Magnetoresistive effects are powerful tools for studying the intricate structure of solid state electronic systems, and have many applications in our current information technology. In particular, the electronic system reflects the crystal symmetry and the orbital structure of the atoms of a given solid, and thus is crucial to understanding magnetism, superconductivity and many other effects which are of key interest to current solid state research. Consequently, studies of the electrical transport properties of solid state matter allow to evaluate this imprint and in turn draw conclusions about the interactions within a material. In this thesis, we will exploit the capabilities of magnetotransport measurements to infer the properties of a multitude of magnetic systems. In turn, this allows us to push the understanding of transport phenomena in magnetic materials. The first part of this work is focused on the magnetoresistance observed in spin Hall active metals in contact with a magnetic insulator. In such bilayers, the interfacial spin accumulation caused by the spin Hall effect in the metal can interact with the magnetic insulator, giving rise to interesting magnetoresistive effects. In the framework of this thesis, bilayers with several magnetic insulators are studied, including antiferomagnets, ferrimagnets and paramagnets (disordered magnets). For the disordered magnetic insulators, we find that the established spin Hall magnetoresistance framework does not allow to consistently describe the observed transport response. Consequently, we propose an alternative explanation of the magnetoresistance in such heterostructures, using the Hanle magnetoresistance and assuming an interface which has a finite electrical conductivity. This alternative model can serve to generalize the theory of the spin Hall magnetoresistance, providing addition information on the microscopic picture for the loss of the transverse spin component. Additionally, by partly removing the magnetic insulator and studying the ensuing changes, we verify that magnons are crucial for the observation of a non-local magnetoresistance in bilayers of a magnetic insulator and a metal. Finally, the local and non-local spin Seebeck effect (i.e. the electric field generated by a thermally driven pure spin current) is investigated in bilayers of Cr2O3 and Pt where the occurrence of a spin superfluid ground state was reported. In our sample, however, the transport response is consistent with the antiferromagnetic spin Seebeck effect mediated by the small magnetic field induced magnetization also reported for other antiferromagnet/metal heterostructures. As such, we cannot verify the presence of a spin superfluid ground state in the system. In the second part of this thesis, the topological properties of the electronic system and the related changes of the magnetoelectric and magnetothermal transport response are investigated. To that end, we first demonstrate a novel measurement technique, the alternating thermal gradient technique, allowing to separate the relevant thermovoltages from spurious other voltages generated within the measurement setup. We employ this novel technique for measuring the topological Nernst effect in Mn 1.8 PtSn and show the possibility to combine the magnetoelectric and magnetothermal transport response to evaluate the presence of topological transport signatures without requiring magnetization measurements. Additionally, we show that the anomalous Nernst effect in the non-collinear antiferromagnet Mn3Sn is connected to the antiferromagnetic domain structure: Using spatially resolved measurements of the anomalous Nernst effect, direct access to the antiferromagnetic domain structure is demonstrated. Additionally, a thermally assisted domain writing scheme is implemented, allowing the preparation of Mn3Sn into a defined antiferromagnetic domain state.

A partir da teoria de resposta linear (formalismo de Kubo) calculamos a condutividade de spin $\\sigma_^$ para um gás bidimensional de elétrons formado num poço quântico com duas subbandas devido a atuação de um novo tipo de interação spin-órbita [Bernardes et al. \\textit{Phys. Rev. Lett.} \\textbf, 076603 (2007) \\& Calsaverini \\textit{et al}. \\textit{Phys. Rev. B} \\textbf, 155313 (2008)]. Este novo termo é não-nulo mesmo em estruturas simétricas e surge devido ao acoplamento entre os estados confinados no poço de paridades diferentes. Encontramos um valor para $\\sigma_^$ não-nulo e não-universal (dependente da intensidade do acoplamento $\\eta$) quando somente uma das subbandas está ocupada, ao contrário de Rashba. Para encontrarmos valores realistas para $\\sigma_^$, determinamos $\\eta$ via cálculo autoconsistente. Esse cálculo é executado para diferentes valores de densidade eletrônica em poços simples e duplos. Obtivemos que $\\sigma_^$ possui um comportamento não-monótono e sofre inversão de sinal como função da energia de Fermi (densidade de elétrons) conforme ela varia entre as duas subbandas. Contudo nossos resultados indicam que a condutividade Hall de spin é muito pequena $\\left(``\\ll \\frac{8\\pi}\"ight)$ nesses sistemas (poços simples e duplos) e possivelmente não mensurável. / Using the Kubo linear response theory, we investigate spin Hall conductivity $\\sigma_^$ in a two-dimensional electron gas in quantum wells with two subbands, when intersubband-induced spin-orbit coupling is operative [Bernardes et al. \\textit{Phys. Rev. Lett.} \\textbf, 076603 (2007) \\& Calsaverini \\textit{et al}. \\textit{Phys. Rev. B} \\textbf, 155313 (2008)]. This new spin-orbit term is non-zero even in symmetric structures and it arises from the distinct parity of the confined states. We find non-zero and non-universal $\\sigma_^$ (dependent on spin-orbit coupling strength $\\eta$) when only one of the subbands is occupied. This is in contrast to the Rashba spin-orbit interaction for which $\\sigma_^$ is identically zero. To obtain realistic values for $\\sigma_^$, we develop a self-consistent scheme to calculate $\\eta$. We performed this calcultion for different values of the eletronic density in single and double wells. We find that $\\sigma_^$ shows a non-monotonic behavior and a sign change as the Fermi energy (carrier density) varies between the two subband edges. However, our results indicate that $\\sigma_^$ is extremely small $\\left(``\\ll \\frac{8\\pi}\"ight)$ and possibly not measurable.

The emerging field of spintronics relies on the manipulation of electron spin in order to use it in spin-based electronics. Such a paradigm change has to tackle several challenges including finding materials with sufficiently long spin lifetimes and materials which are efficient in generating pure spin currents. This thesis predicts that two types of material families could be a solution to the aforementioned challenges: complex oxides and bismuth based materials. We derived a general approach for constructing an effective spin-orbit Hamiltonian which is applicable to all nonmagnetic materials. This formalism is useful for calculating spin-dependent properties near an arbitrary point in momentum space. We also verified this formalism through comparisons with other approaches for III-V semiconductors, and its general applicability is illustrated by deriving the spin-orbit interaction and predicting spin lifetimes for strained SrTiO3 and a two-dimensional electron gas in SrTiO3 (such as at the LaAIO3/SrTiO3 interface). Our results suggest robust spin coherence and spin transport properties in SrTiO3 related materials even at room temperature. In the second part of the study we calculated intrinsic spin Hall conductivities for bismuth-antimony Bi1-xSbx semimetals with strong spin-orbit couplings, from the Kubo formula and using Berry curvatures evaluated throughout the Brillouin zone from a tight-binding Hamiltonian. Nearly crossing bands with strong spin-orbit interaction generate giant spin Hall conductivities in these materials, ranging from 474 ((ћ/e)Ω-1cm-1) for bismuth to 96((ћ/e)Ω-1cm-1) for antimony; the value for bismuth is more than twice that of platinum. The large spin Hall conductivities persist for alloy compositions corresponding to a three-dimensional topological insulator state, such as Bi0.83Sb0.17. The spin Hall conductivity could be changed by a factor of 5 for doped Bi, or for Bi0.83Sb0.17, by changing the chemical potential by 0.5 eV, suggesting the potential for doping or voltage tuned spin Hall current. We have also calculated intrinsic spin Hall conductivities of Bi2Se3 and Bi2Te3 topological insulators from an effective tight-binding Hamiltonian including two nearest-neighbor interactions. We showed that both materials exhibit giant spin Hall conductivities calculated from the Kubo formula in linear response theory and the clean static limit. We conclude that bismuth-antimony alloys and bismuth chalcogenides are primary candidates for efficiently generating spin currents through the spin Hall effect.

In recent years, Spin Seebeck effect (SSE) emerges as one of the efficient and easiest ways to generate pure spin current for spintronics devices. In this dissertation, we have systematically studied the SSE and related phenomena like spin Hall magneto-resistance (SMR), anomalous Nernst effect (ANE) in functional magnetic oxides for both fundamental understanding of their origins and practical ways to apply into technological devices. The research has been performed on three different systems of topical interest: (i) Y3Fe5O12 (YIG)/Pt and YIG/C60/Pt, (ii) CoFe2O4 (CFO)/Pt and CFO/C60/Pt, and (iii) Nd0.6Sr0.4MnO3 (NSMO). In case of the YIG/Pt structure, we have achieved a new consensus regarding the temperature dependence of the longitudinal SSE (LSSE). For the first time, we have demonstrated the temperature dependence of LSSE in association with the magnetocrystalline anisotropy (HK) and surface perpendicular magnetic anisotropy field (HKS) of YIG in the same YIG/Pt system. We show that on lowering temperature, the sharp drop in LSSE signal (VLSSE) and the sudden increases in HK and HKS at ~175 K are associated with the spin reorientation due to single ion anisotropy of Fe2+ ions. The VLSSE peak at ~75 K is attributed to the HKS and MS (saturation magnetization) whose peaks also occur at the same temperature. The effects of surface and bulk magnetic anisotropies are corroborated with those of thermally excited magnon number and magnon propagation length to satisfactorily explain the temperature dependence of LSSE in the Pt/YIG system. As a new way to reduce conductivity mismatch, promote spin transport, and tune the spin mixing conductance (G) at the YIG/Pt interface, we have deposited an organic semiconductor (OSC), C60, between ferrimagnetic material (FM) and Pt. Transverse susceptibility study on YIG/C60/Pt has shown that the deposition of C60 has reduced HKS at the surface of YIG significantly, due to the hybridization between the dz2 orbital in Fe and C atoms, leading to the overall increase in spin moments and G and consequently the LSSE. Upon lowering temperature from 300 K, we have observed an exponential increase in LSSE at low temperature (a ~800% increment at 150 K) in this system, which is attributed to the exponential increase in the spin diffusion length of C60 at low temperature. On the other hand, similar experiments on CoFe2O4 (CFO)/C60/Pt show a reduction in the LSSE signal at room temperature, due to the hybridization between the dz2 orbital in Co and C atoms that results in the increased magnetic anisotropy. Upon decreasing the temperature below 150 K, we have interestingly observed that LSSE signal from CFO/C60/Pt exceeds that of CFO/Pt and increases remarkably with temperature. This finding confirms the important role played by the spin diffusion length of C60 in enhancing the LSSE. A systematic study of SMR, SSE, and HKS on the YIG/Pt system using the same YIG single crystal has revealed a low-temperature peak at the same temperature (~75 K) for all the phenomena. Given the distinct origins of the SSE and SMR, our observation points to the difference in spin states between the bulk and surface of YIG as the main reason for such a low-temperature peak, and suggests that the ‘magnon phonon drag’ theory developed to explain the temperature-dependent SSE behavior should be adjusted to include this important effect. SSE and ANE studies on NSMO films have revealed the dominance of ANE over SSE in this class of perovskite-structured materials. The substrate-dependent study of the films shows that compressive strain developed due to the large lattice mismatch from LAO gives rise to the enhanced ANE signal. On the same substrate, ANE signal strength increases as the thickness increases. A sign change in ANE has been observed at a particular temperature, which explains that the Anomalous Hall effect (AHE) and ANE in these systems arise due to intrinsic scattering mechanisms. Overall, we have performed the SSE and related studies on the three important classes of functional magnetic oxide materials. We demonstrate the important role of magnetic anisotropy in manipulating the SSE in these systems. With this knowledge, we have been able to design the novel YIG/C60/Pt and CFO/C60/Pt heterostructures that exhibit the giant SSEs. The organic semiconductor C60 has been explored for the first time as a means of controlling pure spin current in inorganic magnetic oxide/metal heterostructures, paying the way for future spintronic materials and devices.

The lateral spatial separation between the circular polarization components of a linearly polarized light beam impinging at off-normal incidence on an air-semiconductor interface is investigated experimentally and theoretically. This fundamental optical phenomenon is referred to as the Spin Hall effect of light (SHEL). An optical pump-probe technique is demonstrated to resolve in situ the nanometer size SHEL displacement of a beam transmitted inside an absorptive material. Three different types of optical interactions in silicon and GaAs demonstrate the technique’s general applicability. First, resonant ∼150 fs pump and probe pulses at λ = 820 nm resolve the SHEL displacement via free-carrier absorption in a 10 μm thick silicon sample. The measured SHEL displacements for a p-polarized probe beam are obtained between −10 to 150 nm as a function of the angle of incidence on the sample. Different angles of incidence are achieved by keeping a fixed angular separation between the pump and the probe beams while rotating the sample about the axis perpendicular to the plane of incidence. In another experiment, an optically thin (500 nm thick) GaAs sample allows one to use Pauli-blocking as an optical interaction to investigate the polarization and angular dependence of the SHEL in the probe beam. For such a polarization-dependent imaging technique, the SHEL displacement in the pump beam also contributes to the measured signal and is evaluated experimentally. A probe beam at normal incidence is used to measure a SHEL displacement of ∼180 nm in a transmitted p-polarized pump beam impinging on the sample with an angle of incidence of 55 degrees. Finally, two-photon absorption is used to resolve the SHEL in a (001) oriented 500 μm thick GaAs wafer using an optical source generating sub-bandgap radiation (λ = 1550 nm) with a pulse duration of 120 fs. Linearly p- and s- co-polarized pump and probe beams are also used to investigate the polarization dependence of the SHEL. All the experimental results obtained using these different optical interactions agree with the theory within the experimental error. Finally, analytical expressions of the shifts experienced by the circular components of a beam impinging at an interface between two optical media are also derived for an incident beam with an arbitrary spatial distribution.

The lateral spatial separation between the circular polarization components of a linearly polarized light beam impinging at off-normal incidence on an air-semiconductor interface is investigated experimentally and theoretically. This fundamental optical phenomenon is referred to as the Spin Hall effect of light (SHEL). An optical pump-probe technique is demonstrated to resolve in situ the nanometer size SHEL displacement of a beam transmitted inside an absorptive material. Three different types of optical interactions in silicon and GaAs demonstrate the technique’s general applicability. First, resonant ∼150 fs pump and probe pulses at λ = 820 nm resolve the SHEL displacement via free-carrier absorption in a 10 μm thick silicon sample. The measured SHEL displacements for a p-polarized probe beam are obtained between −10 to 150 nm as a function of the angle of incidence on the sample. Different angles of incidence are achieved by keeping a fixed angular separation between the pump and the probe beams while rotating the sample about the axis perpendicular to the plane of incidence. In another experiment, an optically thin (500 nm thick) GaAs sample allows one to use Pauli-blocking as an optical interaction to investigate the polarization and angular dependence of the SHEL in the probe beam. For such a polarization-dependent imaging technique, the SHEL displacement in the pump beam also contributes to the measured signal and is evaluated experimentally. A probe beam at normal incidence is used to measure a SHEL displacement of ∼180 nm in a transmitted p-polarized pump beam impinging on the sample with an angle of incidence of 55 degrees. Finally, two-photon absorption is used to resolve the SHEL in a (001) oriented 500 μm thick GaAs wafer using an optical source generating sub-bandgap radiation (λ = 1550 nm) with a pulse duration of 120 fs. Linearly p- and s- co-polarized pump and probe beams are also used to investigate the polarization dependence of the SHEL. All the experimental results obtained using these different optical interactions agree with the theory within the experimental error. Finally, analytical expressions of the shifts experienced by the circular components of a beam impinging at an interface between two optical media are also derived for an incident beam with an arbitrary spatial distribution.

京都大学 / 新制・課程博士 / 博士(工学) / 甲第23907号 / 工博第4994号 / 新制||工||1780(附属図書館) / 京都大学大学院工学研究科電子工学専攻 / (主査)教授 白石 誠司, 教授 竹内 繁樹, 准教授 浅野 卓 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DFAM

A partir da teoria de resposta linear (formalismo de Kubo) calculamos a condutividade de spin $\\sigma_^$ para um gás bidimensional de elétrons formado num poço quântico com duas subbandas devido a atuação de um novo tipo de interação spin-órbita [Bernardes et al. \\textit{Phys. Rev. Lett.} \\textbf, 076603 (2007) \\& Calsaverini \\textit{et al}. \\textit{Phys. Rev. B} \\textbf, 155313 (2008)]. Este novo termo é não-nulo mesmo em estruturas simétricas e surge devido ao acoplamento entre os estados confinados no poço de paridades diferentes. Encontramos um valor para $\\sigma_^$ não-nulo e não-universal (dependente da intensidade do acoplamento $\\eta$) quando somente uma das subbandas está ocupada, ao contrário de Rashba. Para encontrarmos valores realistas para $\\sigma_^$, determinamos $\\eta$ via cálculo autoconsistente. Esse cálculo é executado para diferentes valores de densidade eletrônica em poços simples e duplos. Obtivemos que $\\sigma_^$ possui um comportamento não-monótono e sofre inversão de sinal como função da energia de Fermi (densidade de elétrons) conforme ela varia entre as duas subbandas. Contudo nossos resultados indicam que a condutividade Hall de spin é muito pequena $\\left(``\\ll \\frac{8\\pi}\"ight)$ nesses sistemas (poços simples e duplos) e possivelmente não mensurável. / Using the Kubo linear response theory, we investigate spin Hall conductivity $\\sigma_^$ in a two-dimensional electron gas in quantum wells with two subbands, when intersubband-induced spin-orbit coupling is operative [Bernardes et al. \\textit{Phys. Rev. Lett.} \\textbf, 076603 (2007) \\& Calsaverini \\textit{et al}. \\textit{Phys. Rev. B} \\textbf, 155313 (2008)]. This new spin-orbit term is non-zero even in symmetric structures and it arises from the distinct parity of the confined states. We find non-zero and non-universal $\\sigma_^$ (dependent on spin-orbit coupling strength $\\eta$) when only one of the subbands is occupied. This is in contrast to the Rashba spin-orbit interaction for which $\\sigma_^$ is identically zero. To obtain realistic values for $\\sigma_^$, we develop a self-consistent scheme to calculate $\\eta$. We performed this calcultion for different values of the eletronic density in single and double wells. We find that $\\sigma_^$ shows a non-monotonic behavior and a sign change as the Fermi energy (carrier density) varies between the two subband edges. However, our results indicate that $\\sigma_^$ is extremely small $\\left(``\\ll \\frac{8\\pi}\"ight)$ and possibly not measurable.

The impact of the spin degree of freedom on the transport properties of electrons traveling through magnetic materials has been known since the pioneer work of Mott [1]. Since then it has been demonstrated that the spin angular momentum plays a key role in the scattering process of electrons in magnetic multilayers. This role has been emphasized by the discovery of the Giant Magnetoresistance in 1988 by Fert and Grunberg [2, 3]. Among the numerous applications and effects that emerged in mesoscopic devices two mechanisms have attracted our attention during the course of this thesis: the spin transfer torque and the spin Hall effects. The former consists in the transfer of the spin angular momentum from itinerant carriers to local magnetic moments [4]. This mechanism results in the current-driven magnetization switching and excitations, which has potential application in terms of magnetic data storage and non-volatile memories. The latter, spin Hall effect, is considered as well to be one of the most fascinating mechanisms in condensed matter physics due to its ability of generating non-equilibrium spin currents without the need for any magnetic materials. In fact the spin Hall effect relies only on the presence of the spin-orbit interaction in order to create an imbalance between the majority and minority spins. The objective of this thesis is to investigate the impact of disorder on spin dependent transport phenomena. To do so, we identified three classes of systems on which such disorder may have a dramatic influence: (i) antiferromagnetic materials, (ii) impurity-driven spin-orbit coupled systems and (iii) two dimensional semiconducting electron gases with Rashba spin-orbit coupling. Antiferromagnetic materials - We showed that in antiferromagnetic spin-valves, spin transfer torque is highly sensitive to disorder, which prevents its experimental observation. To solve this issue, we proposed to use either a tunnel barrier as a spacer or a local spin torque using spin-orbit coupling. In both cases, we demonstrated that the torque is much more robust against impurities, which opens appealing venues for its experimental observation. Extrinsic spin-orbit coupled systems - In disordered metals accommodating spin orbit coupled impurities, it is well-known that spin Hall effect emerges due to spin dependent Mott scattering. Following a recent prediction, we showed that another effect coexists: the spin swapping effect, that converts an incoming spin current into another spin current by "swapping" the momentum and spin directions. We showed that this effect can generate peculiar spin torque in ultrathin magnetic bilayers. Semiconductors spintronics - This last field of research has attracted a massive amount of hope in the past fifteen years, due to the ability of coherently manipulating the spin degree of freedom through interfacial, so-called Rashba, spin-orbit coupling. However, numerical simulations failed reproducing experimental results due to coherent interferences between the very large number of modes present in the system. We showed that spin-independent disorder can actually wash out these interferences and promote the conservation of the spin signal. In the course of this PhD, we showed that while disorder-induced dephasing is usually detrimental to the transmission of spin information, in selected situation, it can actually promote spin transport mechanisms and participate to the enhancement of the desired spintronics phenomenon.

Functional materials are essential to human welfare and to provide foundations for emerging industries. As an alternative route to experimental materials discovery, computational materials designs are playing an increasingly significant role in the whole discovery process. In this work, we use an in-house developed python utility: PAOFLOW, which generates finite basis Hamiltonians from the projection of first principles plane-wave pseudopotential wavefunctions on pseudo atomic orbitals(PAO) for post-process calculation on various properties such as the band structures, density of states, complex dielectric constants, diffusive and anomalous spin and charge transport coefficients. In particular, we calculated the dielectric function of Sr-, Pb-, and Bi-substituted BaSnO3 over wide concentration ranges. Together with some high-throughput experimental study, our result indicates the importance of considering the mixed-valence nature and clustering effects upon substitution of BaSnO3 with Pb and Bi. We also studied two prototype ferroelectric rashba semiconductors, GeTe and SnTe, and found the spin Hall conductivity(SHC) can be large either in ferroelectric or paraelectric structure phase. Upon doping, the polar displacements in GeTe can be sustained up to a critical hole concentration while the tiny distortions in SnTe vanish at a minimal level of doping. Moreover, we investigated the sensitivity of two dimensional group-IV monochalcogenides to external strain and doping, which reveal for the first time giant intrinsic SHC in these materials, providing a new route for the design of highly tunable spintronics devices based on two-dimensional materials.