Atsuo Shitade - Quantum Spin Hall Effect in Transition Metal Oxides

Master thesis
Quantum spin Hall eect in transition metal oxides

Supervisor: Professor Naoto Nagaosa
February, 2009
Department of Applied Physics School of Engineering University of Tokyo
76505 Atsuo Shitade
Contents
1 Introduction 2 Some backgrounds 2.1 QH eect . . . . . . . . . . . . . . . . . . . . . . . . . . 2.1.1 QH eect and the rst Chern number . . . . . . . 2.1.2 Charge polarization and the rst Chern number . 2.1.3 Haldane model . . . . . . . . . . . . . . . . . . . 2.2 SH eect . . . . . . . . . . . . . . . . . . . . . . . . . . . 2.2.1 Theories of the SH eect in doped semiconductors 2.2.2 Experiments in doped semiconductors . . . . . . . 2.2.3 Experiments in metals . . . . . . . . . . . . . . . 2.2.4 Theories in metals . . . . . . . . . . . . . . . . . 2.3 QSH eect . . . . . . . . . . . . . . . . . . . . . . . . . . 2.3.1 Kane-Mele model . . . . . . . . . . . . . . . . . . 2.3.2 TR polarization and the Z2 number . . . . . . . . 2.3.3 QSH eect and the TR polarization . . . . . . . . 2.3.4 Experimental realizations . . . . . . . . . . . . . 2.4 Relativistic Mott insulator Sr2 IrO4 . . . . . . . . . . . . 3 QSH eect in Na2 IrO3 3.1 Model construction . . . . . . . . . . . . . 3.1.1 Transfer integrals to the NN sites . 3.1.2 Transfer integrals to the NNN sites 3.2 Paramagnetic phase . . . . . . . . . . . . . 3.3 Edge AFM phase . . . . . . . . . . . . . . 3.3.1 Mean eld approximation . . . . . 3.3.2 Fractional charge . . . . . . . . . . 3.4 Experimental proposal . . . . . . . . . . . 3.5 Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3 5 5 5 6 7 8 9 10 12 13 15 15 15 19 22 24 29 29 30 31 35 36 37 39 40 42
4 First principles approach to topological insulators 43 4.1 Na2 IrO3 with the honeycomb lattice . . . . . . . . . . . . . . . . . . . . . . . . . . . 43 4.1.1 Calculations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 43 1
CONTENTS 4.1.2 Discrepancy between calculations and 4.1.3 Extension of the tight binding model Lu2 Ir2 O7 with the pyrochlore lattice . . . . . 4.2.1 Calculations . . . . . . . . . . . . . . experiments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
2 44 46 49 49 53
4.2
5 Summary and future problems
Chapter 1 Introduction
The non-trivial topology of wave functions has attracted intensive interests in condensed matter physics. The Hall conductivity in two-dimensional electron systems was reported to be quantized as long as the Fermi energy lies in localized states [1]. This quantum Hall (QH) eect is experimentally surprising because disorder, the electron correlation, the nite size eect, and three-dimensionality etc. are expected to give some corrections to the Hall conductivity. Thouless, Kohmoto, Nightingale, and den Nijs (TKNN) found that the QH eect can be described by the rst Chern number associated with the Berry curvature [2, 3, 4, 5]. Haldane studied a model on the honeycomb lattice showing the QH eect without Landau levels [6]. In this model, total ux is equal to zero and only breaking of time-reversal (TR) symmetry is essential. Topological numbers give a chance to characterize quantum liquids without the Ginzburg-Landau scheme of symmetry breaking. A recent breakthrough is theoretical predictions and experiments on the quantum spin Hall (QSH) eect in TR invariant systems [7, 8, 9, 10, 11, 12, 13, 14, 15, 16]. Intuitively it can be regarded as two copies of QH systems with up and down spins, but is driven by the relativistic spin-orbit coupling (SOC). Opposite spins have opposite signs of the Hall conductivity and the spin Hall (SH) conductivity is quantized. The Kane-Mele model on the honeycomb lattice [7, 8] is the case. However, the SH conductivity is not quantized generally because spin is not conserved [10]. Then what characterizes a QSH insulator? It is known to be robust against spin nonconserving interactions such as the Rashba coupling, disorder, and the weak electron correlation [7, 8, 17, 18, 19]. In fact, the Z2 number distinguishes a QSH insulator from an ordinary band insulator [7, 20, 21, 22, 23, 13]. It is closely related to Kramers doublets protected by TR symmetry and corresponds to the number of gapless helical edge modes. A HgTe/CdTe quantum well was predicted to show the QSH eect [11] and later experimentally observed [12]. A three-dimensional Bi1x Sbx alloy was found to have the odd number of pairs of helical edge modes by using angleresolved photoemission (ARPES) [15], and now the existence of this novel state of matter has been rmly established. So far, however, QSH insulators are limited only in semiconductors and at low temperature. This is bacause the large SOC and ne tuning of band structures are needed. Therefore one important development is search for more robust QSH insulators at higher temperature with a wider gap. Another development is to study interplay between the non-trivial topology and the electron 3
CHAPTER 1. INTRODUCTION
correlation. Needless to say, the electron correlation and related interplay between spin, orbital, and charge degrees of freedom bring a variety of unusual properties such as high temperature superconductivity (HTSC) in cuprates, the colossal magnetoresistance (CMR) eect in manganites, and so on [24, 25, 26]. Its research targets have been mainly 3d transition metal oxides in which the SOC is negligible or at most perturbative. One example is the single-band (x2 y 2 ) Hubbard model based on cuprates, in which an orbital angular momentum is quenched. Another example is the Dzyaloshinsky-Moriya (DM) antisymmetric interaction in spin systems without inversion symmetry [27, 28]. It can be derived from the second order perturbation of the SOC plus the exchange coupling and can bring the weak FM or the helical magnetism. On the other hand, when we focus on 5d elements going down from 3d elements in the periodic table, the electron correlation becomes smaller because orbitals get more extended, while the SOC becomes larger with increasing atomic number. Both the electron correlation and the SOC play important roles with the same order of magnitudes. A layered perovskite oxide Sr2 IrO4 provides a suggestive example, which is a Mott insulator [29, 30, 31] in sharp contrast to the fact that its 4d version Sr2 RhO4 can be described as a Fermi liquid [32, 33]. Recently Kim et al. found that a narrow band with an eective total angular momentum je = 1/2 is formed and even the relatively weak electron correlation leads to a Mott insulator [34]. Thus 5d elements provide realistic stages to fuse the two separate mainstreams in condensed matter physics, i.e. spintronics in semiconductors and the electron correlation in 3d elements. The nal goal of this thesis is the very term fusion through the study of 5d transition metal oxides from the topological point of view. Although the umklapp scattering term in the strong electron correlation opens up a gap in a helical liquid associated with spontaneous breaking of TR symmetry [18, 19], it is an open problem what about non-magnetic insulators in geometrically frustrated lattices. The Kondo problem in a helical liquid is rather dierent from that in a spinful Tomonaga-Luttinger (TL) liquid [18, 35]. Interplay between the non-trivial topology and the electron correlation in topological transition metal oxides contains such challenging problems. And precisely, the rst problem is whether topological insulators can be realized in transition metal oxides or not. Organization of this thesis is following. In Chapter 2, some backgrounds are explained. The basic notions of topological insulators, both with and without TR symmetry, are reviewed. Since the QSH eect may not be familiar, (not quantum) SH eect is also introduced. At the last Section, the electronic structure of Sr2 IrO4 is discussed, which provided the above big motivation of this thesis. Chapter 3 is devoted to the QSH eect and the related magnetic transition in Na2 IrO3 . The eective model is found to be a QSH insulator and a guiding principle to design QSH transition metal oxides is derived. A new mechanism of the magnetic transition is proposed based on its topological nature. This work is summarized in a paper [36]. In Chapter 4, rst principles band calculations are performed to examine the validity of the eective model on Na2 IrO3 and to search for topological transition metal oxides.
Chapter 2 Some backgrounds

In this Chapter, some basic notions of topological insulators are summarized. The QH eect is a phenomenon in TR breaking topological insulators in two dimensions, which is characterized by the rst Chern number as TKNN pointed out [2, 3, 4, 5]. Before explanations of the main subject of this thesis, the QSH eect, the SH eect is briey introduced. The QSH eect is a phenomenon in TR invariant topological insulators in two and three dimensions, which is characterized by the Z2 number [7, 21, 22, 23]. The physical meanings of these topological numbers are also explained. Finally, we focus on an Ir oxide Sr2 IrO4 , in which the SOC and the electron correlation drastically change its electronic structure.
2.1
QH eect
In a strong magnetic eld and at low temperature, the Hall conductivity H is quantized and there exist gapless edge modes, which is called the QH eect. Although plateaus of H as a function of a magnetic eld are due to localization, we can see the Kubo formula of the Hall conducitvity is associated with the Berry phase of wave functions, leading to the rst Chern number at T = 0 [2, 3, 4, 5]. The charge polarization in one-dimensional insulators provides the physical meaning of the rst Chern number [37, 38]. Haldane invented the model showing the QH eect without Landau levels [6].
2.1.1
QH eect and the rst Chern number
For simplicity, consider the non-interacting Hamiltonian. According to the Kubo formula, the Hall conductivity is given by H = 1 iL2 f ( n (k)) f (
n=m k m (k))
( n (k) f ( n (k))
2 m (k))
n; k|Jx (k)|m; k m; k|Jy (k)|n; k (2.1) ,
1 = 2 iL
n; k|Jx (k)|m; k m; k|Jy (k)|n; k (x y)

m=n
( n (k) 5
2 m (k))
CHAPTER 2. SOME BACKGROUNDS
where |n; k is a Bloch wave function with the eigenvalue n (k), and f ( ) is the Fermi distribution. The matrix elements of J(k) = k H(k) can be rewritten as m; k|J(k)|n; k = ( n (k) for m = n, and then (2.1) is transformed into H = 1 L2 f ( n (k))i
n k m (k)
m; k|
k |n; k
(2.2)
n; k| |n; k (x y) kx ky (2.3)
k
1 = 2 L where An (k) n; k|i leading to
f ( n (k))[
n k
An (k)]z ,
k |n; k
is the Berry connection. At T = 0, n runs over occupied bands,

occ
1 H = 2
d2 k [ 2
1 k An (k)]z 2
occ
Cn .
n
(2.4)
Cn is called the rst Chern number and proved to be an integer as follows. First, we can see that the rst Chern number is invariant under U(1) gauge transformation |n; k ein (k) |n; k , which leads to An (k) An (k) k n (k). This is based on a conjecture that phases of wave functions n (k) can be taken smoothly in the entire Brillouin zone, which is not correct generally. For example, we try to x a gauge so that a|n; k is real. However, the Brillouin zone may contain such k0 as a|n; k0 = 0, where this gauge can not be adopted. Then we adopt another gauge so that b|n; k is real in the nite region D containing k0 . Thus a phase mismatch |n; k D = ein (k) |n; k D occurs at D, leading to the non-zero rst Chern number Cn =
D
d2 k [ 2
D
D k An (k)]z +
d2 k [ 2 1 = 2
AD (k)]z n (2.5) dn (k).

D
1 = 2
dk
[AD (k) n
AD (k)] n
In this way, the rst Chern number reects the non-trivial phase structure of wave functions.
2.1.2
Charge polarization and the rst Chern number
The rst Chern number characterizes change of the charge polarization for a periodic cycle in one dimension. In fact, a QH insulator on a cylinder can be regarded as a one-dimensional insulator. Here we begin with the charge polarization in terms of the Berry connection. Consider a one-dimensional insulator under periodic boundary conditions. The eigenstates can be written as Bloch wave functions y|n (k) = eiky y|n; k . We can dene Wannier wave functions localized at the site Y as dk ik(yY ) e y|n; k . (2.6) y|n; Y = 2
The charge polarization is the shift of the center of Wannier wave functions and can be written as
occ
P =
n
n; Y |(y Y )|n; Y =
dk A(k), 2
(2.7)
where again A(k) is the U(1) Berry connection (but summed over occupied bands here). Note that the charge polarization is well-dened only mod 1. In fact, by performing gauge transformation |1k ei1 (k) |1k , P is transformed into P [1 () 1 ()]/2. This additional term must be an integer due to periodicity of the Brillouin zone. However, change of P induced by adiabatic change of the Hamiltonian H(t) is well-dened. The eigenstates |n; t, k and the Berry connection can be dened at each time t. Then change of P is given by
P (t2 ) P (t1 ) =

dk [Ak (t2 , k) Ak (t1 , k)] 2 dk [Ak (t2 , k) Ak (t1 , k)] + 2 dk t2 dt[ (t,k) A(t, k)]z . 2 t1
t2
dt[At (t, ) At (t, )]

t1
(2.8)
In the second line, the vanishing term At (t, ) At (t, ) = 0 is added and the line integral is performed around a loop in the (t, k)-space, which makes the Stokes theorem applicable in the third line. For a periodic cycle H(t + T ) = H(t), P (T /2) P (T /2) is given by the integral in (2.8) over the entire torus. This is the rst Chern number itself. Thus the rst Chern number chracterizes change of the charge polarization in a periodic cycle. Next we relate two-dimensional QH insulators to one-dimensional insulators. Consider a twodimensional insulator on a cylinder threaded by ux in Figure 2.1 (a). Flux corresponds a vector potential Ax = /L, leading to an electric eld Ex = Ax . From a general argument on electrons in a magnetic eld, a momentum kx is substituted by kx Ax = kx + 2/Lx /0 , where 0 = 2 is a ux quanta. Thus a two-dimensional insulator can be regarded as a parametrized onedimensional insulator, and kx can be identied with . End states of the cylinder as a function of reects edge modes as a function of kx . The rst Chern number, which is dened as the number of charge moving from one end to another for a cycle, guarantees the presence of gapless chiral edge modes as shown in Figure 2.1 (b).
2.1.3
Haldane model
At the end of this Section, the Haldane model on the honeycomb lattice [6] is introduced. This model shows that the QH eect results from breaking of TR symmetry, and in principle even without net ux. It is also important as a forerunner of the Kane-Mele model showing the QSH eect [7, 8]. The Haldane model is a spinless fermion model including (1) transfer integrals to the nearestneighboring (NN) sites t1 , (2) transfer integrals to the next-nearest-neighboring (NNN) sites t2 ei
(a)
(b)
Figure 2.1: (a) A cylinder threaded by ux . (b) Schematic edge modes as a function of kx for C = 1. A shaded area shows bulk states, and red solid and dashed lines indicate evolution of localized states at y = 0 and L. A black dashed line is the Fermi energy.
(a)
(b )
Figure 2.2: (a) The Haldane model dened on the honeycomb lattice. A green arrow indicates transfer integrals t2 ei . (b) Phase diagram of the rst Chern number in the (, M/t2 )-space. The phase boundaries follow |M/t2 | = 3 3| sin | [6]. which break TR symmetry, and (3) staggered on-site potentials M on 1/2 sublattices which break inversion symmetry. It is explicitly written as
NN NNN
H = t1
ij
c cj + t2 i
ij
eiij c cj + M i
i
i c ci . i
(2.9)
Here ij 2/ 3[d1 d2 ]z = 1, where d1 and d2 are unit vectors along the two bonds connecting the site i and j. i = 1 gives staggered on-site potentials M . |t2 /t1 | < 1/3 is assumed to guarantee that the lower band is fully occupied. As seen in Figure 2.2 (b), the TR breaking phase = 0, makes this model non-trivial without a uniform magnetic eld.
2.2
SH eect
In doped semiconductors and metals, transverse charge currents with up and down spins ow in the opposite direction due to the SOC, leading to a pure spin current. This eect is called the SH eect, which has been the active eld in spintronics. It was rst proposed by Dyakonov and Perel, which originates from the extrinsic skew scattering [39]. On the other hand, the intrinsic
SH eect was theoretically predicted in p-type semiconductors [40] and two-dimensional n-type semiconductors [41]. In fact, both the intrinsic and extrinsic contributions are important. Inoue et al. showed that for the Rashba Hamiltonian the vertex correction exactly cancels the bare SH conductivity in the clean limit [42]. Experimentally, Kato et al. observed the SH eect in n-type semiconductors [43], and Wunderlich et al. observed in p-type semiconductors [44]. In this Section, these theoretical and experimental studies are briey introduced. The SH eect in metals, which is more promising candidates for application to spintronics, is also explained.
2.2.1
Theories of the SH eect in doped semiconductors
In p-type semiconductors, six-fold degeneracy of p-orbitals is partially lifted by the SOC, leading to four-fold degenerate states with a total angular momentum j = 3/2 and two-fold degenerate states with j = 1/2. The latter is well-separated from the former and can be neglected. Thus the valence band can be described by j = 3/2-states, which are split into two doubly degenerate bands called the heavy-hole (HH) and light-hole (LH) bands. The k p theory results in the eective Hamiltonian near the -point, H(k) = 1 (1 + 52 /2)k 2 22 2m
2 ka j a2 23 a a=b
ka kb (j a j b + j b j a ) ,
(2.10)
where the sign of energy is inverted. 1 , 2 , and 3 are the Luttinger parameters, which are often approximated as 2 = 3 . Within this approximation, the Hamiltonian is written as H(k) = 1 (1 + 52 /2)k 2 22 (k j)2 . 2m 1 HH LH (3kF kF ), 12 2 (2.11)
Murakami et al. calculated the SH conductivity based on the semi-classical equation of motion, SH = (2.12)
HH LH where kF and kF are the Fermi wave numbers for the HH and LH, respectively [40]. In n-type semiconductors, the SOC is small because the conduction band mainly consists of an s-orbital. However, in two-dimensional electron gas (2DEG) in heterostructures, structural inversion-asymmetry (SIA) induces the Rashba SOC, which reads
H(k) =
k2 + (x ky y kx ). 2m
(2.13)
The coupling constant can be tuned by the gate voltage. Sinova et al. obtained the universal SH conductivity 1 (2.14) SH = 8 from the Kubo formula [41]. The above results are assumed the absence of impurities. There are three impurity eects; (1) the self-energy correction (Figure 2.3 (b)), (2) the side-jump (Figure 2.3 (c)), and (3) the skew
10
(a)
(b)
(c) + c. c. + c. c.
(d)
Figure 2.3: Diagrammatic expressions for (a) the bare SH conductivity, (b) the self-energy corrections, (c) the side-jump terms, (d) the skew scattering terms. The lower panels of (c) and (d) show schematic pictures of the scattering processes. Red and blue arrows indicate motion of up and down spins. scatering (Figure 2.3 (d)). The self-energy correction (1) can be included by the nite 1 and is regarded as correction of the intrinsic SH eect. The side-jump (2) and the skew scattering (3) give the extrinsic SH eect. Inoue et al. evaluated the side-jump eect for the Rashba Hamiltonian (2.13) within the ladder approximation, which exactly cancels the intrinsic term (2.14) in the clean limit [42]. They assumed isotropic short-range potentials, and in addition, many groups found that the SH conductivity vanishes for long-range potentials. On the other hand, for the Luttinger model (2.11) the side-jump eect vanishes within the ladder approximation [45].
2.2.2
Experiments in doped semiconductors
After these theoretical predictions, two seminal experiments were performed. Both observed the spin accumulation at the edges; one is in n-type semiconductors by the Kerr rotation [43], and the other in p-type semiconductors by a light-emitting diode (LED) [44]. Kato et al. prepared thin lms of n-GaAs and n-In0.07 Ga0.93 As with n = 3 1016 cm3 [43]. When an electric eld is applied in the x-direction, an spin current polarized in the z-direction ows in the y-deirection. As a result, spins polarized in the z-direction are accumulated at the edges of the samples. Such distribution of spins can be detected by the Kerr rotation. In this method, a linearly polarized beam is incident normal to the sample. The polarization of the reected beam is rotated by an angle proportional to the z-component of spins. Moreover, when a transverse magnetic eld is applied, spins precess around it. Thus the rotation angle decrease monotonically as A0 /[(L s )2 + 1], where L is the Larmor frequency and s is the spin lifetime. This is known as the Hanle eect. Figure 2.4 shows the experimental data on n-GaAs [43], which strongly supports the SH eect. They also roughly estimated the SH conductivity as SH = 5 103 1 cm1 for n-In0.07 Ga0.93 As [43]. Distribution of spins can be detected by a circularly polarized light. Wunderlich et al. fabricated
11
Figure 2.4: The SH eect in GaAs at T = 30K. (A) Schematic picture of the experimental setup. (B) Kerr rotation as a function of an applied magnetic eld B for x = 35m (red) and x = +35m (blue) for E = 10mVm1 . (C) Kerr rotation as a function of x and B for E = 10mVm1 . (D, E, F) Spatial dependence of the peak Kerr rotation A0 , the spin lifetime s , and reectivity R, respectively. (G) Kerr rotation as a function of E and B at x = 35m. (H, I) E dependence of A0 and s , respectively [43].

(a) (c )
12
(d ) (b )
Figure 2.5: (a) Schematic cross section of the LED. (b) Scanning electron microscope (SEM) image of the LED. (c) Circular polarization along the z-axis for LED 1 for two opposite IP . (d) Circular polarization along the z-axis for xed IP for LED 1 and 2 [44]. LEDs in (Al,Ga)As/GaAs heterostructures in Figure 2.5 (a) and (b) [44]. In usual LEDs, when a forward bias is applied, electrons in the conduction band and holes in the valence band are recombined accompanied with light emission. Now that spins of holes are polarized due to the SH eect, the emitted light is circularly polarized to conserve an angular momentum. Namely, inversion of circular polarization of light in Figure 2.5 (c) and (d) directly shows inversion of spin polarization, which supports the SH eect in p-type semiconductors.
2.2.3
Experiments in metals
The spin Hall eect in metals is more promising than that in semiconductors because (1) the SH conductivity is much larger because of the larger number of carriers, (2) a contact with metallic ferromagnets does not suer from impedance mismatch, and (3) they are more robust against disorder and thermal excitations due to the larger Fermi energy. Recently, 4d and 5d metals with the larger SOC have been focused on [46, 47]. On the other hand, the optical detections used in semiconductors can not be applied to metals because the spin diusion length is much shorter. Therefore in metals, the inverse SH eect, in which a spin current induces a charge current, is widely used. Here we see one of the methods to inject a spin current, the non-local spin injection from metallic ferromagnets [48]. Valenzuela et al. prepared a CoFe/Al device as shown in Figure 2.6 (a), in which a ferromagnetic electrode (FM1) was used to inject a spin-polarized current, and Al was oxidized to make a tunneling barrier [48]. A current I ows from FM1 into the left side of the Al lm in Figure 2.6 (b), and a spin current is injected due to spin diusion. Therefore we can observe the inverse
13
(a)
(d)
(b)
(c)
Figure 2.6: (a) Atomic force microscope (AFM) image of the device. (b) SH measurement. A current I ows from FM1 into the left side of the Al lm, and a SH voltage VSH is measured between the two Hall probes at a distance LSH from FM1. (c) Spin transistor. I ows from FM1 into the right side of the Al lm, and a voltage V is measured between FM2, which is located at a distance LFM from FM1, and the left side of the Al lm [48]. SH eect without suering from the anisotropic magnetoresistance, the ordinary and anomalous Hall eects in FM1. FM1 and another ferromagnetic electrode (FM2) construct a spin transistor in Figure 2.6 (c), which was used to determine the spin polarization P , the spin diusion length sf , and the angle of the magnetization M . With the conguration in Figure 2.6 (b), the SH resistance at LSH is written as RSH RSH = sin (2.15) 2 with P SH LSH /sf RSH = e , (2.16) tAl 2 where tAl is the thickness of the Al lm. Exponential decay in (2.16) was clearly seen in Figure 2.6 (d), and they estimated SH = (3.4 0.6) 101 1 cm1 for tAl = 12nm and SH = (2.7 0.6) 101 1 cm1 for tAl = 25nm, leading to the SH angle of SH SH / = (1 3) 104 at helium temperature. Recently, Kimura et al. observed the SH eect in Pt with the SH conductivity of SH = 2.4 102 1 cm1 and the SH angle of SH = 3.7 103 at room temperature [46]. More recently, the SH angle of SH = 0.113 was reported in a FePt/Au device [47].
2.2.4
Theories in metals
As well as in semiconductors, both the intrinsic and the extrinsic contributions are important in metals. Guo et al. performed relativistic rst principles band calculations for Pt and calculated the intrinsic SH conductivity based on the Kubo formula (Figure 2.7 (a)) [49]. They obtained SH = 22001 cm1 at T = 0 and 2401 cm1 at T = 300K, which is very close to the experimental value [46]. This giant SH conductivity originates from the enhanced Berry curvature z (k) at X-
14
(a)
(b)
(c)
Figure 2.7: (a) Relativistic band structures (left) and the SH conductivity (right) for Pt. Red dashed and blue solid curves indicate scalar relativistic and full relativistic calculations. (b) Berry curvature z (k). (c) n-decomposed Berry curvature n (k). The inset shows the temperature z dependence of the SH conductivity [49]. and L-points due to the SOC-induced anti-crossings as shown in Figure 2.7 (b) and (c). In Pt, the intrinsic contribution is dominant. On the other hand, 4d and 5d metals including Pt were investigated based on the nine-orbital (s, p, and d) tight binding model [50, 51]. Kontani et al. found that the vertex correction due to local impurities is less than 5% within the Born approximation [50]. This is because a p-level, which gives the non-vanishing vertex correction, is 20eV higher than the Fermi energy. Tight binding models are convenient to capture an intuitive origin; the eective Aharonov-Bohm phase due to the SOC involving s- and d-orbitals. Recently, motivated by the giant SH eect in a FePt/Au device [47], the role of the electron correlation was pointed out [52]. Since the Fermi surface of Au is mainly composed of an s-orbital, the intrinsic contribution is expected to be small. They considered three possibilities; (1) Au vacancies, (2) Pt impurities, and (3) Fe impurities. The cases (1) and (2) do not change the electronic structure near the Fermi energy, while LDA+U in the case (3) does change. t2g -orbitals show the resonant peak at the Fermi energy and play the major role in the SH eect. On the other hand, eg -orbitals are 2eV higher than the Fermi energy, leading to the Kondo eect at low temperature. It should be emphasized that the energy splitting between eg - and t2g -orbitals results not from a crystalline eld but from the electron correlation. The SH angle due to the skew scattering is expressed as SH = dI()S() sin 3 (e2i1 1)(e2i2 e2i2 ) = , + 5 dI()(1 cos ) 3 sin2 2 + 2 sin2 2
+
(2.17)
where 2 = j=21/2 is the d-wave phase shift, and 1 is the p-wave one. This quantity was found
15
to be the order of 0.1 when the resonant peak is well-split due to the SOC as shown in the inset of Figure 2.8 (c). In this sense, it can be referred to as the resonant skew scattering.
2.3
QSH eect
The QSH eect was rst theoretically proposed by Kane and Mele in graphene [7, 8]. Intuitively it can be regarded as two copies of QH insulators, but the SH conductivity is not generally quantized because spin is not conserved. On the other hand, a topological number called the Z2 number and helical edge modes persist even in the presence of disorder and the weak electron correlation [18, 19]. In this Section, the TR polarization is dened, which provides the physical meaning of the Z2 number, and then we relate the Z2 number to the QSH eect [20, 13]. This procedure is completely analogous to the charge polarization and the QH eect. Generalization to three dimensions is easy, in which a set of four Z2 numbers distinguishes a strong topological insulator (STI) from a weak topological insulator (WTI) [21, 22, 23]. Experimental realizations are also reviewed.
2.3.1
Kane-Mele model
To begin with, the Kane-Mele model on the honeycomb lattice [7, 8] is explained. This model is just a generalization of the Haldane model showing the QH eect [6] and is explicitly written as
NN NNN NN
H=t
ij
c cj + iSO i
ij
ij c sz cj + iR i
ij
c (s dij )z cj + v i
i
i c ci . i
(2.18)
The second term is the SOC which involves the spin-dependent and complex transfer integrals to the NNN sites, corresponding to = /2 in the Haldane model. The third term is the Rashba interaction, which breaks mirror symmetry and spin conservation. Note that all these terms do not break TR symmetry, which plays a key role in the QSH eect. If R = 0, spin is conserved and the spin Chern number can be dened as the dierence of the rst Chern number between up and down spins, i.e. Cs C C , which leads to the quantized SH conductivity. Also, edge modes crossing at k = 0 or are spin-ltered in the sense that electrons with opposite spin propagate in opposite directions. This is the very intuitive but special case. As shown in Figure 2.9 (a), the region is nite where a pair of gapless helical edge modes exists, which is characterization of the QSH eect. In this region, the charge conductance is predicted to be quantized as G = 2e2 /h for the two-terminal geometry in Figure 2.9 (b). Another characterization by the Z2 number and robustness of helical edge modes against disorder are discussed later.
2.3.2
TR polarization and the Z2 number
In this Subsection, the TR polarization for one-dimensional TR invariant insulators is introduced, and the Z2 number is dened as its change for half a cycle [20]. And then in the next Subsection,
16
Figure 2.8: Partial DOSs for Au with (a) 3.1% Au vacancies, (b) 3.1% Pt impurities, (c) 3.1% Fe impurities in non-magnetic state, and (d) in ferromagnetic state [52].
17
(a)
(b)
Figure 2.9: (a) The band dispersions for the zigzag edge geometry in (left) the QSH phase with v /t = 0.1 and (right) the insulating phase with v /t = 0.4. In both cases SO /t = 0.06 and R /t = 0.05. The inset shows the phase diagram in the (v , R )-space [7]. (b) Schematic picture of the two-terminal measurement. The charge conductance is quantized as G = 2e2 /h. Right picures indicate the population of edge modes [8]. relation between the Z2 number in one dimension and the QSH eect in two dimensions is explained in the same manner of the rst Chern number and the QH eect. In the TR invariant cases, the Kramers theorem guarantees that every Bloch wave function with k is degenerate with its TR partner with k. Therefore 2N eigenstates can be divide into N pairs which satisfy T |n; k =ein (k) |n+; k T |n+; k = ein (k) |n; k (2.19)
where n = 1, , N , and T is the TR operator. Now we can consider the dierence of shift of charge between a Kramers pair. Intuitively it corresponds to shift of spin, but this is not valid in the presence of the SOC. To achieve this purpose, let the pseudospin Berry connection be introduced. TR symmetry (2.19) constrains relation between the pseudospin Berry connections as
N N
A (k) =
n=1 N
n+; k|(ik )|n+; k =

n=1
T n; k|ein (k) (ik )ein (k) |T n; k

N
(2.20) k n (k).
=
n=1
[ n; k|ik |n; k k n (k)] = A (k)

n=1
CHAPTER 2. SOME BACKGROUNDS Then the TR polarization can be dened as
18
P =

dk + A (k) A (k) = 2 dk 2
N
dk + A (k) + A+ (k) A (k) A (k) 2 (2.21)
=
0
k [n (k) n (k)] .
n=1
This can be rewritten in a generic form by introducing a U(2N ) matrix, which is related to TR symmetry, N 0 ein (k) wmn (k) m; k|T |n; k = . (2.22) ein (k) 0
n=1
We can easily see two useful formulas;

N
log det w(k) =i

n=1 N
[n (k) + n (k)] (2.23) n (k ),

n=1
log Pf w(k ) =i
where k = 0 and are TR invariant momenta, where w(k ) is an antisymmetric matrix characterized by Pfaan. Using (2.23), (2.21) is rewritten as
iP =
0
1 1 det w() dk k log det w(k) ik n (k) = log i [n () n (0)] 2 2 det w(0) n=1 n=1
1 det w() Pf w() = log log . 2 det w(0) Pf w(0) Finally, applying the well-known formula det w = (Pf w)2 , we obtain (1)P = det w(0) det w() . Pf w(0) Pf w()
(2.24)
(2.25)
The blanches of det w(k) are chosen to evolve continuously along the path of the integral in (2.24). The TR polarization P distinguishes two phases, i.e. the presence or absence of a Kramers degenerate state at the end of nite systems, though it is meaningless by itself like the charge polarization P . Then again an adiabatic cycle of the Hamiltonian is considered. The Hamiltonian is TR invariant at t = 0 and T /2, at which Wannier wave functions come in pairs. However, in going from t = 0 to t = T /2, Wannier wave functions may switch partners as shown in Figure 2.10 (a), leading to the appearance of an unoccupied state at each end. Thus there must be two-fold
19
(a)
(b)
Figure 2.10: Red and blue lines represent schematic evolution of the centers of a Kramers doublet as a function of t. (a) The non-trivial case with P (T /2) P (0) = 1. Wannier wave functions switch partners, resulting in an unoccupied state at each end. (b) The trivial case with P (T /2) P (0) = 0. degeneracy at each end and four-fold degeneracy in total. On the other hand, there is no degeneracy in the trivial case shown in Figure 2.10 (b). In the result, change of the TR polarization
4
(1) =
i=1
det w(i ) Pf w(i )
(2.26)
denes a Z2 topological invariant which characterizes the presence or absence of a Kramers degenerate state at each end. Here i are four TR invariant points given by (t, k) = (0, 0), (0, ), (T /2, 0) and (T /2, ). To apply (2.26), wave functions must be dened continuously on the entire torus, which is guaranteed by the vanishing rst Chern number due to TR symmetry.
2.3.3
QSH eect and the TR polarization
To relate two-dimensional QSH insulators to the TR polarization, again we consider a cylinder threaded by ux . The Z2 number, change of the TR polarization between two TR invariant time points in terms of one dimension, characterizes in two dimensions how Kramers degenerate states at TR invariant momenta kx = 0 and are connected to each other. Kramers pairs may switch partners associated with the presence of helical edge modes as shown in Figure 2.11 (b), while may not as in Figure 2.11 (c). The former case corresponds to a QSH insulator and the latter to an ordinary band insulator. The Z2 number characterizing two-dimensional insulators is given by
4
(1) =
i=1
i (2.27)
det w(i ) Pf w(i ) wmn (k) = m; k|T |n; k , i =
where i are four TR invariant momenta. The topological number characterizing QSH insulators, the Z2 number, gives only whether the number of pairs of helical edge modes n is even or odd. This reects the fact that two pairs
20
(a)
(b)
(c)
Figure 2.11: (a) A cylinder threaded by ux . (b, c) Schematic edge modes as a function of momentum kx . A shaded area shows bulk states, and red and blue lines indicate evolution of a Kramers doublet. A black dashed line shows the Fermi energy. (b) The non-trivial case with (1) = 1. Since no degeneracy at kx = 0 is assumed, Kramers degeneracy occurs at kx = . (c) The trivial case with (1) = 1. of gapless helical edge modes are generally coupled to open up a gap. To see this, consider the low-energy eective Hamiltonian describing one edge. For n = 1, the non-interacting part can be written as H0 (k) = vF k(R+ R+ L L ), (2.28) where R+ and L are right- or left-propagating edge modes with up or down pseudospins connected by the TR operator. In this case, the single-particle backward scattering term
Hbw (k) = R+ L + h.c.
(2.29)
is forbidden due to TR symmetry. On the other hand, for n = 2, the non-interacting part is given by H0 (k) = vF k(1R+ 1R+ 1L 1L + 2R+ 2R+ 2L 2L ), (2.30) while a possible mass term is
Hbw (k) = (1R+ 2L 1L 2R+ ) + h.c..
(2.31)
Thus even though there exist more than one pair of helical edge modes, every two pairs annihilates and only the last one pair is guaranteed to be gapless by Kramers theorem. In three dimensions, there exist eight TR invariant momenta n1 n2 n3 = (n1 b1 + n2 b2 + n3 b3 )/2 with primitive reciprocal lattice vectors bj and nj = 0, 1. A set of four Z2 numbers (0 ; 1 2 3 ) is dened as (1)0 =
nj nk =1 k
n1 n2 n3 (2.32) n1 n2 n3 .
nj=k
(1)
0 is independent of choice of bj , while k are not. In this sense, 0 is special, and distinguishes STIs from WTIs as seen later. Figure 2.12 shows dierent phases.
21
(0;001) (a) + + + (b) + + + +
(0;011) + + + + + +
(1;111) + + + + + (c) +
Figure 2.12: Dierent phases characterized by (0 ; 1 2 3 ). (a) n1 n2 n3 at eight TR invariant momenta n1 n2 n3 . (b) Schematic contour plot of surface modes as a function of kx and ky . Black and white circles indicate the odd and even TR polarization n1 n2 = n1 n2 0 n1 n2 1 , respectively. Shaded areas represent above the energy shown in (c). (c) Gapless surface modes in the (1; 111) phase. To understand the physical meaning of (2.32), again imagine a generalized cylinder which is open along the z-axis and is periodic along the x- and y-axes. It can be threaded by two independent uxes corresponding kx and ky . At each surface TR invariant momenta in the surface Brillouin zone, the TR polarization is dened as n1 n2 = n1 n2 0 n1 n2 1 . If the TR polarization changes its sign along the path from one surface TR invariant momenta to the other, across the solid curve in terms of Figure 2.12 (b), there exist gapless surface modes. For 0 = 1, one TR polarization diers in sign from the other three as shown in the right panel of Figure 2.12 (b). This means the presence of only one pair of gapless surface modes protected by TR symmetry. Thus the 0 = 1 phases are robust against disorder and the weak electron correlation, which are referred to as STIs. On the other hand, for 0 = 0, two cases are possible. One is that no gapless surface modes exist as shown in the left panel of Figure 2.12 (b). This is an ordinary band insulator. Another is that there exist two pairs of gapless surface modes in the middle panel of Figure 2.12 (b). This can be interpreted as a layered QSH insulator. If the number of layers is odd, it is equivalent to a two-dimensional QSH insulator. However, if the number of layers is even, a weak periodic potential and disorder can easily open up a gap, leading to an ordinary band insulator, as discussed in two dimensions. Therefore the 0 = 0 phases are referred to as WTIs.

(a) (c )
22
(b )
Figure 2.13: (a) The band structures near point for HgTe and CdTe. (b) Schematic picture of a quantum well and lowest subbands for dierent thicknesses. (c) The electronic structure of a quantum well as a function of the thickness of HgTe [9].
2.3.4
Experimental realizations
Up to now, a few specic materials have been conrmed as topological insulators. Various probes can detect helical edge modes, among which ARPES is the most direct. Here we see them in historical order, namely a HgTe quantum well [12], a Bi1x Sbx alloy [15], and Bi2 Se3 and Bi2 Te3 [53, 54, 55]. A HgTe quantum well was the rst experimental realization of the QSH eect [12], following a theoretical prediction by Bernevig et al. [11]. The central idea is band inversion tuned by the thickness of HgTe. See Figure 2.13. CdTe has the normal band structure, in which p-like 7 and 8 are occupied and s-like 6 is empty. On the other hand, HgTe has the inverted one due to the large SOC, in which 7 and 6 are occupied and 8 is empty. Therefore it is expected that as increasing the thickness of HgTe, rst the band structure is normal like CdTe, then a gap between 8 and 6 closes at some critical thickness d = dc , and nally the band structure gets inverted like HgTe. k p model calculation supports this idea and the critical thickness is dc = 6.3nm. Figure 2.14 (a) and (b) show the device used for detection of helical edge modes. Figure 2.14 (c) shows the longitudinal resistance for dierent sizes. (I) is an ordinary band insulator without helical edge modes and has high resistance when the Fermi energy lies in a gap. (II)-(IV) are QSH insulators with helical edge modes. There exist two channels when the Fermi energy lies in a gap, leading to quantization of the conductance as G = 2e2 /h. The conductance of (II) is not quantized because the device size is larger than its inelastic mean free path. These quantitative agreements with k p model calculations strongly support the QSH eect. The second experiment was on a three-dimensional Bi1x Sbx alloy [15], motivated by thoretical predictions by two groups [13, 14]. Bismuth is trivial with the Z2 number of (0; 000) while antimony is non-trivial with the Z2 number of (1; 111). Unfortunately both are semimetal, though Bi1x Sbx is insulator for 0.07 < x < 0.22 as shown in Figure 2.15 (a). Again we can see that the idea of band
23
(b) (a)
(c)
Figure 2.14: (a) Schemaic picture of molecular beam epitaxy (MBE)-grown quantum well structure. (b) The device and helical edge modes. Red and blue arrows indicate up and down spin, respectively. (c) The longitudinal four-terminal resistance R14,23 as a function of the gate voltage at T = 30mK. A black curve (I) is normal (d = 5.5nm < dc ) with the size of (20.0 13.3)m2 . Blue (II), green (III), and red curves (IV) are inverted (d = 7.3nm > dc ) with dierent sizes. R14,23 is not quantized for (II) with the large size of (20.0 13.3)m2 , while quantized for (III) and (IV) with the small size of (1.0 1.0)m2 and (1.0 0.5)m2 [12].
24
(a)
(b )
Figure 2.15: (a) The energy levels of Bi1x Sbx at high symmetric points L, T , and H as a function of x. (b) The surface band dispersion along -M obtained by using ARPES. A white area indicate the bulk band dispersion [15]. inversion is active. Hsieh et al. directly observed surface states by using high-resolution ARPES for x = 0.1 (Figure 2.15 (b)). There exist the odd number of (ve) gapless points, which shows that Bi0.9 Sb0.1 is a STI. Very recently rst principles band calculations for Sb2 Te3 , Sb2 Se3 , Bi2 Te3 , and Bi2 Se3 were performed from the topological viewpoint, which predicted that Sb2 Te3 , Bi2 Te3 , and Bi2 Se3 are STIs while Sb2 Se3 is not [56]. Most astonishing is that Bi2 Se3 has a much larger gap of 0.3eV than room temperature. Bi2 Se3 and Bi2 Te3 were experimentally investigated by scanning tunneling spectroscopy (STS) [53] and ARPES [54, 55]. Note that the STS measurement was done before the proposal of the QSH eect by Kane and Mele [7, 8]. Figure 2.16 clearly shows that the local density of states (DOS) is nite not due to impurity or thermal eects, but due to the presence of surface states [53]. By using ARPES, a single pair of surface states was observed [55] (not shown).
2.4
Relativistic Mott insulator Sr2IrO4
Recently, a layered perovskite iridate Sr2 IrO4 has been focused on as a relativistic Mott insulator. It was an interesting problem why Sr2 IrO4 is a Mott insulator [29, 30, 31], although its 4d version Sr2 RhO4 , with the stronger electron correlation, is a Fermi liquid [32, 33]. Both Sr2 IrO4 and Sr2 RhO4 are distorted by around 10 [29, 57], which was considered to cause band narrowing [30]. In fact, lattice distortion of Sr2 RhO4 provides good explanation for the missing xy-Fermi surface sheet [58]. However, it is not reasonable to apply this idea to Sr2 IrO4 , and we should reexamine the electronic structure focusing on its large SOC. Under an octahedral crystalline eld, ve-fold degenerate d-orbitals split into doubly degenerate eg -orbitals and triply degenerate t2g -orbitals. eg -orbitals are explicitly written as u : 3z 2 r2 and v : x2 y 2 , while t2g -orbitals as : yz, : zx and : xy. Their energy dierence is called 10Dq. In the t2g -manifold an angular momentum is not completely quenched, e = 1. Therefore, with the SOC, we obtain states with total angular momenta je = 3/2 and 1/2. Now that an Ir4+ ion

(a) (b )
25
Figure 2.16: (a) Solid and dashed lines indicate experimental and theoretical tunneling dierential condactance dI/dVB of Bi2 Se3 . A bulk gap is 0.35V < VB < 0V. High reproducibility excludes the possibility of impurity-induced in-gap states and thermal broadening is negligible at low temperature of 4.2K. (b) Partial DOS of Se1 obtained by rst principle band calculations for a twelve-slab geometry [53].
octahedral crystalline field
SOC
Figure 2.17: The electronic structure of an Ir4+ ion under an octahedral crystalline eld and with the SOC. has ve electrons, je = 3/2-states are fully occupied and je = 1/2-states are half-lled. Kim et al. investigated the electronic structure of Sr2 IrO4 by using ARPES, optical conductivity, X-ray absorption spectroscopy (XAS), and rst principles band calculations [34]. The Fermi surface obtained by ARPES in Figure 2.18 (e) cannot be explained without including both the SOC and the electron correlation as shown in Figure 2.18 (a)-(d). Furthermore, the XAS spectra can be well tted by an assumption of : : = 1 : 1 : 1 as shown in Figure 2.19 (b), leading to je = 1/2 states written as 1 |+ = (+| + | + i| ) 3 1 | = (| + | i| ) . 3
(2.33)
26
Tetragonal and rotational distortions seem to be irrelevant. The SOC and the on-site Coulomb interaction are estimated to 0.5eV by optical conductivity in Figure 2.19 (a), which is consistent with the electronic structure obtained by LDA+SOC+U. At the end of this Section, resonant X-ray scattering (RXS) is introduced as more direct probe of relativistic states, which may need some explanations. The RXS process is described by the second order perturbation of the electron-photon coupling, and its amplitude is approximately given by 3 min i|R |n n|R |i f = . (2.34) h hin + i/2 n An electron makes a round trip from and to the initial state |i via all possible intermediate states |n , collecting phase factors. That is why RXS can detect phase factors of relativistic states. On experiments on iridates, L2 (2p1/2 5d) and L3 (2p3/2 5d) edges are focused on. Straightforward calculations on the Clebsch-Gordan coecients leads to the important fact that the intensities at L2 and L3 edges are equal for non-relativistic s = 1/2-states while L2 edge is forbidden for relativistic je = 1/2-states. In the recent RXS study by Kim et al., no intensity was observed at L2 edge in contrast to the resonantly enhanced intensity at L3 edge, which conrmed that je = 1/2-states are realized [59].
27
(a) LDA
(e ARP ) ES
(b LDA+ ) U
(c LDA+ OC ) S
(d LDA+ OC+ ) S U
Figure 2.18: The Fermi surfaces, the band dispersions, and schematic energy diagrams within (a) the local density approximation (LDA), (b) LDA+U with U = 2.0eV, (c) LDA+SOC, and (d) LDA+SOC+U. In the right panel of (b), the unrealistically large U leads to a Mott insulator. (e) ARPES intensity maps at EB = 0.2, 0.3, and 0.4eV. A red square indicates the reduced Brillouin zone neglecting 2 2 distortion [34].
28
Figure 2.19: (a) The optical conductivity at 100K. Peaks A and B are assigned to transition denoted in the right panel of Figure 2.18 (d). The O 1s polarization dependent XAS spectra (dotted lines) compared to the expected one (solid lines) under an assumption of : : = 1 : 1 : 1 [34].
Chapter 3 QSH eect in Na2IrO3

The QSH eect was rst proposed in the Kane-Mele model based on graphene with the honeycomb lattice [7, 8]. The model has the complex and spin-dependent transfer integrals to the NNN sites due to the SOC, in addition to the real and spin-independent ones to the NN sites. These complex and spin-dependent transfer integrals open a gap in bulk and result in gapless helical edge modes. However, the SOC in graphene is so small that the QSH cannot be observed. Here the newly synthesized compound Na2 IrO3 with the honeycomb lattice of iridium [60] is investigated. Antiferromagnetism (AFM) due to the electron correlation is also discussed.
3.1
Model construction
Na2 IrO3 is composed of (Na1/3 Ir2/3 )O2 layers and Na layers shown in Figure 3.1. In a (Na1/3 Ir2/3 )O2 layer, Ir and Na atoms are surrounded by six oxygen atoms, leading to the honeycomb lattice of Ir atoms. Na2 IrO3 is similar to Sr2 IrO4 in that each Ir4+ ion is subject to an octahedral crystalline eld, an eective single-band model can be constructed as basis of je = 1/2-states. The procedure is following: (1) The model is completely two-dimensional, neglecting the interlayer coupling. (2)Lattice distortion is neglected, leading to the perfect honeycomb lattice shown in Figure 3.2
(a) (b)
Figure 3.1: (a) The crystal structure of Na2 IrO3 drawn with VESTA [61]. Yellow, black and red circles indicate Na, Ir and oxygen, respectively. (b) A (Na1/3 Ir2/3 )O2 layer extracted from Na2 IrO3 . 29
CHAPTER 3. QSH EFFECT IN NA2 IRO3
30
(a)
(b)
Figure 3.2: (a) Perfect honeycomb lattice. The x, y and z-axes are dened in an octahedron. (b) Eective model. Black solid arrows are translation vectors a1 and a2 . Blue, red and green dotted arrows indicate the obtained transfer integrals it x , it y and it z , respectively. (a). (3) Oxygen is integrated out since the energy level of p-orbitals ( p ) is around 3eV lower than that of je = 1/2-states ( d ) [31]. The transfer integrals to the NN and NNN sites are calculated with Slater-Koster parameters [62].
3.1.1
Transfer integrals to the NN sites
First the indirect transfer integrals via oxygen are calculated by the second order perturbation. When an electron moves from Ir1 to Ir2 shown in Figure 3.3 (a), two paths exist, via O1 and O2. However, contributions of these independent paths exactly cancel out as seen later. Therefore we consider a O1-O2 bond. Slater-Koster parameters [62] using this and next Subsections are listed in Table 3.1. By using this, channels can be restricted like Table 3.2. When je = 1/2-states are generally expanded as | = ms Cms |ms ( = , m = , , and s =, ), contribution of each state can be written as t2 1 |A1g =
s
22 |H|A1g s A1g s|H|11 = d EA1g (pd) d p + (pp)

2 2 Cs2 + Cs s
(pd)2 d p + (pp)
1 Cs1 + Cs
2 1 Cs Cs s
1 t2 1 |E1g u = 2 t2 1 |E1g v =0
1 t2 1 |E1u u = 2 t2 1 |E1u v = t2 1 |A1u =0.
(pd)2 d p (pp)
(3.1)
Cs2 s 1 2 Cs Cs s
2 Cs
Cs1
1 Cs
(pd)2 d p (pp)
31
() a O2 Ir1 Ir2 O1
() b O5 Ir1
O3 O4 Ir0 O1 O6 Ir2 O2
Figure 3.3: The transfer integrals to (a) the NN sites. (b) the NNN sites. The numbers are assigned to related Ir and oxygen atoms. Red areas indicate the intermediate clusters of the second order perturbation. As a result the indirect transfer integral is given by t2 1 (pd)2 d p
1 2 Cs2 Cs + Cs Cs1 s 1 2 Cs Cs s
(pd)2 (pp) + (pp) d p d p
(pd)2 (pp) d p d p
2 1 Cs2 Cs1 + Cs Cs s
(3.2)
1 (pd)2 (pp) + 3(pp) . t= 3 d p d p Here isotropic je = 1/2-states like (2.33) are assumed. As for the other directions, we only have to permute , and in the rst line of (3.2), while the result is unchanged. In addition to the indirect transfer integrals, the direct transfer integrals are also possible. Again refering to Table 3.1, we obtain 1 1 5 2 + |H|1+ = 2 |H|1 = (dd) + (dd) + (dd), 4 3 12 (3.3)
while the o-diagonal matrix elements are found to vanish. It should be noted that both the indirect part (3.2) and the direct part (3.3) are real and spin-independent. Hereafter (3.2) is written as t, neglecting (3.3).
3.1.2
Transfer integrals to the NNN sites
The transfer integral to the NNN site shown in Figure 3.3 (b) can be calculated in the same way. Here a cluster composed of six oxygen atoms is considered, leading to eighteen states classied in
32
Table 3.1: Slater-Koster parameters [62]. l, m and n are the direction cosines along the x, y and z-axes, respectively. x|H|x l2 (pp) + (1 l2 )(pp) x|H|y lm(pp) lm(pp) x|H|z 2 ln(pp) ln(pp) x|H| 3l m(pd) + m(1 2l2 )(pd) x|H| 3lmn(pd) 2lmn(pd) 2 x|H| n(pd) + n(1 2l2 )(pd) 2 3l 2 2 x|H|v + 2 3l(l2 m2 )(pd)/2 + l(1 l 2 m )(pd) y|H|v 3m(l m )(pd)/2 m(1 + l m2 )(pd) z|H|v 3n(l2 m2 )(pd)/2 n(l2 m2 )(pd) 2 2 2 x|H|u l(2n l m )(pd)/2 3ln2 (pd) y|H|u m(2n2 l2 m2 )(pd)/2 3mn2 (pd) z|H|u n(2n2 l2 m2 )(pd)/2 + 3n(l2 + m2 )(pd) |H| 3l2 m2 (dd) + (l2 + m2 4l2 m2 )(dd) + (n2 + l2 m2 )(dd) |H| 3lm2 n(dd) + ln(1 4m2 )(dd) + ln(m2 1)(dd) |H| 3l2 mn(dd) + mn(1 4l2 )(dd) + mn(l2 1)(dd)
Table 3.2: Classication of six states (= two state |A1g = (|1x + |1y |2x |2y )/2 |E1g u = (|1z |2z )/ 2 |E1g v = (|1x |1y + |2y )/2 |2x |E1u u = (|1z + |2z )/ 2 |E1u v = (|1x |1y + |2x |2y )/2 |A1u = (|1x + |1y + |2x + |2y )/2
atoms three p-orbitals). energy channel (pp) p , , p (pp) , , p + (pp) p + (pp)
33
Table 3.3: Classication of eighteen states (= six atoms three p-orbitals). Here neglecting (pp) and (pp), all states have the same energy p . state channel |A1g = (|1x + |2y + |3z |4x |5y |6z )/ 6 |Eg u = [2|3z 2|6z (|1x + |2y |4x |5y )]/ 12 |Eg v = (|1x |2y |4x + |5y )/2 |T2g = (|2z + |3y |5z |6y )/2 |T2g = (|3x + |1z |6x |4z )/2 |T2g = (|1y + |2x |4y |5x )/2 |T2u = (|2x |3x + |5x |6x )/2 |T2u = (|3y |1y + |6y |4y )/2 |T2u = (|1z |2z + |4z |5z )/2 (1) |T1u = |1x + |4x )/ 2 (1) |T1u = (|2y + |5y )/ 2 (1) |T1u = (|3z + |6z )/ 2 (2) |T1u = (|3x + |6x + |2x + |5x )/2 (2) |T1u = (|1y + |4y + |3y + |6y )/2 (2) |T1u = (|2z + |5z + |1z + |4z )/2 |T1g = (|2z |3y |5z + |6y )/2 |T1g = (|3x |1z |6x + |4z )/2 |T1g = (|1y |2x |4y + |5x )/2 -
CHAPTER 3. QSH EFFECT IN NA2 IRO3 Table 3.3. Then contribution of each state is given by 2 (pd) t2 1 |A1g = 3 d p 1 (pd) t2 1 |T2g = 4 d p t2 1 |T (1)
1u
34
1 Cs2 Cs s 2 Cs Cs1 s 2
1 (pd) = 2 d p
2
(3.4)
1 Cs2 Cs s 2 Cs Cs1 . s
1 (pd) t2 1 |T1g = 4 d p
On the other hand, Eg -states are exceptional because their energy is lowered by the coupling to eg -orbitals of Ir0. Using Eg u|H|u = 3(pd), we can obtain a new eigenstate |Eg u = 1 2 1+ x x2 + 3(pd)2 |Eg u 1 2 1 x x2 + 3(pd)2 |u , (3.5)
with the energy of EEg = 1 t2 1 |Eg u = 2 1+
+x x
x2 + 3(pd)2 , where x ( d + 10Dq p )/2. Thus we obtain 1 6 (pd)2

d 1 Cs2 Cs . s
x2
3(pd)2
x2
3(pd)2
(3.6)
Similarly t |Eg v = 0 is obtained. The resulting transfer integral is written as 1 (pd) t2 1 = 6 d p 1 (pd)2 2 d p
2 2 1 Cs2 Cs 1 s 1 Cs2 Cs s
1 2
1+
x x2 + 3(pd)2
p) d
x2
+ 3(pd)2 x (3.7)
(pd)2 ( d p )( d + 10Dq
p)
(pd)2 ( d + 10Dq
2 p)
2 p)
1 (pd) t = 6 d p (
(pd)2 d p )( d + 10Dq
(pd)2 ( d + 10Dq
iy ,
where s are Pauli matrices for a pseudospin index (+ or ). Hereafter the cocient of (3.7) is denoted as t . As for the other directions, we can obtain it x and it z . The point is that the transfer integrals to the NNN sites are complex and spin-independent similar to Kane-Mele model, leading to the QSH eect as seen in the next Section.
35
Table 3.4: Classication of H0 (k) by a dened by Fu and Kane [13]. P is the space-inversion operater. k1 = k a1 and k2 = k a2 run in the range of [, ). s are Pauli matrices for sublattices. a da (k) a T P 1 t(1 + cos k1 + cos k2 ) x 1 + + 2 t( sin k1 + sin k2 ) y 1 3 2t sin k1 z x 4 2t sin k2 z y 5 2t sin(k1 + k2 ) z z
3.2
Paramagnetic phase
H0 = t
i
From the previous Section, the eective Hamiltonian can be written as d di1 + d 1 2 di1 + d di+a2 1 i2 i2 i+a d 1 1 x di1 + d x di+a1 2 + it i2 i+a
i i
+ it + it
i
d 2 1 y di1 + d y di+a2 2 i2 i+a
(3.8)
d z di+a1 +a2 1 + d 1 +a2 2 z di2 + h.c., i1 i+a
where d (di1 ) is a creation (annihilation) operator at the sublattice 1 of the i-th. unit cell. This i1 model is found to show the QSH eect by the Z2 number and the existence of gapless helical edge modes. To calculate the Z2 number, periodic boundary conditions are imposed. k-component of the Hamiltonian H0 (k) can be written as
5
H0 (k) =
a=1
da (k)a ,
(3.9)
where ds and s are listed in Table 3.4. The components of the other ten matrices ab must vanish due to TR and inversion symmetries. The Z2 number of an inversion symmetric two-band system is determined by the product of (i ) = sgn d1 (i ) [13]. Explicitly i are = [0, 0], M1 = [, 0], M2 = [0, ] and M3 = [, ] in terms of [k1 , k2 ]. It is straightforward to see () = (M1 ) = (M2 ) = 1, while (M3 ) = 1. Their product is negative, which means the Z2 number of (1) = 1. To see gapless helical edge modes directly, the efective Hamiltonian (3.8) is numerically diagonalized under periodic boundary conditions along one axis and open boundary conditions along another. There exist two simple edge geometries, zigzag and armchair. In Figure 3.4, the band dispersion for the zigzag edge geometry is shown. Bulk states are gapped due to the complex and spin-dependent transfer integrals to the NNN sites induced by the SOC, while a pair of helical
36
(a)
(b)
4 3 2 1 0 -1 -2 -3 -4 wavenumber

energy
Figure 3.4: (a) The zigzag edge geometry with N = 4 chains. Periodic boundary conditions are imposed along a1 and a black dotted line indicates a supercell. (b) The band dispersion for t = t = 1 and N = 50. edge modes is gapless at a TR invariant point k = , corresponding to the QSH eect. Note that for the armchair edge geometry a pair of helical edge modes is gapless at k = 0. Now the problem is whether the complex and spin-dependent transfer integrals are peculiar to the honeycomb lattice. A toy model in the xy-plane can answer this problem. Consider projected je = 1/2-states as 1 |+ = (+| + i| ) 2 1 | = (+| i| ) 2
(3.10)
and a pz -orbital. When one oxygen atom is placed as shown in Figure 3.5 (a), we obtain z|H| = i(pd)e i / 2 by using Table 3.1. Then the indirect transfer integral between Ir atoms is given by t = (pd)2 e 2i /2( d p ), which is complex and spin-dependent. Meanwhile when two oxygen atoms are placed as shown in Figure 3.5 (b), phases of two paths cancel out and the resulting transfer integral is real and spin-independent like t = (pd)2 cos 2/( d p ). From the above discussion, we can derive two essences to design QSH transition metal oxides, i.e. (1) complex and spin-dependent states due to the SOC and (2) lattice asymmetry so that phases do not cancel out. As for the NNN sites, Ir and Na atoms are asymmetric, leading to the complex and spin-dependent transfer integrals. These essences can give us even three-dimensional topological insulators.
3.3
Edge AFM phase
In this Section, the eect of the electron correlation is investigated by adding the on-site Coulomb interaction written as H1 = U (ni1+ ni1 + ni2+ ni2 ) , (3.11)
i

(a) (b)
37
Figure 3.5: A toy model in the xy-plane. Black and red clouds indicate a projected je = 1/2-state of an Ir atom and a pz -orbital of an oxygen atom, respectively. Two Ir atoms are on the x-axis. (a) When one oxygen atom is placed at an angle of to the x-axis, the transfer integral between Ir atoms is complex and spin-dependent. (b) When two independent oxygen atoms are symmetrically placed, the transfer integral becomes real and spin-independent. where U is the eective on-site Coulomb interaction in je = 1/2-states. In the large U limit, the real and spin-independent transfer integrals (3.2) result in the AFM exchange interaction between the NN sites,
NN
J
ij 2
si sj .
(3.12)
Here J = 4t /U and s is a spin operator. On the other hand, the complex and spin-dependent transfer integrals (3.7) bring a dierent type of the exchange interaction between the NNN sites,
NNN
J
ij
si sj 2sa sa i j
(a = x, y, z)
(3.13)
with J = 4t 2 /U . In total, the AFM interaction is eective between the NN sites, while the nearly FM interaction between the NNN sites. Therefore AFM is preferred on the honeycomb lattice. However, the paramagnetic phase of Na2 IrO3 is a QSH insulator distinct from an ordinary band insulator. Now a new mechanism of the AFM transition is proposed based on its topological nature. A QSH system consists of the gapped bulk and the gapless edge protected by TR symmetry. The former is dicult to gain the electronic energy and is robust against the AFM order, while the latter is fragile because it breaks TR symmetry. Thus AFM moments are expected to develop rst in the edge and then spread into the bulk as decreasing temperature.
3.3.1
Mean eld approximation
This mechanism can be conrmed within the mean eld approximation on a semi-innite system. The on-site Coulomb interaction can be rewritten as 1 H1 = U 2 2 (ni1+ + ni1 + ni2+ + ni2 ) U 3 s2 + s2 . i1 i2
i
(3.14)

(a) (b)
38
(c)
5 4 3 2 1 0 -1 -2 -3 -4 -5 wavenumber

(d)
5 4 3 2 1 0 -1 -2 -3 -4 -5 wavenumber

energy
energy
Figure 3.6: (a) The edge AFM phase along the X-axis. (b) The bulk AFM phase along the X-axis. Each AFM moment is assumed to have the same length. (c, d) The band dispersions for (a, b) with N = 50 chains and |mn | = 1. The rst term is proportional to the total number of electrons and is constant. Within the mean eld approximation, the quadratic terms of spin operators are approximated as s2 (ln)1 = sn + s(ln)1 sn s2 (ln)2 = sn + s(ln)1 + sn
2 2
2 sn s(ln)1 sn
2 sn s(ln)2 sn 2 ,
(3.15)
where l = 1, . . . , L is the axis with periodic boundary conditions while n = 1, , N is that with open boundary conditions. Hence (3.14) can be written as H1 4 U 3 sn
ln 2
sn s(ln)1 s(ln)2
=
ln
3m2 n 2mn s(ln)1 s(ln)2 U
(3.16)
where the rst constant term of (3.14) is dropped and mn 2U sn /3 is introduced. The total Hamiltonian is H = H0 + H1 . The free energy is optimized via mn and the most stable spin conguration is searched for each temperature. For simplicity spin congurations are restricted to those shown in Figure 3.6 (a) and (b). Figure 3.6 (c) shows that helical edge modes get gapped associated with spontaneous breaking of TR symmetry. The free energy is calculated for L = N = 100. Figure 3.7 shows the existence of the edge AFM phase for U = 10.5, namely, the edge AFM transition occurs at higher temperature than the bulk AFM. It seems that the magnetization changes discontinuously at the transition point from the edge AFM phase to the bulk AFM phase,
39
e g AFM de bulk AFM QS H
Figure 3.7: The temperature dependence of (the upper panel) dierence of the free energy per supercell from the QSH phase and (the lower panel) the magnetization for U = 10.5. As temperature decreases, the edge AFM transition occurs at T = 0.96, and then the bulk AFM transition at T = 0.68. though it should change continuously when n-dependence of mn is considered. An edge mode itself is the most uctuating one-dimensional system and generally the mean eld approximation is not valid. Nonetheless the edge AFM phase is possible in terms of the eective theory of one-dimensional helical liquids [18]. In fact, TR symmetry allows only two kinds of interactions, i.e. the forward and umklapp scatterings Hfw =gfw Hum =gum
dxR+ (x)R+ (x)L (x)L (x)
(3.17) dxe
i4kF x R+ (x)R+ (x
+ a)L (x + a)L (x) + h.c.,
where a is the lattice constant. The forward scattering term gives the non-trivial Luttinger parameter K = (vF gfw )/(vF + gfw ) but a helical liquid remains gapless. On the other hand, according to the renormalization group (RG) analysis of the bozonized Hamiltonian, the umklapp 1/24K scattering term becomes relevant at < 1/2, and a gap K a1 gum opens. For gum < 0, R L is pinned at either 0 or /2, leading to the nite value of the mass order parameter O2 iR L /2a cos 4. Since O2 is TR odd, TR symmetry is spontaneously broken at T = 0. For gum > 0, O1 iR L /2a sin 4 is the order parameter. Anyway, such Ising-like order is not stabilized at nite temperatures in one dimension, though a gap remains. In this sense, the edge AFM phase discussed above is a liquid of Ising domain walls.
3.3.2
Fractional charge
In the edge AFM phase, the fractional charge due to the topological nature of a QSH insulator arises at a domain wall. The idea of the fractional charge goes back to the Su-Schrieer-Heeger
40
model [63]. For spinless fermions, a mass kink induces a localized state with zero energy, which has charge of e/2. However, in realistic systems such as polyacetylene, only the integer charge is carried because of two spin degrees of freedom. On the other hand, helical liquids have half degrees of freedom of spinful TL liquids, i.e. up spins move to the right while down spins to the left. Thus the fractional charge appears at domain walls of helical liquids [64]. To calculate the fractional charge carried by domain walls, we have to dene smooth deformation from a QSH insulator to the vacuum via the edge AFM order. In ve s, only 1 x 1 is TR invariant. Therefore the TR invariant vacuum is described as Hvac (k) = V 1 with V . On the other hand, the AFM order is odd under TR and inversion symmetries, which is describes as H1 = mx 3 + my 4 + mz 5 . Now smooth deformation can be taken as H(k, , ) = 5 da (k, , )a with a=1 t(1 + cos k1 + cos k2 ) + V () t( sin k1 + sin k2 ) x x x , (3.18) 2t sin k1 + mbulk (1 cos )/2 + (medge cos + mDW sin ) sin da (k, , ) = y y y 2t sin k2 + mbulk (1 cos )/2 + (medge cos + mDW sin ) sin z z z 2t sin(k1 + k2 ) + mbulk (1 cos )/2 + (medge cos + mDW sin ) sin where mbulk is the bulk AFM moment, medge are the directions of the edge AFM far away from the domain wall, and mDW is the direction at the domain wall as shown in Figure 3.8. = 0 and correspond to the vacuum and the system, and the domain wall is located between = 0 and . The even function V () satises V (0) = V , V () = 0, and V (/2) = 3t. The last condition V (/2) = 3t is required to guarantee that the level crossing occurs at k = 0 in the QSH phase. One choice of V () is given by V () = 3ta(a + 1) 1 1 a cos a + 1 (3.19)
with a = (1 6t/V )1 . Note that the parameter V should be taken to V > 3t to make sure that = 0 is the trivial vacuum. The net charge carried by the domain wall can be calculated by the skyrmion formula [65] 3 Q= 2 8
abcde 0
d
0
d2 k
da k1 db k2 dc dd de |d(k, , )|5
(3.20)
For mbulk = 0, the bulk is TR invariant and we obtain Q = 1/2 as discussed by Qi et al. [65]. When the bulk TR symmetry is broken with mbulk = 0, the net charge Q deviates from e/2. Thus the edge AFM phase discussed in this Section has the topological property dierent from the bulk AFM phase.
3.4
Experimental proposal
In the realistic three-dimensional compound, the interlayer coupling gives the band dispersion along k3 , leading to two Dirac fermions at k3 = 0 and . In this case, the backward scattering
41
Figure 3.8: Schematic picture of the domain wall. Gray and orange areas indicate the vacuum and system, corresponding = 0 and , respectively. A red curve shows the charge density around at the intersection of the edge and the domain wall.
(a) C B (b) on A and B local DOS A (c) on C local DOS edge
energy 0 bulk 0
energy bulk
Figure 3.9: (a) The schematic picture of a plateau (orange) on the surface. A, B and C are typical points outside, inside and just on the plateau edge, respectively. (b, c) The energy dependence of the local DOS on (b) A, B and (c) C at dierent temperatures T TN (the QSH phase, blue dot line), T > TN (the edge AFM phase, red dash line) and T < TN (the bulk AFM phase, black solid line). between them is possible via a weak periodic potential and disorder, and a helical liquid becomes localized or gapped. In other words, Na2 IrO3 is a WTI. However, if we focus on a plateau on the surface as shown in Figure 3.9 (a), its edge is spatially separated from the edges of underlying layers and is robust. The above topological natures can be detected by STS. When a tip is away from the plateau edge, the local DOS shows a large bulk gap bulk for both the QSH and AFM phases as shown in Figure 3.9 (b). On comparison when the tip is just on the plateau edge, the local DOS remains nite in the QSH phase at T TN , reecting the existence of gapless helical edge modes. Here TN is the bulk Nel temperature. As temperature decreases, a small edge gap e edge opens slightly above TN . Even at T = 0, edge remains smaller than bulk as shown in Figure 3.6. Such temperature dependence is schenatically shown in Figure 3.9 (c).
42
Figure 3.10: The Kitaev model implemented in Na2 IrO3 . Blue, red, and green lines indicate x-, y-, and z-bonds with the superexchange interactions sx sx , sy sy , and sz sz , respectively. i j i j i j
3.5
Discussion
In our approach, the weak electron correlation is added to the non-interacting Hamiltonian with the Z2 non-trivial topology. This is the weak coupling limit. On the other hand, the strong coupling limit is also possible, leading to another interesting phase. Jackeli and Khaliullin derived the superexchange Hamiltonian as
NN
H = J
ij
sc sc , i j
(3.21)
where we label a ij-bond in the ab-plane perpendicular to the c-axis by a c-bond as shown in Figure 3.10. In their theory, the Hund coupling JH plays a crucial role. In fact, without the Hund coupling, J = 42 /3 4t2 /U , with 22 JH /U exactly vanishes due to the lattice symmetry discussed in Section 3.2. This model is included by the Kitaev model generally written as
NN
H=
ij
Jc sc sc , i j
(3.22)
which can be exactly solved, leading to two phases [66]. The phase A, for |Jx | > |Jy | + |Jz | or its cyclic permutations, has a gap asscosiated with Abelian anyons. On the other hand, the phase B, for |Jx | < |Jy | + |Jz | and its cyclic permutations, is gapless with Dirac cones, but acquires a gap in a magnetic eld associated with non-Abelian anyons. Our and their theories are complementary, and it is likely that the realistic compound lies in the intermediate region between two limits, i.e. a QSH insulator and the Kitaev model, leading to a gap and frustration.
Chapter 4 First principles approach to topological insulators

In Chapter 3, we have found that Na2 IrO3 is a WTI based on the tight-binding model, though its validity must be examined by more serious calculations. On the other hand, the search for threedimensional STIs is a challenging problem. To achieve these purposes, rst principles calculations are performed by using the full-potential linearized augmented plane-wave (FP-LAPW) method implemented in WIEN2k [67], which is one of the most accurate methods within the density functional theory (DFT) [68, 69]. The generalized gradient approximation (GGA) by Perdew et al. [70] is used to describe the exchange-correlation potential. The SOC can be included by the second variational method using scalar-relativistic eigenstates as basis [71].
4.1
Na2IrO3 with the honeycomb lattice
In this Section, the electronic structure of Na2 IrO3 is calculated to examine whether several approximations are valid.
4.1.1
Calculations
Since the accurate parameters for the crystal structure of Na2 IrO3 have not been known yet, those of Na2 PtO3 listed in Table 4.1 are used for input. The mun-tin radii RMT are set to 2.05, 2.10 and 1.65a.u. for Ir, Na and oxygen. Wave functions inside atomic spheres are expanded in spherical harmonics up to max = 10, while those outside spheres are expanded in plane-waves with the cut-o RMT Kmax = 7.0. 125 k-points are taken in the whole Brillouin zone, corresponding to 21 k-points in the irreducible Brillouin zone. The convergence criteria are 0.00001Ry for energy and 0.0001 for charge. Figure 4.1 shows the results of the GGA calculations without the SOC. O p-, Ir t2g -, and Ir eg -bands are well-separated by around 4.2eV and 3.6eV, respectively, which are almost consistent with the optical conductivity experiment on Sr2 IrO4 [31]. The bands near the Fermi energy EF
43
CHAPTER 4. FIRST PRINCIPLES APPROACH TO TOPOLOGICAL INSULATORS
44
Table 4.1: The atomic positions for Na2 PtO3 with the monoclinic space group C2/c (No. 15). The lattice constant is a = 5.419, b = 9.385 and c = 10.752 and = 99.67 . Note that WIEN2k has A a limitation that in centered monoclinic lattices only B-setting is allowed. atom x y z Pt1 0 0.249 1/4 Pt2 0 0.584 1/4 Na1 0.261 0.578 0.001 Na2 1/4 1/4 0 Na3 0 0.918 1/4 O1 0.15 0.101 0.148 O2 0.095 0.415 0.149 O3 0.146 0.735 0.148 are mainly composed of Ir t2g -bands (Figure 4.1 (b)), and the nite DOS at EF shows that the compound is a metal within the GGA (not including the SOC). The relativistic calculations including the SOC are shown in Figure 4.3. In Figure 4.3 (b), a dip of the total DOS can be observed at the Fermi energy, in contrast to Figure 4.1 (b). In addition, this double peak is mainly composed of je = 1/2-states as shown in Figure 4.3 (e). Note that the dip becomes deeper after performing optimization of atomic positions. All of these supports our theory that je = 1/2-states on the honeycomb lattice provide a WTI.
4.1.2
Discrepancy between calculations and experiments
Na2 IrO3 is experimentally an insulator, while the above calculations predicted a metal close to an insulator. The possible origins of this discrepancy are (1) the drawback of the LDA, and (2) the eect of the electron correlation. The former is that the eigenvalues of Kohn-Sham equations do not correspond to the single-particle excitation energies, and the LDA usually underestimates the band gap. The latter is very dicult. In cases for the even number of electrons per unit cell, the system is in principle a band insulator in the weak correlation limit, and no distinction exists between a band and Mott insulators. On the other hand, a topological insulator has both charge and spin channels at the edges, while a Mott insulator does not have a charge degree of freedom. Thus we face two challenging problems. One is whether the compound is a topological insulator or a Mott insulator, in other words, where the critical point of the Mott transition is. The other is how the spin channel behaves with the electron correlation. The fractionalized QSH (or quantum spinon Hall) eect proposed by Young et al. [73] may provide a clue, though their model is too articial. These two problems remain to be solved. It should be emphasized that some kinds of frustration are assumed as discussed in Section 3.5. Therefore the Mott transition is not accompanied with breaking of translational and TR symmetries, otherwise, distinction from a Mott insulator is trivial, i.e. the presence or absence of the magnetic order.
45
(a)
40 35 30 25 DOS 20 15 10 5 0 -6 -4 -2 0 energy [eV] 2 4 total Ir eg Ir t2g Op
(b)
40 35 30 25 DOS 20 15 10 5 0 -2 -1.5 -1 -0.5 energy [eV] 0 0.5 total Ir t2g Op
(c)
4 2 energy [eV] 0 -2 -4
(d)
0.5 0 energy [eV]

-0.5 -1 -1.5
-6 -2 Z R Y L X Y Z R Y L X

Figure 4.1: GGA calculations of (a) the total (black) and projected (red, green, and blue for Ir eg , Ir t2g , and O p) DOSs, (b) near EF , and (c) the band structure, (d) near EF . In each panel, the origin of the energy axis is set to EF . See Figure 4.2 (a) for notations of the high symmetric k-points.

(a) (b )
46
Figure 4.2: Brillouin zone for (a) Na2 IrO3 (conventional cell) and (b) Lu2 Ir2 O7 (primitive cell) drawn with XCrySDen [72].
4.1.3
Extension of the tight binding model
Although the bands near the Fermi energy are composed of je = 1/2-states, they appear to be dierent from those expected from the simple tight binding model. This discrepancy is due to the possible existence of the interlayer coupling t and the real and spin-independent transfer integrals to the NNN sites t0 . Especially, since Na2 IrO3 is predicted to be a metal within the GGA+SOC, the transfer integrals t0 are considered to be as large as the transfer integrals t. First of all, we consider the interlayer coupling based on the crystal structure. Black lines in Figure 4.4 shows the considered interlayer coupling. The bond lengths between the interlayer sites are around 5.6, which are the same as those between the NNN sites (5.4). The interlayer A A coupling t is assumed to be real and spin-independent, which can be given by the direct transfer integrals (3.3). The real and spin-independent transfer integrals to the NNN sites can be given by the second order perturbations of those to the NN sites, in addition to the direct ones. Then the three-dimensional 8 8 Hamiltonian can be written as H(k) =
H0 (k) H (k) H (k) H0 (k)
t (1 + eik3 ) t (eik1 + ei(k2 +k3 ) ) H (k) = , t (1 + eik3 ) t (1 + eik3 )
(4.1)
where the two-dimensional 4 4 Hamiltonian H0 (k) is given by (3.9), but d0 (k) = 2t0 (cos k1 + cos k2 + cos(k1 + k2 )). This eective Hamiltonian can be analytically diagonalized along some high symmetric k-points as shown in Table 4.2, which makes it possible to estimate tting parameters t, t , t0 , and t . Figure 4.5 shows the band dispersions for two typical parameters, (a) is for t = 0 and (b) is for t = 0. The trasnfer integrals it a provide no signicant change due to the presence of t , in sharp contrast to the two-dimensional model, which shows that Na2 IrO3 is a WTI. Although it can not be called well-tted, the interlayer coupling t is estimated to be one order of magnitude smaller than t. Discrepancy of the details may be due to lattice distortion, hybridization of je = 3/2-states, and the electron correlation which rst principles calculations can include.
47
(a)
45 40 35 30 25 20 15 10 5 0 total Ir eg Ir t2g Op
(b)
30 25 20 DOS 15 10 5 -6 -4 -2 0 energy [eV] 2 4 0 -2 -1.5 -1 -0.5 energy [eV] 0 0.5 total Ir t2g Op
(c)
4 2 energy [eV] 0 -2 -4 -6
DOS
(d)
0.5 0 energy [eV] Z R
-0.5 -1 -1.5 -2
(e )
Na2IrO3 (with s-o coupling)
2 Jeff=3/2 Jeff=1/2
(f )
0.15 0.1 0.05 energy [eV] 0 -0.05 -0.1 -0.15
0.5
1.5
-0.2 -0.25
-5 -4 -3 -2 -1 Energy (eV) 0 1 2 3
0 -6
L X
Figure 4.3: GGA+SOC calculations of (a) the total (black) and projected (red, green, and blue for Ir eg , Ir t2g , and O p) DOSs, (b) near EF , and (c) the band structure, (d) near EF . (e) Black and red lines indicate the projected DOS of je = 3/2- and je = 1/2-states, respectively. (f) The band structure near EF after optimization of atomic positions.
L X
Z R Y
LX
48
Figure 4.4: Three-dimensional lattice of Ir atoms. The primitive translation vectors a1 , a2 , and a3 are indicated by black arrows. The bond lengths between the NN, NNN (blue, red, and green dotted arrows), and interlayer (black dotted lines) sites are around 3.1, 5.4, and 5.6 A
Table 4.2: Eigenvalues of the eective Hamiltonian (4.1) at some high symmetric k-points. k-point eigenvalues degeneracy 3t + 6t0 , 3t + 6t0 4t 4, 2, 2 2 + 8t 2 + 2t R 5t 4, 4 0 Y 3t + 6t0 4, 4
(a)
energy [eV]
0.15 0.1 0.05 0 -0.05 -0.1 -0.15 -0.2 -0.25
(b )
energy [eV]
0.15 0.1 0.05 0 -0.05 -0.1 -0.15 -0.2 -0.25

L X
L X
Figure 4.5: Comparison between rst principles calculations (small circle) and the extended tight binding model (big square) for t = 0.031145, t0 = 0.013, t = 0.00628375, and (a) t = 0, (b) t = 0.01eV.
49
(a)
(b )
(c )
Figure 4.6: (a) Pyrochlore lattice drawn with VESTA [61]. Yellow, black and red circles indicate Ln, Ir and oxygen, respectively. (b) Network of corner-sharing IrO6 octahedrons. (c) Network of corner-sharing OLn4 tetrahedrons.
4.2
Lu2Ir2O7 with the pyrochlore lattice
The pyrochlore lattice is a three-dimensional geometrically frustrated lattice with corner-sharing tetrahedrons as shown in Figure 4.6. Especially pyrochlore iridates Ln2 Ir2 O7 have attracted much interests because they exhibit unique properties originating from geometrical frustration, f -electrons of Ln ions, and the tunable transfer integrals by Ln ions. Some of them are insulators, and good candidates for STIs. To begin with, the previous studies on pyrochlore iridates are shortly explained. A series of pyrochlore iridates Ln2 Ir2 O7 shows the metal-insulator changeover with decreasing Ln ion radii [74, 75]. Pr2 Ir2 O7 is known as the frustrated Kondo lattice, in which the magnetic long-range order due to the Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction is suppressed by geometrical frustration and the Kondo eect is stabilized [76]. At low temperature, Pr 4f -moments are underscreened, leading to a metallic spin liquid and the unconventional anomalous Hall eect [77]. For Ln = Nd, Sm, and Eu, the metal-insulator transition occurs [75]. The compounds with smaller ions, Ln = Gd, Tb, Dy, Y, Ho, and Yb, are insulators [74], whereas the recent studies by ARPES and rst principles calculations revealed that Y2 Ir2 O7 has the small but non-zero DOS at the Fermi energy [78, 79]. This suggests that the experimentally observed insulating phase is driven by disorder. Therefore the rst problem is whether Lu2 Ir2 O7 , with the smallest ion Lu, is an insulator or not. Since Lu3+ has fourteen f -electrons, we do not suer from the problem of the Kondo lattice.
4.2.1
Calculations
The inputs for band calculations are following. The experimental crystal structure listed in Table 4.3 is used [80]. The cut-o for plane-waves is set to RMT Kmax = 7.0, while that for spherical harmonics is set to max = 10. 512 k-points are taken in the whole Brillouin zone, corresponding to 29 k-points in the irreducible Brillouin zone. The convergence criteria are 0.00001Ry for energy and 0.0001 for charge.
50
Table 4.3: The atomic positions for Lu2 Ir2 O7 with the cubic space group F d (No. 227, origin 3m choice 2). The lattice constant is a = 10.104 [80]. The mun tin radii RMT are also listed (in A the atomic unit). atom x y z RMT Lu 1/2 1/2 1/2 2.38 Ir 0 0 0 2.10 O1 0.340 1/8 1/8 1.67 O2 3/8 3/8 3/8 1.67 The electronic structure without the SOC is shown in Figure 4.7. Ir eg - and t2g -bands are well-split, and narrow Lu f -bands lie in wide O p-bands. The bands near EF are mainly composed of Ir t2g -bands as shown in Figure 4.7 (b), and the depressed but nite DOS at EF shows that the compound is a metal within the GGA. Figure 4.8 is the results of the GGA+SOC calculations. A main dierence from Na2 IrO3 is that t2g -bands are not well-split into je = 1/2- and je = 3/2-bands. In addition, no dip can be observed at the Fermi energy EF . As seen in Figure 4.8 (d), the band across EF is degenerate both with that below EF at point and with that above EF at X point. Thus we conclude that Lu2 Ir2 O7 is not topological nor ordinary band insulators, though it is expected to be the closest to an insulator among pyrochlore iridates.
51
(a)
80 70 60 50 DOS 40 30 20 10 0 -8 -6 -4 -2 0 2 energy [eV] 4 6 8 total Lu d Lu f Ir eg Ir t2g Op
(b)
30 25 20 DOS 15 10 5 0 -2 -1.5 -1 -0.5 energy [eV] 0 0.5 total Ir t2g Op
(c)
8 6 energy [eV] 2 0 -2 -4 -6 -8 X W L

(d)
0.5 0 energy [eV] -0.5 -1 -1.5 -2 X W L

Figure 4.7: GGA calculations of (a) the total (black) and projected (red, green, blue, magenta, and cyan for Lu d, Lu f , Ir eg , Ir t2g , and O p) DOSs, (b) near EF , and (c) the band structure, (d) near EF . In each panel, the origin of the energy axis is set to EF . See Figure 4.2 (b) for notations of the high symmetric k-points.
52
(a)
80 70 60 50 DOS 40 30 20 10 0 -8 -6 -4 -2 0 2 energy [eV] 4 6 8 total Lu d Lu f Ir eg Ir t2g Op
(b)
20 18 16 14 12 10 8 6 4 2 0 -2 -1.5 total Ir t2g Op
DOS
-1 -0.5 energy [eV]
0.5
(c)
8 6 energy [eV] 2 0 -2 -4 -6 -8 X W L

(d)
0.5 0 energy [eV] -0.5 -1 -1.5 -2 X W L

Figure 4.8: GGA+SOC calculations of (a) the total (black) and projected (red, green, blue, magenta, and cyan for Lu d, Lu f , Ir eg , Ir t2g , and O p) DOSs, (b) near EF , and (c) the band structure, (d) near EF .
Chapter 5 Summary and future problems

To conclude this thesis, 5d transition metal oxides have several unique properties due to the SOC and the electron correlation, and especially were investigated from the topological point of view. A newly synthesized Ir oxide Na2 IrO3 , with the layered honeycomb lattice, was found to be a WTI through the study of the eective tight binding model and rst principles calculations. In the eective model, the complex and spin-dependent transfer integrals to the NNN sites it a open up a gap, leading to the QSH eect, i.e. the non-trivial Z2 number (1) = 1 and the presence of helical edge modes. Their origins are the complex and spin-dependent states due to the SOC (je = 1/2-states) and lattice asymmetry so that the eective Aharonov-Bohm phases do not cancel out, which are applicable to the search for STIs in transition metal oxides. The eective tight binding model can roughly explain rst principles band calculations by including the real and spin-independent transfer integrals t0 and the interlayer coupling t , though discrepancy of the details are considered to result from lattice distortion, hybridization of je = 3/2-states, and the electron correlation which the LDA can include. One possible reason of discrepancy between rst principles calculations and experiments is the drawback of the LDA. Another reason is related to the electron correlation, which is discussed as future problems later. In addition, we investigated the interplay between the non-trivial topology and the AFM interaction, and proposed the edge AFM phase within the mean eld approximation. Helical edge modes are robust against TR invariant perturbations, while are fragile against TR breaking perturbations and open up a gap. On the other hand, the gapped bulk is relatively robust than the gapless edge, which leads to the AFM order only at the edge. Interestingly, the fractional charge is localized at the domain wall of the edge AFM, reecting the topological nature of QSH insulators. These topological natures can be observed by the STS measurement on the plateau edge. Since Na2 IrO3 is a WTI, usual methods to detect helical edge modes (ARPES and STS) can not detect its topological natures. To avoid the even/odd problem, we can focus on the plateau, whose edge is spatially separated from the edges of underlying layers. The local DOS at the plateau edge is expected to be suppressed at an onset temperature higher than the bulk Nel temperature. e The interplay between the non-trivial topology and the electron correlation contains many challenging problems, especially in three dimensions and on frustrated lattices. Topological insulators have both charge and spin degrees of freedom at the surface, while in frustrated Mott insulators a charge degree of freedom is frozen. Thus topological insulators and Mott insulators can be dis53
CHAPTER 5. SUMMARY AND FUTURE PROBLEMS
54
tinguished at the surface, in spite of the even number of electrons per unit cell. It is an important problem where the critical point is and how a spin degree of freedom (spinon) behaves. Note that Young et al. proposed the fractionalized QSH (or quantum spinon Hall) eect, in which spinons form edge modes [73]. The Kondo impurity and Kondo lattice in topological metals are another interesting problem. The study of Lu2 Ir2 O7 was considered as the rst step of these problems, in fact, Ln = Yb has one f -hole. We obtained a metal, but instead this problem can be approached by doping of magnetic elements to known STIs. The eective theory of one-dimensional helical liquids predicted that the conductance G is restored at T = 0 due to the formation of a Kondo singlet in the weak correlation region K > 1/4 (K is the Luttinger parameter), while G = 0 in the strong correlation region K < 1/4 [35]. This prediction makes us understand that helical liquids are completely dierent from usual TL liquids, though the behavior of two-dimensional helical liquids remains to be solved. Thus topological transition metal oxides will be developed in various directions.
Acknowledgement
I would like to express my sincere gratitude to my supervisor Professor Naoto Nagaosa for his kind advices and stimulating discussions. I am grateful to Doctor Hosho Katsura, Doctor XiaoLiang Qi, and Professor Shou-Cheng Zhang for their collaborations on Chapter 3 and Doctor Jan Kune on Chapter 4. I would acknowledge the experimental information by Takagi group, and s the computing resources by Tokura group. I would thank all the former and present members of Nagaosa group. Finally I would appreciate my family for their encouragement and support.
55
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Atsuo Shitade - Quantum Spin Hall Effect in Transition Metal Oxides

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Atsuo Shitade - Quantum Spin Hall Effect in Transition Metal Oxides

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Master thesis

Quantum spin Hall eect in transition metal oxides

Department of Applied Physics School of Engineering University of Tokyo

76505 Atsuo Shitade

5 Summary and future problems

Chapter 2 Some backgrounds

QH eect and the rst Chern number

n; k|Jx (k)|m; k m; k|Jy (k)|n; k (2.1) ,

n; k|Jx (k)|m; k m; k|Jy (k)|n; k (x y)

CHAPTER 2. SOME BACKGROUNDS

1 = 2 L where An (k) n; k|i leading to

is the Berry connection. At T = 0, n runs over occupied bands,

AD (k)]z n (2.5) dn (k).

Charge polarization and the rst Chern number

CHAPTER 2. SOME BACKGROUNDS

dt[At (t, ) At (t, )]

CHAPTER 2. SOME BACKGROUNDS

CHAPTER 2. SOME BACKGROUNDS

Theories of the SH eect in doped semiconductors

CHAPTER 2. SOME BACKGROUNDS

Experiments in doped semiconductors

CHAPTER 2. SOME BACKGROUNDS

CHAPTER 2. SOME BACKGROUNDS

CHAPTER 2. SOME BACKGROUNDS

CHAPTER 2. SOME BACKGROUNDS

CHAPTER 2. SOME BACKGROUNDS

TR polarization and the Z2 number

CHAPTER 2. SOME BACKGROUNDS

CHAPTER 2. SOME BACKGROUNDS

n+; k|(ik )|n+; k =

T n; k|ein (k) (ik )ein (k) |T n; k

[ n; k|ik |n; k k n (k)] = A (k)

CHAPTER 2. SOME BACKGROUNDS Then the TR polarization can be dened as

dk + A (k) + A+ (k) A (k) A (k) 2 (2.21)

We can easily see two useful formulas;

log det w(k) =i

[n (k) + n (k)] (2.23) n (k ),

CHAPTER 2. SOME BACKGROUNDS

det w(i ) Pf w(i )

QSH eect and the TR polarization

det w(i ) Pf w(i ) wmn (k) = m; k|T |n; k , i =

CHAPTER 2. SOME BACKGROUNDS

CHAPTER 2. SOME BACKGROUNDS

(0;001) (a) + + + (b) + + + +

CHAPTER 2. SOME BACKGROUNDS

CHAPTER 2. SOME BACKGROUNDS

CHAPTER 2. SOME BACKGROUNDS

Relativistic Mott insulator Sr2IrO4

CHAPTER 2. SOME BACKGROUNDS

octahedral crystalline field

CHAPTER 2. SOME BACKGROUNDS

CHAPTER 2. SOME BACKGROUNDS

CHAPTER 2. SOME BACKGROUNDS

Chapter 3 QSH eect in Na2IrO3

CHAPTER 3. QSH EFFECT IN NA2 IRO3

Transfer integrals to the NN sites

22 |H|A1g s A1g s|H|11 = d EA1g (pd) d p + (pp)

1 t2 1 |E1u u = 2 t2 1 |E1u v = t2 1 |A1u =0.

CHAPTER 3. QSH EFFECT IN NA2 IRO3

(pd)2 (pp) + (pp) d p d p

Transfer integrals to the NNN sites

CHAPTER 3. QSH EFFECT IN NA2 IRO3

atoms three p-orbitals). energy channel (pp) p , , p (pp) , , p + (pp) p + (pp)