Ab Initio Studies of Spin Hall Effect

Ab Initio Studies of Spin Hall Effect

Guang-Yu Guo
Department of Physics and Center for Theoretical Sciences, National Taiwan University, Taipei 106, Taiwan

Spin Hall effect refers to the generation of transverse spin current in a solid by an electric field or current [Fig. 1] . Spin current generation is an important issue in the emerging spintronics technology. Therefore, spin Hall effect has recently become an issue of intensive interests both theoretically and experimentally since the theoretical proposals of the intrinsic spin Hall effect [1, 2]. In this article, we will first give an introduction to ab initio calculation approaches to the various issues in the field of spin Hall effect, in particular, Berry phase theory and ab initio relativistic band structure method for studying intrinsic spin Hall effect. This will be followed by a review on our recent ab initio relativistic band theoretical calculations on the intrinsic spin Hall effect in (1) p-type zincblende semiconductors Si, Ge, GaAs and AlAs, (2) in n-type nitride semiconductor superlattices, and also (3) in platinum and aluminum metals. Extrinsic resonant skew scattering mechanism for the gigantic spin Hall effect observed recently in FePt/Au system [3] will also be discussed.

computer experiments, theoreticians can investigate some important systems where human being cannot conduct experiments yet, such as the physical and chemical processes happening in the interior of our planet [4]. The 1998 Nobel Prize was awarded to W. Kohn for the development of density functional theory [5, 6] upon which many present-day ab initio calculations are based. In condensed matter and material sciences, ab initio calculation has become an indispensable tool for investigation of novel properties of advanced materials and for development and even design of new functional materials. With ab initio calculations, scientists can guide advanced materials development and comprehend how materials form, how they react under changing conditions, and how they can be optimized for better performance. Ab initio calculation has also played a crucial role in the magnetism and magnetic materials research [7] in the past decades. In 1970s, the magnetism research appeared to be hindered by the observation of magnetically dead layers at transition metal surfaces and

Guang-Yu Guo

1. INTRODUCTION

Most theoretical models either have no analytical solutions or their analytical solutions are too difficult to obtain. In the past decades, however, numerical calculation has enabled many theoretical models to be analyzed and their predictions to be compared with experiments. In particular, modern numerical calculations based on ab initio quantum mechanical theories can accurately determine the empirical parameters in many theoretical models without resort to experiments. Furthermore, advanced ab initio theoretical calculations nowadays can predict physical and chemical processes occurring in many real and complex systems. Also, through

interfaces [8] together with subsequent supporting theoretical evidence [9]. However, the field was greatly boosted in part by a number of ab initio calculations [10] which predicted strongly enhanced magnetization on overlayers, interfaces and superlattices. Around 1990, ab initio calculations helped attract further attention into the field of magnetism by predicting gigantic perpendicular magneto-crystalline anisotropy in ultrathin magnetic films [11, 12] which have valuable applications in high density data storage devices. Ab initio calculations [13, 14] have also revealed detailed microscopic mechanism of giant magnetoresistance (GMR) and also tunneling magnetoresistance (TMR) in magnetic multilayers. The discovers of

Fig. 1: (a) Conventional Hall effect and (b) spin Hall effect.

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Celebrating 20 Years of GMR Past, Present, and Future (I)

the GMR, A. Fert and P. Grunberg, won the Nobel Physics Prize last year (2007). Half-metallic magnetic conductors, a class of materials which are important for spintronics, were first predicted by ab initio calculations [15, 16].

relativitic band theory. In this case the current operators j are, ev, ( / 4){z, v} and ( / 2){Lz, v} for the anomalous, spin and orbital Hall effects, respectively. Here , z are the well known 44 Dirac matrices, and v is the velocity operator projected onto states above the electron-positron In this article, however, we will fo- mass gap [18]. The Hall conductivities cus on a different aspect of spintronics, can also be written in terms of Berry phase namely, generation and manipulation of curvature xy(k) [19] as spin current without magnetic materials z z or magnetic fields. In particular, we will xy = e (k) = e fkn n(k) k k n restrict ourselves to the spin Hall effect 2Im[knjxknknvykn] (SHE) [1, 2], an effect which has been a zn(k) = (4) nn (Ekn Ekn )2 source of excitements in the past years. where fkn is the Fermi-Dirac function.

the existence of the intrinsice spin Hall effect in semiconductors structures and that whether it would be cancelled out by the orbital Hall effect, were unsolved. In the meantime, experimental measurements of large SHE for the Rashba two-dimensional electron gas and for n-type bulk semiconductors were reported [26, 27]. Stimulated by the prospect that intrinsic SHE may provide a useful property for spintronics applications, we have carried out ab initio calculations on this effect and related phenomena in the archetypical p-type semiconductors Si, Ge, GaAs and AlAs [28]. We focused on the p-type because the SOC is much stronger in the valence bands, where intrinsic effect has a better chance of dominating over the extrinsic scattering effects. In addition, the calculations may also help resove some of the theoretical issues mentioned above. Our results cover a large range of hole concentration which is beyond the validity regime of the Luttinger model. We found that the spin Hall conductivity (SHC) in hole-doped semiconductors Ge, GaAl and AlAs is large [Fig. 2], showing the possibility of a SHE beyond the four-band Luttinger Hamiltonian. The calculated orbital Hall conductivity is one order of magnitude smaller, indicating no cancellation between the spin and orbital Hall effects in bulk semiconductors. Furthermore, it is found that the spin Hall effect can be strongly manipulated by strains [Fig. 3], and this result on strain effect would help the experimentalists to distinguish intrinsic from extrinsic aspect of the SHE. Finally, we also calculated the ac spin Hall conductivity [Eq. (3)] and found it to be large in both pure and hope-doped semiconductors [28].

2. AB INITIO CALCULATIONS: LINEAR RESPONSE, RELA- 3. INTRINSIC SPIN HALL EFTIVITY AND BERRY PHASE FECT IN ZINCBLENDE SEMIThe intrinsic Hall conductivity of a CONDUCTORS
solid can be evaluated by using the linear-response Kubo formalism [17]. In this approach, the intrinsic Hall effect comes from the static = 0 limit of the off-diagonal element of the conductivity tensor [17]
knjxknknvykn xy= e (fknfkn) E E + + i iVc k nn kn kn

(1) where Vc is the unit cell volume, and kn is the nth Bloch state with crystal momentum k. Setting to zero, one obtains the imaginary part of the off diagonal element xy = e (fkn fkn)Im[knjxkn Vc k nn knvykn](Enn ) (2)

where Enn= Ekn Ekn. As in previous magneto-optical calculations [18], one first calculates the imaginary part of the xy and then obtain the real part from the imaginary part by a Kramers-Kroing transformation
xy() 2 xy= P 0 d 2 2

(3)

where P denotes the principal value of the integral. Since all the intrinsic Hall effects are caused by relativistic spin-orbit coupling, ab initio calculations must be based on a 4

Spin generation and transport in nonmagnetic materials can be induced by an electric field because of relativistic spinorbit coupling (SOC) even in the absence of a magnetic field as demonstrated in a number of recent experiments [20, 21]. This offers the exciting possibility of pure electric driven spintronics in semiconductors, where SOC is relatively strong and which can be more readily integrated with conventional electronics [22]. Earlier theories on electric spin generation and transport were based on extrinsic effects due to SOC in scattering processes [23]. Recently, it was proposed that a transverse spin current response to an electric field, known as the intrinsic SHE, can also occur in pure crystalline materials due to intrinsic SOC in the band structure [1, 2]. A large number of theoretical papers were written addressing various issues about the intrinsic SHE. In particular, in [24], it was argued that spin symmetry consideration would rule out the possibility of such a spin current in the semiconductors described by the Luttinger Hamiltonian which was used in [1]. On the other hand, in [25], it was point out that the intrinsic spin Hall effect predicted in [2], in a two-dimensional electron gas in semicoductors, would be exactly cancelled by the intrinsic orbital angular momentum Hall (orbital) effect. Therefore, fundamental questions such as

4. SPIN HALL EFFECT IN NITRIDE SEMICONDUCTOR SUPERLATTICES

The experimental measurements on the SHE in semiconductors were mostly concentrated on the GaAs systems [26, 27]. Nitride semiconductors represent the most studied material system in semiconduc-

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Ab Initio Studies of Spin Hall Effect

oH sH Fig. 2: Calculated (a) spin (xy ) and (b) orbital (xy )

Hall conductivity as a function of hole concentration (nh) for Si, Ge, GaAs and AlAs [28].

Fig. 4: (upper) Calculated Rashba coupling e(eV) 3 and BIA coupling (eV ) vs in-plane strain. (lower) s Calculated spin Hall conductivity xy and measured circular polarization (CP) vs in-plane strain [30].

Fig. 3: Calculated spin Hall conductivity (xy ) (squares) and energy splitting (diamonds) of heavy-hole and light-hole bands at of GaAs vs. uniaxial strain at the hole concentration nh = 0.1 (e/cell) [28].

sH

By fitting the 2D Hamiltonian [Eq. (5)] to the calculated SOC splitting of the lowest conduction bands near k = 0, we obtained the theoretical e and , as shown in Fig. 4 as a function of the in-plane strain. The theoretical e values are in the same order of magnitude of the effective Rashba coupling measured on AlGaN/GaN [32]. Fig. 4 shows that the SOC e and depend strongly on the in-plane compressive strain. Within the linear-response Kubo formalism, we find the SHC for the 2D Hamiltonian of Eq. (5) as [30] 2m 2 z z xy = xy e [1 + 2 e ( 2 ) ]. (6) 8 3 If = 0, the SHC would be a universal constant as found before [2]. However, in the presence of impurity scattering, the k-linear coupling term would vanish [33]. Therefore, the observed SHE would be mainly due to the k-cubic term, i.e., e 2m 2 z xy 12 ( 2 ) e .This demonstrates that SHE in the wurtzite semiconductor superlattices and multilayers could be enhanced by manipulating the SOC parameters e and which in term can be tuned by the compressive in-plane strain via the piezoelectric field. Fig. 4 shows that the calculated SHC vs the in-plane strain is in good qualitative agreement with the measured circular polarizations [30].

tor community for the past decade. In particular, InGaN/GaN superlattices have become particularly attractive because of their wide applications in light-emitting diodes (LED) and high efficiency laser diodes (LDs) [29]. In Ref. [30], the first experimental observation of current-induced spin polarization in InGaN/GaN was reported. In addition, it was discovered that the SHE can be strongly manipulated by the internal strains [Fig. 4]. Because strains are commonly present in semiconductor multilayers and superlattices due to lattice mismatch, this finding provides a convenient way to control the magnitude of the SHE.

GaN/GaN superlattices, we performed a theoretical investigation of the spin Hall current in n-type two-dimensional (2D) wurtzite structure. Taking into account of the strong polarization field at the interface along the c-axis of wurtzite structure and the bulk inversion asymmetry (BIA), the 2D Hamiltonian can be written as [31]
2 H = k + (e + k )(xky ykx) (5) 2m 2 2

where e = + is the effective Rashba coupling. The coupling is induced by the built-in electric field due to the piezoelectric effect. The coupling and are due to the BIA effect. We performed ab initio relativTo gain a fundamental understand- istic band structure calculations for GaN ing of the strain-dependent SHE in In- under several compressive in-plane strains.

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Celebrating 20 Years of GMR Past, Present, and Future (I)

z 5. NATURE OF LARGE SPIN point is unoccupied, only n(k) for band X point [Fig. 7(a)]. We also showed, by HALL EFFECT IN PLATINUM 4 contributes to the SHE, resulting in modeling these near-degeneracies by an z the large positive peak in (k) near the effective Hamiltonian, that the SHC has METAL

In addition to semiconductors, the SHE in metallic systems is currently attracting interests, stimulated by latest experiments on the SHE or inverse spin Hall effect (ISHE), i.e., the transverse voltage drop due to the spin current [34-36]. The SHC in metals is much larger than that in the semiconductors. Naively, this may be due to the large number of carriers, but the band structure is very important [37]. Furthermore, the Fermi degeneracy temperature is much higher than room temperature, and hence the quantum coherence is more robust against the thermal agitations compared with the semiconductors systems. In recent experiments for metallic systems [34-36] platinum shows the prominent SHE surviving even up to room temperature, whereas aluminum and copper show relatively tiny SHE. However, the mechanism of the SHE in metals was assumed to be extrinsic. In [36], this difference was attributed to a magnitude of SOC for each metal. However, platinum seems to be special among heavy elements. This material dependence strongly suggests a crucial role of intrinsic contributions. Therefore it is highly desired to study the intrinsic SHE of platinum as a representative material for metallic SHE. If this analysis successfully explains the experiment, it will open up the possibility to theoretically design the SHE in metallic systems.

Fig. 5: Temperature-dependence of spin Hall conductivs ity xy in Pt and Au metals [37, 39].

Fig. 6: (a) Band structure and (b) spin Hall conductivity of fcc Pt [37].

Therefore, we recently carried out ab initio calculations for the SHC in platinum. [37] We found that the intrinsic SHC is as large -1 as ~2000 (/e)(cm) at low temperatures, -1 and decreases down to ~200 (/e)(cm) at room temperature [Fig. 5]. It is due to the resonant contribution from the spin-orbit splitting of the doubly degenerated d-bands at high-symmetry L and X points near the Fermi level [Fig. 6]. This perhaps can be best seen from the calculated band- and k-resolved Berry phase curvature zn(k) [Eq. (4)]. Fig. 7 indicates that zn(k) for the doublet bands 4 and 5 near X point are large but have opposite signs [Fig. 7(b)]. However, because band 5 near the X 6

Fig. 7: (a) Berry curvature n(k) and (b) band n-decomz posed Berry curvature n(k) along the symmetry lines z in the Brillouin zone. In (b), n(k) for the nth band has been shifted upwards by (n 1) 500 for clarity [37].

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Ab Initio Studies of Spin Hall Effect

a peak near the Fermi energy and that the vertex correction due to impurity scattering vanishes, indicating that the large SHE observed experimentally in platinum [36] is of intrinsic nature.

down spin DOS has the sharp peak at the Fermi level [Fig. 9]. Furthermore, when SOC is included in the LDA+U calculations, an unquenched orbital moment of

1.54 (B/Fe) is obtained, together with a spin moment of 3.19 (B/Fe). Fig. 9 indicates that the orbital-dependent Kondo effect occurs for Fe in Au, i.e., the eg -orbitals

6. ORIGIN OF GIGANTIC SPIN HALL EFFECT IN FEPT/AU SYSTEM

In bulk Au metal, in contrast, the d-band is completely filled, and the Fermi level falls in the broad 6s6p band where SOC is relatively small [Fig. 8]. As a result, the intrinsic SHC at zero temperature from the relativistic band structure calculation -1 for bulk Au metal is ~400 (/e)(cm) [38, 39]. Nevertheless, the SHC in Au increases steadily with temperature to -1 reach a value of 750 (/e)(cm) at room temperature [Fig. 6], being larger than that of Pt. Surprisingly, the spin Hall effect at room temperature recently observed in a multi-terminal device with a Au Hall cross and an FePt perpendicular spin injector 5 z is gigantic [3]. The measured xy 10 -1 (/e)(cm) is orders of magnitude larger than the intrinsic SHC in bulk Au reported above. This indicates that the SHC due to intrinsic SOC in the band structure of pure Au is not the dominant mechanism in the Au/FePt system. Indeed, the authors of Ref. [3] attributed the giant SHE to the extrinsic mechanism of the skew scattering by impurities in Au. Since in [3], the spin current is supplied from FePt to Au, it is conceivable to consider three kinds of imperfections, namely, (i) Au vacancies, (ii) Pt impurities, and (iii) Fe impurities. We therefore perform ab initio band structure calculations for these three cases, based on the LDA plus on-site Coulomb interaction U (LDA+U) (U = 5.0 eV and J = 0.9 eV) [40]. Fig. 9 shows the DOS in the presence of one impurity in the 2 2 2 supercell. The change in the DOS is confined in the range of 5d bands in the case of (i) vacancy, and (ii) at around -1.5 eV in the case of Pt. No magnetic state could be obtained in both cases. In contrast, the magnetic state is obtained in the case of Fe. Accordingly, the DOS for Fe shows the spin splitting, and

Fig. 8: (a) Band structure and (b) spin Hall conductivity of fcc Au [39].

Fig. 9: Total, site-, orbital- and spin-decomposed DOSs of (a) bulk fcc Au, 3.1% Au-vacancies, (b) 3.1% Pt-impurities, (c) 3.1% Fe-impurities in nonmagnetic state and (d-e) in ferromagnetic state [40].

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Celebrating 20 Years of GMR Past, Present, and Future (I)

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