LETTER

pubs.acs.org/NanoLett

Graphene-based Spin Caloritronics

Minggang Zeng,†,‡ Yuanping Feng,‡ and Gengchiau Liang*,†
†
Department of Electrical and Computer Engineering, 4 Engineering Drive 3, National University of Singapore, Singapore 117576,
Republic of Singapore
‡
Department of Physics, 2 Science Drive 3, National University of Singapore, Singapore 117542, Republic of Singapore

ABSTRACT: Thermally induced spin transport in magnetized

zigzag graphene nanoribbons (M-ZGNRs) is explored using first-
principles calculations. By applying temperature difference be-
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tween the source and the drain of a M-ZGNR device, spin-up and
spin-down currents flowing in opposite directions can be induced.
This spin Seebeck effect in M-ZGNRs can be attributed to the
asymmetric electron-hole transmission spectra of spin-up and
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spin-down electrons. Furthermore, these spin currents can be

modulated and completely polarized by tuning the back gate
voltage. Finally, thermal magnetoresistance of ZGNRs between ground states and magnetized states can reach 104% without an
external bias. Our results indicate the possibility of developing graphene-based spin caloritronic devices.
KEYWORDS: Graphene, spin caloritronics, spintronics, spin Seebeck effect, thermal magnetoresistance effect, thermal spin
components

spin caloritronics.8 In this Letter, using first-principles calcula-

D issipating heat, or waste energy, is one of the critical issues of
electronic devices as they shrink toward nanoscale dimen-
sion and increase in operating speed. To realize energy saving
tions, the physical insights of spin caloritronics based on magne-
tized zigzag graphene nanoribbons (M-ZGNRs) and their
and improve the performance and reliability of electronic devices, possible applications are investigated. We demonstrate that
waste energy should be reduced or utilized. In this regard, opposite spin currents can be generated in M-ZGNRs with a tem-
spintronics offers a promising path to achieve lower energy perature difference, rather than bias voltage, between the source
consumption.1-3 Thermoelectronics, on the other hand, ex- and the drain. This interesting spin Seebeck effect is attributed to
plores the possibility of directly converting heat into electrical the asymmetric transmission spectra of spin-up and spin-down
power.4-8 An exciting new research field taking advantage of electrons in M-ZGNRs.23 Furthermore, a back gate voltage can
both spintronics and thermoelectronics, called spin caloritronics, be implemented to modulate the spin currents, which creates a
is attracting a growing interest.9 Thermally assisted reversal of thermal spin transistor with complete spin polarization. Finally,
magnetization is an example of spin caloritronics, where the very large thermal magnetoresistance (MR) effect, which is
spintronics components can benefit from the controlled thermal related to the magneto Seebeck effect, is found when the
currents.10 Furthermore, spintronics components may be oper- magnetic state of ZGNRs is transformed from ferromagnetic
ated with thermally induced spin currents in the absence of state to ground state. Our results show that magnetized ZGNRs
external bias voltage. One of the milestones of spin caloritronics are promising for spin caloritronic applications.
is the recent discovery of spin Seebeck effect in ferromagnetic Methodology. First-principles bandstructure calculations are
metal (NiFe alloy), semiconductor (GaMnAs) and insulator performed with ATK package24,25 employing the local spin
(LaY2Fe5O12).11-13 In these experiments, spin-up current and density approximation (LSDA) with the Perdew-Zunger ex-
spin-down current can be generated without using an electrical change-correlation functional.26 The vacuum layers between two
bias but with temperature difference instead. Furthermore, these sheets are 15 Å to avoid the artificial Coulomb interactions between
thermally induced spin-up and spin-down currents flow in the contents in two neighboring cells. Moreover, a cutoff energy of
opposite directions, which can be converted to a spin voltage 150 Ry and a Monkhorst-Pack k-mesh of 1
1
100 are chosen to
measured via inverse spin Hall effect (ISHE).14-16 These inter- achieve the balance between calculation efficiency and accuracy. A
esting phenomena indicate the possibility of applying spin calori- double-ζ polarized (DZP) basis set is adopted for electron wave
tronics in energy harvesting devices to directly convert heat into function and the spin-dependent current through the system is
electricity, as well as in low-power-consumption devices. calculated using the Landauer Formula
Z
On the other hand, graphene is an invigorating research field vð V Þ e ¥ vð V Þ
currently and recent studies have show that it has strong I ¼ fT ðεÞ½fS ðε, TS Þ - fD ðε, TD Þgdε ð1Þ
h -¥
potentials for spintronic applications.17-23 However, most stud-
ies were focused on the spin currents generated by an external Received: January 1, 2011
bias, and very little attention has been paid to the possibility of Revised: February 8, 2011
thermally induced spin-polarized currents for graphene-based Published: February 23, 2011

r 2011 American Chemical Society 1369 dx.doi.org/10.1021/nl2000049 | Nano Lett. 2011, 11, 1369–1373
Nano Letters LETTER

Figure 1. (a) The schematic illustration of M-ZGNRs based thermal Figure 2. (a) The Fermi distribution of the source (the left panel-higher
spin devices. A M-ZGNRs, with spin-up polarization, is placed on a temperature) and the drain (the right panel-lower temperature). The
substrate. TSD represent the temperature difference between the source electron current (Ie) and the hole current (Ih) are created due to the
(TS) and the drain (TD), i.e., TD - TS. A back-gate voltage is used to difference of carrier concentration at the two terminals. (b) The spin
control the thermal spin polarized currents. (b) The spin dependent dependent transmission spectrum and the bandstructure of M-ZGNR.
currents versus TS for different TSD. The spin-up current and the spin- (c) The spin-down current spectra for different TS (TSD = 60 K). (d)
down current flow in opposite directions (spin Seebeck effects). (c) The width dependence of spin currents for different TS (TSD = 60 K).
lg(ISD) - TS curve for the spin-up current and the spin down current
with TSD = 60 K. by the Fermi distribution (fS(E,TS) - fD(E,TD)), which is
intimately related to the electron temperature at the two
where fS(D)(ε) is the Fermi-Dirac distribution for the source terminals as shown in Figure 2a. Because of difference in the
(drain), and Tv(V)(ε) is the spin-resolved transmission of spin-up Fermi distribution, carriers with energy higher than the Fermi
(down) electrons calculated by the number of transport modes energy flow from the source (higher temperature) to the drain
from the bandstructure mentioned above. (lower temperature), resulting in electron current Ie. Conversely,
A schematic illustration of the proposed ZGNRs-based device carriers with energy lower than the Fermi energy flow in the
is shown in Figure 1a. The magnetic state of ZGNRs can be opposite direction, resulting in hole current Ih. If the transmis-
controlled by an external magnetic field.23 Except in special sion is energy independent, Ie and Ih will cancel out each other,
notes, the width of the ZGNR in our discussion is 1.36 nm, that is, leading to a zero net thermal current.
6ZGNR with six carbon dimers.28 In this work, we focus on However, as shown in the left panel of Figure 2b, the spin-
currents driven by temperature difference (TSD), the difference dependent transmission spectrum for M-ZGNR has a peak in the
between the source temperature (TS) and the drain temperature energy range -0.323 eV < E - EF < -0.213 eV and 0.156 eV <
(TD), that is, TS - TD. E - EF < 0.168 eV for the spin-up electrons and the spin-down
Results and Discussion. In Figure 1b, we plot the spin electrons, respectively. The origin of this transmission peak can
dependent currents versus TS with different TSD. It is clearly be attributed to the unique bandstructure of M-ZGNR.23,29,30
seen that there is a threshold temperature Tth,v(∼250 K) and As shown in the right panel of Figure 2b, the bandstructure of
Tth,V(∼200 K) for the spin-up current and the spin-down current, the spin-up electrons displays a double degenerate band tail
respectively. When TS < Tth,v (Tth,V), the spin-up (down) current near the x-point. As a result, the number of transport channels
is approximately zero. When TS > Tth,v (Tth,V), the spin-up for the spin-up electrons in the energy range -0.323 eV < E -
(down) current increases with increasing TS. Similarly, as TSD EF < -0.213 eV is three. On the other hand, the π and π* band
increases, ISD increases, cf., Figure 1c, and the ratio of Ion/Ioff for of spin-down electrons intersect each other within a narrow
spin-up (down) current can be as high as 108 (105) with a TSD of energy range (0.156 eV < E - EF < 0.168 eV) near the x-point,
60 K. Furthermore, it is worthy to note that the spin-up current leading to a transmission fluctuation in this energy region. The
and the spin-down current flow in opposite directions, indicating band tail and intersection near the x-point for the spin electrons
spin Seebeck effect11-13 in M-ZGNRs.27 However, graphene may be caused by the interaction between the strongly spin
may not be a good thermal electric conversion material due to its polarized edge states.23,29,30 As a result, these transmission peaks
low figure of merit (ZT),32,33 therefore, instead of evaluating the break the electron-hole symmetry in the transmission spectrum,
Seebeck coefficient, we focus on the mechanism to create spin leading to the nonzero net thermal spin currents. To further
polarized currents in magnetized ZGNRs and their possible illustrate this point, the transmission peak of spin-down electrons
applications. occurs at energies above Fermi level, and hence, Ie dominates Ih
To understand the fundamental mechanism of these interest- for the spin-down electrons, resulting in the negative spin-down
ing characteristics, we first consider the electron distribution at current (from the drain to the source). On the other hand, the
the source and the drain. Since the contacts are the same material behavior of the spin-up electrons is opposite to that of the spin-
and possess the same density of states, the difference in carrier down electrons, and the positive spin-up current is generated
concentrations between the source and the drain is determined from the source to the drain, exhibiting the spin Seebeck effect in
1370 dx.doi.org/10.1021/nl2000049 |Nano Lett. 2011, 11, 1369–1373
Nano Letters LETTER

M-ZGNRs. Furthermore, it is found that the spin-down current

is larger than spin-up current even though the transmission peak
of spin-down electrons is much narrower than that of spin-up
electrons. This can be attributed to the fact that the transmission
peak of spin-down electrons is closer to the Fermi energy as
compared to the peak of spin-up electrons.
Because of the exponential decaying nature of the Fermi
distribution, and the fact that the transmission peaks are relatively
far away from the Fermi level, a sufficiently high temperature is
required to broaden the distribution to overlap with the trans-
mission peaks and turn on the spin currents. For example, as the
current spectra (J(E) = T(E)(fS(E,TS) - fD(E,TD)) of spin-
down electrons shown in Figure 2c, when TS < Tth,V, the curve of
(fS(E,TS) - fD(E,TD)) remains close to zero within the energy
windows where the transmission peak exists (0.156 eV < E - EF <
0.168 eV). Therefore, as the black line (TS = 100 K) shown in the
inset of Figure 2c, J(E) is equal to zero within the energy range of
the transmission peak, indicating that the transmission peak does
not have a large net effect on the current. Thus, the electron-
hole symmetry for spin-down current is not broken, which leads
to the suppressed spin-down current. However, when TS > Tth,V,
the overlap between the curve (fS(E,TS) - fD(E,TD)) and the
transmission peak initiate the effect of transmission peak (see
J(E) for TS = 200 K and TS = 300 K in the inset of Figure 2c, and
break the electron-hole symmetry, giving a nonzero net thermal
spin-down current. A similar effect can be observed for the spin-
up current with the small peak in the current spectra generated by Figure 3. (a) Output characteristics of thermal spin-up currents as a
the electron-hole asymmetry appearing in the positive side of E function of TSD under different negative back-gate voltage (VG) (TS =
- EF. Furthermore, we also investigate spin currents of 400 K). (b) Output characteristics of thermal spin-down currents as a
M-14ZGNR as a function of TS as shown in Figure 2d. It is function of TSD under different positive back-gate voltage (VG) (TS =
found that compared to M-6ZGNR, Tth decreases slightly, and 400 K). (c) The current spectra for different TSD (VG = 0 V, TS = 400 K).
The inset shows the zoom in current spectra in the energy range -0.24
the thermally induced spin currents are enhanced for 14ZGNR
eV < E - EF < -0.2 eV. (d) The current spectra for different VG (TSD =
case. The reasons of these phenomena can be attributed to the 60 K, TS = 400 K). (e) The gate dependent spin-up current and spin-
distance of the asymmetric transmission peaks of spin-up and down current. (f) The polarization of spin current (SP = (|Iup| -
spin-down electrons to the intrinsic Fermi level. It has been |Idown|)/(|Iup| þ |Idown|)
100) as a function of VG for 6ZGNR and
studied that the peaks of the wider width M-ZGNR systems are 14ZGNR.
closer to the Fermi level.28,29 As a result, higher thermal-induced
spin currents can be obtained easier in wider M-ZGNR systems. application of these novel green transistors in low-power circui-
Furthermore, we would like to note that from a linear-response try. To understand the device physics of M-ZGNRs spin
quantum transport’s viewpoint, the mechanisms of the currents caloritronics, current spectra for spin-up current at different
induced by the voltage and the temperature difference are TSD with VG = 0 V is presented in Figure 3c. We found that
controlled by the carrier transmission function of the systems. the current spectra for TSD of 40, 80, and 150 K show distinct
However, the former is induced by a difference in Fermi features, leading to a nonlinear increasing thermal current under
distributions caused by the different voltages (i.e., different low TSD. However, the current spectra for TSD of 150 and 200 K
chemical potentials at the two leads), and the latter is caused are almost overlapping, resulting in a saturated current. Further-
by the different temperatures. In addition, because of the unique more, to explore the gate-dependent saturation currents, the
properties of ZGNRs it has been shown that the current driven current spectra at different back-gate voltage for a fixed TSD (150 K)
by a voltage difference is controlled by the wave function are shown in Figure 3d. It is found that shifting the Fermi level with a
symmetry of the spin-up and the spin-down channels.23 On negative VG closer to the spin-up electron transmission peak may
the other hand, the mechanism of the currents generated from a enhance the impact of electron-hole asymmetry and greatly
temperature difference in this study is attributed to the electron increase the thermally induced spin-up current. Because of the
bandstructure, characterized by electron-hole asymmetry, of opposite effect of the back-gate voltage on the spin-up current and
the spin-up and the spin-down channels. the spin-down current, completely spin polarized current can be
Next, we investigate the effect of back-gate voltage on the obtained via back-gate voltage tuning. Figure 3e shows the spin
thermally induced spin currents of M-ZGNRs. Figure 3a,b show currents as a function of back-gate voltage for a fixed TSD (150 K)
the spin-up current and the spin-down current as a function of and TS (400 K), and it is found that the spin-up (spin-down)
TSD and VG, respectively. As VG is fixed and TSD increases, spin current predominates the other one in the negative (positive) VG.
currents (ISD) increase and reach saturation; as TSD is fixed and Moreover, the transport directions of the spin-up current and the
the amplitude of VG increases, ISD increase. These behaviors are spin-down current change to the opposite side as the higher negative
very similar to those of conventional field-effect transistors and positive gate bias are applied. The reason of this can be
(FETs) operated under external bias. However, the absence understood from the chemical potential passing the transmission
of the source-drain bias in our study indicates a potential peak to cause the change in the carrier type from electrons (holes)
1371 dx.doi.org/10.1021/nl2000049 |Nano Lett. 2011, 11, 1369–1373
Nano Letters LETTER

metal-based MR devices, which have successful applications in

digital storage, but face difficulties in integrating with other spin
components so that logic operation and digital storage can be
performed in the same devices.2,35
Conclusion. We have shown that M-ZGNRs driven by
temperature difference pose several intriguing properties for spin
caloritronics. By breaking the electron-hole symmetry, a
strongly spin polarized current can be generated in M-ZGNRs
using temperature difference instead of external electrical bias.
Moreover, this thermally induced spin polarized current in
Figure 4. (a) The spin dependent transmission spectrum and band- M-ZGNRs can be controlled by thermal (i.e., temperature),
structure for GS-ZGNR. (b) The spin currents as a function of TSD for electrical (gate voltage) or magnetic means, thereby providing a
M-ZGNR and GS-ZGNR (VG = -0.02 V, TS = 400 K). The inset shows rich set of thermal spin components (spin filter, spin diode,
MR can be as high as 5
104% by translating ZGNRs from ferromag- spin FET, MR device). The results in this study show an
netic to ground state. MR is calculated based on the following formula: approach to create and control thermally induced spin-polarized
MR = (RM - RGS)/(RGS)
100 = ((|IGS|)/(|IM|) -1)
100, where currents in nanodevices and pave the way for carbon-based spin
RM = TSD/|IM| and RGS = TSD/|IGS| are the thermal-induced resistances caloritronics.
in the M-ZGNR and GS-ZGNR, respectively.
to holes (electrons) for spin-up (spin-down) current as discussed in ’ AUTHOR INFORMATION
Figure 2a. We further calculate the spin polarization of the spin
currents, cf., Figure 3f, and find that it can approach -100% (100%) Corresponding Author
under the positive (negative) back-gate voltage. Similarly, the spin *E-mail: elelg@nus.edu.sg.
polarization of a wider ZGNR (14ZGNR) under the same tem-
perature conditions also shows the same behaviors, except that the ’ ACKNOWLEDGMENT
turnover voltage, that is, |Iup| = |Idown|, is reduce to VG = 0. This is We thank Professor M. B. A. Jalil, Dr. L. Shen, and Mr. K. T.
because the distances of the transmission peak of spin-up and spin- Lam for the helpful discussion. The computations were per-
down electrons to the Fermi level are the same in the wider ZGNR formed on the cluster of Computational Nanoelectronics and
case, resulting in the equal spin-up and spin-down current. This Nanodevice Laboratory, National University of Singapore. This
promising characteristic of M-ZGNRs based on spin caloritronics work was supported in part by the Ministry of Education of
indicates a potential application as a perfect bipolar spin filter.31 Singapore under Grant R263000578112.
In addition, we investigate the impact of magnetic field in
thermally driven currents in ZGNRs. In principle, the M-ZGNR
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