Giant spin Seebeck effect in a non-magnetic material
Giant spin Seebeck effect in a non-magnetic material
Giant spin Seebeck effect in a non-magnetic material
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LETTER<br />
doi:10.1038/nature11221<br />
<strong>Giant</strong> <strong>sp<strong>in</strong></strong> <strong>Seebeck</strong> <strong>effect</strong> <strong>in</strong> a <strong>non</strong>-<strong>magnetic</strong> <strong>material</strong><br />
C. M. Jaworski 1 , R. C. Myers 2,3 , E. Johnston-Halper<strong>in</strong> 3 & J. P. Heremans 1,3<br />
The <strong>sp<strong>in</strong></strong> <strong>Seebeck</strong> <strong>effect</strong> is observed when a thermal gradient applied<br />
to a <strong>sp<strong>in</strong></strong>-polarized <strong>material</strong> leads to a spatially vary<strong>in</strong>g transverse<br />
<strong>sp<strong>in</strong></strong> current <strong>in</strong> an adjacent <strong>non</strong>-<strong>sp<strong>in</strong></strong>-polarized <strong>material</strong>, where it<br />
gets converted <strong>in</strong>to a measurable voltage. It has been previously<br />
observed with a magnitude of microvolts per kelv<strong>in</strong> <strong>in</strong> <strong>magnetic</strong>ally<br />
ordered <strong>material</strong>s, ferro<strong>magnetic</strong> metals 1 , semiconductors 2 and <strong>in</strong>sulators<br />
3 . Here we describe a signal <strong>in</strong> a <strong>non</strong>-<strong>magnetic</strong> semiconductor<br />
(InSb) that has the hallmarks of be<strong>in</strong>g produced by the <strong>sp<strong>in</strong></strong> <strong>Seebeck</strong><br />
<strong>effect</strong>, but is three orders of magnitude larger (millivolts per kelv<strong>in</strong>).<br />
We refer to the phenome<strong>non</strong> that produces it as the giant <strong>sp<strong>in</strong></strong><br />
<strong>Seebeck</strong> <strong>effect</strong>. Quantiz<strong>in</strong>g <strong>magnetic</strong> fields <strong>sp<strong>in</strong></strong>-polarize conduction<br />
electrons <strong>in</strong> semiconductors by means of Zeeman splitt<strong>in</strong>g, which<br />
<strong>sp<strong>in</strong></strong>–orbit coupl<strong>in</strong>g amplifies by a factor of 25 <strong>in</strong> InSb. We propose<br />
that the giant <strong>sp<strong>in</strong></strong> <strong>Seebeck</strong> <strong>effect</strong> is mediated by pho<strong>non</strong>–electron<br />
drag, which changes the electrons’ momentum and directly modifies<br />
the <strong>sp<strong>in</strong></strong>-splitt<strong>in</strong>g energy through <strong>sp<strong>in</strong></strong>–orbit <strong>in</strong>teractions. Ow<strong>in</strong>g to<br />
the simultaneously strong pho<strong>non</strong>–electron drag and <strong>sp<strong>in</strong></strong>–orbit<br />
coupl<strong>in</strong>g <strong>in</strong> InSb, the magnitude of the giant <strong>sp<strong>in</strong></strong> <strong>Seebeck</strong> voltage<br />
is comparable to the largest known classical thermopower values.<br />
At present, we understand 4–6 that the <strong>sp<strong>in</strong></strong> <strong>Seebeck</strong> <strong>effect</strong> (SSE) <strong>in</strong><br />
ferromagnets results from the <strong>in</strong>teraction between pho<strong>non</strong>s and excitations<br />
of <strong>magnetic</strong> moments (mag<strong>non</strong>s), which creates a gradient <strong>in</strong><br />
the magnetization across the sample. At the steady state, the pho<strong>non</strong><br />
driven excitation of mag<strong>non</strong>s out-of-equilibrium is balanced by<br />
damp<strong>in</strong>g back to equilibrium. This dissipation of angular momentum<br />
generates a <strong>sp<strong>in</strong></strong> current flow<strong>in</strong>g <strong>in</strong>to an adjacent <strong>non</strong>-<strong>magnetic</strong> metal,<br />
a process called <strong>sp<strong>in</strong></strong>-pump<strong>in</strong>g 7,8 . The generated <strong>sp<strong>in</strong></strong> current can be<br />
electrically detected because <strong>sp<strong>in</strong></strong>-polarized electrons are selectively<br />
scattered to one side of a heavy metal (plat<strong>in</strong>um), thereby generat<strong>in</strong>g<br />
a transverse voltage via the <strong>in</strong>verse <strong>sp<strong>in</strong></strong>-Hall <strong>effect</strong> (ISHE) 9 . The SSE is<br />
enhanced by pho<strong>non</strong>–mag<strong>non</strong> drag: 4,5 <strong>in</strong> the GaMnAs/GaAs system it<br />
reaches a maximum near 5 mVK 21 when the lattice thermal conductivity<br />
and pho<strong>non</strong>–electron drag (PED) are maximal. Here we select a<br />
system <strong>in</strong> which PED, <strong>sp<strong>in</strong></strong>–orbit coupl<strong>in</strong>g and <strong>sp<strong>in</strong></strong> polarizability are<br />
maximized, namely, InSb.<br />
SSE is a thermal <strong>sp<strong>in</strong></strong> <strong>effect</strong>, belong<strong>in</strong>g to the class of irreversible<br />
thermodynamic <strong>effect</strong>s <strong>in</strong> the absence of time-reversal symmetry.<br />
Other such <strong>sp<strong>in</strong></strong>–heat <strong>in</strong>teractions <strong>in</strong>clude thermal <strong>sp<strong>in</strong></strong> torque 10 and<br />
thermally driven <strong>sp<strong>in</strong></strong> <strong>in</strong>jection 11 , offer<strong>in</strong>g new possibilities for heatdriven<br />
<strong>sp<strong>in</strong></strong>tronics. Conversely, opportunities exist for new all-solidstate<br />
energy conversion devices based on SSE, along the l<strong>in</strong>es of current<br />
thermoelectric devices. The optimization of the efficiency of thermoelectric<br />
<strong>material</strong>s <strong>in</strong>volves reach<strong>in</strong>g a compromise between mutually<br />
counter-<strong>in</strong>dicated properties (thermopower, electrical and thermal<br />
conductivities) of a s<strong>in</strong>gle <strong>material</strong>. Conversely, SSE-based thermoelectrics<br />
<strong>in</strong>volve properties (pho<strong>non</strong>–<strong>sp<strong>in</strong></strong> <strong>in</strong>teractions, <strong>sp<strong>in</strong></strong>–orbit<br />
<strong>in</strong>teractions) of at least two different <strong>material</strong>s that can be optimized<br />
<strong>in</strong>dependently to achieve higher efficiency.<br />
SSE was first measured 1–3 us<strong>in</strong>g the ISHE <strong>in</strong> Pt strips oriented perpendicular<br />
to the thermal gradient, which is the same geometry that we<br />
use <strong>in</strong> this study (Fig. 1a, <strong>in</strong>set); the SSE can also be measured us<strong>in</strong>g a<br />
longitud<strong>in</strong>al temperature gradient applied uniformly 12 or locally 13 .<br />
Here, a slab of <strong>material</strong> is subject to a temperature gradient = x T (blue<br />
represents cold <strong>in</strong> the figures, and red hot), applied parallel to a<br />
<strong>magnetic</strong> field B x , which controls the magnetization (M) and <strong>sp<strong>in</strong></strong><br />
polarization (s) aligned along x. Pt strips are evaporated onto the<br />
top surface of the slab: when a flux of <strong>sp<strong>in</strong></strong>s (J S ) diffuses along z <strong>in</strong>to<br />
the Pt strips, it generates an electric field (E ISHE ) detected as a transverse<br />
voltage (V y ; ref. 14) shown schematically <strong>in</strong> Fig. 1a and given by<br />
V y =W~E ISHE ~D ISHE (J s |s) where W is the strip width and D ISHE is<br />
the ISHE coefficient of Pt. V y scales l<strong>in</strong>early with = x T, so that the slope<br />
def<strong>in</strong>es the <strong>sp<strong>in</strong></strong> <strong>Seebeck</strong> coefficient S xy :E ISHE =(+ x T), <strong>in</strong> the same<br />
units (V K 21 ) as a thermoelectric power (or ‘charge <strong>Seebeck</strong>’ coefficient).<br />
S xy changes polarity near the middle of the sample, yield<strong>in</strong>g<br />
opposite polarity between hot and cold sides.<br />
The macroscopic (,5mm3 15 mm 3 0.5 mm) InSb samples<br />
studied here are Te-doped n-type (electron concentration n 5 3.7<br />
3 10 15 cm 23 ) and have high mobility (m < 120,000 cm 2 V 21 s 21 at<br />
5 K). The work function of Pt is larger than the electron aff<strong>in</strong>ity of<br />
InSb: a high sheet density (p 1 ) of holes accumulates <strong>in</strong> InSb<br />
(,10 15 cm 22 ; Fig. 1b) at the InSb/Pt <strong>in</strong>terface, so the p 1 -InSb/Pt<br />
<strong>in</strong>terface is Ohmic. In this p 1 -InSb region, the light hole band is<br />
<strong>non</strong>-parabolic (almost l<strong>in</strong>ear) and subject to strong <strong>sp<strong>in</strong></strong>–orbit coupl<strong>in</strong>g<br />
(<strong>sp<strong>in</strong></strong>–orbit coupl<strong>in</strong>g energy at C for the light hole band is<br />
0.8 eV) 15 , so it is likely to contribute to E ISHE . Away from the InSb/Pt<br />
<strong>in</strong>terface, we have n-InSb; the depletion region at the n/p 1 <strong>in</strong>terface is<br />
th<strong>in</strong>, <strong>in</strong>terband tunnell<strong>in</strong>g gives quasi-ohmic behaviour, and we<br />
observe l<strong>in</strong>ear current–voltage relations.<br />
In an applied <strong>magnetic</strong> field B x , electrons <strong>in</strong> n-InSb move <strong>in</strong> a helical<br />
fashion, spirall<strong>in</strong>g <strong>in</strong> the y–z plane as they translate along x. If they can<br />
complete several orbits without phase change or scatter<strong>in</strong>g (the latter<br />
a 20<br />
b Detection Polarization<br />
0.6<br />
(1,↑) (0,↓)<br />
Pt InSb<br />
15<br />
(0,↑)<br />
ε F<br />
0.3<br />
z y<br />
10<br />
CB<br />
B<br />
+ x<br />
+ – x<br />
ε F<br />
0<br />
5 –<br />
Pt<br />
VB ε g<br />
InSb<br />
0 –0.3<br />
0 2 4 6 –10 0 10 20<br />
B (T)<br />
z (nm)<br />
ε (meV)<br />
Figure 1 | Detection scheme for measurement of the SSE <strong>in</strong> <strong>non</strong>-<strong>magnetic</strong><br />
InSb. a, Landau energy levels (labels on coloured l<strong>in</strong>es) for orbital and <strong>sp<strong>in</strong></strong><br />
quantized electrons <strong>in</strong> InSb, together with calculated e F (Fermi level; black<br />
curve) as a function of the applied <strong>magnetic</strong> field B. e, k<strong>in</strong>etic energy of<br />
electrons. Inset, experimental geometry for <strong>sp<strong>in</strong></strong> <strong>Seebeck</strong> detection, not to scale;<br />
red denotes the hot side, blue the cold. b, The Pt-InSb band edge diagram,<br />
show<strong>in</strong>g, from left to right, an <strong>in</strong>terface (bold vertical l<strong>in</strong>e) between Pt and p 1 -<br />
InSb layers, followed by a th<strong>in</strong> tunnel junction bracketed by the two grey<br />
vertical l<strong>in</strong>es, and an n-InSb layer with n 5 3.7 3 10 15 cm 23 where the <strong>sp<strong>in</strong></strong><br />
polarization orig<strong>in</strong>ates. e g is the bandgap, e F the Fermi level (dashed horizontal<br />
l<strong>in</strong>e). Conduction electrons <strong>in</strong> Pt are hatched purple. In InSb, the conduction<br />
band (CB) is hatched p<strong>in</strong>k, the valence band (VB) dark blue. The<br />
<strong>sp<strong>in</strong></strong>-polarization can be detected by either holes <strong>in</strong> InSb or electrons <strong>in</strong> Pt.<br />
ε (eV)<br />
1 Department of Mechanical Eng<strong>in</strong>eer<strong>in</strong>g, The Ohio State University, Columbus, Ohio 43210, USA. 2 Department of Materials Science and Eng<strong>in</strong>eer<strong>in</strong>g, The Ohio State University, Columbus, Ohio 43210,<br />
USA. 3 Department of Physics, The Ohio State University, Columbus, Ohio 43210, USA.<br />
210 | NATURE | VOL 487 | 12 JULY 2012<br />
©2012 Macmillan Publishers Limited. All rights reserved
LETTER<br />
RESEARCH<br />
when mB x . 1), the only rema<strong>in</strong><strong>in</strong>g degree of freedom is their wave<br />
vector k which has only one component k x parallel to B x The Lorentz<br />
force conf<strong>in</strong>es the motion to cyclotron orbits that are quantized <strong>in</strong>to<br />
Landau levels with orbital quantum number i (5 0, 1, 2…). Each<br />
Landau level becomes further divided <strong>in</strong>to two <strong>sp<strong>in</strong></strong>-polarized levels.<br />
The equation of motion for the k<strong>in</strong>etic energy (e) of such electrons is<br />
described by the k x -dependence of the energy function c(e) for a given<br />
orbital (i) and <strong>sp<strong>in</strong></strong> (s x ) quantum number, which is given by: 16<br />
c(e) i,sx :e(1z e )~ B2 k 2 x<br />
e g 2m z(iz 1 2 )Bv czgm B s x B x ð1Þ<br />
where e g is the band gap, m* the <strong>effect</strong>ive mass, B the reduced Planck<br />
constant, v c (5 eB x /m c ) the cyclotron frequency, m c<br />
the cyclotron<br />
mass, g the <strong>effect</strong>ive g-factor (a function of n and Fermi energy), m B<br />
the Bohr magneton, and s x (6K) is the projection of <strong>sp<strong>in</strong></strong> along x. The<br />
Zeeman <strong>sp<strong>in</strong></strong> splitt<strong>in</strong>g energy De"# 5 gm B B x is the energy difference<br />
between s x 51K and s x 52K levels. For e , e g , c!e!B 2 k 2 x<br />
and the<br />
energy bands are free-electron-like; for high e . e g , c!e 2 !B 2 k 2 x and<br />
the relation between e and k x becomes l<strong>in</strong>ear. The Fermi surface for<br />
lightly doped n-InSb at low temperatures is spherical and located at<br />
the centre of the Brillou<strong>in</strong> zone, lead<strong>in</strong>g to isotropic behaviour<br />
with m c 5 m* 5 0.0136 m 0 (the free electron mass), g < 249 for<br />
n < 2 3 10 15 cm 23 , and e g 5 0.235 eV at 4.2 K (ref. 15). Figure 1a<br />
shows the B x dependence of each energy level (i, s x ) from equation<br />
(1) at k x 5 0. For n 5 3.7 310 15 cm 23 , we calculate the location of the<br />
Fermi level e F at T 5 0 K (an acceptable approximation for T , 20 K),<br />
shown as a full l<strong>in</strong>e <strong>in</strong> Fig. 1a. Therefore, at fields B x . 1.6 T most<br />
electrons occupy the lowest energy <strong>sp<strong>in</strong></strong>-polarized Landau level<br />
(i 5 0, s x 51K), called the ultra-quantum limit (UQL). At T . 0<br />
and under the <strong>in</strong>fluence of = x T, a small fraction of these electrons<br />
populate the next (i 5 0, s x 52K) level follow<strong>in</strong>g Fermi–Dirac<br />
statistics. Magnetoresistance below ,10 K shows quantum oscillations,<br />
the Shubnikov–de Haas <strong>effect</strong> 16 , as a function of B x as e F crosses<br />
different Landau levels (these are reported and analysed <strong>in</strong><br />
Supplementary Information). The last oscillation is observed at<br />
1.6 T, above this the sample is <strong>in</strong> the UQL.<br />
Figure 2 shows S xy as a function of B x , for four J S -sensitive Pt strips,<br />
two at the hot end (red, orange traces) and two at the cold end (green,<br />
blue traces) of the sample at four different temperatures. V y (= x T 5 0,<br />
B x 5 0) has a residual <strong>non</strong>-zero value, especially at low T, which was<br />
subtracted from the data <strong>in</strong> Fig. 2a–e. As was the case for the SSE <strong>in</strong><br />
ferro<strong>magnetic</strong> <strong>material</strong>s, S xy changes polarity at some location near the<br />
middle of the sample, yield<strong>in</strong>g signals of opposite polarity between<br />
hot and cold sides (although not perfectly antisymmetric). The traces<br />
show a large even-symmetric dependence on B x, and a small oddsymmetric<br />
one, especially below the UQL. The even-symmetric part<br />
(V y ) even :½V y (B z x )zV y(B { x )Š=2; Bz x ~{B{ x measured at 31.2 K on<br />
the hottest and coldest Pt strip is shown <strong>in</strong> Fig. 2e. These voltages<br />
are plotted as a function of the DT x between thermometers located<br />
on the samples’ hot and cold ends (not shown <strong>in</strong> Fig. 2g) <strong>in</strong> Fig. 2f,<br />
which illustrates that V y varies l<strong>in</strong>early with = x T, aga<strong>in</strong> as was the case<br />
for the SSE signal <strong>in</strong> ferro<strong>magnetic</strong> <strong>material</strong>s; this justifies a posteriori<br />
the def<strong>in</strong>ition of the quantity S xy ; E y /(= x T) 5 V y L/(DT x W), where<br />
L is the length between the thermometers. As <strong>in</strong> the case of the SSE<br />
signal <strong>in</strong> ferro<strong>magnetic</strong> <strong>material</strong>s, this signal is not observed when<br />
<strong>sp<strong>in</strong></strong>-<strong>in</strong>sensitive In-po<strong>in</strong>t contacts are used on the sample (see<br />
Fig. 3). It displays polarity <strong>in</strong>version near the middle of the sample,<br />
and is l<strong>in</strong>ear <strong>in</strong> = x T. For those reasons, and because the signal is much<br />
larger and has a different B x -dependence from the classical thermo<strong>magnetic</strong><br />
<strong>effect</strong>s taken <strong>in</strong> the same geometry (Fig. 3), we conclude that<br />
Fig. 2 shows signals similar to the SSE that orig<strong>in</strong>ate from the <strong>effect</strong> of<br />
= x T on the <strong>sp<strong>in</strong></strong>-polarized carriers <strong>in</strong> the n-type InSb; because of their<br />
amplitude, we call them the giant <strong>sp<strong>in</strong></strong> <strong>Seebeck</strong> <strong>effect</strong> (GSSE).<br />
Below the UQL <strong>in</strong> the Shubnikov–de Haas regime, S xy shows an<br />
oscillatory dependence on B x with the same period <strong>in</strong> 1/B x as the<br />
a<br />
S xy (μV K –1 )<br />
c<br />
S xy (μV K –1 )<br />
e<br />
(V y ) even (μV)<br />
g<br />
2,000<br />
μV K –1<br />
4.3 K<br />
1,500<br />
μV K –1 150<br />
μV K –1<br />
0.5 μV<br />
6.3 K<br />
–8 –4 0 4 8<br />
B x (T)<br />
∇ x T<br />
Increas<strong>in</strong>g ∇ x T<br />
Hot Pt bar<br />
Cold Pt<br />
bar<br />
Increas<strong>in</strong>g ∇ x T<br />
0 2 4 6 8<br />
B x (T)<br />
B x<br />
Pt bars<br />
InSb<br />
Shubnikov–de Haas oscillations observed <strong>in</strong> resistivity or thermopower.<br />
Interest<strong>in</strong>gly, above the UQL S xy cont<strong>in</strong>ues to change as a<br />
function of B x ; even though S xy is sensitive to orbital quantization,<br />
its orig<strong>in</strong> is clearly different from that of the Shubnikov–de Haas<br />
oscillations. The maximum value of S xy reaches 8 mV K 21 near<br />
2.8 K, more than 1,000 times larger than the largest value of SSE<br />
measured <strong>in</strong> a ferro<strong>magnetic</strong> <strong>material</strong> 4 .<br />
The amplitude of the maximum at B x 5 2.7 T is plotted as a function<br />
of T <strong>in</strong> Fig. 2h. This shows that GSSE persists above the UQL up to<br />
40 K, a temperature far <strong>in</strong> excess of the 10–15 K where the Shubnikov–de<br />
Haas oscillations disappear. We also plot <strong>in</strong> Fig. 2h a temperature amplitude<br />
reduction function<br />
R T ~ 2p2 k B T<br />
gm B B<br />
b<br />
S xy (μV K –1 )<br />
d<br />
S xy (μV K –1 )<br />
f<br />
(V y ) max<br />
even (μV)<br />
h<br />
|S xy | max (μV K –1 )<br />
1,000<br />
μV K –1<br />
–8<br />
0.5<br />
0<br />
–0.5<br />
10.4 K<br />
–4 0 4 8<br />
B x (T)<br />
0 0.1 0.2 0.3 0.4<br />
Δ x T (K)<br />
10 3<br />
R T<br />
10 4 10 20 30 40<br />
10 2<br />
0<br />
31.2 K<br />
25.1 K<br />
T (K)<br />
Figure 2 | Experimental data on the SSE <strong>in</strong> InSb. a–d, Sp<strong>in</strong> <strong>Seebeck</strong><br />
coefficient S xy (def<strong>in</strong>ed <strong>in</strong> text) as a function of applied <strong>magnetic</strong> field (B x )on<br />
first sample. The zero is the horizontal l<strong>in</strong>e <strong>in</strong> the middle of each panel. e, Evensymmetric<br />
part (V y ) even of the transverse voltage at selected temperature<br />
differences DT x between hottest and coldest strip on second sample at 31.2 K,<br />
and f, maximum of (V y ) even <strong>in</strong> e versus DT x . g, Diagram (not to scale) of InSb<br />
sample, Pt bar colour corresponds to a–d. h, Absolute value of maximum of<br />
S xy (B x ) at 2.7 T of the cold Pt bar, and function R T (see text). Error bars, s.d.<br />
{1<br />
s<strong>in</strong>h ( 2p2 k B T<br />
gm B B )<br />
ð2Þ<br />
©2012 Macmillan Publishers Limited. All rights reserved<br />
12 JULY 2012 | VOL 487 | NATURE | 211
RESEARCH<br />
LETTER<br />
a<br />
–α xxx (mV K –1 )<br />
1<br />
0.1<br />
0.01<br />
0<br />
V x<br />
V y<br />
In B b<br />
4.04 K<br />
x 0<br />
5.63 K<br />
8.28 K<br />
11.3 K<br />
InSb<br />
–20<br />
15.8 K<br />
–40<br />
c<br />
0<br />
α xxx (0T)<br />
–0.4<br />
3.8 K<br />
α xxx (7T)–α xxx (0T)<br />
–0.8<br />
8.2 K<br />
SSE (normalized)<br />
16.1 K<br />
–1.2<br />
25 50 75 100<br />
–8 –4 0 4 8<br />
T (K)<br />
B x (T)<br />
α xxx (mV K –1 ) α xyx (μV K –1 )<br />
Figure 3 | Classical thermo<strong>magnetic</strong> properties of InSb. a, Thermopower<br />
a xxx as a function of T <strong>in</strong> zero field (green open dots) and excess thermopower<br />
a xxx (B x ) 2 a xxx (B x 5 0) measured <strong>in</strong> longitud<strong>in</strong>al applied <strong>magnetic</strong> field B x //<br />
= x T at B x 5 7 T (yellow dots). The dashed blue l<strong>in</strong>e is the function R T from<br />
Fig. 2h, the amplitude of the GSSE signal as a function of T. Inset, diagram of In<br />
which, with the literature value of g 5249 and B x 5 2.7 T and only the<br />
absolute amplitude as adjustable parameter, follows the data over<br />
almost three orders of magnitude. R T was derived 16 to express the <strong>effect</strong><br />
on transport, thermal and <strong>magnetic</strong> properties of the f<strong>in</strong>ite probability<br />
of occupation of Zeeman-split Landau levels at a temperature T. In<br />
equation (2), R T depends on the ratio between the thermal energy<br />
k B T and the Zeeman energy gm B B x of conduction electrons on helical<br />
trajectories. R T is dist<strong>in</strong>ct from the Brillou<strong>in</strong> or Langev<strong>in</strong> functions that<br />
characterize the same <strong>effect</strong>s <strong>in</strong> <strong>magnetic</strong> systems where the <strong>magnetic</strong><br />
moments are due to bound electrons. We contrast R T <strong>in</strong> Fig. 2h with the<br />
much faster temperature-<strong>in</strong>duced decay <strong>in</strong> the Shubnikov–de Haas<br />
oscillations <strong>in</strong> resistivity, analysed <strong>in</strong> Supplementary Information,<br />
which <strong>in</strong>volve the orbital quantum number. Both the T and B x dependence<br />
<strong>in</strong> Fig. 2 give evidence that S xy exists <strong>in</strong> InSb even when orbital<br />
quantization is no longer resolved, and is driven by <strong>sp<strong>in</strong></strong>-polarization of<br />
conduction electrons.<br />
The classical charge-transport properties of the samples (made<br />
without Pt strips but with In po<strong>in</strong>t contacts) with B x aligned<br />
parallel to heat flux as <strong>in</strong> the SSE are reported <strong>in</strong> Fig. 3a–c. More<br />
thermo<strong>magnetic</strong> measurements are reported <strong>in</strong> the Supplementary<br />
Information, where the notation used is also expla<strong>in</strong>ed. Figure 3a shows<br />
the thermopower a xxx (B x 5 0 T) at zero field and the difference<br />
a xxx (B x 5 7T)2 a xxx (B x 5 0 T). This difference was attributed to the<br />
PED contribution to a xxx (B) (ref. 17): the magnitude and temperature<br />
dependence of the excess <strong>in</strong>dicates that PED dom<strong>in</strong>ates the thermopower<br />
<strong>in</strong> our samples, and persists above 50 K. PED is a long-range<br />
<strong>effect</strong>. Pho<strong>non</strong>–electron and pho<strong>non</strong>–pho<strong>non</strong> <strong>in</strong>teraction lengths at<br />
T , 50 K are of the order of the macroscopic sample size, as shown<br />
experimentally <strong>in</strong> measurements of size-<strong>effect</strong>s at the millimetre scale 17 .<br />
We add to Fig. 3a, as a dashed l<strong>in</strong>e, the temperature dependence of the<br />
GSSE <strong>effect</strong> from Fig. 2h, re<strong>in</strong>forc<strong>in</strong>g the conclusion that its temperature<br />
dependence is limited by equation (2), and not by PED. Figure 3b shows<br />
a pseudo-thermopower a xyx ; its purpose is to show that the E y picked up<br />
<strong>in</strong> the same configuration as the GSSE shown <strong>in</strong> Fig. 2 is negligibly small<br />
<strong>in</strong> the absence of a <strong>sp<strong>in</strong></strong>-sensitive detector. Although great care was taken<br />
to avoid small misalignments <strong>in</strong> the (x,z) plane, the reported a xyx<br />
probably has no physical significance. The <strong>magnetic</strong> field dependence<br />
of a xxx (B x ) is shown <strong>in</strong> Fig. 3c, and is quite dist<strong>in</strong>ct from that of the<br />
GSSE signals. Except for the transverse magnetothermopower a xxz (B z ),<br />
a configuration very different from the one <strong>in</strong> Fig. 2, <strong>non</strong>e of the<br />
potential parasitic <strong>effect</strong>s has the same magnitude, <strong>magnetic</strong> field<br />
dependence, or position dependence along the sample length as the<br />
GSSE.<br />
We now dist<strong>in</strong>guish the B x dependence of GSSE <strong>in</strong> <strong>non</strong>-<strong>magnetic</strong><br />
InSb from that of the SSE <strong>in</strong> ferro<strong>magnetic</strong> <strong>material</strong>s. First, the evensymmetric<br />
nature of S xy (B x ) with B x above the UQL is opposite to that<br />
po<strong>in</strong>t contacts on InSb. b, Transverse thermally <strong>in</strong>duced voltage observed with<br />
a <strong>magnetic</strong> field B x applied <strong>in</strong> the sample plane, a xyx , most probably aris<strong>in</strong>g<br />
from small parasitic misalignments. c, a xxx as a function of B x at different<br />
temperatures. Error bars, s.d.<br />
<strong>in</strong> ferro<strong>magnetic</strong> <strong>material</strong>s where S xy (B x ) is odd-symmetric with B x .<br />
Second, pho<strong>non</strong>–mag<strong>non</strong> <strong>effect</strong>s dom<strong>in</strong>ate <strong>in</strong> ferro<strong>magnetic</strong> <strong>material</strong>s,<br />
while there are no mag<strong>non</strong>s <strong>in</strong> InSb, but long-range 17 and <strong>in</strong>tense<br />
PED especially <strong>in</strong> the UQL. The sign of the momentum exchange <strong>in</strong><br />
pho<strong>non</strong>–mag<strong>non</strong> drag is not important <strong>in</strong> ferro<strong>magnetic</strong> <strong>material</strong>s<br />
because the change <strong>in</strong> M is due to heat<strong>in</strong>g or cool<strong>in</strong>g. Therefore, for<br />
a fixed= x T, the sign of the <strong>sp<strong>in</strong></strong>-current (and result<strong>in</strong>g E ISHE ) is determ<strong>in</strong>ed<br />
by the orientation of M and S xy is odd with B x . The reverse holds<br />
true when <strong>sp<strong>in</strong></strong>–orbit coupl<strong>in</strong>g is strong, because then the orientation<br />
of electron <strong>sp<strong>in</strong></strong>s (determ<strong>in</strong>ed by their total <strong>sp<strong>in</strong></strong> splitt<strong>in</strong>g De"#) is<br />
coupled to their Fermi wavevector (k F ). Sp<strong>in</strong>–orbit coupl<strong>in</strong>g <strong>in</strong> bulk<br />
InSb (ref. 18) is the orig<strong>in</strong> of the very narrow gap, small m*, large<br />
negative g, and <strong>non</strong>-parabolic dispersion (see equation (1)). Thus,<br />
when a pho<strong>non</strong> drags an electron, result<strong>in</strong>g <strong>in</strong> a Dk F , De"# changes<br />
by an amount we label De k "#. We suggest that a two-step mechanism<br />
(pho<strong>non</strong> momentum gives Dk F by PED, and Dk F gives De k "# by <strong>sp<strong>in</strong></strong>–<br />
orbit coupl<strong>in</strong>g) results <strong>in</strong> the GSSE <strong>effect</strong>, as described below.<br />
By analogy with the SSE <strong>in</strong> ferro<strong>magnetic</strong> <strong>material</strong>s, which required<br />
a mag<strong>non</strong> population out of thermal equilibrium with the pho<strong>non</strong><br />
population, the GSSE requires the electrons to be out of thermal equilibrium<br />
4–6 . Follow<strong>in</strong>g similar arguments, the imposition of the thermal<br />
gradient implies an equilibrium between pho<strong>non</strong>s and electrons near<br />
the middle of the sample, and we set the Zeeman splitt<strong>in</strong>g energy there<br />
as De 0"# 5 gm B B x , as well as Dk F 5 0. At the hot end, PED adds<br />
momentum (Dk F . 0) to the electrons above the thermal equilibrium<br />
value set <strong>in</strong> the middle of the sample; at the cold end, PED subtracts<br />
momentum from the equilibrium value (Dk F , 0). While k F and the<br />
netmotion<strong>in</strong>equation(1)alignwithB x along the x axis, the electron<br />
trajectory is helical, with a component <strong>in</strong> the (y,z)-plane; Dk F results <strong>in</strong> a<br />
change of orbital velocity, which, through <strong>sp<strong>in</strong></strong>–orbit <strong>in</strong>teractions, results<br />
<strong>in</strong> a <strong>sp<strong>in</strong></strong>–orbit field DB s-o oriented along x. DB s-o adds (hot side) or<br />
subtracts (cold side) from the applied field B x , result<strong>in</strong>g <strong>in</strong> a perturbation<br />
De k "# 5 gm B DB s-o of the Zeeman energy, De"# 5 De 0"# 1 De k "# 5 gm B<br />
(B x 1 DB s-o ). Def<strong>in</strong><strong>in</strong>g b ; de"#/dk F , the sign of this <strong>effect</strong> is shown <strong>in</strong><br />
Fig. 4. When B x is parallel to= x T (B x . 0, Fig. 4b), for the hot side Dk F . 0,<br />
and, assum<strong>in</strong>g b . 0, De k "# . 0. At the cold side, Dk F ,0 and De k "# , 0.<br />
The orientation of B x has no <strong>effect</strong> on the orientation of DB s-o , as shown<br />
<strong>in</strong> Fig. 4. Because the perturbation of <strong>sp<strong>in</strong></strong>-up and <strong>sp<strong>in</strong></strong>-down states is<br />
<strong>in</strong>dependent of applied field direction, the result<strong>in</strong>g S xy is <strong>in</strong>dependent<br />
of the sign of the background <strong>sp<strong>in</strong></strong> splitt<strong>in</strong>g, result<strong>in</strong>g <strong>in</strong> the evensymmetric<br />
behaviour observed. The sign of the <strong>sp<strong>in</strong></strong> polarization of<br />
the <strong>sp<strong>in</strong></strong> current <strong>in</strong> Pt is solely determ<strong>in</strong>ed by the direction of PED,<br />
which determ<strong>in</strong>es the sign of Dk F and the result<strong>in</strong>g De k "#.<br />
To estimate the order of magnitude of the <strong>effect</strong> of the above mechanism,<br />
we derive the slope b from the experimental dependence of g on<br />
n (dg/dn < 25 3 10 222 m 23 ; ref. 15); <strong>in</strong> that experiment, the <strong>effect</strong> of<br />
212 | NATURE | VOL 487 | 12 JULY 2012<br />
©2012 Macmillan Publishers Limited. All rights reserved
LETTER<br />
RESEARCH<br />
a<br />
InSb<br />
b<br />
Pt<br />
+½βΔk<br />
ε<br />
–½βΔk<br />
c<br />
–½βΔk<br />
ε<br />
+½βΔk<br />
–q x 0 +q x Δk<br />
B x //∇ x T<br />
–gμ B<br />
B<br />
–gμ B<br />
B<br />
B x //–∇ x T<br />
+½βΔk<br />
–½βΔk<br />
–½βΔk<br />
+½βΔk<br />
Figure 4 | How pho<strong>non</strong>–electron drag causes the SSE <strong>in</strong> InSb through the<br />
<strong>sp<strong>in</strong></strong>-orbit <strong>in</strong>teraction. a, Sample geometry (not to scale), with the grey bar<br />
show<strong>in</strong>g the change <strong>in</strong> electron momentum Dk due to drag by pho<strong>non</strong>s of<br />
momentum q x correspond<strong>in</strong>g to the applied temperature gradient. b, c, The<br />
<strong>sp<strong>in</strong></strong>-up and <strong>sp<strong>in</strong></strong>-down electron energy levels are plotted at the cold, middle<br />
and hot side of the sample (coloured blue, pale grey and p<strong>in</strong>k respectively) for<br />
the applied <strong>magnetic</strong> field (B x ) parallel (b, green arrows) and anti-parallel<br />
(c, brown arrows) to = x T. At the cold end, pho<strong>non</strong> drag reduces (<strong>in</strong>creases) the<br />
<strong>sp<strong>in</strong></strong>-down (<strong>sp<strong>in</strong></strong>-up) energy irrespective of the sign of B x , while the reverse<br />
holds true at the hot end. Therefore the sign of the <strong>sp<strong>in</strong></strong> <strong>Seebeck</strong> <strong>effect</strong> depends<br />
on the direction of pho<strong>non</strong> drag, not on the sign of B x .<br />
<strong>sp<strong>in</strong></strong>–orbit <strong>in</strong>teractions is parameterized <strong>in</strong> the value of g(n), rather<br />
than a separate term DB s-o . We further use the k F dependence of the<br />
electron concentration on a s<strong>in</strong>gle Landau level 16 dn/dk F 5 eB/(2p 2 B),<br />
and write b 5 m B B x (dg/dn)(dn/dk F ). The temperature difference of<br />
DT will then change pho<strong>non</strong> momentum by Dq ; k B DT/(Bc) where c<br />
is the average sound velocity. If we assume that PED fully transfers this<br />
to electrons, Dk F 5 Dq. For DT 5 40 mK, as we use near 5 K<br />
(k B T < 430 meV), jDe k "#j is of the order of 150 meV at 7 T, quite<br />
enough to alter the statistical distribution and therefore the <strong>sp<strong>in</strong></strong>-polarization<br />
of electrons. Note that <strong>in</strong> the absence of a quantitative measure<br />
of the <strong>sp<strong>in</strong></strong> transfer efficiency across the Pt/InSb <strong>in</strong>terface, translat<strong>in</strong>g<br />
this energy <strong>in</strong>to an estimated magnitude of the GSSE signal is not<br />
possible at present.<br />
There is a small odd-symmetric component of S xy (B x ), especially<br />
below the UQL where Shubnikov–de Haas oscillations are observed.<br />
We suggest that it arises from the classical magneto-thermopower, an<br />
even-symmetric function of B x , of the electrons on the (i 5 0, s x 5 K)<br />
level. Because their polarization flips with the direction of B x , the<br />
perturbation of their distribution due to PED <strong>in</strong> = x T creates a SSE<br />
signal that is odd <strong>in</strong> B x .<br />
The magnitude and generality of GSSE and SSE, and the fact that the<br />
thermal voltages are generated <strong>in</strong> metallic electrodes that have a low<br />
source impedance, suggest the potential for further optimization of<br />
these <strong>effect</strong>s and perhaps of all solid-state <strong>sp<strong>in</strong></strong>-thermal devices.<br />
METHODS SUMMARY<br />
Several parallelepiped-shaped samples (z 5 0.5 mm thick, y 5 3–5 mm wide and<br />
x 5 10–20 mm long) were cleaved from a Te-doped InSb wafer along the [110]<br />
direction. For GSSE measurements, 10 nm of Pt was deposited on top of a<br />
1-nm-thick Ti adhesion layer on the InSb. To perform classical galvano<strong>magnetic</strong><br />
and thermo<strong>magnetic</strong> measurements, different samples were equipped with<br />
diffused In po<strong>in</strong>t contacts. All contacts were verified to be ohmic with I/V curves<br />
at the millivolt scale. Measurements were made us<strong>in</strong>g the conventional heater and<br />
s<strong>in</strong>k method <strong>in</strong> a modified Thermal Transport Option <strong>in</strong> the Quantum Design<br />
PPMS system 2 . Out-of-plane temperature gradients are avoided 19 by the use of<br />
bulk samples with m<strong>in</strong>imized heat leaks through contacts (40-mm copper wires<br />
attached to the Pt bars with silver epoxy, or soldered to the In po<strong>in</strong>t contacts as<br />
voltage leads), and with m<strong>in</strong>imized radiative or convective losses (fully gold-plated<br />
cryopumped sample chamber). The top and bottom surfaces of the samples are<br />
<strong>in</strong>dium-soldered to the heat source/s<strong>in</strong>k. Cernox thermometry (Lakeshore CX-<br />
1050-BR) calibrated as a function of T is used. For GSSE measurements, we fix<br />
cryostat temperature and heater power and sweep B while record<strong>in</strong>g V y across the<br />
Pt strips us<strong>in</strong>g a Keithley 2182A nanovoltmeter. Relative error <strong>in</strong> S xy (B) is readily<br />
apparent <strong>in</strong> the noise <strong>in</strong> Fig. 2; the ma<strong>in</strong> source of absolute error is <strong>in</strong> DT x , and is<br />
<strong>in</strong>dividually estimated for each po<strong>in</strong>t <strong>in</strong> Fig. 2f and h. The SSE data were reproduced<br />
on a second, <strong>in</strong>dependently prepared sample, and further S xy (B x ) data are<br />
reported <strong>in</strong> Supplementary Information. Reproducibility of the amplitude is<br />
limited by the reproducibility of the quality of the Pt/InSb <strong>in</strong>terfaces.<br />
Received 16 February; accepted 8 May 2012.<br />
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Supplementary Information is l<strong>in</strong>ked to the onl<strong>in</strong>e version of the paper at<br />
www.nature.com/nature.<br />
Acknowledgements We thank Y. Kato, H. Adachi, S. Maekawa and D. Stroud for<br />
discussions, and K. Wickey for assistance. This work was supported by the NSF<br />
CBET-1133589 (data acquisition and <strong>in</strong>terpretation) and by DMR-0820414 (sample<br />
preparation). C.M.J. has a fellowship from the DOE GATE Center of Excellence FG26<br />
05NT42616.<br />
Author Contributions C.M.J., R.C.M. and J.P.H. conceived the study; C.M.J. designed the<br />
experiments, prepared the samples with help from E.J.-H., and collected and carried out<br />
analysis of the data. R.C.M. and J.P.H. developed the explanation. All authors discussed<br />
the results and participated <strong>in</strong> writ<strong>in</strong>g the manuscript.<br />
Author Information Repr<strong>in</strong>ts and permissions <strong>in</strong>formation is available at<br />
www.nature.com/repr<strong>in</strong>ts. The authors declare no compet<strong>in</strong>g f<strong>in</strong>ancial <strong>in</strong>terests.<br />
Readers are welcome to comment on the onl<strong>in</strong>e version of this article at<br />
www.nature.com/nature. Correspondence and requests for <strong>material</strong>s should be<br />
addressed to J.P.H. (heremans.1@osu.edu).<br />
h<br />
©2012 Macmillan Publishers Limited. All rights reserved<br />
12 JULY 2012 | VOL 487 | NATURE | 213