A first-principles description of the spin Nernst effect, denoting the occurrence of a transverse spin current due to a temperature gradient, is presented. The approach, based on an extension to the Kubo-Streda equation for spin transport, supplies in particular the formal basis for investigations of diluted as well as concentrated alloys. Results for corresponding applications to the alloy system Au-Cu give the intrinsic and extrinsic contributions to the relevant transport coefficients. Using scaling laws allows in addition to split the extrinsic contribution into its skew scattering and side-jump parts.
A first-principles description of the spin Nernst effect, denoting the occurrence of a transverse spin current due to a temperature gradient, is presented. The approach, based on an extension to the Kubo-Streda equation for spin transport, supplies in particular the formal basis for investigations of diluted as well as concentrated alloys. Results for corresponding applications to the alloy system Au-Cu give the intrinsic and extrinsic contributions to the relevant transport coefficients. Using scaling laws allows in addition to split the extrinsic contribution into its skew scattering and sid…
In this study, we implemented a finite-difference algorithm for computing anomalous Hall and Nernst conductivity. Based on the expression to evaluate the Berry curvature in an insulating system [J. Phys. Soc. Jpn. 74 1674(2005)], we extended the methods to a metallic system. We calculated anomalous Hall conductivity and Nernst conductivity in a two-dimensional ferromagnetic material FeCl$_2$ and three-dimensional ferromagnetic transition metals bcc-Fe, hcp-Co, and fcc-Ni. Our results are comparable to previously reported results computed by Kubo-formula or Wannier representation. To evaluate a…
Thermoelectric properties of a model Skyrmion crystal were theoretically investigated, and it was found that its large anomalous Hall conductivity, corresponding to large Chern numbers induced by its peculiar spin structure leads to a large transverse thermoelectric voltage through the anomalous Nernst effect. This implies the possibility of finding good thermoelectric materials among Skyrmion systems, and thus motivates our quests for them by means of the first-principles calculations as were employed here.
The generation of spin and orbital currents is of crucial importance in the field of spin-orbitronics. In this work, using relativistic density functional theory and the Kubo linear-response formalism, we systematically investigate the spin Hall and orbital Hall effects for 40 monoatomic metals. The spin Hall conductivity (SHC) and orbital Hall conductivity (OHC) are computed as a function of the electrochemical potential and the influence of the spin-orbit interaction strength is also investigated. Our calculations predict a rather small OHC in $sp$ metals, but a much larger OHC in $d$-band m…
Anomalous Nernst effect generates a transverse voltage perpendicular to the temperature gradient. It has several advantages compared with the longitudinal thermoelectricity for energy conversion, such as decoupling of electronic and thermal transports, higher flexibility, and simpler lateral structure. However, a design principle beyond specific materials systems for obtaining a large anomalous Nernst conductivity (ANC) is still absent. In this work, we theoretically demonstrate that a pair of Dirac nodes under a Zeeman field manifests a double-peak anomalous Hall conductivity curve with respe…
We have performed systematic density functional calculations and evaluated thermoelectric properties, See- beck coefficient and anomalous Nernst coefficient of half-Heusler comounds CoMSb(M=Sc, Ti, V, Cr, and Mn). The carrier concentration dependence of Seebeck coefficients in nonmagnetic compounds are in good agreement with experimental values. We found that the half-metallic ferromagnetic CoMnSb show large anomalous Nernst effect originating from Berry curvature at the Brillouin zone boundary. These results help to understanding for the mechanism of large anomalous Nernst coefficient and giv…
Based on first-principles calculations, the anomalous Hall (AHC) and anomalous Nernst conductivities (ANC) of the XMnP (X=Ti, Zr, Hf) compounds were evaluated, and the possibility to tailor such properties by changing the magnetization directions was also investigated. We observed that nodal lines and small gap areas consist the dominant contributions to AHC and ANC, where the significant variations in AHC and ANC when altering the magnetization direction originate from the whole Brillouin zone. Our studies gave a promising clue on engineering magnetic intermetallic compounds for tunable trans…
Based on high-throughput first-principles calculations, we evaluated the anomalous Hall and anomalous Nernst conductivities of 266 transition-metal-based ferromagnetic compounds. Detailed analysis based on the symmetries and Berry curvatures reveals that the origin of singular-like behaviour of anomalous Hall/Nernst conductivities can be mostly attributed to the appearance of Weyl nodes or nodal lines located in the proximity of the Fermi energy, which can be further tailored by external stimuli such as biaxial strains and magnetic fields. Moreover, such calculations are enabled by the automat…
MnP and FeP are show complex magnetic spiral states with geometric phase contributions to the anomalous Hall effect and the topological Hall effect, where both have thermoelectric Nernst counterparts. We use state of the art first principle calculations to show that both Hall and Nernst effects are enhanced in MnP and FeP due to the temperature dependent magnetic texture. At ambient pressure the inversion breaking crystals shows a transition from a double-spiral helimagnetic phase to a topologically trivial magnetic phase. This helimagnetic structure is determined by exchange frustration and t…
Temperature gradient in a ferromagnetic conductor may generate a spontaneous transverse voltage drop in the direction perpendicular to both magnetization and heat current. This anomalous Nernst effect (ANE) has been considered to be proportional to the magnetization, and thus observed only in ferromagnets, while recent theories indicate that ANE provides a measure of the Berry curvature at the Fermi energy $E_{\rm F}$. Here we report the observation of a large ANE at zero field in the chiral antiferromagnet Mn$_3$Sn. Despite a very small magnetization $\sim 0.002$ $μ_{\rm B}/$Mn, the transvers…
Applying a temperature gradient in a magnetic material generates a voltage that is perpendicular to both the heat flow and the magnetization. This is the anomalous Nernst effect (ANE) which was thought to be proportional to the value of the magnetization for a long time. However, more generally, the ANE has been predicted to originate from a net Berry curvature of all bands near the Fermi level. Subsequently, a large anomalous Nernst thermopower has recently been observed in topological materials with no net magnetization but large net Berry curvature around E$_F$. These experiments clearly fa…
Ferrimagnetic Mn$_4$N is a promising material for heat flux sensors based on the anomalous Nernst effect (ANE) because of its sizable uniaxial magnetic anisotropy ($K_{\rm u}$) and low saturation magnetization ($M_{\rm s}$). We experimentally and theoretically investigated the ANE and anomalous Hall effect in sputter-deposited Mn$_4$N films. It was revealed that the observed negative anomalous Hall conductivity ($σ_{xy}$) could be explained by two different coexisting magnetic structures, that is, a dominant magnetic structure with high $K_{\rm u}$ contaminated by another structure with neglig…
Nodal-Surface and Flat-Band Driven Large Anomalous Nernst Effect in Epitaxial Ferromagnetic Weyl Metal Fe5Si3
Indian Institute of Technology Delhi（印度德里理工学院）；Indian Institute of Technology Hyderabad（印度海得拉巴理工学院）；National Institute for Materials Science（日本国立材料研究所）
In this article, we show fundamentals and recent advances on the transverse thermoelectric generation, in which a thermopower is generated in the direction perpendicular to an applied temperature gradient. Transverse thermoelectric generation is one of the central topics in condensed matter physics, and can be a breakthrough approach to solve long-standing technological problems with contact resistances in thermoelectric generators. We review here the six currently known driving mechanisms: the ordinary Nernst effect, the anomalous Nernst effect, goniopolar materials, the spin Seebeck effect, …
Simultaneous achievement of large anomalous Nernst effect and reduced thermal conductivity in sintered polycrystalline topological Heusler ferromagnets
The negative sign of the anomalous Nernst thermopower ($S_\text{ANE}$) observed in Mn-Ga ordered alloys is an attractive property for thermoelectric applications exploiting the anomalous Nernst effect (ANE); however, its origin has not been clarified. In this study, to gain insight into the negative $S_\text{ANE}$, we prepared epitaxial thin films of Mn$_{x}$Ga$_{100-x}$ with $x$ ranging from 56.2 to 71.7, and systematically investigated the structural, magnetic, and transport properties including the anomalous Hall effect (AHE) and the ANE. The measured $S_\text{ANE}$ is negative for all samp…
The anomalous Nernst effect (ANE), a thermoelectric phenomenon in magnetic materials, has potential for novel energy harvesting applications because its orthogonal relationship between the temperature gradient and the electric field enables us to utilize the large area of non-flat heat sources. In this study, the required thermopower of ANE for practical energy harvesting applications is evaluated in simulations of electric power obtainable from ANE using a low-temperature heat source. A strategy for finding magnetic materials having large ANEs is proposed, which suggests that a large ANE orig…
All-$d$ Heuslers are a category of novel compounds combining versatile functionalities such as caloric responses and spintronics with enhanced mechanical properties. Despite the promising transport properties (anomalous Hall (AHC) and anomalous Nernst (ANC) conductivities) shown in the conventional Co$_2$XY Heuslers with $p$-$d$ hybridization, the all-$d$ Heuslers with only $d$-$d$ hybridization open a new horizon to search for new candidates with outstanding transport properties. In this work, we evaluate the AHC and ANC for thermodynamically stable ferro/ferri-magnetic all-$d$-metal regular …
Since spin currents can be generated, detected, and manipulated via the spin Hall effect (SHE), the design of strong SHE materials has become a focus in the field of spintronics. Because of the recent experimental progress also the spin Nernst effect (SNE), the thermoelectrical counterpart of the SHE, has attracted much interest. Empirically strong SHEs and SNEs are associated with $d$-band compounds, such as transition metals and their alloys -- the largest spin Hall conductivity (SHC) in a $p$-band material is $\sim 450$ $\left(\hbar/e\right)\left(Ω\cdot cm\right)^{-1}$ for a Bi-Sb alloy, wh…
Motivated by the recent discovery of a large anomalous Nernst effect in Co$_2$MnGa, Fe$_3X$ ($X$=Al, Ga) and Co$_3$Sn$_2$S$_2$, we performed a first-principles study to clarify the origin of the enhancement of the transverse thermoelectric conductivity ($α_{ij}$) in these ferromagnets. The intrinsic contribution to $α_{ij}$ can be understood in terms of the Berry curvature ($Ω$) around the Fermi level, and $Ω$ is singularly large along nodal lines (which are gapless in the absence of the spin-orbit coupling) in the Brillouin zone. We find that not only the Weyl points but also stationary point…
Topological Lifshitz transition-induced bipolarity of anomalous Nernst effect in kagome magnet YCo3
Zhejiang University of Technology（浙江工业大学）；Hefei National Laboratory（合肥国家实验室）；Collaborative Innovation Center of Advanced Microstructures, Nanjing University（南京大学先进微结构协同创新中心）
The giant anomalous Hall and Nernst effects in Kagome permanent magnets RCo5
School of Physics & Astronomy and Center for Advanced Quantum Studies, Beijing Normal University（北京师范大学物理与天文学学院及先进量子研究中心）；Key Laboratory of Multiscale Spin Physics (Ministry of Education), Beijing Normal University（北京师范大学多尺度自旋物理教育部重点实验室）
The anomalous Nernst effect (ANE) - the generation of a transverse electric voltage by a longitudinal heat current in conducting ferromagnets or antiferromagnets - is an appealing approach for thermoelectric power generation in spin caloritronics. The ANE in antiferromagnets is particularly convenient for the fabrication of highly efficient and densely integrated thermopiles as lateral configurations of thermoelectric modules increase the coverage of heat source without suffering from the stray fields that are intrinsic to ferromagnets. In this work, using first-principles calculations togethe…
Exchange splitting as a descriptor for giant anomalous Hall and Nernst effects in ferromagnets
National Institute for Materials Science (NIMS)（物质材料研究机构）；Zhejiang Key Laboratory of Magnetic Materials and Applications, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences（中国科学院宁波材料技术与工程研究所磁材料与应用浙江省重点实验室）；Kyoto Institute of Technology（京都工艺纤维大学）
Utilizing the first-principles density functional theory calculations together with group theory analyses, we systematically investigate the spin order-dependent magneto-optical effect (MOE), anomalous Hall effect (AHE), and anomalous Nernst effect (ANE) in a recently discovered two-dimensional room-temperature ferromagnet $1T$-CrTe$_2$. We find that the spin prefers an in-plane direction by the magnetocrystalline anisotropy energy calculations. The MOE, AHE, and ANE display a period of $2π/3$ when the spin rotates within the atomic plane, and they are forbidden if there exists a mirror plane …
Influence of strain on the anomalous Hall and Nernst effects in Fe thin films
Graduate School of Science and Technology, University of Tsukuba（筑波大学科学技术研究科教）；Research Center for Magnetic and Spintronic Materials (CMSM), National Institute for Materials Science (NIMS)（物质材料研究机构磁性自旋材料研究中心）；Electronic Mechanical Engineering Department, National Institute of Technology, Oshima college（国立丰岛工业高等专门学校电子机械工程系）；Faculty of Electrical Engineering and Electronics, Kyoto Institute of Technology（京都工艺纤维大学电气电子学部）
Large Anomalous and Topological Hall Effect and Nernst Effect in a Dirac Kagome Magnet Fe3Ge
Ningbo University（宁波大学）；Michigan State University（密歇根州立大学）；Weizmann Institute of Science（魏茨曼科学研究所）；Oak Ridge National Laboratory（橡树岭国家实验室）；Zhejiang University of Technology（浙江工业大学）
Fe3Ge单晶表现出大异常霍尔效应和能斯特效应，其横向热电导率达4.6 A m^-1 K^-1，源于Dirac间隙的 Berry 曲率，同时拓扑霍尔电阻率和能斯特系数也显著，展示了动量和实空间中 Berry 阶段的联合影响。
Intrinsic Berry Curvature Driven Anomalous Hall and Nernst Effect in Co$_2$MnSn
Indian Institute of Technology Bombay（印度理工学院孟买分校）；Saha Institute of Nuclear Physics, A CI of Homi Bhabha National Institute（萨哈核物理研究所，霍米·巴巴国立学院成员机构）；University of South Florida（南佛罗里达大学）；Technical University of Denmark（丹麦技术大学）；Università di Cagliari（卡利亚里大学）；Pennsylvania State University（宾夕法尼亚州立大学）
Kagome metal TbMn6Sn6 was recently discovered to be a ferrimagnetic topological Dirac material by scanning tunneling microscopy/spectroscopy measurements. Here, we report the observation of large anomalous Nernst effect and anomalous thermal Hall effect in this compound. The anomalous transverse transport is consistent with the Berry curvature contribution from the massive Dirac gaps in the 3D momentum space as demonstrated by our first-principles calculations. Furthermore, the transverse thermoelectric transport exhibits asymmetry with respect to the applied magnetic field, i.e., an exchange-…
Materials exhibiting controllable magnetic phase transitions are currently in demand for many spintronics applications. Here we investigate from first principles the electronic structure and intrinsic anomalous Hall, spin Hall and anomalous Nernst response properties of the FeRh metallic alloy which undergoes a thermally driven antiferromagnetic-to-ferromagnetic phase transition. We show that the energy band structures and underlying Berry curvatures have important signatures in the various Hall effects. Specifically, the suppression of the anomalous Hall and Nernst effects in the AFM state an…
The electric and thermo-magneto-electric transport of the prototypical ferromagnetic transition-metal alloy system fcc-Co$_x$Pd$_{1-x}$ has been investigated on the basis of Kubo's linear response formalism. The results for the full electric conductivity tensor allow to discuss the spin-orbit induced anisotropic magneto-resistance (AMR) and the anomalous Hall effect (AHE). These are complemented by results for the corresponding thermo-magneto-electric transport properties anisotropy of the Seebeck effect (ASE) and anomalous Nernst effect (ANE). The relation between the respective response coef…
Utilizing the first-principles calculations together with the group theory analysis, we systematically investigate the magnetocrystalline anisotropy energy, magneto-optical effect, and anomalous transport properties (including anomalous Hall, Nernst, and thermal Hall effects) of monolayer and bilayer Fe$_n$GeTe$_2$ ($n$ = 3, 4, 5). The monolayer Fe$_n$GeTe$_2$ ($n$ = 3, 4, 5) exhibits the out-of-plane, in-plane, and in-plane ferromagnetic orders with considerable magnetocrystalline anisotropy energies of -3.17, 4.42, and 0.58 meV/f.u., respectively. Ferromagnetic order is predicted in bilayer …
Transverse thermoelectric devices produce electric fields perpendicular to an incident heat flux. Classically, this process is driven by the Nernst effect in bulk solids, wherein a magnetic field generates a Lorentz force on thermally excited electrons. The spin Seebeck effect (SSE) also produces magnetization-dependent transverse electric fields. SSE is traditionally observed in thin metallic films deposited on electrically insulating ferromagnets, but the films' high resistance limits thermoelectric conversion efficiency. Combining Nernst and SSE in bulk materials would enable devices with s…
Co-based shandite Co$_3$Sn$_2$S$_2$ is a representative example of magnetic Weyl semimetals showing rich transport phenomena. We thoroughly investigate magnetic and transport properties of hole-doped shandites Co$_3$In$_x$Sn$_{2-x}$S$_2$ by first-principles calculations. The calculations reproduce nonlinear reduction of anomalous Hall conductivity with doping In for Co$_3$Sn$_2$S$_2$, as reported in experiments, against the linearly decreased ferromagnetic moment within virtual crystal approximation. We show that a drastic change in the band parity character of Fermi surfaces, attributed to th…
Using the model of classical Heisenberg exchange and Dzyaloshinskii-Moriya (DM) interaction we show that the ground state of B20 FeGe chiral magnet is a superposition of twisted helical spin-density waves formed by different sublattices of the crystal. Such twisted spin-density waves propagate in the same direction but with different phases and different directions of the rotation axes. We derive an advanced micromagnetic expression describing the exchange and DM interaction for such magnetic structures. By employing first-principles calculations based on density functional theory and using ou…
A tight-binding model is fit to first-principles calculations for copper that include structures distorted according to elastic constants and high-symmetry phonon modes. With the resulting model the first-principles-based phonon dispersion and the free energy are calculated in the quasi-harmonic approximation. The resulting thermal expansion, the temperature- and volume-dependence of the elastic constants, the Debye temperature, and the Gruneisen parameter are compared with available experimental data.
We present a first-principles description of anisotropic materials characterized by having both weak (dispersion-like) and strong covalent bonds, based on the Adiabatic--Connection Fluctuation--Dissipation Theorem within Density Functional Theory. For hexagonal boron nitride the in-plane and out of plane bonding as well as vibrational dynamics are well described both at equilibrium and when the layers are pulled apart. Also bonding in covalent and ionic solids is described. The formalism allows to ping-down the deficiencies of common exchange-correlation functionals and provides insight toward…
The description of the molecular solid phase of O$_2$, especially its ground-state antiferromagnetic insulating phase, is known to be quite unsatisfactory within the conventional local and semilocal density functional approximations used in the Kohn-Sham formalism of density functional theory. The recently-developed van der Waals functionals that take into account nonlocal correlations have also shown subpar performance in this regard. The difficulty lies in the subtle balance between the van der Waals interactions and the exchange coupling between the antiferromagnetic and ferromagnetic molec…
Recently, the two-dimensional magnetic semiconductor CrSBr has attracted considerable attention due to its excellent air-stable property and high magnetic critical temperature. Here, we systematically investigate the electronic structure, magnetocrystalline anisotropy energy, first-order magneto-optical effects (Kerr and Faraday effects) and second-order magneto-optical effects (Schafer-Hubert and Voigt effects) as well as intrinsically anomalous transport properties (anomalous Hall, anomalous Nernst, and anomalous thermal Hall effects) of two-dimensional van der Waals layered magnets CrXY (X …
Phenomenological orbital-polarization (OP) terms have been repeatedly introduced in the single-particle equations of spin-density-functional theory, in order to improve the description of orbital magnetic moments in systems containing transition metal ions. Here we show that these ad hoc corrections can be interpreted as approximations to the exchange-correlation vector potential A_xc of current-density-functional theory (CDFT). This connection provides additional information on both approaches: Phenomenological OP terms are connected to first-principles theory, leading to a rationale for thei…
Modeling the high-$T$ paramagnetic state of bulk UO$_2$ by a non-spin-polarized calculation and neglecting the Hubbard-U correction for the $f$ electrons in U atoms, the lattice thermal conductivity of bulk UO$_2$ is investigated by the exact solution of the Boltzmann transport equation for the steady-state phonon distribution function. The results show that TA branches corresponding to U-atoms vibrations have the largest lifetimes and therefore have dominant role in thermal conductivity, while the optical branches corresponding mainly to O-atoms vibrations have the shortest lifetimes. Using t…
We examine the influence of the main approximations employed in density-functional theory descriptions of the solid phase of molecular hydrogen near dissociation. We consider the importance of nuclear quantum effects on equilibrium properties and find that they strongly influence intramolecular properties, such as bond fluctuations and stability. We demonstrate that the combination of both thermal and quantum effects make a drastic change to the predicted optical properties of the molecular solid, suggesting a limited value to dynamical, e.g., finite-temperature, predictions based on classical…
A general approach to calculate the diabatic surfaces for electron-transfer reactions is presented, based on first-principles molecular dynamics of the active centers and their surrounding medium. The excitation energy corresponding to the transfer of an electron at any given ionic configuration (the Marcus energy gap) is accurately assessed within ground-state density-functional theory via a novel penalty functional for oxidation-reduction reactions that appropriately acts on the electronic degrees of freedom alone. The self-interaction error intrinsic to common exchange-correlation functiona…
Using a combination of density-functional perturbation theory and the itinerant coherent potential approximation, we study the effects of atomic relaxation on the inelastic incoherent neutron scattering cross sections of disordered Ni$_{50}$Pt$_{50}$ alloys. We build on previous work, where empirical force constants were adjusted {\it ad hoc} to agree with experiment. After first relaxing all structural parameters within the local-density approximation for ordered NiPt compounds, density-functional perturbation theory is then used to compute phonon spectra, densities of states, and the force c…
