R),
and index of agreement (IA) for various meteorological, trace gas, and aerosol quantities.

Aerosol Modeling Testbed
The extensive data collected during CalNex and CARES are an ideal testbed for
evaluating photochemical and aerosol models; therefore, they have been merged into a single
dataset used by the Aerosol Modeling Testbed (AMT). The AMT [Fast et al., 2011] consists of a
host model, testbed cases, and post-processing software. The host model is the Weather Research
and Forecasting (WRF-Chem) community model [Skamarock et al., 2005] that permits on-line
coupling of meteorology and chemistry [Grell et al., 2005; Fast et al., 2006]. Since detailed
measurements of aerosol properties are not routinely collected aloft, the AMT uses
meteorological, trace gas, and aerosol measurements from field campaigns to define each testbed
case. The analysis software extracts simulated variables in a manner compatible with the
available measurements using instrument simulators. Examples of instrument simulators
include the interpolation of model output in space and in time along research aircraft flight tracks
and over vertical profiles sampled by radar wind profilers and lidars. Statistical and graphical
programs are also available in the analysis software. While the AMT has been designed for use
with WRF, the analysis software can be modified for other models. For example, Ensberg et al.
[2013] used the AMT software coupled with the Community Multiscale Air Quality (CMAQ)
modeling system to evaluate simulated aerosol concentration and composition in the Los Angeles
Basin using the CalNex CIRPAS Twin Otter measurements.
The field campaign and operational data used for the CalNex/CARES testbed case have
been provided through several archives with a variety of formats (e.g. ASCII, ICARTT, NetCDF,
HDF, Microsoft Excel). Modelers need to write software that handles the variety of formats,
which usually changes from field campaign to field campaign. Inevitably, each user that
processes the same field dataset creates different software scripts or programs. As part of the
AMT, a common ASCII format is employed for most of the data and data has been organized into
common types including surface, aircraft, profile, and satellite. Subdirectories are created for
each supersite or operational network in the case of surface instrumentation, and for each research
aircraft in the case of airborne sampling. The directory structure for the AMT CalNex/CARES
testbed case is given in Fig. S1. Some of the sub-directories contain data exclusively from
CalNex or CARES, while other sub-directories contain data from both campaigns, e.g., in the
case of instrument platforms participating in both, such as the B-200 and NOAA Twin Otter
aircraft. In addition to data from the radiosonde, radar wind profiler, CARB, IMPROVE,
AERONET networks, satellite measurements of aerosol optical depth from the Moderate
Resolution Imaging Spectroradiometer (MODIS) on the Aqua and Terra satellites are also
included in the testbed case. An identical directory structure is employed for model output
extracted to be temporally and spatially compatible with the measurements, enabling graphics and
statistics to evaluate model performance. In this way, the AMT permits users to spend more time
on science issues (rather than on tedious and repetitive tasks associated with data processing),
target specific aerosol processes and other atmospheric processes affecting aerosol evolution, and
document improvements in parameterizations.
The testbed case containing the CARES and operational data as well as the analysis
toolkit software is available to download from the Atmospheric Radiation Measurement (ARM)
research climate facility archive at http://www.arm.gov/data/eval/59. Users are encouraged to
contact Jerome Fast (Jerome.Fast@pnnl.gov) for an updated version of the dataset.

Evaluation of Meteorological Quantities
Since the current model configuration is somewhat different than previous studies
[Angevine et al., 2012; Fast et al., 2012], some comparisons of observed and simulated
temperature, humidity, wind speed and direction, and solar radiation from the DEF_ANT
simulation are presented here to demonstrate the performance of the model in representing the
meteorological conditions that affect the vertical mixing, transport, chemical transformation, and
removal of trace gases and aerosols.
An example of the simulated surface meteorology at the Pasadena supersite over May
and June of 2010 as well as the diurnal averages is shown in Fig. S2. The model is able to
reproduce the multi-day variability of temperature and relative humidity although the simulated
nighttime temperatures are a few degrees warmer than observed and the relative humidity is
generally 10% lower than observed at all times of the day. As seen in the solar radiation, the
mostly sunny conditions occurred on the majority of the days. While the model correctly
produces clouds on some days when they occurred (May 17 18, June 8-9, the overall reduction
in downward shortwave radiation due to clouds is less than observed suggesting that the
simulated liquid or ice water path is too low. The near-surface winds at Pasadena exhibit nearly
the same diurnal variation from day to day, with southwesterly winds during the day that become
weaker and southerly to southeasterly at night. While the model reproduces the diurnal
variability in wind direction, the predicted wind speeds are too high. The over-prediction in wind
speeds is likely due to two factors: 1) urban canopy effects that are not included in the current
model configuration of the model, and 2) sub-grid scale terrain effects since the site is located
near the edge of the San Gabriel Mountains. The performance of near surface winds is usually
better at other stations located outside of urban areas and/or in flat terrain (not shown).
Table 4 summaries statistics that quantify model performance for the simulated near-
surface temperature, relative humidity, wind speed, and wind direction average over California
and averaged over smaller geographic regions depicted in Fig. 1c. As with the Pasadena site,
simulated temperatures are usually 0.2 to 0.9 K too low and the diurnal and multi-day temporal
variations are similar to observations. Relatively humidity is usually lower than observed by 5.5
to 7.0% over the San Joaquin Valley and southern California, but is generally within 1% of the
observations on average elsewhere. Simulated near surface wind speeds are usually higher than
observed with the largest biases for stations in the coastal region. The average bias in wind
direction is less than 10 degrees for the San Joaquin Valley, Sacramento Valley, and coastal
regions, but between 17.6 and 22.5 degrees over southern California and the interior mountains.
While the model qualitatively captures the diurnal and multi-day variability in wind direction, it
is not surprising that it cannot represent the high frequency variations especially when wind speed
are low (< 1 m s
-1
) as shown in Fig. S2e. This is the primary reason for the low wind direction
correlations in Table 4.
Statistics summarizing the performance in simulated temperature, relative humidity, wind
speed, and wind direction for all of the G-1, CIRPAS Twin Otter, and WP-3D flight paths and the
R/V Atlantis deployment are shown in Table 5. In general, the spatial and temporal variability in
temperature in the lower troposphere is reasonably simulated as reflected by the relatively high
correlation coefficients that are similar to the surface measurements; however, the model is 2 to 3
degrees colder than observed on average. Conversely, the near surface temperatures over the
ocean are about 1 degree warmer on average than those from the R/V Atlantis. The relative
humidity statistics are similar to those at the surface measurement sites with the model being 4 to
7% drier than observed, except along the G-1 flight paths that had a very small bias. The wind
speeds aloft along the G-1 and WP-3D flight paths are very similar to observed and consequently
the errors are much smaller than at the surface measurement sites. Nevertheless, the correlation
coefficients indicate that the model did not represent all of the spatial and temporal variability in
wind speed. Wind speed variability is better represented over southern California where the WP-
3D usually flew than over northern California where the G-1 flew. Statistics for individual
aircraft flights and daily statistics for the R/V Atlantis sampling are given in Tables S1 S14.
It is also important to evaluate the evolving simulated winds throughout the boundary
layer and lower troposphere when assessing the ability of a model to simulate horizontal transport
downwind of emissions sources; therefore the simulated winds aloft have been evaluated with
measurements from the radar wind profiler network shown in Fig. 1c. While Fast et al. [2012]
demonstrated that the observed and simulated wind speed and direction, associated with varying
synoptic conditions and thermally-driven flows, was similar in the vicinity of Sacramento during
June, this study quantifies model performance over all of California for May and June. Statistics
that summarize the model performance at all the radar wind profiler sites at three altitudes are
given in Tables 6 and 7. The performance varies among the sites and with altitude as expected.
Figure S3 shows the observed and simulated diurnally-averaged winds over May and June of
2010 at the Sacramento, Bakersfield, and USC radar wind profilers based on the time series
shown in Fig. S4. The simulated wind speed and direction at Sacramento (Fig. S2a) is very close
to observed, except for a few periods during the night that differ by as much as 30 degrees. Both
the observed and simulated winds at Bakersfield are usually northwesterly all day (Fig S2b), but
the model overestimates the wind speeds at night. Low-level jets frequently occur in the San
Joaquin Valley, but the simulated wind speeds are too strong on some nights consistent with Bao
et al. [2008] in their WRF simulation of winds during the Central California Ozone Study. At
USC (Fig. S2c), the model reproduces the overall diurnal variation in wind speed and direction at
this altitude, but the wind speeds are generally 1-2 m s
-1
higher than observed during the night
and early morning and the simulated wind directions are more westerly than observed. When
comparing Fig. S2d and Fig. S4c, the daytime wind speed bias decreases significantly with
height, but the bias at night is similar at both altitudes.
Boundary-layer depth is an important meteorological quantity, since it defines the vertical
extent of turbulent mixing that dilutes the concentrations of near-surface trace gases and aerosols
and alters chemical transformation. The performance of the model in simulated boundary-layer
depth compared with the radiosondes collected at the T0 and T1 sites is nearly identical to Fast et
al. [2012] and is not included here. Scarino et al. [2013] present a methodology of deriving
boundary layer heights from backscatter profiles measured by the HRSL on the B-200 aircraft.
An advantage of this data set is that the simulated spatial and temporal variability in boundary
layer height can be evaluated, as opposed to comparing model predictions to infrequent soundings
made at a few locations. Scarino et al. [2013] use the results from the DEF_ANT simulation to
show that the simulated spatial and temporal variations in boundary layer depths are usually
similar to those derived along the B-200 aircraft flight paths. Statistics that summarize the model
performance during the day also show that the model boundary layer depths are somewhat too
low over southern California during the CalNex flights, but are closer to observed over northern
California during the CARES flights.

Table S1. Performance of simulated temperature (T) in terms of bias, RMSE, R, and IA for the
individual G-1 aircraft flight paths.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
T (K)
June 03a 849 292.0 -2.9 3.1 0.96 0.69
June 06a 1164 296.3 -4.0 4.3 0.39 0.33
June 06b 989 296.1 -4.5 4.7 0.97 0.85
June 08a 1170 293.2 -2.4 3.3 0.27 0.47
June 08b 1213 292.7 -5.0 5.5 0.95 0.73
June 10a 1113 290.0 -1.7 2.2 0.93 0.91
June 12a 1093 293.8 -2.7 3.3 0.67 0.63
June 12b 1001 298.0 -1.7 2.2 0.90 0.85
June 14a 1168 296.6 -1.7 2.3 0.73 0.75
June 15a 1103 290.2 -1.1 2.2 0.05 0.42
June 15b 1116 292.1 -3.8 5.1 0.94 0.82
June 18a 1164 293.2 -0.2 2.5 0.93 0.96
June 19a 1120 290.9 -2.3 3.2 0.90 0.83
June 21a 1130 291.8 -2.0 2.8 -0.17 0.38
June 21b 1126 296.6 -2.7 3.0 0.98 0.95
June 23a 1180 292.6 -2.4 3.8 0.90 0.85
June 23b 1106 296.1 -3.2 4.5 0.93 0.87
June 24a 1173 292.3 1.4 3.6 -0.12 0.34
June 24b 1034 294.7 -3.7 5.0 0.92 0.76
June 27a 1215 298.7 -1.7 2.2 0.80 0.79
June 28a 1139 301.3 -2.5 2.9 0.85 0.74
June 28b 847 306.0 -0.9 2.3 0.88 0.89

Table S2. Performance of simulated relative humidity (RH) in terms of bias, RMSE, R, and IA
for the individual G-1 aircraft flight paths.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
RH (%)
June 03a 849 60.2 7.2 10.9 0.22 0.47
June 06a 1117 55.5 6.9 9.1 0.23 0.42
June 06b 988 41.3 10.4 18.8 -0.20 0.23
June 08a 1170 56.3 3.9 9.4 0.55 0.70
June 08b 1212 40.1 -1.8 19.4 0.20 0.49
June 10a 1111 38.9 1.2 12.0 0.18 0.51
June 12a 1093 28.2 -1.8 5.3 -0.16 0.26
June 12b 991 25.5 2.3 4.7 0.56 0.67
June 14a 1168 32.2 2.6 9.6 0.54 0.70
June 15a 1103 55.4 2.5 13.3 0.71 0.79
June 15b 1115 42.4 -4.0 20.7 0.24 0.44
June 18a 1142 25.2 -5.1 10.5 0.68 0.77
June 19a 1097 39.3 2.7 11.8 0.35 0.60
June 21a 1130 43.4 -5.1 8.2 0.56 0.65
June 21b 1126 21.4 2.0 6.6 0.63 0.78
June 23a 1180 40.5 -6.2 15.3 0.28 0.56
June 23b 1077 30.5 0.7 14.4 -0.01 0.42
June 24a 1173 44.3 -5.5 18.6 -0.08 0.35
June 24b 1005 37.3 1.4 13.7 0.13 0.42
June 27a 1215 41.4 -9.6 16.0 0.37 0.59
June 28a 1136 38.3 2.2 7.9 0.51 0.71
June 28b 843 25.2 -0.4 4.9 0.58 0.73

Table S3. Performance of simulated wind speed (WS) in terms of bias, RMSE, R, and IA for
the individual G-1 aircraft flight paths.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
WS (m s
-1
)
June 03a 849 7.0 -1.3 3.3 -0.16 0.35
June 06a 1117 3.5 -0.2 1.8 -0.01 0.36
June 06b 989 6.1 -0.4 2.6 0.81 0.90
June 08a 1170 3.8 -1.2 2.3 0.23 0.52
June 08b 1213 5.3 -0.2 1.9 0.60 0.77
June 10a 1112 8.0 0.5 1.8 0.55 0.70
June 12a 1093 11.0 0.1 4.1 0.53 0.66
June 12b 1001 9.8 -1.6 3.9 -0.15 0.27
June 14a 1168 4.5 0.1 3.2 -0.23 0.27
June 15a 1103 4.6 1.0 2.5 0.17 0.49
June 15b 1115 5.5 0.8 2.6 0.54 0.70
June 18a 1142 6.3 -2.0 3.6 0.23 0.50
June 19a 1097 5.7 -0.5 2.1 -0.01 0.39
June 21a 1130 4.5 2.7 4.3 0.60 0.66
June 21b 1060 6.1 -2.0 12.3 0.06 0.11
June 23a 1180 3.5 0.1 2.6 0.55 0.67
June 23b 1077 3.9 0.8 2.6 0.35 0.56
June 24a 1173 5.8 -2.0 3.4 0.37 0.57
June 24b 1005 4.9 1.5 2.8 -0.06 0.32
June 27a 1215 2.4 -0.2 1.9 -0.14 0.30
June 28a 1136 2.8 -0.2 2.7 0.14 0.45
June 28b 843 4.3 -1.2 2.4 -0.01 0.42

Table S4. Performance of simulated wind direction (WD) in terms of bias, RMSE, R, and IA
for the individual G-1 aircraft flight paths.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
WD ()
June 03a 849 225.0 31.1 41.3 0.41 0.50
June 06a 1117 255.0 1.0 48.3 0.21 0.55
June 06b 989 255.0 27.4 47.8 0.28 0.51
June 08a 1170 165.0 45.8 83.7 0.31 0.64
June 08b 1213 195.0 4.5 39.2 0.01 0.39
June 10a 1112 315.0 -0.2 18.3 -0.03 0.55
June 12a 1093 345.0 21.9 34.8 0.42 0.99
June 12b 1001 315.0 15.6 26.7 0.08 0.75
June 14a 1168 195.0 15.2 63.2 0.12 0.50
June 15a 1103 195.0 4.9 40.4 0.61 0.79
June 15b 1115 195.0 8.3 31.2 0.25 0.54
June 18a 1142 315.0 16.2 51.8 0.71 0.78
June 19a 1097 195.0 3.7 20.2 0.55 0.73
June 21a 1130 345.0 2.2 62.8 0.57 0.83
June 21b 1060 285.0 -6.4 40.5 0.07 0.89
June 23a 1180 165.0 2.5 72.7 -0.11 0.69
June 23b 1077 255.0 -0.4 53.8 0.17 0.49
June 24a 1173 165.0 27.6 49.9 0.58 0.72
June 24b 1005 165.0 -5.7 39.1 0.30 0.51
June 27a 1215 285.0 12.2 100.3 -0.09 0.75
June 28a 1136 255.0 -49.2 108.2 -0.12 0.59
June 28b 843 255.0 45.1 70.5 -0.08 0.47

individual WP-3D aircraft flight paths.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
T (K)
May 04 17219 287.5 -4.7 6.0 0.88 0.85
May 07 24839 288.3 -5.5 6.4 0.90 0.84
May 08 25439 286.6 -3.6 5.1 0.87 0.86
May 11 25799 275.8 -5.2 6.1 0.97 0.95
May 12 27489 285.1 -4.7 6.9 0.91 0.89
May 14 22259 285.6 -0.4 3.9 0.87 0.93
May 16 27899 286.5 -2.8 4.4 0.87 0.89
May19 24239 287.0 -3.2 4.8 0.86 0.87
May 21 10722 286.8 0.4 1.5 0.82 0.89
May 24 22619 283.4 -1.2 2.5 0.98 0.98
May 30 20879 293.5 -0.7 2.3 0.87 0.92
May 31 21278 292.3 -0.2 3.8 0.75 0.85
June 02 22259 287.1 0.8 2.8 0.71 0.82
June 03 24179 290.8 0.0 4.0 0.70 0.77
June 14 26459 289.0 -3.5 4.5 0.97 0.97
June 16 24899 289.7 -3.3 4.8 0.84 0.85
June 18 25499 288.6 -2.0 3.6 0.88 0.91
June 20 25619 290.6 -3.2 4.9 0.70 0.76
June 22 22679 287.3 -9.6 10.1 0.92 0.74

for the individual WP-3D aircraft flight paths.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
RH (%)
May 04 17219 22.5 -7.4 13.6 0.72 0.73
May 07 24839 25.8 4.3 12.1 0.18 0.49
May 08 25439 30.2 -0.9 15.1 0.72 0.83
May 11 25799 39.4 6.5 19.2 0.67 0.79
May 12 27489 41.6 1.4 21.4 0.51 0.71
May 14 22259 49.3 -10.6 24.8 0.50 0.61
May 16 27899 51.9 -6.2 19.4 0.81 0.89
May19 24239 44.2 -14.6 21.3 0.58 0.64
May 21 10722 40.5 -6.4 17.5 0.83 0.90
May 24 22619 39.5 -6.6 16.3 0.36 0.59
May 30 20879 21.7 -4.0 11.7 0.78 0.76
May 31 21278 27.3 -10.1 19.9 0.57 0.58
June 02 22259 59.6 -12.2 20.2 0.41 0.57
June 03 24179 51.2 -8.7 18.6 0.73 0.64
June 14 26459 30.1 5.3 13.8 0.70 0.82
June 16 24899 38.1 -1.6 18.2 0.70 0.83
June 18 25499 41.5 0.3 14.7 0.84 0.92
June 20 25619 35.6 -10.1 17.4 0.82 0.81
June 22 22679 16.8 -0.7 8.8 0.18 0.47

Table S7. Performance of wind speed (WS) in terms of bias, RMSE, R, and IA for the

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
WS (m s
-1
)
May 04 17219 4.9 1.5 3.3 0.35 0.61
May 07 24839 4.5 0.5 2.6 0.81 0.89
May 08 25439 7.9 0.1 3.6 0.76 0.87
May 11 25799 11.0 2.3 7.6 0.85 0.86
May 12 25289 7.3 0.3 6.3 0.49 0.62
May 14 22259 3.1 -0.3 2.3 0.23 0.55
May 16 27899 5.1 -1.7 3.1 0.44 0.60
May19 24239 8.4 -1.4 4.8 0.67 0.79
May 21 10722 10.4 1.6 3.9 0.83 0.90
May 24 22619 6.2 -1.7 3.1 0.61 0.70
May 30 20879 5.5 0.2 3.6 0.11 0.45
May 31 21278 4.1 1.1 3.8 0.11 0.48
June 02 22259 3.4 1.1 3.7 0.13 0.47
June 03 24179 3.3 0.5 2.7 0.39 0.62
June 14 26459 7.4 -1.7 3.3 0.73 0.81
June 16 24899 7.6 -0.3 3.1 0.79 0.88
June 18 25499 7.8 -1.8 3.8 0.75 0.83
June 20 25619 4.8 0.4 2.6 0.64 0.79
June 22 22679 6.5 -1.9 3.8 0.70 0.77
June 20 25619 255.0 24.4 70.5 0.34 0.61
June 22 22679 225.0 14.4 65.7 0.30 0.78

Table S8. Performance of wind direction (WD) in terms of bias, RMSE, R, and IA for the

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
WD ()
May 04 17219 285.0 7.5 53.1 0.09 0.57
May 07 24839 345.0 -10.3 76.4 0.16 0.81
May 08 25439 255.0 -1.7 53.4 0.20 0.49
May 11 25799 345.0 1.3 40.1 0.11 0.85
May 12 25289 315.0 -2.4 62.4 0.04 0.48
May 14 22259 255.0 20.6 99.2 -0.11 0.73
May 16 27899 285.0 -24.6 95.2 -0.02 0.57
May19 24239 345.0 1.9 74.8 0.29 0.68
May 21 10722 315.0 -1.1 35.0 0.26 0.52
May 24 22619 315.0 -24.1 38.0 0.34 0.64
May 30 20879 285.0 -2.1 66.1 0.42 0.90
May 31 21278 315.0 -18.1 87.3 0.12 0.70
June 02 22259 285.0 -11.8 84.2 0.23 0.84
June 03 24179 345.0 -10.1 84.3 0.17 0.84
June 14 26459 255.0 -16.8 57.6 0.51 0.84
June 16 24899 315.0 -7.5 39.2 0.28 0.80
June 18 25499 255.0 -3.2 47.0 0.57 0.83
individual CIRPAS Twin Otter aircraft flight paths.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
T (K)
May 04 187 293.7 -2.3 3.5 0.14 0.40
May 05 228 291.8 -2.0 3.6 -0.09 0.33
May 06 179 290.0 -2.0 2.6 0.17 0.46
May 07 194 294.9 -3.6 5.0 0.09 0.32
May 10 182 286.7 -1.1 2.4 0.48 0.54
May 12 195 291.9 -4.8 5.5 0.67 0.54
May 13 174 294.3 -2.3 3.6 0.76 0.80
May14 189 289.5 0.4 1.5 0.68 0.77
May 15 185 292.2 -1.7 2.7 0.72 0.74
May 18 183 283.6 -2.5 3.5 0.96 0.93
May 19 192 290.6 -1.1 2.1 0.37 0.54
May 20 192 288.0 -4.6 5.3 0.85 0.74
May 21 192 288.7 -2.4 3.0 0.58 0.63
May 22 195 279.1 -4.3 4.7 0.95 0.87
May 24 189 285.8 -5.7 6.7 0.87 0.76
May 25 191 289.8 -5.7 6.5 0.81 0.63
May 27 176 287.9 -3.4 4.1 0.28 0.32
May 28 192 288.1 -4.2 4.7 0.38 0.27

for the individual CIRPAS Twin Otter aircraft flight paths.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
RH (%)
May 04 187 40.1 -10.1 12.1 0.87 0.78
May 05 228 51.9 -16.2 19.0 0.78 0.67
May 06 178 57.4 -17.2 41.4 0.29 0.37
May 07 194 36.0 -9.3 20.8 0.57 0.61
May 10 182 61.6 4.8 13.0 -0.12 0.27
May 12 195 35.9 6.7 11.7 0.85 0.88
May 13 174 31.8 -3.6 10.1 0.79 0.82
May14 189 65.1 -18.2 22.2 0.67 0.55
May 15 185 57.3 -12.7 18.3 0.71 0.75
May 18 183 48.5 -1.8 14.6 0.90 0.90
May 19 192 64.8 -18.2 21.9 0.62 0.51
May 20 192 38.9 6.4 22.5 0.78 0.82
May 21 192 64.3 -18.5 26.4 0.56 0.63
May 22 194 38.2 1.7 25.9 0.46 0.68
May 24 189 35.9 4.2 13.0 0.73 0.85
May 25 191 38.5 0.1 11.1 0.72 0.85
May 27 176 66.1 7.3 15.6 -0.29 0.13
May 28 192 54.9 -6.9 12.4 0.68 0.68

R/V Atlantis paths by day.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
T (K)
May 14 359 287.6 -1.9 2.0 0.03 0.17
May 15 1409 286.6 0.6 1.3 -0.43 0.11
May 16 1424 285.9 1.6 1.7 0.25 0.35
May 17 1433 285.0 0.8 1.0 0.12 0.46
May 18 1413 285.7 0.7 1.0 0.35 0.53
May 19 1427 286.8 0.5 0.9 -0.57 0.31
May 20 1439 288.0 -0.1 1.9 0.43 0.62
May 21 1433 288.1 1.6 2.7 -0.23 0.12
May 22 1417 288.4 1.5 2.1 0.12 0.47
May 23 1440 286.1 1.1 1.3 0.48 0.51
May 24 1429 286.2 0.7 0.9 -0.07 0.44
May 25 1440 286.0 0.9 1.2 -0.17 0.44
May 26 1440 288.2 -0.5 1.1 0.90 0.89
May 27 1440 288.6 0.4 1.4 0.51 0.70
May 28 1440 287.8 0.8 1.5 0.46 0.59
May 29 1440 287.5 0.6 1.4 0.24 0.45
May 30 1434 288.9 1.6 3.3 0.11 0.34
May 31 1432 287.1 3.7 4.8 -0.18 0.12
June 01 1440 285.1 1.6 1.7 0.67 0.45
June 02 1440 285.0 0.5 1.4 0.29 0.48
June 03 1440 291.2 3.8 4.5 0.79 0.74
June 04 1440 293.4 0.2 2.8 -0.30 0.12
June 05 1440 294.1 -2.3 5.2 -0.66 0.31
June 06 1440 290.6 5.1 6.7 0.66 0.55
June 07 1440 285.9 0.6 1.3 0.87 0.86
June 08 720 285.8 1.8 2.1 0.84 0.41

for the R/V Atlantis paths by day.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
RH (%)
May 14 359 79.7 14.5 14.6 0.14 0.12
May 15 1409 88.2 2.4 6.4 -0.07 0.33
May 16 1424 92.8 -2.3 3.8 -0.05 0.40
May 17 1433 94.7 -2.3 4.4 0.46 0.56
May 18 1413 94.8 -1.6 3.0 0.06 0.42
May 19 1427 94.3 -3.8 4.7 -0.11 0.37
May 20 1439 91.4 -4.3 13.4 0.35 0.46
May 21 1433 83.5 -13.2 17.7 -0.11 0.21
May 22 1417 71.3 -7.8 11.5 0.27 0.53
May 23 1440 67.5 3.6 5.4 0.84 0.86
May 24 1429 80.0 -3.4 4.7 0.58 0.57
May 25 1440 85.0 -9.2 12.5 -0.52 0.20
May 26 1440 81.2 2.1 5.8 0.90 0.94
May 27 1440 76.2 -1.7 9.6 0.63 0.79
May 28 1440 78.4 -13.8 16.8 0.67 0.51
May 29 1440 84.4 -10.3 13.9 0.03 0.30
May 30 1434 86.4 -20.6 28.3 0.22 0.46
May 31 1432 91.7 -29.9 33.3 -0.13 0.09
June 01 1440 95.9 -3.2 8.8 0.14 0.35
June 02 1440 93.1 -8.8 11.6 0.41 0.53
June 03 1440 79.1 -9.0 14.6 0.71 0.74
June 04 1440 71.3 -3.5 14.6 -0.11 0.29
June 05 1440 74.0 6.3 23.2 -0.68 0.20
June 06 1440 84.1 -28.0 32.2 0.59 0.51
June 07 1440 95.6 1.5 2.8 0.95 0.97
June 08 720 89.2 -10.3 11.2 0.91 0.37

Table S13. Performance of simulated wind speed (WS) in terms of bias, RMSE, R, and IA for
the R/V Atlantis paths by day.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
WS (ms
-1
)
May 14 359 4.4 -1.0 1.3 0.42 0.48
May 15 1408 3.3 0.4 2.0 0.15 0.41
May 16 1424 3.6 1.8 2.6 0.46 0.56
May 17 1433 2.8 0.2 2.6 -0.31 0.23
May 18 1413 4.4 -2.7 3.6 0.45 0.50
May 19 1427 5.2 1.0 2.6 0.01 0.43
May 20 1439 4.3 1.4 2.6 0.02 0.43
May 21 1433 4.5 4.4 5.8 -0.05 0.34
May 22 1417 2.8 4.4 4.9 0.84 0.53
May 23 1440 9.6 2.5 4.1 0.34 0.49
May 24 1429 5.9 7.8 8.8 -0.71 0.34
May 25 1440 4.7 3.8 5.6 -0.07 0.40
May 26 1440 4.4 3.0 3.6 0.26 0.47
May 27 1440 2.6 3.1 3.4 -0.28 0.33
May 28 1440 5.4 3.8 4.5 0.31 0.46
May 29 1440 3.7 6.1 6.7 -0.22 0.28
May 30 1434 4.3 3.5 4.5 0.14 0.45
May 31 1432 2.9 0.5 3.2 0.35 0.41
June 01 1440 7.9 2.0 4.3 0.41 0.63
June 02 1440 4.4 6.3 8.5 -0.20 0.35
June 03 1440 5.6 0.8 2.3 0.28 0.49
June 04 1440 4.8 -0.5 1.5 0.12 0.33
June 05 1440 3.3 -1.8 2.4 0.84 0.59
June 06 1440 6.5 -0.5 2.1 0.01 0.38
June 07 1440 10.9 -2.2 3.4 0.47 0.56
June 08 720 5.7 3.5 4.1 0.35 0.41

Table S14. Performance of simulated wind direction (WD) in terms of bias, RMSE, R, and IA
for the R/V Atlantis paths by day.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
WD ()
May 14 359 225.0 -9.0 29.7 -0.45 0.21
May 15 1408 255.0 0.4 65.5 -0.09 0.43
May 16 1424 195.0 41.0 90.4 0.25 0.52
May 17 1433 255.0 -40.7 99.6 -0.36 0.20
May 18 1413 105.0 65.4 129.3 0.46 0.54
May 19 1427 255.0 19.1 29.2 0.47 0.51
May 20 1439 225.0 51.0 73.3 0.22 0.52
May 21 1433 225.0 -9.3 71.1 0.43 0.60
May 22 1417 255.0 22.9 55.4 0.20 0.44
May 23 1440 285.0 5.2 16.8 0.32 0.51
May 24 1429 255.0 16.2 104.1 0.82 0.63
May 25 1440 285.0 16.7 80.7 0.43 0.55
May 26 1440 285.0 17.0 57.4 -0.25 0.45
May 27 1440 285.0 9.9 87.1 0.26 0.52
May 28 1440 285.0 13.0 63.0 -0.41 0.41
May 29 1440 255.0 -17.6 82.6 -0.50 0.73
May 30 1434 105.0 -18.7 118.2 -0.20 0.60
May 31 1432 315.0 32.6 91.8 0.46 0.58
June 01 1440 315.0 -7.4 39.1 0.67 0.72
June 02 1440 285.0 19.3 77.1 0.16 0.53
June 03 1440 225.0 18.5 35.8 0.19 0.48
June 04 1440 195.0 18.6 32.1 0.24 0.45
June 05 1440 135.0 -5.5 54.6 0.52 0.70
June 06 1440 285.0 14.9 25.6 0.80 0.78
June 07 1440 315.0 11.4 24.3 0.89 0.77
June 08 720 225.0 31.9 35.7 -0.03 0.38

Table S15. Performance of simulated carbon monoxide (CO), the sum of nitrogen oxide and
nitrogen dioxide (NO
x
), sulfur dioxide (SO
2
), and ozone (O
3
), from the DEF_ANT
simulation in terms of bias, RMSE, R, and IA relative to observations at the four
supersites (Fig. 1a,b) and the surface operational air quality sampling stations
depicted in Fig. 1d. Statistics given for all of California (CA) and by regions as
shown in Fig. 1c.

Table S15. (continued).

Variables
Regions and
Supersites
Observed
Mean Bias RMSE R IA
CO (ppbv)
CA 269.9 -2.0 260.0 0.14 0.39
Southern CA 319.8 1.3 298.4 0.03 0.35
San Joaquin 172.9 31.2 115.2 0.20 0.45
Coastal 206.2 -25.0 143.2 0.24 0.48
Interior Mountains 249.0 -59.3 424.0 0.07 0.11
Bakersfield 166.7 48.1 81.3 0.47 0.50
Pasadena 306.6 225.6 291.9 0.45 0.36
T0 154.5 79.5 129.1 0.23 0.38
T1 122.8 69.1 86.0 0.31 0.33
NO
x
(ppbv)
CA 9.7 6.2 22.4 0.33 0.46
Southern CA 13.1 9.1 29.7 0.24 0.40
San Joaquin 8.3 5.8 15.8 0.52 0.55
Coastal 4.5 2.4 8.9 0.36 0.52
Bakersfield ! ! ! ! !
Pasadena 16.3 40.8 50.5 0.45 0.27
T0 7.0 8.3 14.7 0.25 0.34
T1 ! ! ! ! !
SO
2
(ppbv)
CA 0.8 0.9 3.5 0.05 0.17
Southern CA 0.9 1.4 4.4 0.03 0.14
San Joaquin 1.3 -0.3 1.1 0.14 0.45
Coastal 0.4 0.7 2.5 -0.07 0.12
Bakersfield 0.8 0.0 1.0 -0.21 0.24
Pasadena 0.3 1.4 2.0 0.05 0.14
T0 0.4 0.4 0.9 0.32 0.47
T1 ! ! ! ! !
O
3
(ppbv)
CA 36.6 -3.9 13.9 0.71 0.83
Southern CA 38.5 -2.8 15.9 0.65 0.80
San Joaquin 38.7 -8.6 14.0 0.84 0.86
Sacramento Valley 30.4 -6.1 12.5 0.77 0.83
Coastal 29.5 -2.2 11.4 0.61 0.77
Bakersfield 39.1 -13.2 17.8 0.84 0.83
Pasadena 33.1 -14.8 20.4 0.68 0.70
T0 32.1 -8.0 13.5 0.86 0.87
T1 39.7 -5.4 13.0 0.76 0.84

Table S16. Same as Table S15, except from 50%_ANT simulation.

Variable
Regions and
Supersites
Observed
Mean Bias RMSE R IA
CO (ppbv)
CA 269.9 -71.9 243.7 0.17 0.37
Southern CA 319.8 -92.5 273.5 0.07 0.38
San Joaquin 172.9 -10.3 106.0 0.20 0.35
Coastal 206.2 -56.6 146.6 0.25 0.45
Bakersfield 166.7 -0.9 39.8 0.49 0.69
Pasadena 306.6 24.6 105.6 0.43 0.63
T0 154.5 18.9 72.0 0.26 0.46
T1 122.8 32.1 45.5 0.27 0.46
NO
x
(ppbv)
CA 9.74 -2.05 13.4 0.33 0.56
Southern CA 13.1 -2.45 17.6 0.24 0.51
San Joaquin 8.30 -1.42 8.1 0.53 0.70
Coastal 4.51 -1.09 6.0 0.36 0.57
Pasadena 16.3 11.03 17.9 0.47 0.53
T0 7.00 0.36 7.3 0.26 0.47
T1 ! ! ! ! !
SO
2
(ppbv)
CA 0.77 0.88 3.5 0.05 0.17
Southern CA 0.88 1.35 4.4 0.03 0.14
San Joaquin 1.28 -0.34 1.1 0.15 0.46
Coastal 0.41 0.71 2.5 -0.07 0.13
Bakersfield 0.79 0.00 1.0 -0.21 0.24
Pasadena 0.32 1.34 2.0 0.05 0.14
T0 0.38 0.42 0.9 0.33 0.48
T1 ! ! ! ! !
O
3
(ppbv)
CA 36.6 -4.0 13.1 0.70 0.81
Southern CA 38.5 -1.7 14.9 0.63 0.79
San Joaquin 38.7 -8.9 13.0 0.83 0.85
Coastal 29.5 -2.6 10.5 0.61 0.77
Bakersfield 39.1 -12.2 16.0 0.85 0.83
Pasadena 33.1 -8.4 16.9 0.66 0.77
T0 32.1 -7.0 11.6 0.85 0.88
T1 39.7 -9.1 13.2 0.77 0.80

Table S17. Same as Table S15, except from 0%_ANT simulation.

Variable
Regions and
Supersites
Observed
Mean Bias RMSE R IA
CO (ppbv)
CA 269.9 -140.2 268.2 0.19 0.37
Southern CA 319.8 -183.9 304.8 0.17 0.40
San Joaquin 172.9 -51.3 118.1 0.13 0.39
Coastal 206.2 -87.5 164.0 0.11 0.42
Interior Mountains 249.0 -125.7 438.7 -0.03 0.15
Bakersfield 166.7 -49.6 62.8 0.27 0.43
Pasadena 306.6 -171.9 194.8 -0.05 0.37
T0 154.5 -41.3 74.7 0.33 0.39
T1 122.8 -5.1 28.3 -0.16 0.26
NO
x
(ppbv)
CA 9.74 -9.57 15.2 0.18 0.38
Southern CA 13.1 -12.94 19.4 0.13 0.39
San Joaquin 8.30 -8.11 11.2 0.39 0.39
Coastal 4.51 -4.42 7.3 0.21 0.38
Pasadena 16.3 -16.1 18.7 -0.10 0.38
T0 7.00 -6.77 9.1 0.37 0.38
T1 ! ! ! ! !
SO
2
(ppbv)
CA 0.77 -0.70 1.2 0.04 0.40
Southern CA 0.88 -0.76 1.3 0.01 0.40
San Joaquin 1.28 -1.28 1.5 -0.04 0.39
Sacramento Valley 0.72 -0.71 1.2 -0.01 0.43
Coastal 0.41 -0.41 0.7 0.01 0.47
Interior Mountains 0.86 -0.85 1.8 -0.02 0.35
Bakersfield 0.79 -0.79 1.0 -0.15 0.42
Pasadena 0.32 -0.24 0.4 -0.12 0.37
T0 0.38 -0.37 0.7 0.05 0.35
T1 ! ! ! ! !
O
3
(ppbv)
CA 36.6 -9.8 18.6 0.39 0.57
Southern CA 38.5 -8.1 20.7 0.24 0.50
San Joaquin 38.7 -14.8 19.9 0.60 0.59
Coastal 29.5 -6.2 12.5 0.48 0.62
Bakersfield 39.1 -16.4 22.6 0.67 0.59
Pasadena 33.1 -5.4 20.2 0.26 0.53
T0 32.1 -12.2 17.3 0.67 0.63
T1 39.7 -19.9 23.5 0.52 0.51

Table S18. Performance of simulated carbon monoxide (CO) from the DEF_ANT simulation in
terms of bias, RMSE, R, and IA for each for the G-1 flights.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
CO
(ppbv)
June 03a 800 129.7 0.8 14.8 0.12 0.44
June 06a 1097 120.6 11.8 20.3 0.81 0.76
June 06b 943 124.8 -2.1 16.8 0.31 0.59
June 08a 1142 156.1 -7.1 20.2 0.54 0.71
June 08b 1147 149.0 7.9 28.6 0.71 0.69
June 10a 1068 126.3 -5.0 9.3 0.18 0.43
June 12a 1042 113.2 10.6 16.7 0.13 0.33
June 12b 950 127.7 4.5 10.6 0.03 0.41
June 14a 1120 164.7 5.3 35.1 0.36 0.60
June 15a 1055 144.9 32.7 37.5 0.73 0.49
June 15b 1071 150.5 25.3 35.1 0.29 0.44
June 18a 1114 132.9 -2.6 24.4 0.39 0.58
June 19a 1050 135.3 27.6 31.6 0.41 0.36
June 21a 1077 134.6 14.9 25.3 0.54 0.63
June 21b 1043 128.0 18.0 26.0 0.39 0.48
June 23a 1012 171.8 3.6 49.8 -0.16 0.27
June 23b 1003 157.3 27.6 42.0 0.24 0.42
June 24a 1122 110.4 25.1 57.7 -0.37 0.26
June 24b 922 120.8 17.5 42.7 0.35 0.52
June 27a 1163 147.4 42.6 62.2 0.36 0.49
June 28a 1051 166.3 54.0 78.7 0.65 0.64
June 28b 750 155.7 0.6 24.2 0.54 0.71

Table S19. Performance of simulated nitrogen oxide (NO) from the DEF_ANT simulation in

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
NO
(ppbv)
June 03a 816 0.3 0.4 0.9 0.59 0.52
June 06a 1069 0.2 0.6 1.2 0.85 0.48
June 06b 946 0.1 0.0 0.2 0.14 0.42
June 08a 1119 1.0 0.4 1.5 0.65 0.73
June 08b ! ! ! ! ! !
June 10a 1066 0.2 0.1 0.2 0.38 0.57
June 12a 1048 0.2 0.0 0.2 0.64 0.80
June 12b 952 0.2 0.0 0.1 0.28 0.53
June 14a 1117 1.0 0.4 2.0 0.17 0.40
June 15a 1054 1.0 1.8 2.7 0.80 0.58
June 15b 1067 0.2 0.1 0.2 0.54 0.69
June 18a 1097 0.2 0.0 0.3 0.49 0.65
June 19a 995 0.2 0.0 0.1 0.70 0.81
June 21a 1080 0.8 0.5 1.4 0.32 0.53
June 21b 1045 0.2 0.1 0.3 0.20 0.40
June 23a 1129 0.4 0.1 0.9 0.67 0.79
June 23b 975 0.2 0.0 0.2 0.49 0.66
June 24a 1083 1.1 0.2 1.9 0.32 0.55
June 24b 899 0.4 0.6 1.2 0.74 0.49
June 27a 1131 0.1 0.2 0.5 0.64 0.52
June 28a 1054 0.5 1.1 2.6 0.29 0.28
June 28b 749 0.2 0.0 0.1 0.25 0.50

Table S20. Performance of simulated nitrogen dioxide (NO
2
) from the DEF_ANT simulation in

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
NO
2

(ppbv)
June 03a 777 0.7 0.2 0.8 0.66 0.72
June 06a 1016 0.6 0.7 1.3 0.84 0.61
June 06b 899 0.4 0.1 0.4 0.45 0.59
June 08a 1061 2.2 -0.4 1.6 0.67 0.79
June 08b ! ! ! ! ! !
June 10a 965 0.6 0.1 0.3 0.42 0.60
June 12a 995 0.4 0.0 0.3 0.73 0.84
June 12b 900 0.5 0.1 0.3 0.53 0.64
June 14a 1060 2.2 1.2 3.4 0.33 0.51
June 15a 1003 1.7 2.3 3.0 0.81 0.60
June 15b 1009 0.9 0.5 1.0 0.46 0.60
June 18a 1042 0.9 0.0 0.9 0.66 0.76
June 19a 948 0.0 0.9 1.1 -0.27 0.03
June 21a 1024 1.8 0.5 1.8 0.46 0.65
June 21b 991 0.7 0.5 1.3 0.34 0.36
June 23a 1072 0.9 0.3 1.6 0.73 0.80
June 23b 928 0.9 0.4 0.9 0.61 0.66
June 24a 1027 1.7 0.0 2.0 0.41 0.65
June 24b 856 1.1 1.3 2.5 0.74 0.56
June 27a 1078 0.5 0.7 1.4 0.62 0.46
June 28a 1001 2.0 3.2 6.4 0.50 0.48
June 28b 709 1.0 0.2 0.6 0.40 0.62

Table S21. Performance of simulated sulfur dioxide (SO
2

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
SO
2

(ppbv)
June 03a 808 -0.3 0.5 1.0 -0.08 0.34
June 06a 1048 0.2 -0.1 0.8 0.11 0.22
June 06b 941 -0.1 0.2 0.8 0.00 0.23
June 08a ! ! ! ! ! !
June 08b ! ! ! ! ! !
June 10a ! ! ! ! ! !
June 12a ! ! ! ! ! !
June 12b ! ! ! ! ! !
June 14a ! ! ! ! ! !
June 15a 1037 0.8 0.0 0.4 0.69 0.82
June 15b 1046 0.8 -0.4 0.7 0.31 0.53
June 18a 1082 0.8 -0.7 1.1 0.13 0.43
June 19a 1028 0.7 -0.3 0.5 0.51 0.63
June 21a 1071 0.6 -0.3 0.8 0.11 0.43
June 21b 1037 0.5 -0.2 0.6 0.40 0.60
June 23a 1112 0.7 -0.4 0.6 0.41 0.53
June 23b 955 1.0 -0.7 0.9 0.39 0.46
June 24a 944 0.5 0.1 0.9 0.19 0.44
June 24b 889 1.0 -0.7 0.9 0.30 0.49
June 27a 1093 0.6 -0.1 0.6 0.50 0.55
June 28a 1031 0.9 -0.6 1.0 0.10 0.45
June 28b 722 0.6 -0.5 0.8 0.29 0.44

Table S22. Performance of simulated ozone (O
3
) from the DEF_ANT simulation in terms of
bias, RMSE, R, and IA for each for the G-1 flights.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
O
3

(ppbv)
June 03a 835 38.2 -9.2 10.7 0.55 0.54
June 06a 1132 29.0 -1.8 6.8 0.48 0.70
June 06b 969 48.9 -10.3 17.9 -0.07 0.32
June 08a 1152 44.0 -5.0 10.8 0.83 0.85
June 08b 1194 60.2 -3.2 7.3 0.79 0.86
June 10a 1088 43.5 -4.7 5.7 0.51 0.51
June 12a 1078 37.2 5.3 5.8 0.80 0.57
June 12b ! ! ! ! ! !
June 14a 1075 44.9 6.8 9.8 0.49 0.58
June 15a 1065 36.4 -1.2 5.8 0.81 0.89
June 15b 1082 63.5 6.1 9.6 0.09 0.36
June 18a 1145 52.1 1.0 8.6 0.64 0.80
June 19a 1101 49.1 7.7 10.3 0.28 0.36
June 21a 1128 34.8 0.8 5.5 0.61 0.77
June 21b 1035 55.9 4.7 9.2 0.02 0.40
June 23a 1167 58.5 7.2 10.9 0.81 0.83
June 23b 1024 71.5 18.4 20.8 0.39 0.35
June 24a 1125 32.2 6.0 14.2 0.59 0.66
June 24b 951 44.5 1.1 7.2 0.52 0.69
June 27a 1152 48.5 18.0 21.2 0.26 0.29
June 28a 1121 55.4 11.4 21.5 0.34 0.56
June 28b 759 65.6 10.4 17.7 0.53 0.66

Table S23. Performance of simulated isoprene from the DEF_ANT simulation in terms of bias,
RMSE, R, and IA for each for the G-1 flights.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
isoprene
(ppbv)
June 03a 854 -0.2 0.2 0.3 0.71 0.44
June 06a 1133 0.4 -0.3 0.6 0.61 0.52
June 06b 705 0.1 -0.1 0.2 0.25 0.46
June 08a 1190 0.4 -0.3 0.5 0.61 0.47
June 08b 1140 0.0 0.0 0.4 0.34 0.19
June 10a 1113 0.1 0.0 0.1 0.47 0.61
June 12a 1114 0.2 -0.1 0.2 0.69 0.81
June 12b ! ! ! ! ! !
June 14a 1168 0.3 -0.1 0.4 0.25 0.43
June 15a 1110 0.3 -0.2 0.3 0.41 0.55
June 15b 1115 0.5 -0.4 0.6 0.47 0.51
June 18a 632 0.2 -0.1 0.6 0.17 0.13
June 19a 1071 1.0 -0.8 0.9 0.28 0.28
June 21a 1075 0.4 -0.3 0.3 0.53 0.52
June 21b 1126 0.4 -0.3 0.4 0.57 0.47
June 23a 1079 0.6 -0.4 0.7 0.73 0.64
June 23b 1106 1.2 -1.1 1.5 0.32 0.47
June 24a 1173 0.3 -0.3 0.5 -0.09 0.33
June 24b 1034 0.8 -0.7 1.1 -0.07 0.45
June 27a 840 1.6 -1.2 2.3 0.83 0.54
June 28a 1105 1.5 -1.2 2.3 0.76 0.51
June 28b 755 1.1 -0.9 1.4 0.61 0.48

Table S24. Performance of simulated methyl-vinyl-ketone + methacrolein (MVK+MACR) from
the DEF_ANT simulation in terms of bias, RMSE, R, and IA for each for the G-1
flights.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
MVK+
MACR
(ppbv)
June 03a 854 0.0 0.0 0.1 0.68 0.59
June 06a 1133 0.4 -0.2 0.3 0.72 0.67
June 06b 705 0.2 0.0 0.1 0.65 0.76
June 08a 1190 0.4 -0.2 0.4 0.62 0.56
June 08b 1140 0.7 -0.6 0.7 0.52 0.50
June 10a 1113 0.1 -0.1 0.1 0.72 0.73
June 12a 1114 0.2 0.0 0.1 0.60 0.75
June 12b ! ! ! ! ! !
June 14a 1168 0.4 -0.1 0.3 0.39 0.54
June 15a 1110 0.4 -0.1 0.3 0.78 0.71
June 15b 1115 0.6 -0.4 0.6 0.63 0.53
June 18a 633 0.1 0.0 0.1 0.48 0.52
June 19a 1071 0.4 -0.3 0.3 0.65 0.47
June 21a 1075 0.3 -0.1 0.2 0.48 0.62
June 21b 1126 0.3 -0.1 0.2 0.47 0.55
June 23a 1079 0.8 -0.4 0.6 0.76 0.70
June 23b 1106 0.9 -0.8 1.1 0.63 0.49
June 24a 1173 0.3 -0.2 0.4 0.28 0.42
June 24b 1034 1.0 -0.9 1.3 0.11 0.47
June 27a 840 1.4 -0.9 1.6 0.84 0.60
June 28a 1106 2.3 -1.7 2.4 0.64 0.51
June 28b 755 0.9 -0.5 0.8 0.17 0.45

Table S25. Performance of simulated toluene from the DEF_ANT simulation in terms of bias,
RMSE, R, and IA for each for the G-1 flights.

Variable
Flight
Date
Number of
Data Points
Observed
Mean Bias RMSE R IA
toluene
(ppbv)
June 03a 851 0.1 -0.1 0.2 0.32 0.51
June 06a ! ! ! ! ! !
June 06b 705 0.1 0.0 0.0 0.26 0.54
June 08a 1190 0.1 0.0 0.1 0.40 0.52
June 08b 1140 0.0 0.1 0.1 0.45 0.45
June 10a 1113 0.0 0.0 0.0 0.03 0.39
June 12a 1114 0.0 0.0 0.0 0.23 0.51
June 12b ! ! ! ! ! !
June 14a 1168 0.1 0.1 0.2 0.25 0.48
June 15a 1110 0.1 0.2 0.2 0.43 0.31
June 15b 1115 0.1 0.0 0.1 0.23 0.49
June 18a 633 0.1 0.0 0.1 0.21 0.53
June 19a 1071 0.1 0.0 0.0 0.40 0.64
June 21a 1075 0.1 0.1 0.1 0.43 0.56
June 21b 1126 0.1 0.0 0.1 0.11 0.40
June 23a 1079 0.1 0.0 0.2 0.45 0.49
June 23b 1106 0.1 0.0 0.1 -0.01 0.38
June 24a 1173 0.1 0.0 0.1 0.21 0.40
June 24b 1034 0.1 0.1 0.2 0.33 0.45
June 27a 840 0.1 0.0 0.1 0.58 0.63
June 28a 1106 0.2 0.2 0.3 0.49 0.49
June 28b 755 0.1 -0.1 0.1 0.24 0.46

Table S26. Performance of simulated terpene (TERP) from the DEF_ANT simulation in terms of
bias, RMSE, R, and IA for each for the G-1 flights.

Variable
Flight
Date
Number
of Data
Points
Observed
Mean Bias RMSE R IA
TERP
(ppbv)
June 03a 854 0.0 0.0 0.1 0.43 0.43
June 06a 1133 0.0 0.0 0.1 0.02 0.37
June 06b 705 0.0 0.0 0.1 0.02 0.27
June 08a 1190 0.0 0.0 0.1 0.05 0.44
June 08b 1140 0.0 0.0 0.1 0.07 0.40
June 10a 1113 0.0 0.0 0.0 0.01 0.39
June 12a 1114 0.0 0.0 0.0 0.10 0.43
June 12b ! ! ! ! ! !
June 14a 1168 0.1 -0.1 0.1 -0.03 0.41
June 15a 1110 0.0 0.0 0.1 -0.09 0.39
June 15b 1115 0.1 -0.1 0.1 0.28 0.46
June 18a 633 0.1 0.0 0.1 0.16 0.45
June 19a 1071 0.1 -0.1 0.1 -0.08 0.42
June 21a 1075 0.1 0.0 0.1 0.14 0.45
June 21b 1126 0.1 -0.1 0.1 0.15 0.44
June 23a 1079 0.1 -0.1 0.1 0.35 0.50
June 23b 1106 0.1 -0.1 0.1 0.23 0.43
June 24a 1173 0.1 -0.1 0.1 0.07 0.44
June 24b 1034 0.1 -0.1 0.1 -0.16 0.41
June 27a 840 0.1 -0.1 0.1 0.46 0.51
June 28a 1106 0.1 -0.1 0.1 0.25 0.46
June 28b 755 0.1 -0.1 0.1 0.16 0.44

Table S27. Performance of simulated carbon monoxide (CO) from the DEF_ANT simulation in
terms of bias, RMSE, R, and IA for each for the WP-3D flights.

Variable Flight Date
Number
of Data
Points
Observed
Mean Bias RMSE R IA
CO
(ppbV)
May 4 16011 166.3 42.5 69.4 0.75 0.79
May 7 23212 161.7 9.3 35.5 0.78 0.86
May 8 24182 177.0 8.6 44.2 0.80 0.89
May 11 24549 145.6 0.0 13.6 0.82 0.90
May 12 26169 153.7 10.4 26.4 0.85 0.90
May 14 20857 172.1 29.6 56.4 0.83 0.87
May 16 26495 168.6 30.0 50.9 0.90 0.89
May 19 22960 173.5 15.9 52.3 0.86 0.92
May 212 10366 150.8 -5.7 16.6 0.90 0.94
May 22 21538 142.3 0.2 20.3 0.80 0.84
May 23 19728 150.9 27.5 59.4 0.57 0.58
May 24 20125 164.2 49.9 80.8 0.76 0.69
May 25 21126 158.6 12.9 34.4 0.73 0.83
June 3 22894 179.3 27.0 61.2 0.80 0.86
June 14 25077 123.3 11.0 30.2 0.82 0.89
June 16 23692 133.2 8.1 35.4 0.82 0.80
June 18 24262 120.2 6.9 20.3 0.88 0.92
June 20 24350 164.8 21.0 54.2 0.79 0.79
June 22 4536 136.3 25.9 50.9 0.62 0.68

Table S28. Performance of simulated nitrogen oxide (NO) from the DEF_ANT simulation in

Variable
Flight
Date
Number
of Data
Points
Observed
Mean Bias RMSE R IA
NO
(ppbV)
May 4 15868 1.0 0.6 2.4 0.63 0.74
May 7 23049 0.4 0.4 1.5 0.59 0.72
May 8 23923 0.6 0.2 2.7 0.19 0.32
May 11 21719 0.4 0.1 0.7 0.87 0.91
May 12 25402 0.6 0.1 1.5 0.65 0.78
May 14 ! ! ! ! ! !
May 16 26574 0.2 0.5 1.5 0.72 0.56
May 19 22654 2.3 1.0 3.5 0.77 0.83
May 21 8785 0.8 -0.3 3.0 0.49 0.54
May 22 20434 0.1 0.2 1.3 0.60 0.54
May 23 19471 0.0 0.0 0.9 0.46 0.14
May 24 19906 0.0 0.1 1.2 0.28 0.28
May 25 21034 0.1 0.2 2.1 0.17 0.07
June 3 22893 0.2 0.3 1.8 0.62 0.71
June 14 23681 0.2 0.1 1.4 0.80 0.84
June 16 23026 0.4 0.3 1.7 0.87 0.76
June 18 23687 0.3 0.2 1.0 0.77 0.74
June 20 23911 0.4 1.7 5.1 0.37 0.19
June 22 4357 0.4 0.1 1.6 0.50 0.67

Table S29. Performance of simulated nitrogen dioxide (NO
2

Variable
Flight
Date
Number
of Data
Points
Observed
Mean Bias RMSE R IA
NO
2

(ppbV)
May 4 13716 3.0 1.1 4.7 0.73 0.84
May 7 19543 1.3 1.1 4.7 0.35 0.51
May 8 23562 2.0 0.4 3.3 0.63 0.77
May 11 20335 0.9 0.1 0.9 0.91 0.95
May 12 24752 1.6 0.2 2.4 0.82 0.88
May 14 ! ! ! ! ! !
May 16 25836 0.9 1.5 3.9 0.87 0.69
May 19 22016 4.1 1.2 4.1 0.85 0.90
May 212 8569 1.1 -0.1 2.4 0.69 0.78
May 22 19838 0.9 0.7 1.9 0.85 0.82
May 23 19019 1.4 2.6 5.7 0.61 0.56
May 24 19676 1.5 3.5 7.1 0.61 0.53
May 25 20812 1.5 0.9 4.1 0.54 0.58
June 3 22697 2.3 4.1 8.3 0.52 0.55
June 14 22767 0.8 0.4 2.1 0.83 0.89
June 16 22390 1.0 0.6 2.3 0.91 0.82
June 18 23234 0.9 0.4 1.5 0.84 0.84
June 20 23475 1.1 2.6 6.0 0.61 0.44
June 22 4228 0.9 0.3 2.5 0.52 0.69

Table S30. Performance of simulated ammonia (NH
3
) from the DEF_ANT simulation in terms
of bias, RMSE, R, and IA for each for the WP-3D flights.

Variable
Flight
Date
Number
of Data
Points
Observed
Mean Bias RMSE R IA
NH
3

(ppbV)
May 4 8506 3.7 -1.6 8.9 0.44 0.28
May 7 14716 24.2 -19.5 42.9 0.56 0.36
May 8 13058 5.0 -2.9 7.7 0.59 0.41
May 11 10948 4.3 -3.3 4.7 0.49 0.51
May 12 16250 11.2 -8.7 17.9 0.70 0.42
May 14 14387 5.3 -3.5 12.2 0.57 0.28
May 16 20454 3.2 -1.8 13.1 0.42 0.16
May 19 18686 13.3 -10.9 49.3 0.54 0.15
May 21 8783 1.7 -0.9 5.0 0.47 0.50
May 22 17075 5.8 -3.3 15.6 0.17 0.18
May 23 18552 0.9 0.5 2.1 0.46 0.55
May 24 18966 3.0 -0.9 9.2 0.18 0.20
May 25 19875 3.3 -1.4 11.3 0.46 0.33
June 3 17383 3.2 -0.9 6.9 0.03 0.20
June 14 19974 4.1 -2.8 5.7 0.75 0.57
June 16 21467 7.8 -4.2 10.4 0.65 0.50
June 18 19080 7.7 -5.9 18.0 0.35 0.25
June 20 22002 2.4 -0.2 4.0 0.47 0.57
June 22 3573 5.7 -3.9 8.0 0.68 0.47

Table S31. Performance of simulated sulfur dioxide (SO
2

Variable
Flight
Date
Number
of Data
Points
Observed
Mean Bias RMSE R IA
SO
2

(ppbV)
May 4 15413 0.4 -0.1 0.8 0.41 0.60
May 7 22412 0.8 -0.5 0.9 0.38 0.54
May 8 23025 0.7 -0.3 0.9 0.45 0.62
May 11 23401 0.1 0.0 0.3 0.44 0.61
May 12 24820 0.4 -0.3 0.7 0.31 0.49
May 14 20161 0.5 0.0 0.6 0.80 0.89
May 16 25416 0.3 0.1 0.7 0.40 0.53
May 19 22073 0.3 0.0 0.6 0.58 0.74
May 212 9942 0.3 -0.3 1.2 0.15 0.16
May 22 20576 0.4 -0.3 0.6 0.26 0.50
May 23 19016 0.4 -0.1 1.4 0.24 0.23
May 24 19306 0.6 -0.1 1.1 0.44 0.52
May 25 20316 0.4 -0.1 1.1 0.16 0.24
June 3 22020 0.6 -0.1 0.7 0.47 0.62
June 14 23709 0.4 -0.2 0.6 0.49 0.53
June 16 22677 0.7 -0.5 0.9 0.22 0.47
June 18 23319 0.4 -0.2 0.7 0.27 0.49
June 20 23384 0.4 0.3 1.6 0.26 0.29
June 22 4307 0.5 -0.2 0.9 0.11 0.35

Table S32. Performance of simulated ozone (O
3
bias, RMSE, R, and IA for each for the WP-3D flights.

Variable Flight Date
Number
of Data
Points
Observed
Mean Bias RMSE R IA
O
3

(ppbV)
May 4 16552 68.0 -2.3 8.5 0.54 0.71
May 7 23787 62.6 -5.4 10.0 0.60 0.70
May 8 24401 75.7 -8.9 12.4 0.75 0.75
May 11 25079 50.9 -4.1 15.9 0.69 0.69
May 12 26879 51.7 4.0 10.6 0.52 0.64
May 14 ! ! ! ! ! !
May 16 27326 66.6 -1.5 13.1 0.63 0.78
May 19 23389 51.3 -4.8 11.1 0.58 0.71
May 21 9855 57.5 -10.4 13.4 0.87 0.74
May 22 21551 56.7 -12.6 14.8 0.69 0.55
May 23 20158 63.9 -10.8 13.5 0.61 0.59
May 24 20628 63.4 -9.0 14.2 0.39 0.52
May 25 21733 49.9 -2.2 13.5 0.43 0.65
June 3 23712 53.3 -14.9 21.2 0.19 0.46
June 14 24837 58.8 1.7 9.7 0.74 0.86
June 16 24068 55.0 -4.6 9.1 0.77 0.84
June 18 24639 51.2 -4.8 10.2 0.79 0.85
June 20 24574 66.9 -10.7 16.0 0.51 0.64
June 22 4598 68.7 -5.1 12.1 0.44 0.59

Table S33. Performance of simulated isoprene from the DEF_ANT simulation in terms of bias,
RMSE, R, and IA for each for the WP-3D flights.

Variable
Flight
Date
Number
of Data
Points
Observed
Mean Bias RMSE R IA
isoprene
(ppbV)
May 4 616 0.1 0.0 0.1 0.53 0.71
May 7 937 0.1 0.0 0.1 0.63 0.77
May 8 1371 0.1 0.0 0.1 0.56 0.73
May 11 1118 0.0 0.0 0.0 0.52 0.70
May 12 1464 0.0 0.0 0.1 0.68 0.81
May 14 1160 0.1 0.0 0.1 0.84 0.88
May 16 1448 0.0 0.0 0.1 0.75 0.81
May 19 912 0.1 0.0 0.1 0.76 0.85
May 21 465 0.0 0.0 0.0 0.69 0.78
May 22 1222 0.0 0.0 0.0 0.56 0.67
May 23 1122 0.0 0.0 0.1 0.36 0.56
May 24 1149 0.0 0.0 0.1 0.15 0.38
May 25 1199 0.0 0.0 0.0 0.18 0.37
June 3 1300 0.0 0.0 0.0 0.18 0.42
June 14 1326 0.1 0.0 0.2 0.66 0.78
June 16 1077 0.0 0.0 0.1 0.52 0.70
June 18 808 0.0 0.0 0.1 0.47 0.68
June 20 1419 0.1 0.0 0.1 0.59 0.74
June 22 267 0.1 0.0 0.2 0.35 0.52

Table S34. Performance of simulated methyl-vinyl-ketone + methacrolein (MVK+MACR) from
the DEF_ANT simulation in terms of bias, RMSE, R, and IA for each for the WP-3D
flights.

Variable
Flight
Date
Number
of Data
Points
Observed
Mean Bias RMSE R IA
MVK+
MACR
(ppbV)
May 4 70 0.2 0.0 0.2 0.00 0.16
May 7 70 0.1 0.1 0.1 0.08 0.42
May 8 71 0.2 0.1 0.1 0.21 0.49
May 11 71 0.1 0.0 0.1 -0.19 0.28
May 12 70 0.1 0.1 0.1 -0.33 0.30
May 14 70 0.1 0.0 0.1 -0.48 0.12
May 16 71 0.1 0.1 0.1 0.08 0.37
May 19 71 0.1 0.1 0.1 -0.02 0.39
May 212 71 -0.1 0.2 0.5 0.23 0.28
May 22 71 -0.3 0.4 0.7 0.55 0.39
May 23 58 -0.1 0.3 0.6 0.21 0.38
May 24 71 -0.1 0.2 0.5 -0.12 0.27
May 25 65 -0.1 0.2 0.5 0.09 0.30
June 3 71 0.0 0.1 0.5 0.07 0.20
June 14 71 -0.1 0.3 0.8 -0.23 0.33
June 16 70 -0.2 0.4 0.7 -0.25 0.37
June 18 71 -0.1 0.4 0.7 0.08 0.36
June 20 71 -0.2 0.5 0.9 0.10 0.41
June 22 71 0.2 0.0 0.3 -0.16 0.12

Table S35. Performance of simulated terpene (TERP) from the DEF_ANT simulation in terms of
bias, RMSE, R, and IA for each for the WP-3D flights.

Variable
Flight
Date
Number
of Data
Points
Observed
Mean Bias RMSE R IA
TERP
(ppbv)
May 4 745 0.0 0.0 0.0 0.51 0.46
May 7 1147 0.0 0.0 0.0 0.28 0.41
May 8 1202 0.0 0.0 0.0 0.50 0.49
May 11 1282 0.0 0.0 0.0 0.18 0.38
May 12 1464 0.0 0.0 0.0 0.46 0.41
May 14 1160 0.0 0.0 0.0 0.75 0.65
May 16 1448 0.0 0.0 0.0 0.54 0.59
May 19 1247 0.0 0.0 0.1 0.60 0.50
May 21 573 0.0 0.0 0.0 0.77 0.25
May 22 1221 0.0 0.0 0.0 0.24 0.21
May 23 1122 0.0 0.0 0.0 0.44 0.56
May 24 1148 0.0 0.0 0.0 0.42 0.49
May 25 1198 0.0 0.0 0.0 0.13 0.24
June 3 1300 0.0 0.0 0.0 0.18 0.40
June 14 1326 0.0 0.0 0.0 0.25 0.32
June 16 1388 0.0 0.0 0.0 0.49 0.32
June 18 1177 0.0 0.0 0.0 0.27 0.19
June 20 1302 0.0 0.0 0.0 0.42 0.59
June 22 266 0.0 0.0 0.1 0.65 0.28

Table S36. Performance of simulated formaldehyde (CH
2
O) from the DEF_ANT simulation in

Variable
Flight
Date
Number
of Data
Points
Observed
Mean Bias RMSE R IA
CH
2
O
(ppbv)
May 4 780 1.9 -0.4 0.9 0.81 0.86
May 7 1323 1.7 -0.4 0.7 0.75 0.79
May 8 1372 2.1 -1.0 1.3 0.83 0.73
May 11 1379 0.9 -0.3 0.5 0.56 0.64
May 12 1464 1.4 -0.4 0.6 0.76 0.79
May 14 1200 1.6 -0.4 0.9 0.78 0.83
May 16 1501 1.6 -0.5 0.9 0.88 0.86
May 19 1306 2.1 -0.8 1.2 0.85 0.79
May 212 574 1.1 -0.5 0.7 0.73 0.69
May 22 1222 1.1 -0.3 0.5 0.50 0.58
May 23 1123 1.8 -0.3 0.7 0.72 0.79
May 24 1150 2.1 -0.3 0.8 0.73 0.79
May 25 1199 2.0 -0.8 1.0 0.55 0.56
June 3 1300 2.6 -1.0 1.2 0.80 0.66
June 14 1478 2.9 -1.3 1.6 0.84 0.77
June 16 1388 2.1 -0.8 1.0 0.72 0.66
June 18 1388 2.1 -0.9 1.3 0.31 0.50
June 20 1419 2.7 -1.3 1.5 0.81 0.66
June 22 267 2.7 -1.5 1.6 0.50 0.44

Table S37. Performance of simulated black carbon (BC) from the DEF_ANT simulation in terms
of bias, RMSE, R, and IA for each for the G-1, WP-3D, and CIRPAS Twin Otter
flights.

Flight Date
Number
of Data
Points
Observed
Mean
(g/m3)
Bias
(g/m3) RMSE R IA
G-1, June 03a 787 0.03 0.03 0.04 0.36 0.40
G-1. June 06a 1083 0.02 0.08 0.09 0.54 0.24
G-1, June 06b 658 0.02 0.07 0.09 0.10 0.14
G-1, June 08a 1144 0.09 0.07 0.10 0.10 0.36
G-1, June 08b 883 0.07 0.08 0.09 0.67 0.41
G-1, June 10a 786 0.03 0.03 0.04 0.32 0.29
G-1, June 12a 1090 0.02 0.05 0.06 0.47 0.24
G-1, June 12b 713 0.02 0.05 0.05 -0.02 0.16
G-1, June 14a 1139 0.08 0.10 0.12 0.50 0.48
G-1, June 15a 1075 0.07 0.16 0.16 0.65 0.32
G-1, June 15b 830 0.09 0.08 0.09 0.58 0.46
G-1, June 18a 786 0.05 0.04 0.07 0.17 0.33
G-1, June 19a ! ! ! ! ! !
G-1, June 21a 1107 0.07 0.12 0.18 0.21 0.31
G-1, June 21b 797 0.06 0.05 0.08 0.42 0.53
G-1, June 23a 1145 0.09 0.09 0.10 0.44 0.39
G-1, June 23b 769 0.10 0.09 0.10 0.36 0.40
G-1, June 24a 1140 0.06 0.07 0.10 0.06 0.36
G-1, June 24b 703 0.08 0.05 0.08 0.48 0.61
G-1, June 27a 1185 0.07 0.15 0.16 0.73 0.27
G-1, June 28a 1091 0.13 0.17 0.21 0.56 0.51
G-1, June 28b 579 0.11 0.06 0.09 0.11 0.42
WP-3D, May 4 8197 0.02 0.13 0.14 0.59 0.27
WP-3D, May 7 24831 0.08 0.07 0.12 0.73 0.74
WP-3D, May 8 25375 0.09 0.09 0.15 0.66 0.63
WP-3D, May 11 25780 0.03 0.05 0.08 0.65 0.64
WP-3D, May 12 25020 0.08 0.06 0.10 0.68 0.73
WP-3D, May 14 19087 0.14 0.12 0.19 0.79 0.80
WP-3D, May 16 21321 0.09 0.16 0.22 0.75 0.53
WP-3D, May 19 24221 0.15 0.06 0.15 0.80 0.87
WP-3D, May 21 10357 0.05 0.02 0.05 0.88 0.92
WP-3D, May 22 22536 0.03 0.05 0.08 0.55 0.60
WP-3D, May 23 20827 0.04 0.11 0.16 0.63 0.45
WP-3D, May 24 20661 0.07 0.14 0.22 0.44 0.46
WP-3D, May 25 20469 0.09 0.08 0.17 0.49 0.54
WP-3D, June 3 23570 0.16 0.07 0.15 0.66 0.77
WP-3D, June 14 26406 0.07 0.05 0.16 0.51 0.62
WP-3D, June 16 22634 0.07 0.04 0.08 0.75 0.78
WP-3D, June 18 24707 0.05 0.04 0.07 0.77 0.83
WP-3D, June 20 24681 0.07 0.14 0.23 0.67 0.46
WP-3D, June 22 4907 0.07 0.08 0.15 0.67 0.72
Twin Otter, May 6 179 0.16 0.34 0.37 0.51 0.27
Twin Otter, May 7 194 0.22 0.36 0.51 0.61 0.30
Twin Otter, May 10 186 0.07 0.19 0.21 0.51 0.22
Twin Otter, May 12 195 0.14 0.24 0.32 0.63 0.37
Twin Otter, May 13 178 0.12 0.31 0.48 0.26 0.19
Twin Otter, May 14 189 0.15 0.44 0.48 0.42 0.23
Twin Otter, May 15 185 0.16 0.34 0.39 0.35 0.22
Twin Otter, May 18 183 0.03 0.07 0.09 0.62 0.41
Twin Otter, May 19 116 0.18 0.39 0.43 0.25 0.25
Twin Otter, May 20 192 0.06 0.08 0.12 0.92 0.69
Twin Otter, May 21 192 0.15 0.20 0.25 0.33 0.33
Twin Otter, May 22 195 0.03 0.04 0.07 0.76 0.47
Twin Otter, May 24 173 0.07 0.08 0.09 0.89 0.68
Twin Otter, May 25 191 0.10 0.12 0.14 0.80 0.53
Twin Otter, May 27 176 0.11 0.20 0.23 0.08 0.21
Twin Otter, May 28 192 0.16 0.20 0.37 -0.12 0.13

Table S38. Performance of simulated organic aerosol (OA) from the DEF_ANT simulation in
terms of bias, RMSE, R, and IA for each for the G-1, WP-3D, and CIRPAS Twin
Otter flights.

Flight Date
Number
of Data
Points
Observed
Mean
(g/m3)
Bias
(g/m3) RMSE R IA
G-1, June 03a 674 0.88 -0.09 0.67 0.37 0.64
G-1. June 06a 918 1.90 -0.78 1.25 0.53 0.59
G-1, June 06b 510 2.05 -0.94 1.66 0.13 0.48
G-1, June 08a 946 4.02 -1.67 2.30 0.76 0.65
G-1, June 08b 957 3.92 -1.26 1.67 0.79 0.78
G-1, June 10a 882 1.17 -0.35 0.52 0.49 0.58
G-1, June 12a 882 0.91 -0.51 0.61 0.47 0.47
G-1, June 12b 793 2.17 -1.54 1.66 -0.33 0.29
G-1, June 14a 928 4.08 -2.32 2.65 0.52 0.47
G-1, June 15a 878 2.64 -0.45 1.31 0.25 0.50
G-1, June 15b 882 4.93 -0.97 1.99 0.46 0.60
G-1, June 18a 922 2.14 -0.36 2.13 0.12 0.35
G-1, June 19a 887 2.16 0.30 1.00 0.45 0.66
G-1, June 21a 898 3.05 -1.55 2.48 0.45 0.49
G-1, June 21b 894 3.23 -1.38 1.90 0.59 0.59
G-1, June 23a 942 6.12 -1.99 3.01 0.48 0.57
G-1, June 23b 874 6.25 -0.81 2.17 0.53 0.64
G-1, June 24a 934 2.07 -0.22 1.84 0.13 0.45
G-1, June 24b 816 3.21 -1.33 2.28 0.28 0.51
G-1, June 27a 960 9.73 -4.88 5.68 0.69 0.59
G-1, June 28a 902 13.42 -7.60 8.87 0.75 0.54
G-1, June 28b 668 10.83 -7.02 8.45 0.60 0.47
WP-3D, May 4 1495 1.51 1.30 1.75 0.79 0.77
WP-3D, May 7 2383 2.02 0.36 1.03 0.84 0.90
WP-3D, May 8 2304 2.03 0.01 1.18 0.81 0.89
WP-3D, May 11 244 0.12 0.29 0.43 0.70 0.73
WP-3D, May 12 ! ! ! ! ! !
WP-3D, May 14 1765 1.92 1.18 1.91 0.70 0.76
WP-3D, May 16 2012 2.29 0.66 2.02 0.66 0.79
WP-3D, May 19 2102 1.85 0.20 1.21 0.87 0.91
WP-3D, May 21 434 1.14 -0.37 1.23 0.79 0.78
WP-3D, May 22 1912 0.67 0.44 0.73 0.54 0.67
WP-3D, May 23 1906 1.04 0.30 0.71 0.66 0.75
WP-3D, May 24 1938 1.86 0.00 1.30 0.71 0.77
WP-3D, May 25 1879 1.52 0.39 0.97 0.48 0.67
WP-3D, June 3 2215 2.37 0.08 1.19 0.70 0.83
WP-3D, June 14 2438 1.88 -0.22 1.62 0.74 0.83
WP-3D, June 16 2367 1.65 0.17 0.87 0.80 0.89
WP-3D, June 18 2341 1.00 0.31 0.88 0.75 0.84
WP-3D, June 20 2389 2.66 -0.97 2.00 0.83 0.73
WP-3D, June 22 481 1.01 0.94 1.51 0.29 0.51
Twin Otter, May 18 183 1.80 -0.58 1.31 0.69 0.74
Twin Otter, May 19 146 3.51 0.77 1.16 0.51 0.62
Twin Otter, May 20 192 1.30 0.40 0.71 0.92 0.94
Twin Otter, May 21 192 2.27 0.55 0.88 0.68 0.74
Twin Otter, May 22 195 0.93 -0.19 0.44 0.86 0.90
Twin Otter, May 24 173 1.50 0.17 0.67 0.64 0.78
Twin Otter, May 25 191 1.10 1.32 1.54 0.45 0.43
Twin Otter, May 27 176 2.00 -0.39 0.76 0.15 0.47
Twin Otter, May 28 192 2.27 -0.09 0.96 0.05 0.43

Table S39. Performance of simulated sulfate (SO
4
2-
bias, RMSE, R, and IA for each for the G-1, WP-3D, and CIRPAS Twin Otter
flights.

Flight Date
Number
of Data
Points
Observed
Mean
(g/m3)
Bias
(g/m3) RMSE R IA
G-1, June 03a 674 0.51 -0.04 0.24 -0.16 0.28
G-1. June 06a 918 0.32 0.06 0.23 0.16 0.35
G-1, June 06b 510 0.44 -0.12 0.18 -0.23 0.35
G-1, June 08a 946 0.72 -0.24 0.34 0.16 0.45
G-1, June 08b 957 0.88 -0.20 0.37 0.59 0.70
G-1, June 10a 882 0.25 0.06 0.13 0.30 0.52
G-1, June 12a 882 0.13 0.17 0.18 -0.11 0.30
G-1, June 12b 793 0.12 0.16 0.17 -0.05 0.31
G-1, June 14a 928 0.40 0.18 0.30 0.57 0.69
G-1, June 15a 878 0.54 -0.08 0.17 0.56 0.60
G-1, June 15b 882 0.67 -0.07 0.22 0.39 0.60
G-1, June 18a 926 0.28 0.05 0.23 0.18 0.47
G-1, June 19a 887 0.46 0.45 0.56 0.23 0.30
G-1, June 21a 899 0.39 0.04 0.19 -0.03 0.36
G-1, June 21b 894 0.39 0.04 0.19 0.39 0.60
G-1, June 23a 944 0.58 -0.13 0.29 0.19 0.47
G-1, June 23b 874 0.91 -0.31 0.44 0.43 0.51
G-1, June 24a 934 0.69 -0.15 0.41 0.30 0.56
G-1, June 24b 816 0.65 -0.06 0.39 0.30 0.59
G-1, June 27a 960 0.75 -0.04 0.32 0.63 0.71
G-1, June 28a 902 0.72 -0.13 0.39 0.17 0.42
G-1, June 28b 668 0.79 -0.34 0.52 0.41 0.48
WP-3D, May 4 1495 0.42 0.17 0.29 0.70 0.76
WP-3D, May 7 2383 0.49 -0.09 0.31 0.42 0.60
WP-3D, May 8 2304 0.78 -0.18 0.76 0.18 0.38
WP-3D, May 11 244 0.32 -0.03 0.22 0.36 0.61
WP-3D, May 12 ! ! ! ! ! !
WP-3D, May 14 1765 0.93 -0.24 0.49 0.82 0.81
WP-3D, May 16 2012 1.19 -0.20 0.53 0.73 0.82
WP-3D, May 19 2105 0.75 -0.19 0.37 0.83 0.81
WP-3D, May 21 434 0.74 -0.37 0.42 0.61 0.47
WP-3D, May 22 1912 0.51 -0.24 0.32 0.20 0.44
WP-3D, May 23 1907 0.35 0.12 0.27 0.41 0.59
WP-3D, May 24 1938 0.59 0.05 0.28 0.83 0.90
WP-3D, May 25 1879 1.16 -0.39 0.59 0.70 0.73
WP-3D, June 3 2215 1.26 -0.44 0.72 0.51 0.63
WP-3D, June 14 2440 0.55 -0.16 0.34 0.56 0.64
WP-3D, June 16 2368 0.78 -0.41 0.51 0.67 0.59
WP-3D, June 18 2341 0.48 -0.14 0.28 0.64 0.69
WP-3D, June 20 2389 0.99 -0.41 0.56 0.62 0.66
WP-3D, June 22 481 0.81 -0.38 0.56 0.35 0.49
Twin Otter, May 18 183 1.13 -0.70 1.23 -0.80 0.38
Twin Otter, May 19 146 0.77 0.44 0.57 0.56 0.58
Twin Otter, May 20 192 0.57 -0.08 0.46 -0.06 0.31
Twin Otter, May 21 192 0.50 0.13 0.25 0.41 0.57
Twin Otter, May 22 195 0.47 -0.21 0.29 0.67 0.59
Twin Otter, May 24 173 0.32 -0.02 0.11 0.62 0.65
Twin Otter, May 25 191 0.17 0.32 0.33 0.56 0.25
Twin Otter, May 27 176 0.80 -0.13 0.38 0.17 0.42
Twin Otter, May 28 192 0.69 -0.10 0.41 0.38 0.41

Table S40. Performance of simulated nitrate (NO
3
-
bias, RMSE, R, and IA for each for the G-1, WP-3D, and CIRPAS Twin Otter
flights.

Flight Date
Number
of Data
Points
Observed
Mean
(g/m3)
Bias
(g/m3) RMSE R IA
G-1, June 03a 674 0.12 0.00 0.11 0.07 0.37
G-1. June 06a 918 0.09 0.01 0.06 0.33 0.56
G-1, June 06b 510 0.10 -0.01 0.06 0.01 0.37
G-1, June 08a 946 0.21 -0.05 0.10 -0.04 0.38
G-1, June 08b 957 0.21 0.02 0.10 0.59 0.73
G-1, June 10a 882 0.07 0.02 0.05 0.07 0.39
G-1, June 12a 882 0.05 0.06 0.07 -0.08 0.40
G-1, June 12b 793 0.06 0.04 0.06 -0.05 0.43
G-1, June 14a 928 0.14 0.03 0.08 0.48 0.66
G-1, June 15a 878 0.17 -0.02 0.10 0.29 0.55
G-1, June 15b 882 0.20 0.07 0.17 0.14 0.30
G-1, June 18a 926 0.18 -0.04 0.19 0.37 0.60
G-1, June 19a 887 0.17 0.14 0.19 0.41 0.43
G-1, June 21a 899 0.14 0.01 0.08 0.12 0.41
G-1, June 21b 894 0.12 0.02 0.07 0.45 0.62
G-1, June 23a 944 0.21 -0.04 0.11 0.04 0.40
G-1, June 23b 874 0.25 -0.01 0.13 0.10 0.39
G-1, June 24a 934 0.15 0.02 0.12 0.16 0.48
G-1, June 24b 816 0.14 0.04 0.14 0.28 0.53
G-1, June 27a 960 0.21 0.02 0.08 0.62 0.75
G-1, June 28a 902 0.24 -0.04 0.10 0.44 0.55
G-1, June 28b 668 0.19 -0.03 0.10 0.50 0.52
WP-3D, May 4 1495 0.61 0.47 2.05 0.57 0.63
WP-3D, May 7 2383 0.89 0.41 1.52 0.63 0.72
WP-3D, May 8 2304 0.65 0.22 1.60 0.63 0.68
WP-3D, May 11 244 0.11 0.09 0.28 0.84 0.86
WP-3D, May 12 ! ! ! ! ! !
WP-3D, May 14 1765 0.82 0.75 2.23 0.34 0.50
WP-3D, May 16 2012 1.19 0.57 1.62 0.80 0.87
WP-3D, May 19 2105 2.95 -1.73 3.74 0.78 0.72
WP-3D, May 21 434 0.72 -0.26 0.83 0.89 0.93
WP-3D, May 22 1912 0.09 0.00 0.26 0.37 0.56
WP-3D, May 23 1907 0.07 -0.04 0.23 0.23 0.38
WP-3D, May 24 1938 0.29 0.50 1.79 0.64 0.49
WP-3D, May 25 1879 0.80 -0.13 1.22 0.59 0.76
WP-3D, June 3 2215 1.26 0.14 2.33 0.56 0.72
WP-3D, June 14 2440 0.13 -0.13 0.42 0.43 0.35
WP-3D, June 16 2368 0.36 -0.06 0.64 0.52 0.69
WP-3D, June 18 2341 0.30 -0.16 0.50 0.65 0.79
WP-3D, June 20 2389 0.45 -0.02 1.09 0.58 0.66
WP-3D, June 22 481 0.32 -0.11 0.94 0.95 0.85
Twin Otter, May 18 183 1.05 -0.53 1.39 0.65 0.73
Twin Otter, May 19 146 5.43 -2.42 3.44 0.59 0.62
Twin Otter, May 20 192 1.51 -0.20 1.99 0.49 0.67
Twin Otter, May 21 192 2.32 -1.17 2.33 0.31 0.56
Twin Otter, May 22 195 0.65 0.41 1.01 0.64 0.65
Twin Otter, May 24 173 0.94 -0.35 0.99 0.54 0.70
Twin Otter, May 25 191 0.81 0.55 1.68 0.57 0.61
Twin Otter, May 27 176 2.48 -2.22 2.89 0.32 0.47
Twin Otter, May 28 192 1.59 0.28 1.53 0.45 0.67

Table S41. Performance of simulated ammonium (NH
4
+
terms of bias, RMSE, R, and IA for each for the G-1, WP-3D, and CIRPAS Twin
Otter flights.

Flight Date
Number
of Data
Points
Observed
Mean
(g/m3)
Bias
(g/m3) RMSE R IA
G-1, June 03a 674 0.09 0.04 0.21 0.11 0.25
G-1. June 06a 918 0.13 -0.13 0.16 -0.22 0.43
G-1, June 06b 510 0.11 -0.11 0.14 0.01 0.42
G-1, June 08a 946 0.42 -0.35 0.41 -0.04 0.35
G-1, June 08b 957 0.29 -0.27 0.34 -0.01 0.43
G-1, June 10a 882 0.11 -0.11 0.15 0.06 0.38
G-1, June 12a 882 0.06 -0.06 0.07 -0.03 0.39
G-1, June 12b 793 0.10 -0.10 0.10 ! 0.30
G-1, June 14a 928 0.34 -0.34 0.40 0.06 0.43
G-1, June 15a 878 0.47 -0.24 0.40 0.40 0.58
G-1, June 15b 882 0.53 -0.24 0.57 0.09 0.38
G-1, June 18a 926 0.60 -0.41 1.00 0.38 0.48
G-1, June 19a 887 0.25 -0.24 0.29 0.05 0.40
G-1, June 21a 899 0.31 -0.31 0.50 0.01 0.32
G-1, June 21b 894 0.19 -0.19 0.24 -0.11 0.42
G-1, June 23a 944 0.40 -0.38 0.48 -0.11 0.30
G-1, June 23b 874 0.36 -0.25 0.46 -0.02 0.30
G-1, June 24a 934 0.23 -0.20 0.31 -0.15 0.39
G-1, June 24b 816 0.25 -0.25 0.29 0.01 0.41
G-1, June 27a 960 0.43 -0.43 0.47 0.19 0.39
G-1, June 28a 902 0.61 -0.61 0.69 -0.14 0.40
G-1, June 28b 668 0.40 -0.40 0.45 -0.13 0.39
WP-3D, May 4 1495 0.36 0.12 0.67 0.57 0.70
WP-3D, May 7 2383 0.48 0.03 0.48 0.64 0.79
WP-3D, May 8 2304 0.50 -0.10 0.56 0.57 0.71
WP-3D, May 11 244 0.10 0.01 0.10 0.83 0.90
WP-3D, May 12 ! ! ! ! ! !
WP-3D, May 14 1765 0.61 0.06 0.66 0.54 0.72
WP-3D, May 16 2012 0.86 -0.01 0.55 0.82 0.90
WP-3D, May 19 2105 1.15 -0.62 1.25 0.80 0.73
WP-3D, May 21 434 0.50 -0.27 0.44 0.88 0.88
WP-3D, May 22 1912 0.20 -0.11 0.19 0.18 0.49
WP-3D, May 23 1907 0.13 0.02 0.20 0.10 0.29
WP-3D, May 24 1938 0.31 0.13 0.50 0.73 0.75
WP-3D, May 25 1879 0.64 -0.17 0.49 0.67 0.79
WP-3D, June 3 2215 0.80 -0.11 0.74 0.63 0.78
WP-3D, June 14 2440 0.18 -0.08 0.23 0.58 0.57
WP-3D, June 16 2368 0.37 -0.19 0.32 0.61 0.72
WP-3D, June 18 2341 0.21 -0.11 0.24 0.75 0.79
WP-3D, June 20 2389 0.45 -0.17 0.44 0.56 0.69
WP-3D, June 22 481 0.34 -0.14 0.42 0.90 0.77
Twin Otter, May 18 183 0.73 -0.46 0.75 0.44 0.55
Twin Otter, May 19 146 2.31 -1.01 1.33 0.47 0.53
Twin Otter, May 20 192 1.05 -0.54 0.79 0.65 0.66
Twin Otter, May 21 192 1.49 -1.03 1.28 0.30 0.49
Twin Otter, May 22 195 0.43 -0.07 0.33 0.58 0.74
Twin Otter, May 24 173 0.40 -0.16 0.39 0.49 0.65
Twin Otter, May 25 191 0.43 0.11 0.50 0.55 0.67
Twin Otter, May 27 176 1.23 -0.93 1.16 0.14 0.45
Twin Otter, May 28 192 0.85 -0.11 0.57 0.22 0.55

Figure S1. Directory structure of the Aerosol Modeling Testbed for the CalNex/CARES testbed
case. Blue, red, and green denote data from CalNex, CARES, and both campaigns,
respectively.

Figure S2. Time series (left panels) and diurnal average (right panels) of (a) temperature, (b)
relative humidity, (c) downward shortwave radiation, (d) wind speed, and (e) wind
direction at the Pasadena supersite. Observed values are hourly averages, while
simulated values are instantaneous values at hourly intervals. Gray shading denotes
night and R is the correlation coefficient.

Figure S3. Observed and simulated diurnally-averaged wind speed and direction over the 2-
month period approximately 1 km AGL at the (a) SAC, (b) BAK, and (c) USC radar
wind profiler sites. Gray shading denotes night

Figure S4. Comparison of observed and simulated wind speed and direction over May and June
2010 approximately 1 km AGL at the (a) SAC, (b), BAK, and (c) USC radar wind
profiler sites.

Figure S5. Observed and simulated carbon monoxide (CO) at the (a) Pasadena, (b) Bakersfield,
(c) T0, and (d) T1 supersites. Gray shading denotes night.

Figure S6. Observed and simulated nitrogen oxide (NO) at the (a) Pasadena, (b) Bakersfield, and
(c) T0 supersites. Gray shading denotes night.

Figure S7. Observed and simulated nitrogen dioxide (NO
2
) at the (a) Pasadena, (b) Bakersfield,
and (c) T0 supersites. Gray shading denotes night.

Figure S8. Observed and simulated ammonia (NH
3
) at the (a) Pasadena and (b) Bakersfield
supersites. Gray shading denotes night.

Figure S9. Observed and simulated nitric acid (HNO3
3
) at the (a) Pasadena and (b) Bakersfield

Figure S10. Observed and simulated sulfur dioxide (SO
2
) at the (a) Pasadena, (b) Bakersfield, and
(c) T0 supersites. Gray shading denotes night.

Figure S11. Observed and simulated isoprene at the (a) Pasadena, (b) Bakersfield, (c) T0, and (d)
T1 supersites. Gray shading denotes night.

Figure S12. Observed and simulated terpene at the (a) Pasadena, (b) T0, and (c) T1 supersites.
Gray shading denotes night.

Figure S13. Observed and simulated methyl-vinyl-ketone + methacrolein (MVK+MACR) at the
(a) Pasadena, (b) T0, and (c) T1 supersites. Gray shading denotes night.

Figure S14. Observed and simulated toluene at the (a) Pasadena, (b) Bakersfield, (c) T0, and (d)
T1 supersites. Gray shading denotes night.

Figure S15. Observed and simulated formaldehyde (CH
2
O) at the (a) Pasadena, (b) Bakersfield,
(c) T0, and (d) T1 supersites. Gray shading denotes night.

Figure S16. Observed and simulated ozone at the (a) Pasadena, (b) Bakersfield, (c) T0, and (d) T1

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Atmos. Chem. Phys.

, 14, 1001310060, 2014

showed that while predicted annual mean

W, 240 mm.s.l.) (Chan

W, 123 mm.s.l.) (Alm et al.,

W, 30 mm.s.l.) and the other in

W, 450 mm.s.l.), a small

) G-1 23 988 195.0 9.6 57.60 0.36 0.84

N (as high as 5.6 kmm.s.l.), and the entire RV-Atlantis

N, (c) WP-3D ight ights south of 35

N, and (d) the

N, and (c) WP-3D ight ights south of 35

N. Vertical lines denote 5th

N have similar medians and range of

N, except that the overall con-

is too low while the simulated PM

N where the simulated val-

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