ARTICLES

PUBLISHED ONLINE: 18 APRIL 2016 | DOI: 10.1038/NMAT4618

Inverse spin Hall effect from pulsed spin current

in organic semiconductors with tunable
spinorbit coupling
Dali Sun, Kipp J. van Schooten, Marzieh Kavand, Hans Malissa, Chuang Zhang,
Matthew Groesbeck, Christoph Boehme* and Z. Valy Vardeny*
Exploration of spin currents in organic semiconductors (OSECs) induced by resonant microwave absorption in ferromagnetic
substrates is appealing for potential spintronics applications. Owing to the inherently weak spinorbit coupling (SOC) of
OSECs, their inverse spin Hall effect (ISHE) response is very subtle; limited by the microwave power applicable under
continuous-wave (cw) excitation. Here we introduce a novel approach for generating significant ISHE signals in OSECs using
pulsed ferromagnetic resonance, where the ISHE is two to three orders of magnitude larger compared to cw excitation. This
strong ISHE enables us to investigate a variety of OSECs ranging from -conjugated polymers with strong SOC that contain
intrachain platinum atoms, to weak SOC polymers, to C60 films, where the SOC is predominantly caused by the curvature of
the molecules surface. The pulsed-ISHE technique offers a robust route for efficient injection and detection schemes of spin
currents at room temperature, and paves the way for spin orbitronics in plastic materials.

oupled charge and spin-transport phenomena have drawn

great attention in the past few years as they allow one to
investigate the influence of the spin degree of freedom on the
charge currents through spinorbit coupling (SOC)1 , a relativistic
effect in condensed matter systems. For example, the spin Hall effect
causes a transverse spin current induced by a longitudinal charge
current24 ; whereas the inverse spin Hall effect (ISHE) produces a
transverse charge current that is caused by a pure spin current (see
Fig. 1a)57 . The ISHE can be used to determine the spin-mixing
conductance across ferromagnet/metal interfaces and the spin Hall
angle of heavy-atom metals that possess strong SOC812 . In contrast,
light-element metals13,14 , semiconductors15,16 , and organic materials1720 are characterized by intrinsically weak SOC, which restricts
the magnitude of the ISHE signals owing to the small spin-current
charge-current conversion efficiency. The technical limitation
and weak ISHE responses in these pioneering reports originate from
the low applicable maximum power in most continuous-wave (cw)
microwave (MW) ISHE experiments (<200 mW). Furthermore,
small cw-ISHE signals are often concealed by potentially confounding spurious signals such as the anomalous Hall effect (AHE), spin
backflow, anisotropic magnetoresistance (AMR), resonant heating,
and so on15,21,22 . Thus, the formation, manipulation and detection
of spin currents in weak SOC solids has proved to be challenging;
however, at the same time, it is the focus of recent research referred
to in the literature as spin orbitronics1 .
Pulsed magnetic resonance techniques have been widely employed for the study of spin interactions that affect the optoelectronic properties of organic solids23,24 using powers in the kW range
on nanosecond timescales. Based on previous cw-ISHE results and
the prediction of current spin-pumping models, the ISHE response
should increase linearly with the MW power8,9,21 . During such
pulsed excitation at ferromagnetic resonance (FMR)2528 , a much
greater spin current density can be generated that is capable of

inducing a large pulse-ISHE (p-ISHE) response that may be measurable even for materials with very weak SOC. In addition, benefiting
from the versatility of organic semiconductor (OSEC) synthesis,
their SOC can be enhanced by integrating intrachain heavy metal
atoms (such as Pt, Ir, and so on)29,30 , in contrast to the passive
intrinsic systematic variation of SOC in transition metals13,14 . Therefore, by chemically adjusting the heavy metal concentrations in
the polymer chains, the SOC strength in OSECs can be systemically tuned30 and quantitatively investigated by means of the ISHE
response generated from pulsed-FMR (p-FMR).
Here we present the experimental realization of p-FMR for generating and detecting spin currents in OSEC compounds with tunable
SOC through the p-ISHE response. Using this technique we develop
methods to effectively eliminate various spurious effects, such as
AMR, the AHE and resonant MW heating, that interfere with
the p-ISHE current. To highlight the usefulness of these technical
advances, we report a systematic study of the p-ISHE response
in a variety of OSEC materials with tunable SOC, ranging from
-conjugated polymers (PCP) having strong SOC that contain intrachain Pt atoms with various concentrations, to PCP that have
very weak SOC and are fully organic, to C60 films. We unravel the
important role of SOC in spin-current charge-current conversion
within these materials, and quantitatively determine the value of the
spin-diffusion length and spin Hall angle in each compound, exploring potential candidate materials for organic spin orbitronics3137 .

The pulsed-ISHE technique

Distinct from conventional cw-ISHE devices8,9 , the p-ISHE devices
presented here and their electrical connections are deposited as
thin-film structures23,24 with a slightly altered geometry (see Fig. 1a
and Methods). The pulsed dynamics of the magnetization vector,
M, in a ferromagnetic (FM) metal such as Ni80 Fe20 (NiFe) under
p-FMR induces a pulsed spin current in the adjacent non-magnetic

Department of Physics & Astronomy, University of Utah, Salt Lake City, Utah 84112, USA. These authors contributed equally to this work.
*e-mail: boehme@physics.utah.edu; val@physics.utah.edu
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NATURE MATERIALS DOI: 10.1038/NMAT4618

Device B
plane

Cu

JC

EISHE

IISHE

VISHE

+0.5 mV
+0.1 mV
0.3 mV
0.7 mV
1.1 mV
1.5 mV

6
4
2
60

120

B ()

Vp-ISHE (mV)

100
105
110
115
120
125
130
135

180
135
110

180

80
45
0
40 20

20

0.0

Vcw-ISHE at 200 mW 10

0.5
1.0

Vp-ISHE
1.5 at 1,000 W

2.0
50

1.0
0.5
0.0

25
0
25
BBres (mT)

0.0 0.1 0.2 0.3

B12 (mT2)

50

1.0

0.5
0.0
0.5
1.0
10

0 1 2 3 4 5 6 7 8
Acquisition time (s)

0.5

2
4
6
8
Acquisition time (s)

Vp-ISHE (a.u.)

Bres (102 mT)

B (mT)

JS

Vp-ISHE in NiFe/Pt

1.0

B1

0.5
1.5

0.5
0.0

50 nm

NiFe
Polymer

d
MW pulse sequence

FMR (a.u.)

1.5
1.0

SiO
NiF 2
e
C
60
Cu

Cu

trodes

ec
Copper el

Polymer

Vp-ISHE (normalized)

NiFe ferromagnet

Vp-ISHE (mV)

V/VMAX

ARTICLES

NiFe/Pt
NiFe only
5

0
5
BBres (mT)

10

40

BBres (mT)

60

120

180

B ()

Figure 1 | Detection of pulsed spin current through the p-ISHE response. a, Schematic illustration (not to scale) of the NiFe/OSEC/Cu device on a glass
template held by a sample rod with a built-in contact system for thin-film electrical connections23 . The inset shows a transmission electron microscope
image for the cross-section of an organic-based p-ISHE device fabricated as sketched in the main panel. Different layers can be distinguished as labelled.
B, B1 and M denote, respectively, the static external magnetic field, the magnetic component of the pulsed MW field, and the dynamic magnetization in the
NiFe film, which precesses around B. JS , S, JC , EISHE , VISHE and IISHE denote, respectively, the flow of the pulsed spin current, the spin polarization vector, the
generated electric current, the generated electric field, the detected p-ISHE voltage and the detected p-ISHE current. b,c, Time (t) and field (B) responses
of the p-ISHE voltage (Vp-ISHE ) measured for the prototype NiFe (15 nm)/Pt (10 nm)/Cu (30 nm) device under 1 kW microwave excitation. The blue solid
line in b shows the one-pulse MW excitation. The red solid line indicates the moving-average ISHE voltage response. The colour plot in c shows a
resonance at B = Bres = 120 mT. The two spurious regions outside the MW pulse originate from MW switching artefacts and non-resonant inductive
coupling. d, Comparison of Vp-ISHE (at 1 kW) and the maximum cw-ISHE (at 200 mW) response on the same NiFe/Pt/Cu device. The inset shows the MW
power dependence response of Vp-ISHE ; it increases linearly with MW power ( B21 ) in range used in this work (see Supplementary Discussion 2). eh, Field
(B) and angular (B ) dependencies of FMR absorption and p-ISHE response, respectively, in the NiFe/Pt/Cu device. e, Comparison of the NiFe FMR
response before (red) and after (black) the deposition of Pt. f, Resonance field as a function of B , as obtained from FMR in the NiFe film. g, Normalized
Vp-ISHE (B, B ) response, where Bres is normalized. h, Normalized Vp-ISHE amplitude and polarity versus B .

layer as a result of spin pumping. The existence of a pulsed spin

current (JS ) in materials with a finite spin Hall angle (SH ) leads to
an electric field EISHE (ref. 5). EISHE is transverse to the spin current
JS and spin polarization S, such that the induced charge current
JC EISHE SH JS S, where is the material conductivity along
the interface (see Fig. 1a). Therefore, by measuring VISHE or JC in
the sample film adjacent to the FM layer, the ISHE can be used
for sensitive detection of the spin Hall angle, which is strongly
influenced by the material SOC.
A typical p-ISHE response from a prototype NiFe/Pt system
measured in an in-plane (that is, B = 0 ) external magnetic field,
B, is shown in Fig. 1b. Pt is used here because of its strong SOC,
which generates a large ISHE response. The transient voltage was
measured between the two Cu contacts underneath the Pt film
after a single-pulse excitation of 5 s duration that is averaged
over 10,240 MW pulses at the resonance magnetic field B = Bres
in the FMR spectrum (Fig. 1c). The p-ISHE voltage shows a step
function response of 1.3 mV that occurs simultaneously with
the MW pulse. The abrupt VISHE rise and decay times are 5 ns,
consistent with the timescale of free induction decay for FMR (see
Supplementary Discussion 1). This indicates that the processes of
magnon activation, spin current injection and ISHE generation in Pt
2

metals all have ultrafast responses25,26 . Possible contributions to the

observed ISHE from parametrically excited magnons28 can be ruled
out as it occurs at half the resonant field. Figure 1c depicts a twodimensional data set that shows the obtained values of VISHE (B, t),
and Fig. 1d shows the VISHE (B, t = 3 s) response has a full-width at
half-maximum 1B 10 mT, which is in agreement with the FMR
linewidth from the same device (shown in Fig. 1e).
A comparison between the cw- and p-ISHE responses is
performed using the same NiFe/Pt device with an in-plane B
(see Methods and Supplementary Discussion 2). The p-ISHE
response (VISHE 1.6 mV) is about two orders of magnitude larger
than the cw-ISHE response (VISHE 25 V); this is also one order
of magnitude higher than previously reported ac-ISHE using a.c.
spin pumping22,38,39 . However, a relatively high cw-ISHE response in
Pt obtained from the cw-FMR of an alternative magnetic insulator
layer (yttrium-iron-garnet (YIG)) cannot be directly compared with
a NiFe/Pt device because of the different spin-pumping efficiency of
YIG and different device geometries (ref. 40).
Figure 1e shows the respective FMR spectra (in terms of
dI (B)/dB) for the NiFe/Pt device and a NiFe-only film. The FMR
linewidth enhancement (1Hpp ) indicates an increased magnon
damping, which demonstrates the injection of spin current from

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NATURE MATERIALS DOI: 10.1038/NMAT4618

Pt

P(n-Bu)3

Ph

IC
Cu

Pt

P(n-Bu)3

P(n-Bu)3 N

Pt

P(n-Bu)3

p-ISHE -Is (nA)

FL

Ph

300

100
0
100
200
180

300

0.0
1.5

2.0

2.5
3.0
Energy (eV)

B ()

Pt-1

200

0.0

0.5

0
90 45 0 45 90

3.5

4.0

1
20

IS

FL
Pt-Q

IF

Cu

P(n-Bu)3

Pt-3

0.5

1.0

NiFe
OSC

dN

FL

0.0

Bres (T)

Ph

FMR (a.u.)

Pt-1

0.5

1.0

P(n-Bu)3

p-ISHE -Is (normalized)

1.0

40

20

20

NiFe only
NiFe/Pt-1
10

0
BBres (mT)

1,000 W
500 W
250 W
125 W

1.0
0.8
0.6

p-ISHE
normalized

Electroluminescence intensity (a.u.)

ARTICLES

10

20

0
500 1,000
0
MW power (W)

0.4
0.2
0.0

40

BBres (mT)

60

30

0
30
BBres (mT)

60

Figure 2 | Electroluminescence spectra of the Pt-polymer series studied here, and observation of the p-ISHE response in Pt-1 polymer. a, Normalized
electroluminescence spectra for Pt-1 (black), Pt-3 (red) and Pt-Q (blue) polymers, respectively. The SOC strengths can be estimated from the
electro-Ph/FL intensity ratios30 . The insets show the building blocks of the studied Pt-polymers. The spacer in Pt-1 has a single phenyl ring, whereas that
of Pt-3 has three phenyl rings. b, Schematic illustration of the p-ISHE-IS current response in OSEC-based devices. IC , IF and IS are, respectively, the electric
current source generated by the ISHE in the organic layer, the AHE in the NiFe thin film (suppressed by capacitor geometry) and the current response
detected by the preamplifier; dN and l are the material thickness and length of device, respectively. c, FMR spectra of the Cu/Pt-1 polymer/NiFe/SiO2 /Cu
device measured by MW transmission without (black) and with (red) the spin-coated Pt-1 polymer. The inset shows the FMR resonance field, Bres versus
the external field angle, B . d, Typical p-ISHE(B) response (in terms of current, IS ) in the Pt-1 polymer device (ISHE/AHE ratio 9). The black squares and
red circles in d are data with the in-plane magnetic field B (at 0 ) and B (at 180 ), respectively. e, p-ISHE(B) response versus the MW power, as denoted.
The inset shows the obtained linear IS versus MW power dependence.

NiFe into the Pt layer by spin pumping41,42 . Figure 1fh shows

the FMR resonance fields, the p-ISHE(B) response, and p-ISHE
magnitudes measured for the NiFe/Pt device as a function of the
out-of-plane angle (B ) between the device plane and B. On varying
B , the p-ISHE signal disappears at B = 90 , changing polarity
between B = 0 and B = 180 , which is consistent with the ISHE(B )
characteristic response21 . These results also demonstrate that thermoelectric artefacts43 are largely suppressed in low pulse-duty cycle
p-ISHE experiments. The asymmetry of the p-ISHE(B) response
seen in Fig. 1d originates from the extrinsic electromagnetic AHE,
which is due to the electric field (E1 ) component of the resonant
MW in the NiFe film, when the sample is placed slightly off the
resonator centre5,21 . To substantially reduce the AHE contribution
and other spurious effects in the p-ISHE measurements, especially
for OSEC samples with a small spin Hall angle, we integrated a MW
shunt capacitor layer (SiO2 /Cu) into the device geometry, which is
designed to absorb the electric field component of the MW that
crosses the FM layer (see Supplementary Discussion 3)44 .

Pulsed-ISHE studies of various organic semiconductors

Having reduced the various artefact contributions, we have
measured the p-ISHE response in a variety of OSEC compounds
with tunable SOC values. The generally weak SOC of OSEC
materials can be enhanced by incorporating intrachain heavy atoms,
such as Pt29 , which can be tuned by changing the intrachain Pt
atom concentration, through incorporation of different organic
ligand spacers30 . Triggered by the enhanced SOC, these polymers
show substantial phosphorescence (Ph) emission from the lowest
triplet state, and consequently their emission spectra contain both
fluorescence (FL) and Ph bands29,30 ; this can conveniently serve to

provide estimates of the relative SOC strength from the intensity

ratio of the Ph/FL in the electroluminescence spectra of organic
light-emitting diodes (OLEDs) based on these polymers29 .
In Fig. 2a we show the chemical structures of three Pt-containing
polymers that we synthesized and study here30 . It is seen that one
spacer unit contains a single phenyl ring, dubbed here as Pt-1;
whereas the other spacer unit contains three phenyl rings, dubbed as
Pt-3. The Pt-Q polymer has a similar structure to that of Pt-1, except
that the phenyl rings in the chain are replaced by a 5,8-diethynyl2,3-diphenylquinoxaline unit. The normalized electroluminescence
spectra of these three polymers (Fig. 2a) show both electro-FL and
electro-Ph bands. From the ratio of Ph/FL we conclude that the
SOC strength decreases from Pt-1 to Pt-3 to Pt-Q (see Table 1)30 .
In addition to Pt-containing polymers with tunable SOC, we also
studied several more conventional PCPs having very weak SOC,
including poly(3,4-ethylenedioxythiophene):polystyrene sulfonate
(PEDOT:PSS), poly(dioctyloxy)phenylenevinylene (DOO-PPV),
and
poly[2,5-bis(3-tetradecylthiophen-2-yl)thieno[3,2-b]thiophene] (PBTTT-C14), as well as the fullerene C60 . Their respective
repeat units are shown in the appropriate panels of Fig. 3.
Figure 2b shows the schematic illustration of the p-ISHE current
response in OSEC-based devices. Figure 2c compares the FMR(B)
response obtained from the NiFe films as deposited on glass
and on a spin-coated Pt-1 polymer film. The broadening of the
FMR(B) response in the NiFe/Pt-1 film indicates the occurrence
of spin pumping at the NiFe/OSEC interface41,42 . Figure 2d shows
the p-ISHE(B) response (as a series current, IS , between the Cu
electrodes (see Methods)) at MW pulse peak power, P = 1 kW.
The maximum IS occurs at Bres , and reverses sign when the inplane magnetic field direction is reversed from B = 0 to B = 180 .

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NATURE MATERIALS DOI: 10.1038/NMAT4618

ARTICLES

Table 1 | Summary of the p-ISHE parameters for the investigated OSEC materials obtained from the experiments.
Materials
Pt
Pt-1
Pt-3
Pt-Q
PEDOT
DOO-PPV
C60

SOC (Ph/FL)
N/A
27
12
0.75
N/A
N/A
N/A

Vp-ISHE (V)
1,615
76
52
26
17
15
209

p-ISHE-IS (nA)

SH (nm)

2,892
246
231
145
69
54
668

+12.0 0.3 102

4.0 0.1 103
3.0 0.1 103
1.5 0.1 103
+1.9 0.4 103
6.0 0.2 104
+7.1 0.1 102

(nm)
0.3 ,

SH
3.410

1.5
1.5 0.5
5 1 , 3
10 2
40 10 , 2719
25 10 , 1646,
5 2 , 1250,

+3.9 0.3 102

2.7 1.0 103
1.4 0.4 103
1.5 0.3 104
+5.3 0.3 105
8.2 1.2 105
+1.4 0.2 102

The relative SOC for the three Pt-polymers was obtained from the intensity ratio of the electro-Ph/FL in OLED devices. Vp-ISHE and p-ISHE-IS are the ISHE voltage and current, respectively, between the
Cu electrodes measured at Bres using a MW power of 1 kW. SH is the lambda-theta product obtained from the fit to the ISHE response versus the OSEC thickness using equations (1)(3) (or
Supplementary Equations 68). is the spin-diffusion length extracted from equation (2) (or Supplementary Equation 6) (marked by ), independent values from GMR response in OSVs at low
temperature (marked by ), or literature reports. SH (in radians) is the spin Hall angle calculated from independent spin-diffusion length estimations (see Supplementary Table 2).

The IS (B ) sign reversal is consistent with the reversal of the spin

current polarization induced by spin pumping21,45 . The remaining
asymmetry of IS (B) is due to a residual AHE(B) contribution caused
by the finite thickness of the shunt capacitor. Figure 2e shows the
expected1921 linear increase of IS with the MW power.
Figure 3 shows IS (B) responses for the other six NiFe/OSEC
devices with various thicknesses. The ISHE response component
was found to scale with the SOC strength of the materials. This
explains the weak ISHE signals obtained in the fully organic PCPs,
which have very weak SOC. We note our ability to still observe
an ISHE response in DOO-PPV, a polymer previously used in
spin valve experiments from which the spin-diffusion length was
inferred46 . This demonstrates that the dual use of p-ISHE response
detection and a microwave shunt capacitor layer provides a highly
sensitive method for obtaining a larger, artefact-free ISHE response,
which is crucial for continuing spin-pumping studies in OSEC
materials; whereas the mechanism responsible for the ISHE is still
the same as in d.c. measurements.
When PBTTT-C14 is used, no p-ISHE current is detected
(Fig. 3e), although the broadening of the FMR linewidth
indicates that spin pumping indeed occurs at the interface of
NiFe/PBTTT-C14. The absence of a detectable p-ISHE response in
PBTTT-C14 is consistent with the previously reported extremely
weak SOC20 in this polymer. Furthermore, this data can serve as a
control experiment for the exclusion of measurement artefacts in
our experiments.
Figure 3f shows the p-ISHE response of a NiFe/C60 device. Surprisingly, we found that C60 film (25 nm thick) exhibits a large ISHE
response, in spite of the fact that it only contains carbon atoms with
relatively small SOC. We measured an IS value of 600 nA, which is
a larger response than in Pt-1. This cannot be explained by a possible
artefact, because the ISHE response obtained lacks the usual AHE
component (see Supplementary Discussion 46); therefore the large
ISHE response is a genuine characteristic response of the C60 film.

Determination of SH in OSEC with tunable SOC

The p-ISHE responses observed in this study exhibit experimental characteristics similar to those reported for other inorganic
and organic materials by cw spin pumping, such as Pt5 and PEDOT:PSS19 . The p-ISHE current dependency on B , the MW power
P, as well as the polarity of B and the FMR(B) resonance field
are all in agreement with the existing understanding of the ISHE
phenomenon (see Supplementary Discussion 7). This shows that the
pulsed measurements are indeed a consequence of spin-current
charge-current conversion in the OSEC, generated by spin pumping through the NiFe/OSEC interface. Consequently, the p-ISHE
experiments may be used to probe the spin charge conversion
efficiency in various OSEC materials by determining the spin Hall
angle, SH (see Methods and Supplementary Discussions 711), as
summarized in Table 1.
4

For metallic spin-transport layers with conductivity N

comparable to that of a ferromagnetic injector, F , the expression
for VISHE is21
 
lSH N tanh(dN /2N ) 2e 0
j
(1)
V (ISHE) =
dN N + dF F
} S
where N is the spin-diffusion length in the non-magnetic layer;
dF is the FM thickness; l is the FM length parallel to the
interface, and j0S is the spin current density injected into the
non-magnetic layer, which can be calculated from the FMR(B)
response (see Fig. 1e, and Supplementary Discussion 7). For the
present p-ISHE experiments, equation (1) has to be modified (see
Supplementary Equation (6)) to account for the various frequencydependent impedances of the experimental set-up (Supplementary
Discussions 7). Nevertheless, it is clear from equation (1) (and
Supplementary Equation (6)) that measurements of VISHE versus
dN reveal both N and SH , as long as dN < 2N , that is, when
tanh(dN /2N ) in equation (1) is not saturated at 1. This is the
case for the NiFe/Pt device, where the Pt layer thickness could
be controlled within 1 nm. Equation (1) (and Supplementary
Equation (6)) shows thatVISHE (dN ) first increases with dN ; but when
tanh(dN /2N ) saturates, then VISHE (dN ) decreases approximately as
1/dN . This is shown for the NiFe/Pt device in Fig. 4a. We measured
VISHE (dN ) in devices based on several thin Pt layers for which
dN < 2N ; from the fit to the data using equation (1) (Fig. 4a)
we independently obtained N (Pt) = 1.5 0.3 nm and SH = 0.080
(see Supplementary Table 2). These values are consistent with the
literature values10,47 , validating our method and the approximation
made in the equivalent circuit (Supplementary Fig. 11).
For the OSEC layers, especially the Pt-polymers, it is difficult
to control their thickness to be within dN < 2N 10 nm; in
addition, it is possible that, at such a small dN , the longitudinal
transport mode would be tunnelling rather than drift. Under these
conditions the fabricated OSEC thickness dN > 2N for most of
the NiFe/OSEC devices. Consequently, tanh(dN /2N ) 1, rendering
the two fitting parameters N and SH inseparable; thus, according
to equation (1), their product is treated as one fitting parameter
(dubbed here the lambda-theta product, N SH ). Neither N nor SH
can be independently obtained from IS (dN ) when dN > 2N . Similar
issues for the determination of N and SH have been reported for
metals such as Pt, where values of N and SH varied widely among
the different sources, whereas the resulting N SH products were
reproduced well10 .
Unless N can be determined independently from other
experiments, the spin Hall angle in OSEC materials in general
cannot be determined accurately. One such independent estimate
of N in OSEC can be made, for example from the giant
magnetoresistance (GMR) in organic spin valves (OSVs)31 .
Although OSV fabrication using OSEC with relatively strong

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NATURE MATERIALS DOI: 10.1038/NMAT4618

180
0

500

150

1,000

MW power (W)

ISHE/AHE: 3

150

FMR (a.u.)

60

20

30

180
0

1,000
500
MW power (W)

60

10
0
10
BBres (mT)

40

20

20

d
n

S
O

ISHE/AHE: 7

0
1

50
100

30

150
60

60
10
0
10
BBres (mT)

20

30

C8H17

ISHE/AHE: 4

1
0
1
20 10 0 10
BBres (mT)

PEDOT:PSS

30

180

1
20

C8H17

30

60

40

20

180

300

30

p-ISHE-Is (nA)

C14H29

0
FMR (a.u.)

30

60
30

600

10
0
10
BBres (mT)

20

10

40

20

60

30

180
0
500
1,000
MW power (W)

ISHE/AHE: 33

300

PBTTT
10

600

20

20

1
20

p-ISHE normalized

p-ISHE-Is (nA)

f
0

FMR (a.u.)

0
BBres (mT)

C14H29

60

DOO-PPV

20

BBres (mT)

C8H17
O

FMR (a.u.)

S
O

FMR (a.u.)

p-ISHE-Is (nA)

50

180

p-ISHE-Is (nA)

40

C8H17

60

SO3 SO3H SO3 SO3H

O

20

BBres (mT)

150
100

Pt-Q
0

BBres (mT)

ISHE/AHE: 6

1
20

300

Pt-3

30

150

1
20 10
0
10
BBres (mT)

300

p-ISHE normalized

FMR (a.u.)

p-ISHE-Is (nA)

150

300

p-ISHE-Is (nA)

300

p-ISHE normalized

ARTICLES

1
20

10
0
10
BBres (mT)

40

BBres (mT)

20

20

C60
0

20

40

60

BBres (mT)

Figure 3 | p-ISHE(B) response in various OSEC materials with tunable spinorbit coupling. af, p-ISHE(B) current response in a variety of NiFe/OSEC/Cu
devices as denoted, measured under a 1 kW pulsed MW excitation with a 500 Hz repetition rate. The OSEC materials are four pristine -conjugated
polymers, PCPs (a, b, d, and e), one heavily doped PCP (c), and a fullerene (C60 ; f). Their respective molecular structures and ISHE/AHE ratios are shown in
the appropriate panels. All devices are capped with a SiO2 /Cu capacitor layer to suppress the AHE(B) response component. The open black squares and
red circles represent an in-plane field B (at 0 ) and B (at 180 ), respectively. When Bres is reversed from B = 0 to B = 180 , all signals reverse polarity,
as expected for the ISHE. For the NiFe/Pt-3 and NiFe/Pt-Q bilayers, the proper IS values for the ISHE (that is, after separating the ISHE and AHE
components) are 230 nA and 150 nA, respectively. When the Pt-containing polymer is replaced by a fully OSEC polymer (that is, PEDOT:PSS or
DOO-PPV), IS is significantly reduced (69 nA for PEDOT:PSS; 54 nA for DOO-PPV). The respective insets show the NiFe FMR(B) responses measured by
MW absorption in devices, with (red) and without (black) the OSEC overlayer (for details on the broadening of FMR linewidth due to the spin pumping, see
Supplementary Discussion 7) and, in a,b and f, the obtained p-ISHE response versus MW power (see also Supplementary Fig. 14). The red lines through the
data points show a linear fit. The connecting line in f is a guide for the eye.

SOC materials is challenging, we nevertheless successfully

fabricated OSVs based on C60 and Pt-3 polymer in our
laboratory, and extracted N from the GMR response versus

dN (Supplementary Fig. 16 and Table 1). In Table 1 (indicated

by the reference number) we also include N values obtained
from the literature, whenever possible. In addition, in Table 1

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NATURE MATERIALS DOI: 10.1038/NMAT4618

ARTICLES
a

NiFe/Pt

0.8

Pt = 1.5 0.3 nm

800

150
NiFe/Pt-1

100

Pt-1 = 1.5 0.5 nm

50

0.4

Thickness (nm)

10

600
NiFe/C60

400

C60 = 5 2 nm

200

0
2

p-ISHE-Is (nA)

1.2

0.0

1,000

200
p-ISHE-Is (nA)

p-ISHE (mV)

1.6

250

20

40

60

80

100

Thickness (nm)

30

60

90

120

150

Thickness (nm)

Figure 4 | p-ISHE(B) responses versus the OSEC thickness. ac, Thickness dependence of the p-ISHE (IS ) responses (open squares) in NiFe/Pt/Cu,
NiFe/Pt-1/Cu and NiFe/C60 /Cu, respectively. Red solid lines are fits to the p-ISHE data using equation (1) (for Pt) and Supplementary Equation (6)
(for Pt-1 and C60 ). The respective spin-diffusion length extracted from the fit of each OSEC device is denoted. The error bars are determined from the noise
level in the time/field-dependent p-ISHE(B) response, which varies with the individual device under operational conditions (see Methods and
Supplementary Fig. 1).

we show values of N (marked by ) and SH that we obtained

from a method that uses Supplementary Equation (6), keeping l
and j0S constant, and focusing on the tanh(dN /2N ) value close to
saturation (Supplementary Fig. 15). For this, we first obtained a
crude estimation of N , and then calculated SH . The fits obtained to
JS versus dN for Pt-1 and C60 devices using the N and SH values from
Table 1 are shown in Fig. 4b,c, respectively; the good fits support
our approach. We note that spin backflow from the OSEC into the
NiFe film is not considered in our SH calculations22,48,49 . Most of
our p-ISHE measurements were done on devices where the organic
thickness dN  N . In this case, the influence of the spin backflow
(if at all relevant with OSEC) saturates48 , namely it does not change
the spin-mixing conductance with dN ; see Supplementary Fig. 19.
Therefore the equations that we used to extract SH are correct;
except that a constant spin backflow might reduce the real SH . The
SH values obtained are therefore a lower limit22 .
The results summarized in Table 1 show that SH scales with the
SOC strength of the OSEC layers; this validates the measurement
technique and the procedure employed for estimating SH . We note
that the SH obtained for PEDOT:PSS is slightly higher than the
literature report19 . This difference is most likely due to the different
types of PEDOT:PSS polymers used for the two ISHE measurements
(see Methods). We also note that an enhancement of the measured

SH (compared to the intrinsic SH

) occurs in the various OSEC
due to their anisotropic conductivity (see Supplementary Figs 20
and 21, and Supplementary Tables 1 and 2). We found that, for all
PCPs studied here, except PEDOT-PSS, SH has an opposite polarity
compared to that of Pt. In contrast to the previous studies on 3d,
4d and 5d transition metals, in which the sign and the magnitude
of SH is mainly dominated by the d-electron configurations and
atomic number (Z 4 )13,14 , the ISHE polarity in OSEC materials
may be influenced by several factors. For example, the SOC sign
in the highest occupied molecular orbital (HOMO) and lowest
unoccupied molecular orbital (LUMO) bands, and the SOC sign
of the heavy atoms embedded in the OSEC; for example, the SOC
of Pt atoms in the Pt-polymer chains may have opposite polarity
compared to that in Pt metal.
Surprisingly, we found that C60 films have an anomalously large
SH which is bigger than that of Pt-1 polymer, but smaller than in
Pt. This shows that the p-ISHE experiment is capable of obtaining
important information about the SOC even in unusual cases such
as C60 (ref. 50). The -electrons alone cannot be responsible for
the large SH in C60 film, because the SOC of these electrons is
identically zero. However, carbon electrons can also contribute
to the SOC in C60 , because of the mixing that occurs between
and electrons due to the strong curvature of the molecule
surface50 . Moreover, after carefully performing measurements of the
6

ISHE MW power dependence in the C60 device, we observed an

unusual nonlinear behaviour (see inset of Fig. 3f and Supplementary
Fig. 14f). The ISHE response increases markedly between 200
and 500 W, then returns to a linear response as the MW power
increases. As we discussed above (see Supplementary Figs 3, 9
and 10), there are no other artefacts (such as MW heating, spin
Seebeck, parametric pumping, or spurious effects from the NiFe
electrode) that could account for this result. Therefore, this finding
may be a signature that the SOC strength in C60 can be tuned
by electric fields (here the electric field generated by the ISHE
response), as proposed in C60 organic spin valves50 . Electric-fieldtuned SOC would provide a new avenue to actively control the SOC
strength in organic semiconductors.

Outlook
The pulsed, high MW power detection allows experimental access
to the ISHE dynamics with an approximately 5 ns time resolution,
suggesting that the p-ISHE response may have potential for fast
spin-orbitronics-based logic applications. It also enables the use
of traditional ferromagnets (for example, NiFe) instead of the
technically more demanding magnetic insulators (such as yttrium
iron garnet)13,14,40 , thus opening many research opportunities for
both the organic and inorganic spintronics communities. The ability
to pump large pure spin currents into most classes of OSEC offers
a robust methodology for investigating spin-transport properties,
and a simple method to probe the strength of SOC in OSEC-based
devices. Our work also indicates the possibility of tunable SOC in
OSECseither passively, through chemical synthesis, or actively,
using an electric fieldpaving the way for the future studies of spin
orbitronics in plastic materials.

Methods
Methods and any associated references are available in the online
version of the paper.
Received 6 January 2015; accepted 3 March 2016;
published online 18 April 2016

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Acknowledgements
We acknowledge support by the National Science Foundation (DMR-1404634) for sample
preparation, execution of the experiments and data processing of the ISHE experiments.
We also acknowledge the NSF-Material Science & Engineering Center (DMR-1121252)
for supporting Pt-polymer synthesis, execution of the OSV experiments and development
of the ISHE device structures, as well as support for the device preparation facilities.

Author contributions
D.S., K.J.v.S., C.B. and Z.V.V. conceived this study and the experiments. D.S. fabricated the
devices. K.J.v.S., D.S. and H.M. implemented the p-ISHE set-up. K.J.v.S., H.M. and M.K.
measured the p-ISHE response; D.S., M.K. and C.Z. measured the device conductivity
and capacitance. C.Z. and D.S. measured the Pt-polymer electroluminescence spectra.
M.G. measured the frequency dependence of the FMR spectra. D.S. carried out the
circuit modelling for the p-ISHE current. C.B. and Z.V.V. were responsible for the project
planning, group management, and final writing of the manuscript . All authors discussed
the results, and worked on data analysis and manuscript preparation.

Additional information
Supplementary information is available in the online version of the paper. Reprints and
permissions information is available online at www.nature.com/reprints.
Correspondence and requests for materials should be addressed to C.B. or Z.V.V.

Competing financial interests

The authors declare no competing financial interests.

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NATURE MATERIALS DOI: 10.1038/NMAT4618

ARTICLES
Methods
Device preparation for the p-ISHE measurements. Al thin-film electrodes
(150 nm) on glass templates (3 50 mm) were fabricated by sputtering and using
conventional optical lithography23,24 . Two Cu contacts with a gap of 50 m
(extended from an Al bottom electrode) were grown by e-beam evaporation
through a shadow mask in a glove-box-integrated vacuum deposition chamber
(Angstrom Engineering), dedicated to metal deposition, having a base pressure of
3 108 torr. Cu is chosen as the electrode material because it has negligible SOC,
and thus does not interfere with the ISHE from the spin current diffusion through
the OSEC film into the underlying electrode20 . The templates were subsequently
transferred into a second glove box that is dedicated to OSEC spin coating through
an antechamber under a nitrogen atmosphere (0.1 ppm).
The Pt-1, Pt-3, Pt-Q and DOO-PPV PCPs were synthesized in house using
literature methods30 . The PEDOT:PSS polymer (Clevios, P VP AI 4083) was
purchased from Heraeus, and the PBTTT-C14 polymer was purchased from
Luminescence Technology Corp (Lumtec) and used without further purification.
The polymer/chloroform solutions were spin-coated onto the templates at various
spinning speeds (from 1,000 to 8,000 r.p.m.) to obtain different OSEC film
thicknesses, followed by a post-annealing procedure (100 C for 30 min) in the
glove box. The C60 powder was purchased from American Dye Source, and C60
films were thermally evaporated onto the template at a rate of 0.5 to 1.0 s1 . The
OSEC-coated templates were transferred in a nitrogen atmosphere back to the first
glove box, with the vacuum deposition chamber.
Ni80 Fe20 ferromagnetic layers (15 nm thickness) were grown by e-beam
evaporation through a shadow mask on the spin-coated polymer thin films.
Without breaking the vacuum, the fabricated structures were transferred with
another shadow mask back to the deposition chamber for e-beam evaporation of a
SiO2 (150 to 750 nm) dielectric layer and a top Cu thin film (30 nm). All thin-film
thicknesses were calibrated using a profilometer. The active device area was
0.7 mm 1.0 mm .
p-ISHE measurement set-up. The p-ISHE measurements were carried out at room
temperature in a Bruker ElexSys E580 X-band (9.7 GHz) pulsed EPR
spectrometer equipped with a dielectric resonator (Bruker FlexLine ER 4118
X-MD5). Both cw and pulsed MWs were applied to the p-ISHE templates under a
rough vacuum. The purpose of the all-thin-film device design is to ensure that all
conducting components are thinner than the MW skin depth at 9.7 GHz, leaving
the device mostly unperturbed by the intense E-fields within the cavity. Figure 1a
illustrates a p-ISHE device on a glass template that was designed specifically to fit
in the MW resonator. The position of the template during operation is such that its
contact pads are well outside the resonator volume whereas the actual sample
structure is located at the opposing far end in the centre of the resonator. The MW
pulse duration time was either 2 s or 5 s (chosen depending on the rise time of
the current amplifier being used) at a repetition rate of 500 Hz. The device
geometry is chosen such that it places the sample at a position within the
cylindrical MW cavity where the B1 field is both maximal and homogeneous,
whereas the E1 field is minimal. The maximum pulsed MW power was 1 kW,
resulting in an amplitude B1 = 1.1 mT at the sample location.
The p-ISHE responses were detected by means of the induced electromotive
force, VISHE , using a Femto DHPCA 100 for metals, and a Stanford Research SRS
570 current preamplifier for OSEC material (that is, IS , see Supplementary
Discussion 7), with a bandwidth setting of 100 Hz1 MHz. The current-amplifier
output was connected to the input of a Bruker SpecJet transient recorder
(250 MS s1 , 8-bit digitizer) that is built into the ElexSys spectrometer. The
sensitivity of the current preamplifier was chosen to be 103 A V1 (Femto
DHPCA-100) or 20 A V1 (SRS 570). The p-ISHE(B) response measurements and

time dynamics required averaging over 10,240 shots. The error bar is determined
from the maximum noise level in the time/field-dependent p-ISHE(B) response
from each device (for example, Supplementary Fig. 1), which depends randomly on
the power fluctuation in each MW pulse (maximum: 10%) and the device stability
under the pulsed MW operational conditions. For the cw-ISHE measurement we
used a cw MW source with a power of 200 mW applied to the same resonator and
VISHE (as a derivative spectrum) was measured by magnetic field modulation and
lock-in amplification. The VISHE (B) spectrum is converted to a voltage amplitude
by numerical integration. The parallel capacitance and resistance in the devices
were measured using an Agilent E4980A precision LCR meter. The out-of-plane
and in-plane conductivities for various materials were measured by a Keithley 4200
at room temperature.
Spin Hall angle calculation. The observed p-ISHE responses enable us to calculate
the spin Hall angles (SH ) for various OSEC materials. Here we quantify the values
of SH based on a phenomenological model21 and equivalent circuit model of our
set-up (see Supplementary Fig. 11). The p-ISHE response is measured during each
MW pulse excitation (5 s duration) at a repetition rate of 500 Hz. Consequently,
the generated p-ISHE response contains a wide bandwidth of a.c. signals (from
100 Hz to 1 MHz, see Supplementary Discussion 7). The capacitance of each
OSEC film, CN , also needs to be considered in the circuit model (Supplementary
Fig. 11). By taking into account the device structure, detection electronics, and
the a.c. response of each electronic component, a simplified expression may
be written:
#
"
(IC + IF )RF
(2)
IS (pISHE) = Re SUM
SUM
RS + RF + (2RSUM
)
N /1 + i( j CN (j) RN (j) )
where RF and RSUM
are the series resistances of the NiFe film and
S
current-preamplifier impedance, respectively. j , CN (j) = (N (j) w(l/2))/dN and
RN (j) = dN /(N (j) W (l/2)) are, respectively, the jth frequency component
(established by the finite Fourier transform), parallel capacitance and resistance of
the organic layer at j (see Supplementary Discussion 7 for the derivation). The
variables N (j) and N (j) are the dielectric constant and conductivity of the OSEC
material at j . RSUM
and (j CN (j) RN (j) )SUM are the respective sum of parallel
N
resistance and sum of the CN RN product terms averaged over the entire frequency
range of the measurement apparatus (Supplementary Figs 12 and 13). The
parameter w is the width of NiFe layer and l is the length of NiFe thin film. The
currents IC and IF are the generated ISHE responses at the NiFe/OSEC interface
and the AHE response from the NiFe thin film, respectively. The latter response is
greatly suppressed by the MW shunt capacitor incorporated into our devices
(Fig. 2), but not completely eliminated. The spin-pumping-related IC through the
OSEC layer can be expressed as21 :

IC = lSH

2e
}

N tanh

dN
2N

j0S

(3)

where SH and N are the respective spin Hall angle and spin-diffusion length in the
OSEC, and j0S is the spin current in the OSEC perpendicular to the NiFe/OSEC
interface and along l (ref. 21). By measuring the IC dependence on the OSEC
thickness, dN at fixed l and j0S , we can obtain N from a normalized version of
equation (3) (see Fig. 4 and Supplementary Fig. 15). The spin current j0S is obtained
from the attenuation of the FMR response (that is, FMR(B ) resonant field and
spectral width dependencies, see Supplementary Fig. 18). The lambda-theta
product ( SH ) can be accurately calculated by substituting the above parameters
into equations (2) and (3)21 .

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