Journal of Environmental Radioactivity 140 (2015) 114e122

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Journal of Environmental Radioactivity

journal homepage: www.elsevier.com/locate/jenvrad

Impact of Fukushima-derived radiocesium in the western North

Pacic Ocean about ten months after the Fukushima Dai-ichi nuclear
power plant accident
Yuichiro Kumamoto a, *, Michio Aoyama b, Yasunori Hamajima c, Akihiko Murata a,
Takeshi Kawano a
a

Research and Development Center for Global Change, Japan Agency for Marine-Earth Science and Technology, 2-15 Natushima-cho, Yokosuka, Kanagawa
237-0061, Japan
Institute of Environmental Radioactivity, Fukushima University, 1-1 Kanayagawa, Fukushima 960-1296, Japan
c
Low Level Radioactivity Laboratory, Kanazawa University, Wake, Nomi, Ishikawa 923-1224, Japan
b

a r t i c l e i n f o

a b s t r a c t

Article history:
Received 3 July 2014
Received in revised form
7 November 2014
Accepted 14 November 2014
Available online

We measured vertical distributions of radiocesium (134Cs and 137Cs) at stations along the 149
E meridian
in the western North Pacic during winter 2012, about ten months after the Fukushima Dai-ichi Nuclear
Power Plant (FNPP1) accident. The Fukushima-derived 134Cs activity concentration and water-column
inventory were largest in the transition region between 35 and 40
N approximately due to the
directed discharge of the contaminated water from the FNPP1. The bomb-derived 137Cs activity concentration just before the FNPP1 accident was derived from the excess 137Cs activity concentration
relative to the 134Cs activity concentration. The water-column inventory of the bomb-derived 137Cs was
largest in the subtropical region south of 35
N, which implies that the Fukushima-derived 134Cs will also
be transported from the transition region to the subtropical region in the coming decades. Mean values of
the water-column inventories decay-corrected for the Fukushima-derived 134Cs and the bomb-derived
137
Cs were estimated to be 1020 80 and 820 120 Bq m2, respectively, suggesting that in winter
2012 the impact of the FNPP1 accident in the western North Pacic Ocean was nearly the same as that of
nuclear weapons testing. Relationship between the water-column inventory and the activity concentration in surface water for the radiocesium is essential information for future evaluation of the total
amount of Fukushima-derived radiocesium released into the North Pacic Ocean.
2014 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license
(http://creativecommons.org/licenses/by/3.0/).

Keywords:
Fukushima Dai-ichi nuclear power plant
accident
Radiocesium
Seawater
Western North Pacic Ocean
Nuclear weapons testing

1. Introduction
The massive Tohoku earthquake and consequent giant tsunamis
on 11 March 2011 resulted in serious damage to the Fukushima Daiichi Nuclear Power Plant (FNPP1) in eastern Japan (Prime Minister
of Japan and His Cabinet, 2011). Radiocesium (134Cs and 137Cs)
derived from the damaged FNPP1 caused radioactive contamination of the islands of Japan and the North Pacic Ocean (Yoshida
and Kanda, 2012). Most of the Fukushima-derived radiocesium
deposited on the Japanese islands has remained in the soil, and
measurement of radiocesium activity in the soil (Nuclear
Regulation Authority, 2012) has revealed that the radioactivities

* Corresponding author. Tel.: 81 46 867 9505; fax: 81 46 867 9835.

E-mail address: kumamoto@jamstec.go.jp (Y. Kumamoto).

of 134Cs and 137Cs released from the FNPP1 were approximately

equivalent. The estimated total amount of 137Cs (or 134Cs) activity in
the islands of Japan is 2.4 PBq (1015 Bq), based on soil measurements and the air dose rate derived from airborne monitoring
(Morino et al., 2013). In contrast, radiocesium released into the
North Pacic Ocean was immediately diluted by water advection
and diffusion. As a result, it has been difcult to collect enough
seawater samples for a quantitative discussion of the total amount
of Fukushima-derived radiocesium in the vast ocean.
The Fukushima-derived radiocesium were released into the
North Pacic, mostly in March and April 2011, through two major
pathways: direct discharge of radioactive water and atmospheric
deposition. In late March 2011, the Tokyo Electric Power Company
and the Japanese Government began marine monitoring in the
coastal area within a radius of about 30 km from the FNPP1
(Nuclear Regulation Authority, 2011; Oikawa et al., 2013; Tokyo

http://dx.doi.org/10.1016/j.jenvrad.2014.11.010
0265-931X/ 2014 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/3.0/).

Y. Kumamoto et al. / Journal of Environmental Radioactivity 140 (2015) 114e122

Electric Power Company, 2011). The decay-corrected 134Cs/137Cs

ratio in those monitoring data was almost 1 and in agreement with
the ratio in standing water in the damaged FNPP1 (Nishihara et al.,
2012). Thus, the activity concentrations of 134Cs and 137Cs in the
radioactive water directly discharged from the FNPP1 were also
approximately equivalent. These measurements have facilitated
evaluation of the total amount of 137Cs (or 134Cs) derived from the
directly discharged radioactive water. Many estimations were in
the range between 2 and 6 PBq (Estournel et al., 2012; Kawamura
et al., 2011; Miyazawa et al., 2013; Nair et al., 2014; Prime
Minister of Japan and His Cabinet, 2011; Tsumune et al., 2012).
However, temporal or spatial extrapolating in the calculation
resulted in a larger amount ranged from 11 to 27 PBq (Bailly du Bois
et al., 2012; Charette et al., 2013; Rypina et al., 2013).
Efforts to obtain data of Fukushima-derived radiocesium in the
open ocean have continued, and radiocesium measurements made in
both surface water (Aoyama et al., 2013; Honda et al., 2012;
Kaeriyama et al., 2013; Kamenk et al., 2013; Karasev, 2012) and the
ocean interior (Buesseler et al., 2012; Kaeriyama et al., 2014;
Kumamoto et al., 2014; Povinec et al., 2013; Ramzaev et al., 2014)
have been reported. These data obtained in the open ocean have
revealed that the Fukushima-derived radiocesium released into the
North Pacic Ocean has been transported eastward by surface currents and conveyed southward across the Kuroshio Extension current
in subsurface layers. However, the available data are still insufcient
for evaluation of the total amount of radiocesium, including that from
atmospheric deposition, in the vast North Pacic Ocean. Atmospheric
deposition has been estimated by using atmospheric model simulations (Estournel et al., 2012; Kawamura et al., 2011; Kobayashi et al.,
2013; Miyazawa et al., 2013; Morino et al., 2011, 2013; Stohl et al.,
2012). The results of these model simulations consistently show
that a large portion of the radiocesium released to the atmosphere
from the FNPP1 was subsequently deposited on the North Pacic
Ocean. However, the simulated total amount of 137Cs (or 134Cs)
deposited on the ocean ranges widely, from 5 to 30 PBq.
The two major isotopes in the Fukushima-derived radiocesium
are 134Cs and 137Cs. These radiocesium isotopes were also released
into the environment before the FNPP1 accident by atmospheric
nuclear weapons testing, mainly in the 1950s and 1960s; nuclear
fuel reprocessing, mainly in the 1980s; and the Chernobyl accident
in 1986. In the North Pacic Ocean the major source of radiocesium
was atmospheric deposition due to the nuclear weapons testing
(Aoyama et al., 2006). The bomb-derived 137Cs released into the
North Pacic was still there just before the accident because its
half-life is long, 30.04 y. In the 2000s, 137Cs activity concentration of
1.0e2.5 Bq m3 was widely observed in surface seawaters of the
North Pacic Ocean (Aoyama et al., 2012a). After the FNPP1 accident, the Fukushima-derived 137Cs was of course added to the
bomb-derived 137Cs. In contrast, the 134Cs released before the accident had disappeared, because its half-life is only 2.07 y, which
indicates that 134Cs can be used as a tracer of radiocesium from the
FNPP1 accident. The Fukushima-derived radiocesium measurements in the past suggested that the activities of 134Cs and 137Cs
released from the FNPP1 were equivalent. Thereby, after the decaycorrection, the excess 137Cs activity concentration relative to the
134
Cs activity concentration in seawaters collected after the FNPP1
accident represents the bomb-derived 137Cs activity concentration.
By measuring both 134Cs and 137Cs activity concentrations, both the
Fukushima-derived and the bomb-derived 137Cs activity concentrations can be determined simultaneously. A few studies have
already calculated the bomb-derived 137Cs activity concentrations
in seawaters of the North Pacic Ocean in this way (Inoue et al.,
2012; Kamenk et al., 2013; Ramzaev et al., 2014). However, they
did not compare the activity concentrations and inventories of the
Fukushima-derived and bomb-derived 137Cs quantitatively.

115

Here we report the vertical distributions of 134Cs and 137Cs activity concentrations at stations along 149
E between approximately 42
N and 4
S in winter 2012, about ten months after the
FNPP1 accident. We preliminarily reported the distribution and
behavior of the Fukushima-derived 134Cs only prior to the bombderived 137Cs along this meridional line between 42
N and 10
N
(Kumamoto et al., 2014). In the preliminary report, we found that
activity concentration of the Fukushima-derived 134Cs in surface
water was highest in the transition region between the subarctic
and Kuroshio Extension fronts (approximately 35e40
N), where
the FNPP1 is situated (Fig. 1). In addition, a subsurface maximum of
the Fukushima-derived 134Cs was found in the subtropical region
south of the Kuroshio Extension Current, and southward transportation of the Fukushima-derived 134Cs was evaluated. In this
report, we (1) additionally publish 134Cs and 137Cs activity concentrations observed between 10
N and 4
S, which was not
published in the previous report, (2) compare them between 42
N
and 4
S to estimate the bomb-derived 137Cs, which was not
calculated in the previous report, and (3) discuss the impact of the
Fukushima-derived radiocesium on the bomb-derived radiocesium, which had existed since before the FNPP1 accident, in the
western North Pacic in winter 2012. In addition, we evaluated the
relationship between the activity concentration in surface water
and the water-column inventory of the radiocesium. These results
will contribute to the eventual determination of the total amount of
the Fukushima-derived radiocesium in the North Pacic Ocean.
2. Samples and experimental procedures
Seawater samples for radiocesium measurements (about
20 dm3 each) were collected during cruise MR11-08 of the Research
Vessel Mirai from December 2011 to February 2012. This cruise also
performed repeat hydrography along one of the observation lines of
the World Ocean Circulation Experiment (WOCE) in the western
Pacic Ocean (the WOCE-P10/P10N line), which approximately
follows the 149
E meridian. We collected surface seawater using a
bucket at 38 stations along the line between 42
N and 4
S (Fig. 1).
Along this line, the area north of the subarctic front (approximately
40
N) is dened as the subarctic region, that south of the Kuroshio
Extension front (approximately 35
N) is dened as the subarctic,
and the area between the two fronts, in which the FNPP1 is also
situated, is designated the transition region (Fig. 1) (Kumamoto
et al., 2014). Although the boundary between the subtropical and
tropical regions is not clear, the area south of the North Equatorial
current (approximately 12
N) is provisionally regarded as the
tropical region. At 18 of the 38 stations, seawater samples from the
surface to 800 m depth were collected using 12-Liter polyvinyl
chloride bottles (Model 1010X NISKIN-X, General Oceanics Inc.).
The seawater was ltered through a 0.45 mm pore size membrane
lter (HAWP14250, Millipore) and acidied on board ship by adding 40 cm3 of concentrated nitric acid (Nitric Acid 70% AR, RCI
Labscan, Ltd.) within 24 h after sampling. After the cruise, radiocesium in the seawater sample was concentrated on ammonium
phosphomolybdate (Aoyama and Hirose, 2008) in onshore laboratories for measurement of gamma-ray activity.
The radiocesium activity of the ammonium phosphomolybdate
was measured in a laboratory of the Mutsu Oceanographic Institute
at the Japan Agency for Marine-Earth Science and Technology
(MIO/JAMSTEC) or the Low Level Radioactivity Laboratory at
Kanazawa University (LLRL/KU). In the MIO/JAMSTEC laboratory,
the radiocesium was measured with low-background Ge-detectors
(Well-type GCW2022-7915-30-ULB, Canberra Industries, Inc.) that
were calibrated with gamma-ray volume sources (Eckert & Ziegler
Isotope Products) certied by Deutscher Kalibrierdienst. The averages of the analytical uncertainties (standard deviations) for the

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Y. Kumamoto et al. / Journal of Environmental Radioactivity 140 (2015) 114e122

Fig. 1. Water sampling locations for radiocesium measurements. White circles denote stations for surface sampling only, and black circles denote stations where a deep hydrocast to
a depth of 800 m was also made. The cross shows the location of the Fukushima Dai-ichi Nuclear Power Plant. Arrows schematically show the locations and directions of surface
currents in the North Pacic Ocean. The map in this gure was drawn using Ocean Data View software (Schlitzer, 2014).

134

Cs and 137Cs measurements were calculated to be 13% and 7%,

respectively; this 134Cs uncertainty includes the uncertainty of the
cascade summing effect. The radiocesium activity concentration
was also measured in the LLRL/KU laboratory with ultra-lowbackground Ge-detectors (Hamajima and Komura, 2004). The averages of the analytical uncertainties for 134Cs and 137Cs were
calculated to be 11% and 6%, respectively. Activities of 134Cs and
137
Cs in certied reference materials, IAEA-443 (Pham et al., 2011)
and IAEA-445 (International Atomic Energy Agency, 2011) were
also measured, and the results obtained in the two laboratories
agreed within the uncertainties. This agreement conrms the
comparability of the radiocesium measurements performed in the
two laboratories. Details of the sampling and analytical methods
above were given in Kumamoto et al. (2014).
We also measured 137Cs activity concentration at seven stations
along the 149
E meridian between 15
N and 22
N in June 2005
during cruise MR05-02. The surface seawaters (about 20 dm3 each)
were collected using a pump from about 4 m depth and the deeper
seawaters (about 6e20 dm3 each) to 800 m depth were collected

using 12-L polyvinyl chloride bottles (Model 1010X NISKIN-X,

General Oceanics Inc.). The seawater was ltered through the lter and acidied on board ship by adding of the concentrated nitric
acid. After the cruise, 137Cs in the seawater sample was concentrated on ammonium phosphomolybdate (Aoyama and Hirose,
2008). The 137Cs activity concentration was measured in the LLRL/
KU laboratory with the ultra-low-background Ge-detectors. The
134
Cs activity concentration in the samples collected in June 2005
was lower than the detection limit, about 0.1 Bq m3.
3. Results and discussion
3.1.

134

Cs versus

137

Cs activity concentrations

Activity concentrations of 134Cs and 137Cs measured in winter 2012

and June 2005, decay-corrected to the date of the FNPP1 accident (11
March 2011), are shown in the supplementary data table. The 134Cs
and 137Cs activity concentrations in winter 2012 show an approximately one-to-one relationship (Fig. 2; slope 1.009 0.006), which

Y. Kumamoto et al. / Journal of Environmental Radioactivity 140 (2015) 114e122

Fig. 2. Scatter plot of 137Cs activity concentration (Bq m3) against 134Cs activity
concentration (Bq m3) in seawaters collected at stations along approximately 149
E
meridian in winter 2012. The activity concentrations have been corrected to the date of
the accident, 11 March 2011. The error bars indicate measurement standard deviations.
The solid line shows the one-to-one relationship between 134Cs and 137Cs activity
concentrations. Linear regression analysis of the data yielded the equation
[137Cs] 1.009 [134Cs] 1.10 (r2 0.993, n 217).

is consistent with the isotopic relationships in the North Pacic Ocean

reported by previous studies (Aoyama et al., 2012a, 2012b; Buesseler
et al., 2012; Inoue et al., 2012; Kaeriyama et al., 2013; Kamenk et al.,
2013; Kofuji and Inoue, 2013; Ramzaev et al., 2014) and which also
supports the assumption that the total radioactivities of Fukushimaderived 134Cs and 137Cs released into the North Pacic Ocean were
approximately equivalent. The intercept value, 1.10 0.04 Bq m3
(Fig. 2), represents the average excess 137Cs relative to 134Cs activity
concentrations decay-corrected. In the North Pacic Ocean, as
mentioned above, most of the excess 137Cs was derived from the
nuclear weapons testing. Therefore the excess 137Cs is expressed as
the bomb-derived 137Cs. The average bomb-derived 137Cs activity
concentration, 1.1 Bq m3 agrees with reported values in the North
Pacic (1.0e1.7 Bq m3) in previous works (Buesseler et al., 2012;
Inoue et al., 2012; Kamenk et al., 2013; Kofuji and Inoue, 2013;
Ramzaev et al., 2014).
3.2. Activity concentration in surface water
In winter 2012, the Fukushima-derived 134Cs activity concentration in surface seawater along approximately 149
E was highest
(more than 20 Bq m3) in the transition region between 35
N and
40
N (Fig. 3). In the adjacent subarctic and subtropical regions the
activity concentration decreased sharply at greater distances from
the FNPP1. This latitudinal distribution was mainly derived from the
direct discharge of contaminated water from the FNPP1 (Kumamoto
et al., 2014). At stations in the south of 25
N and at 42
N, the activity
concentration in surface water less than 1 Bq m3 was detected. The
widespread distribution of Fukushima-derived 134Cs from 42
N to
4
S in the North Pacic Ocean can be attributed to atmospheric
deposition. In an atmospheric model simulation, the Fukushimaderived 134Cs spread to the tropical region (Kobayashi et al., 2013).
However, to the south of 20
N, 134Cs was detected only in surface
waters collected using the bucket, which is unlikely because
seawater in surface mixed layer (to approximately 200 m depth) is
well mixed vertically. It is implied that a little radioactive contamination on the bucket during the cruise (Kumamoto et al., 2014).
The bomb-derived 137Cs in surface seawater ranged between 0.4
and 2.2 Bq m3 (Fig. 3) in winter 2012. The mean value in the

117

Fig. 3. Activity concentrations (Bq m3) of the Fukushima-derived 134Cs (open circles)
and the bomb-derived 137Cs (closed circles) in surface water along approximately
149
E meridian in winter 2012. All of the radiocesium data were decay-corrected to 11
March 2011. Activity concentrations of 137Cs (Bq m3) in surface water observed in
2005, which were corrected to the date of the accident by using the apparent half-life
of 13 y (Povinec et al., 2005), are also shown (open triangles). The error bars indicate
standard deviations. The bomb-derived 137Cs activity concentration in the surface
water at station P10-102 is not shown because a negative value was calculated. The
vertical broken lines indicate the approximate boundaries between the four regions
(tropical, subtropical, transition, and subarctic).

tropical region south of 12
N and the subtropical region between

12
N and 35
N were 1.2 0.2 Bq m3 (n 9) and 1.5 0.1 Bq m3
(n 17), respectively. In the transition and subarctic regions north
of the Kuroshio Extension, the mean value of 1.1 0.5 Bq m3
(n 12) coincides with those in the tropical and subtropical regions
within the error range. Small spatial variation in the activity concentration in surface water was also observed in the 2000s
(Aoyama et al., 2012a). As a result, the bomb-derived 137Cs activity
concentration was higher (lower) than the Fukushima-derived
134
Cs activity concentration at most stations in the tropical and
subtropical (transition and subarctic) regions south (north) of the
Kuroshio Extension Current, suggesting larger impact of the directdischarged contaminated water on the radiocesium activity concentration in the western North Pacic Ocean.
In June 2005, about 6 y before the FNPP1 accident, we also
measured 137Cs activity concentration in surface waters collected at
stations between 15
N and 22
N along 149
E meridian. Activity
concentration of 137Cs in surface water in 2005 ranged from 1.7 to
2.5 Bq m3. During the past several decades, 137Cs activity concentration in the surface seawater in the open ocean has decreased
(Hirose and Aoyama, 2003; Inomata et al., 2009; Povinec et al.,
2005) at an apparent rate (or half-life) of about 2e10%/y (i.e, a
half-life of 5e30 y). This apparent half-life, which is shorter than
that due to radioactive decay (30.04 y), suggests that the surface
137
Cs has been diluted by mixing of the surface water with deeper
water in which the 137Cs activity concentration is low. For the North
Pacic Ocean, the apparent half-life of 137Cs in surface water has
been calculated to be 13 1 y (Povinec et al., 2005). We corrected
the activity concentrations of 137Cs in surface water obtained in
2005 to the date of the FNPP1 accident by using this apparent halflife of 13 1 y and obtained good agreement between the decaycorrected 137Cs activity concentrations in 2005 (open triangles in
Fig. 3) and the bomb-derived 137Cs in winter 2012. This agreement
validates that the bomb-derived 137Cs calculated corresponds to
137
Cs just before the FNPP1 accident.
3.3. Vertical distribution and water-column inventory
Vertical proles of the Fukushima-derived 134Cs activity concentration in winter 2012 are shown in Fig. 4. The activity concentration in the surface mixed layer (to approximately 200 m

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Y. Kumamoto et al. / Journal of Environmental Radioactivity 140 (2015) 114e122

Fig. 4. Vertical proles of the activity concentrations (Bq m3) of the Fukushima-derived 134Cs (open circles) and the bomb-derived 137Cs (closed circles) at stations P10-023 (a and f,
1.3
N/146.5
E), P10-060 (b and g, 19.8
N/149.3
E), P10-077 (c and h, 30.0
N/149.3
E), P10-098 (d and i, 37.4
N/147.2
E), and P10-106 (e and j, 40.1
N/145.4
E). All of the
radiocesium data were decay-corrected to 11 March 2011. Activity concentrations of 137Cs (Bq m3) observed in 2005 at stations P10-060 and 062 (g, 19.8
N/149.3
E and 21.2
N/
149.3
E, respectively), which were corrected to the date of the accident by using the apparent half-life of 13 y (Povinec et al., 2005), are also shown (open triangles). The error bars
indicate standard deviations. A datum without the error bar indicates that the activity concentration was below detection limit.

depth) was almost uniform vertically. As a result, the activity concentration in the mixed layer was highest in the transition region
(Fig. 4d) as shown in the latitudinal distribution of the activity
concentration in surface water. In the transition and subarctic regions (Fig. 4d, e), the activity concentration decreased monotonically with depth below the mixed layer. This vertical prole in
the transition and subarctic regions can be primarily explained by
vertical mixing between the surface mixed and deeper layers and
by upwelling of deep water. In the subtropical region south of the
Kuroshio Extension, the activity concentration in the surface mixed
layer was lower than those in the transition and subarctic regions.
However, just below the surface mixed layer around 200e400 m
depth, there were subsurface maxima (Fig. 4b, c). From a crosssectional view, Kumamoto et al. (2014) found that a tongueshaped subsurface plume of the Fukushima-derived 134Cs between 35 and 20
N in the subtropical region. Because this subsurface plume appeared on a subsurface minimum of potential
vorticity, they concluded that the Fukushima-derived 134Cs subsurface maximum was derived from formation and subduction of
the Subtropical Mode Water (STMW, Masuzawa, 1969). In the
tropical region, the Fukushima-derived 134Cs was not observed
except in the surface water (Fig. 4a).
Vertical proles of the bomb-derived 137Cs activity concentration in winter 2012 are also shown in Fig. 4. In the tropical region
(Fig. 4f) the bomb-derived 137Cs activity concentration was almost
uniform vertically in the surface mixed layer, and then it decreased
monotonically with depth. Similar vertical proles of the bombderived 137Cs were observed in the transition and subarctic regions (Fig. 4i, j) north of the Kuroshio Extension, although the uncertainties of the activity concentrations in the surface mixed layer
were large. The vertical proles in the tropical, transition, and

subarctic regions can be primarily explained by one-dimensional

advection-diffusion model as same as those of the Fukushimaderived 134Cs were.
In the subtropical region (Fig. 4g, h), as in the other regions, the
bomb-derived 137Cs activity concentration was uniform in the
surface mixed layer, but just below the mixed layer, in the
200e600 m approximate depth range, we observed a subsurface
maximum. Below this maximum, the activity concentration
decreased with depth. A similar subsurface 137Cs maximum was
also observed at stations in the subtropical region in 2005 (open
triangles in Fig. 4g). Vertical proles of 137Cs activity concentration
in 2005 agreed with those of the bomb-derived 137Cs in winter
2012 after decay-correction to the FNPP1 accident date. In addition,
the subsurface maximum in the subtropical region has been reported since the 1970s (Aoyama et al., 2008; Povinec et al., 2003).
Aoyama et al. (2008) proposed that the subsurface 137Cs maximum
was due to subduction and horizontal movement of the mode
waters, STMW and the denser Central Mode Water (CMW, Suga
et al., 1997) and that the bomb-derived 137Cs circulated clockwise
in the North Pacic Ocean along the subtropical gyre. Radiocarbon
(14C) concentrations due to nuclear weapons testing, like 137Cs activity concentrations, also show a similar subsurface maximum in
the subtropical region of the North Pacic (Kumamoto et al., 2013).
The bomb-derived 137Cs, which originated mainly from the
nuclear weapons testing in the 1950s and 1960s, is now, about a
half century since its atmospheric deposition in the North Pacic
Ocean, accumulated in the subsurface of about 200e600 m depth
in the subtropical region and is recirculating within the subtropical
gyre due to formation and the subduction of STMW and CMW. The
Fukushima-derived 134Cs was also transported into the subtropical
region, which occurred within 1 y as a result of STMW formation

Y. Kumamoto et al. / Journal of Environmental Radioactivity 140 (2015) 114e122

and subduction around 200e400 m depth (Kaeriyama et al., 2014;

Kumamoto et al., 2014). The shallower penetration of the
Fukushima-derived 134Cs than the bomb-derived 137Cs was derived
from slower advection speed of denser CMW. The Fukushimaderived 134Cs activity concentration was still high in the transition region than in other regions because of the direct discharge of
contaminated water from the FNPP1, which is located at 37.4
N
(Fig. 1). The behavior of the bomb-derived 137Cs in past decades
suggests that the Fukushima-derived 134Cs will become concentrated in the subtropical region due to formation of the mode waters (Kumamoto et al., 2014).
We determined the vertical water-column inventory (Bq m2) of
the Fukushima-derived 134Cs between surface and 800 m depth by
simple trapezoidal integration of the activity concentration versus
depth proles (Fig. 5). The total amount of the Fukushima-derived
134
Cs activity along the meridional line (Bq m1) in the each region
was also calculated by simple trapezoidal integration of the watercolumn inventory versus distance between the stations. Then a
mean of the water-column inventory (Bq m2) in the each region
was determined by division of the total amount (Bq m1) by the
total distance between the northernmost and southernmost stations in the region. Among the four regions, the mean inventory of
the Fukushima-derived 134Cs was largest in the transition region
(4710 310 Bq m2) because of the direct discharge of contaminated water from the FNPP1. The mean inventories in the adjacent
subarctic and subtropical regions were just 760 70 and
1300 110 Bq m2, respectively, but in the northern subtropical
region, where the subsurface maximum of 134Cs was observed, the
inventories were as large as those in the transition region. By
contrast, the 134Cs inventories were less than 5 Bq m2 in the
tropical region, where 134Cs was observed only in surface seawater.
We also show the water-column inventories of the bombderived 137Cs for comparison with the Fukushima-derived 134Cs
inventories (Fig. 5). The mean inventory of the bomb-derived 137Cs
was calculated to be 510 30 and 590 120 Bq m2 in the tropical
and subarctic regions, respectively. These values are signicantly
lower than the water-column inventory in the subtropical region,
1080 150 Bq m2. The larger mean water-column inventory in the
subtropical region reects the subsurface maximum there (Fig. 4g,
h), and the water-column inventories of the 137Cs activity concentrations in 2005, decay-corrected to the FNPP1 accident date in this

Fig. 5. Water-column inventories (Bq m2) between surface and 800 m depth of the
Fukushima-derived 134Cs (open circles) and the bomb-derived 137Cs (closed circles)
along approximately 149
E meridian in winter 2012. All of the radiocesium data were
decay-corrected to 11 March 2011. Water-column inventories of 137Cs (Bq m2)
observed in 2005, which were corrected to the date of the accident by using the
apparent half-life of 13 y (Povinec et al., 2005), are also shown (open triangles). Error
bars show standard deviations. In the inventory calculations, data with a standard
deviation (error) larger than the measured value were omitted to reduce uncertainty.
Closed triangles indicate latitudinal locations of ve stations where vertical proles of
the radiocesium were shown in.Fig. 4.

119

region agreed well with the winter 2012 inventories (open triangles
in Fig. 5). The mean inventory of the bomb-derived 137Cs in the
transition region of 900 Bq m2 is comparable to that in the subtropical region, although the uncertainty (370 Bq m2) is large.
The mean inventory of the Fukushima-derived 134Cs was larger
than that of the bomb-derived 137Cs in the subarctic, transition, and
subtropical regions. The decay-corrected ratio of the 134Cs and 137Cs
inventories was calculated to be 1.3 0.3 and 1.2 0.2 in the
subarctic and subtropical regions, respectively. The larger ratio of
5.2 2.2 (4710 310 Bq m2 versus 900 370 Bq m2) in the
transition region suggests a higher impact of the Fukushimaderived radiocesium there. The mean inventories of the
Fukushima-derived 134Cs and the bomb-derived 137Cs along the
whole meridional line between 42
N and 4
S, decay-corrected to
the date of the FNPP1 accident, were estimated to be 1020 80 and
820 120 Bq m2, respectively. The overall ratio of the Fukushimaderived 134Cs versus the bomb-derived 137Cs inventories, 1.3 0.2,
suggests that in winter 2012 in the western North Pacic Ocean the
impact of the FNPP1 accident was nearly the same as that of the
nuclear weapons tests.
3.4. Relation between activity concentration in surface water and
water-column inventory
We plotted the water-column inventories against activity concentrations in surface water for the bomb-derived 137Cs (Fig. 6a)
and obtained two clusters of data, one for the subtropical and the
other for the subarctic/tropical regions. We calculated regression
lines for each data cluster passing through the origin. The calculated slopes of these regressions, about 720 m for the subtropical
region and about 450 m for the subarctic/tropical regions, indicate
the mean penetration depth (MPD), dened as the water-column
inventory (Bq m2) divided by the activity concentration in surface water (Bq m3), of the bomb-derived 137Cs in winter 2012. The
MPD is an indicator of the one-dimensional penetration of the
tracer into the ocean, and it is proportional to the square root of the
penetration time. The larger MPD in the subtropical region (720 m)
compared with that in the subarctic and tropical regions (450 m)
implies that in the subtropical region the bomb-derived 137Cs
intruded deeply into the ocean interior as a result of the convergence of surface waters there. However, estimation of the MPD in
the subtropical region was disturbed by the subsurface maximum
due to the horizontal subduction of the mode waters (Fig. 4g, h).
The overlap of the 2005 (open triangles in Fig. 6a) and 2012 137Cs
data also implies that the vertical transport of the bomb-derived
137
Cs in the subtropical region was not controlled by a simple
one-dimensional advection/diffusion process.
In the subarctic and tropical regions, the bomb-derived 137Cs
activity concentration decreased monotonically with depth, and no
subsurface maximum was observed (Fig. 4f, j). This result implies
that in these regions the bomb-derived 137Cs penetrated into
deeper waters through a one-dimensional advection/diffusion
process. The MPD of bomb-derived 137Cs in winter 2012 can be
compared with that of tritium, obtained during the Geochemical
Ocean Sections Study project in the 1970s, because both the bombderived 137Cs and the tritium were produced by atmospheric nuclear weapons testing and deposited on the ocean surface simultaneously mainly in the early 1960s. The estimated MPD of the
bomb-derived tritium in 1973 was 310 m in the subarctic and
225 m in the tropical region of the North Pacic (about 270 m in
average, Broecker and Peng, 1982). If it is assumed that the penetration process was not changed during the past decades, the
temporal increase in the MPD between 1973 and 2012, about 180 m
(450 me270 m) indicates penetration of the bomb-derived 137Cs
(and tritium) started in approximately 1960, which is consistent

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Y. Kumamoto et al. / Journal of Environmental Radioactivity 140 (2015) 114e122

overestimated due to the subsurface maximum (Fig. 4b, c). In June

2011, about seven months earlier, Buesseler et al. (2012) observed
the MPD of Fukushima-derived radiocesium in the transition region to be 42 m. The MPD of 42 m and the penetration time of about
3 months (from March to June 2011) suggest that the MPD of
Fukushima-derived radiocesium in January 2012 should have been
about 80 m. The MPD of the Fukushima-derived 134Cs observed in
January 2012 (about 220 m) is thus about three times the MPD
estimated by using the data of June 2011 (about 80 m). The deeper
observed MPD implies that the Fukushima-derived 134Cs, especially
that derived from the direct discharge of contaminated water from
the FNPP1, was explained not by a simple one-dimensional
advection/diffusion process but by strong coastal and tidal currents.
By using the relationship between water-column inventories
and activity concentrations in surface water of the Fukushimaderived 134Cs in winter 2012, we could obtain better coverage of
the water-column inventory because we have surface 134Cs data
from a larger set of locations (e.g., Aoyama et al., 2013). As a result, it
is possible to obtain a better estimate of the total amount of radiocesium released from the FNPP1 into the Pacic Ocean. In the
same way, by using the relationship between water-column inventories and activity concentrations in surface water of the bombderived 137Cs in this study, we could obtain larger coverage of the
total inventory of the bomb-derived 137Cs just before the accident.
Because of the short half-life of 134Cs (2.07 y), the Fukushimaderived 134Cs activity concentration is decreasing rapidly, and it
will decay to less than the detection limit within the coming
decade. Thus, in the future the Fukushima-derived radiocesium will
be estimated using 137Cs, which has a half-life of 30.04 y, instead of
134
Cs. The water-column inventory of the Fukushima-derived 137Cs
will be obtained by subtracting the inventory of the bomb-derived
137
Cs from the observed 137Cs inventory.
4. Conclusions
Fig. 6. (a) Water-column inventories (Bq m2) plotted against activity concentrations
in surface water (Bq m2) for the bomb-derived 137Cs. Open and closed circles indicate
data from stations in the subarctic/tropical and subtropical regions, respectively. All
inventories and activity concentrations were decay-corrected to the date of the accident, 11 March 2011. The data from stations in the transition region (P10-094, 098, and
102) are not shown because the bomb-derived 137Cs activity concentrations in the
surface water are negative or have a large error. The solid and broken lines are
regression lines passing through the origin for the data in the subarctic/tropical and
subtropical regions, respectively. The slope for the subarctic/tropical data is 453 m, and
that for the subtropical region is 716 m. The 137Cs data observed in 2005, which were
corrected to the date of the accident by using the apparent half-life of 13 y (Povinec
et al., 2005), are also shown (open triangles). Error bars indicate standard deviations. (b) The same as (a) but for the Fukushima-derived 134Cs. Open and closed
circles indicate data from stations in the subarctic/transition/tropical and subtropical
regions, respectively. The line is a regression line passing through the origin for the
data in the subarctic and transition regions. The slope of the regression line was
calculated to be 216 m.

with the main atmospheric deposition in the early 1960s. This

implies that deep penetration of the bomb-derived tracers was
primarily controlled by the one-dimensional process in the divergence (subarctic and tropical) regions.
On the scatter plot of the water-column inventories of the
Fukushima-derived 134Cs against its activity concentrations in
surface water (Fig. 6b), the slope of the regression line passing
through the origin calculated with the data from the subarctic and
transition regions was about 220 m. Because in the tropical region
the Fukushima-derived 134Cs was measured only in the surface
seawater, its water-column inventory there was vanishingly
smaller than those the subarctic and transition regions (Fig. 5). As
with the MPD of the bomb-derived 137Cs, the MPD of the
Fukushima-derived 134Cs in the subtropical region was likely

In winter 2012, about ten months after the FNPP1 accident, the
Fukushima-derived 134Cs activity concentration and water-column
inventory were largest in the transition region due to the directed
discharge of the contaminated water from the FNPP1 (Kumamoto
et al., 2014). We also evaluated the bomb-derived 137Cs activity
concentration, that is, the activity concentration just before the
FNPP1 accident, along 149
E meridian to be about
1.10 0.04 Bq m3 on average from the excess 137Cs activity concentration relative to the 134Cs activity concentration observed in
winter 2012. The estimated the bomb-derived 137Cs activity concentration agrees well with that obtained in 2005 after decaycorrection using the apparent half-life of 13 1 y (Povinec et al.,
2005). The bomb-derived 137Cs activity concentration, which is
due mainly to nuclear weapons testing in the 1950s and 1960s, is at
present concentrated in the subtropical region of the North Pacic.
This implies that the Fukushima-derived 134Cs will also be transported from the transition to subtropical regions in the coming
decades by way of the thermocline circulation, including the subduction of the mode waters. Mean values of the water-column inventories for the Fukushima-derived 134Cs and the bomb-derived
137
Cs, both decay-corrected to the date of the FNPP1 accident,
were estimated to be 1020 80 and 820 120 Bq m2, respectively.
The ratio of the Fukushima-derived 134Cs versus the bomb-derived
137
Cs inventories, 1.3 0.2, suggests that the impact of the FNPP1
accident in the western North Pacic Ocean in winter 2012 was
nearly the same as that of nuclear weapons testing. The Fukushimaderived 134Cs will decay to less than the detection limit within the
coming decade because of its short half-life. After that, it will be
necessary to employ 137Cs to estimate the Fukushima-derived
radiocesium instead of 134Cs, a unique tracer of radiocesium

Y. Kumamoto et al. / Journal of Environmental Radioactivity 140 (2015) 114e122

released by the FNPP1 accident. Knowledge of the bomb-derived

137
Cs activity concentration will be essential to evaluation of the
total amount of Fukushima-derived 137Cs activity concentration.
Acknowledgments
We thank the crew of the R/V Mirai and the staff of Marine
Works Japan, Ltd. for their help during onboard sample collection.
This work was partially supported by a Grant-in-Aid for Scientic
Research on Innovative Areas from the Ministry of Education, Culture, Sports, Science and Technology of Japan (KAKENHI), Interdisciplinary Study on Environmental Transfer of Radionuclides
from the Fukushima Dai-ichi NPP Accident (#24110005).
Appendix A. Supplementary data
Supplementary data related to this article can be found at http://
dx.doi.org/10.1016/j.jenvrad.2014.11.010.
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