Phonon Hall effect (PHE) has attracted a lot of attention in recent years with many theoretical and experimental explorations published. While experiments work on complicated materials, theoretical studies are still hovering around the phenomenon-based models. Moreover, previous microscopic theory was found unable to explain large thermal Hall conductivity obtained by experiments in strontium titanate (STO). Therefore, as a first attempt to bridge this gap, we implement first-principles calculations to explore the PHE in real materials. Our work provides a new benchmark of the PHE in sodium chloride (NaCl) under a large external magnetic field. Moreover, we demonstrate our results in barium titanate (BTO), and discuss the results in STO in detail about their deviation from experiments. As a possible future direction, we further propose that the inner electronic Berry curvature plays an important role in the PHE in STO.
Berry curvature (BC) governs topological phases of matter and generates anomalous transport. When a magnetic field is applied, phonons can acquire BC indirectly through spin-lattice coupling, leading to a linear phonon Hall effect. Here, we show that polar lattice distortion directly couples to a phonon BC dipole, which causes a switchable non-linear phonon Hall effect. In a SnS monolayer, the in-plane ferroelectricity induces a phonon BC and leads to the phononic version of the non-volatile BC memory effect. As a new type of ferroelectricity-phonon coupling, the phonon Rashba effect emerges a…
Since the first experimental observation of the phonon Hall effect (PHE) in 2005, its physical origin and theoretical explanation have been extensively investigated. While spin-orbit interactions are believed to play important roles under external magnetic fields, nonmagnetic effects are also possible. Here, we propose a mechanism of PHE which is induced by electric current in a nonequilibrium system through electron-phonon interactions. The influence of the drift electrons to the phonon degrees of freedom, as a correction to the Born-Oppenheimer approximation, is represented by an antisymmetr…
Valley Hall effect is an appearance of the valley current in the direction transverse to the electric current. We develop the microscopic theory of the valley Hall effect in two-dimensional semiconductors where the electrons are dragged by the phonons or photons. We derive and analyze all relevant contributions to the valley current including the skew-scattering effects together with the anomalous contributions caused by the side-jumps and the anomalous velocity. The partial compensation of the anomalous contributions is studied in detail. The role of two-phonon and two-impurity scattering pro…
We generalize the notion of dissipationless, topological Hall viscosity tensor to optical phonons in thin film Weyl semimetals. By using the strained Porphyrin thin film Weyl semimetal as a model example, we show how optical phonons can couple to Weyl electrons as chiral pseudo gauge fields. These chiral vector fields lead to a novel dissipationless two-rank viscosity tensor in the effective dynamics of optical phonons whose origin is the chiral anomaly. We also compute the contribution to this two rank Hall viscosity tensor due to the presence of an external magnetic field, whose origin is th…
A mechanism for phonon Hall effect (PHE) in non-magnetic insulators under an external magnetic field is theoretically studied. PHE is known in (para)magnetic compounds, where the magnetic moments and spin-orbit interaction play an essential role. In sharp contrast, we here show that a non-zero Berry curvature of acoustic phonons is induced by an external magnetic field due to the correction to the adiabatic Born-Oppenheimer approximation. This results in the finite thermal Hall conductivity $κ_H$ in nonmagnetic band insulators. Our estimate of $κ_H$ for a simple model gives $κ_H \sim 1.0\times…
We establish the general phonon dynamics of magnetic solids by incorporating the Mead-Truhlar correction in the Born-Oppenheimer approximation. The effective magnetic-field acting on the phonons naturally emerges, giving rise to the phonon Hall effect. A general formula of the intrinsic phonon Hall conductivity is obtained by using the corrected Kubo formula with the energy magnetization contribution incorporated properly. The resulting phonon Hall conductivity is fully determined by the phonon Berry curvature and the dispersions. Based on the formula, the topological phonon system could be ri…
We provide a topological understanding on phonon Hall effect in dielectrics with Raman spinphonon coupling. A general expression for phonon Hall conductivity is obtained in terms of the Berry curvature of band structures. We find a nonmonotonic behavior of phonon Hall conductivity as a function of magnetic field. Moreover, we observe a phase transition in phonon Hall effect, which corresponds to the sudden change of band topology, characterized by the altering of integer Chern numbers. This can be explained by touching and splitting of phonon bands.
Spin Hall effect is the transverse flow of the electron spin in conductors under external electric field. Similarly, thermal gradient in magnetic insulators can drive a transverse flow of the spin angular momentum of magnons, which provides a thermal alternative for spin manipulation. Recently, the phonon angular momentum (PAM), which is the angular momentum of atoms as a result of their orbital motion around their equilibrium positions, has garnered attention as a quantity analogous to the magnon spin. However, can we manipulate PAM like magnon spin? Here, we show that temperature gradient ge…
We present a systematic theory of the phonon Hall effect in a ballistic crystal lattice system, and apply it on the kagome lattice which is ubiquitous in various real materials. By proposing a proper second quantization for the non-Hermite Hamiltonian in the polarization-vector space, we obtain a new heat current density operator with two separate contributions: the normal velocity responsible for the longitudinal phonon transport, and the anomalous velocity manifesting itself as the Hall effect of transverse phonon transport. As exemplified in kagome lattices, our theory predicts that the dir…
The quantum anomalous Hall effect, an exotic topological state first theoretically predicted by Haldane and recently experimentally observed, has attracted enormous interest for low-power-consumption electronics. In this work, we derived a Schr{ö}dinger-like equation of phonons, where topology-related quantities, time reversal symmetry and its breaking can be naturally introduced similar as for electrons. Furthermore, we proposed a phononic analog of the Haldane model, which gives the novel quantum (anomalous) Hall-like phonon states characterized by one-way gapless edge modes immune to scatte…
The origin of phonon thermal Hall Effect (THE) observed in a variety of insulators is yet to be identified. Here, we report on the observation of a thermal Hall conductivity in a non-magnetic elemental insulator, with an amplitude exceeding what has been previously observed. In black phosphorus (BP), the longitudinal ($κ_{ii}$), and the transverse, $κ_{ij}$, thermal conductivities peak at the same temperature and at this peak temperature, the $κ_{ij}/κ_{jj}/B $ is $\approx 10^{-4}$-$10^{-3}$ T$^{-1}$. Both these features are shared by other insulators displaying THE, despite an absolute amplit…
We investigate the thermal Hall effect in a Kitaev-Heisenberg system, a model for Kitaev candidate $α$-RuCl$_3$, in the presence of the coupling between spin and phonon arising from chlorine atoms' vibration. We observe that the coupling modifies the relative stability between different magnetic states under a magnetic field, especially stabilizing a canted zigzag antiferromagnetic state. Remarkably, the spin-phonon interaction has distinct effects on the thermal Hall conductivity in different magnetically ordered states. For the canted zigzag state, which is relevant to $α\text{-RuCl}_3$, the…
A distinct thermal Hall signal is observed in a quantum spin liquid candidate Ba$_3$CuSb$_2$O$_9$. The transverse thermal conduction shows a power-law temperature dependence below 40 K where a spin gap opens. We suggest that, through the very low longitudinal thermal conductivity and the thermal Hall signals, a phonon Hall effect is induced by strong phonon scatterings by orphan Cu$^{2+}$ spins formed in random domains of Cu$^{2+}$-Sb$^{5+}$ dumbbells.
In this study, we report first experimental evidence of spin-momentum locking in the topological phonons in an inhomogeneously strained Si thin film. The spin-momentum locking in the topological phonons lead to a longitudinal spin texture or spatially inhomogeneous spin distribution in the freestanding sample structure. The spin texture was uncovered using location dependent Hall effect and planar Hall effect measurement. The charge carrier density and anomalous Hall resistance showed a linear behavior along the length of the sample. Similarly, the planar Hall resistance related with the spin …
SrTiO$_3$, a quantum paralectric, displays a detectable phonon thermal Hall effect (THE). Here we show that the amplitude of THE is extremely sensitive to stoichiometry. It drastically decreases upon substitution of a tiny fraction of Sr atoms with Ca, which stabilizes the ferroelectric order. It drastically increases by an even lower density of oxygen vacancies, which turn the system to a dilute metal. The enhancement in the metallic state exceeds by far the sum of the electronic and the phononic contributions. We explain this observation as an outcome of three features: i) heat is mostly tra…
Recently, a series of two-dimensional (2D) nonmagnetic layered materials XSi2Y4 (X=transition metals; Y=pnictogens) having similar crystal structures with transition-metal dichalcogenides (TMDs) were proposed for their potential application value. Like TMDs, we propose that chiral phonon involved valley-selective optical circular dichroism can be also obtained in XSi2Y4, and it can be further entangled with multiple Hall effects. However, it is difficult to compare such effect between XSi2Y4 and TMDs due to the non-unified conventions for pseudo-angular momentum (PAM) in the previous studies. …
Thermal Hall resistivity and transverse entropy production in a phonon gas
Wuhan National High Magnetic Field Center and School of Physics, Huazhong University of Science and Technology（华中科技大学物理学院）；CPHT, CNRS, École polytechnique, Institut Polytechnique de Paris（巴黎理工学院）；Laboratoire de Physique et d’Étude de Matériaux (CNRS) ESPCI Paris, PSL Research University（巴黎高等物理化工大学）
Electron-phonon ($e$-ph) interactions are key to understanding the dynamics of electrons in materials, and can be modeled accurately from first-principles. However, when electrons and holes form Coulomb-bound states (excitons), quantifying their interactions and scattering processes with phonons remains an open challenge. Here we show a rigorous approach for computing exciton-phonon (ex-ph) interactions and the associated exciton dynamical processes from first principles. Starting from the ab initio Bethe-Salpeter equation, we derive expressions for the ex-ph matrix elements and relaxation tim…
In this paper, the chiral Hall effect of strained Weyl semimetals without any external magnetic field is proposed. Electron-phonon coupling emerges in the low-energy fermionic sector through a pseudogauge potential. We show that, by using chiral kinetic theory, the chiral Hall effect appears as a response to a real time-varying electric field in the presence of structural distortion and it causes spatial chirality and charges separation in a Weyl system. We also show that the coupling of the electrons to acoustic phonons as a gapless excitation leads to emerging an optical absorption peak at $…
The thermal Hall effect, which arises when heat flows transverse to an applied thermal gradient, has become an important observable in the study of quantum materials. Recent experiments found a large thermal Hall conductivity $κ_{xy}$ in many high-temperature cuprate superconductors, including deep inside the Mott insulator, but the underlying mechanism remains unknown. Here, we uncover a surprising linear temperature dependence for the inverse thermal Hall resistivity, $1/ρ_H=-κ_{xx}^2/κ_{xy}$, in the Mott insulating cuprates $\mathrm{La_2CuO_4}$ and $\mathrm{Sr_2CuO_2Cl_2}$. We also find thi…
Recent theoretical studies inspired by experiments on the Kitaev magnet $α$-RuCl$_3$ highlight the nontrivial impact of phonons on the thermal Hall conductivity of chiral topological phases. Here we introduce mixed mesoscopic-macroscopic devices that allow refined thermal-transport probes of non-Abelian spin liquids with Ising topological order. These devices feature a quantum-coherent mesoscopic region with negligible phonon conductance, flanked by macroscopic lobes that facilitate efficient thermalization between chiral Majorana edge modes and bulk phonons. We show that our devices enable $(…
It has become common knowledge that phonons can generate thermal Hall effect in a wide variety of materials, although the underlying mechanism is still controversial. We study longitudinal $κ_{xx}$ and transverse $κ_{xy}$ thermal conductivity in Pr$_2$Ir$_2$O$_7$, which is a metallic analogue of spin ice. Despite the presence of mobile charge carriers, we find that both $κ_{xx}$ and $κ_{xy}$ are dominated by phonons. A $T/H$ scaling of $κ_{xx}$ unambiguously reveals that longitudinal heat current is substantially impeded by resonant scattering of phonons on paramagnetic spins. Upon cooling, th…
The phonon mode parameters and anisotropic mid-infrared dielectric function tensor components of high- Al-content Al$_x$Ga$_{1-x}$N alloys in dependence of the Al content $x$ are precisely determined from mid-infrared spectroscopic ellipsometry measurements for a set of high-quality Si-doped Al$_x$Ga$_{1-x}$N epitaxial layers on 4H-SiC substrates. Two-mode behavior of the $E_1$(TO) modes and one-mode behavior of the $A_1$(LO) mode are found in agreement with previous Raman scattering spectroscopy reports. The composition dependencies of the IR active phonon frequency parameters are established…
We have studied the influence of magnetic order on the optical phonons of the geometrically frustrated spinel ZnCr$_2$O$_4$ from first-principles. By mapping the first-principles phonon calculations onto a Heisenberg-like model, we developed a method to calculate exchange derivatives and subsequently the spin-phonon couping parameter from first-principles. All calculations were performed within LSDA+U.
Phonon Thermal Hall Effect: The Roles of Disorder, Annealing, and Metallic Contacts
Wuhan National High Magnetic Field Center and School of Physics, Huazhong University of Science and Technology（华中科技大学物理学院与武汉国家强磁场中心）；Laboratoire de Physique et d’Étude des Matériaux (ESPCI - CNRS - Sorbonne Université), PSL Research University（巴黎高等物理化工大学院校物理与材料实验室（ESPCI-法国国家科学研究中心-索邦大学），PSL研究大学）
We carry out a detailed analysis of the short-wave (semiclassical) approximation for the linear equations of the elasticity in a smoothly inhomogeneous isotropic medium. It is shown that the polarization properties of the transverse waves are completely analogous to those of electromagnetic waves and can be considered as spin properties of optical phonons. In particular, the Hamiltonian of the transverse waves contains an additional term of the phonon spin-orbit interaction arising from the Berry gauge potential in the momentum space. This potential is diagonal in the basis of the circularly p…
Phonon plays essential roles in dynamical behaviors and thermal properties, which are central topics in fundamental issues of materials science. The importance of first principles phonon calculations cannot be overly emphasized. Phonopy is an open source code for such calculations launched by the present authors, which has been world-widely used. Here we demonstrate phonon properties with fundamental equations and show examples how the phonon calculations are applied in materials science.
First-principles calculations combining density functional theory and many-body perturbation theory can provide microscopic insight into the dynamics of electrons and phonons in materials. We review this theoretical and computational framework, focusing on perturbative treatments of scattering, dynamics and transport of coupled electrons and phonons. We discuss application of these first-principles calculations to electronics, lighting, spectroscopy and renewable energy.
Observation of anomalous thermal Hall effect in altermagnets
Fudan University（复旦大学）；Shanghai Research Center for Quantum Sciences（上海量子科学研究与创新中心）；ShanghaiTech University（上海科技大学）；Hefei National Laboratory（合肥国家实验室）；Collaborative Innovation Center of Advanced Microstructures（先进微结构协同创新中心）
Lattice thermal conductivities of two SiO$_2$ polymorphs, i.e., $α$-quartz (low) and $α$-cristobalite (low), were studied using first-principles anharmonic phonon calculation and linearized phonon Boltzmann transport equation. Although $α$-quartz and $α$-cristobalite have similar phonon densities of states, phonon frequency dependencies of phonon group velocities and lifetimes are dissimilar, which results in largely different anisotropies of the lattice thermal conductivities. For $α$-quartz and $α$-cristobalite, distributions of the phonon lifetimes effective to determine the lattice thermal…
In this paper, thermal conductivity of crystalline GaAs is calculated using first-principles lattice dynamics. The harmonic and cubic force constants are obtained by fitting them to the force-displacement data from density functional theory calculations. Phonon dispersion is calculated from dynamical matrix constructed using the harmonic force constants and phonon relaxation times are calculated using Fermi Golden rule. The calculated GaAs thermal conductivity agrees well with experimental data. Thermal conductivity accumulations as a function of phonon mean free path and as a function of wave…
First principles calculation supports the occurence of a phonon anomaly along [211] in Ni$_2$FeGa that was observed experimentally for the first time as structural modulations along [211] direction. Fermi surface scans have been performed in both austenite and martensite phase to observe the possible Fermi nesting features in the system. The magnitude of observed Fermi surface nesting vectors in (211) plane exactly match the phonon anomaly wavevectors along [211] direction. Electron-phonon calculations in the austenite phase shows that there is significant electron-phonon coupling in the syste…
It has been known for more than a decade that phonons can produce an off-diagonal thermal conductivity in presence of magnetic field. Recent studies of thermal Hall conductivity, $κ_{xy}$, in a variety of contexts, however, have assumed a negligibly small phonon contribution. We present a study of $κ_{xy}$ in quantum paraelectric SrTiO$_3$, which is a non-magnetic insulator and find that its peak value exceeds what has been reported in any other insulator, including those in which the signal has been qualified as 'giant'. Remarkably, $κ_{xy}(T)$ and $κ(T)$ peak at the same temperature and the …
In the context of recent experimental observations of an unexpectedly large thermal Hall conductivity, $κ_H$, in insulating $\mathrm{La_2CuO_4}$ (LCO) and $\mathrm{SrTiO_3}$ (STO), we theoretically explore conditions under which acoustic phonons can give rise to such a large $κ_H$. Both the intrinsic and extrinsic contributions to $κ_H$ are large in proportion to the dielectric constant, $ε$, and the flexoelectric coupling, $F$. While the intrinsic contribution is still orders of magnitude smaller than the observed effect, an extrinsic contribution proportional to the phonon mean free path app…
Phonon energies at finite temperatures shift away from their harmonic values due to anharmonicity. In this paper, we have realized the rigorous calculation of phonon energy shifts of silicon by three and four-phonon scattering from first principles. The anharmonic fourth-order force constants are calculated by considering up to the fifth nearest neighbors. The results agree reasonably well with available data from inelastic neutron scattering throughout the Brillouin zone. Surprisingly, the frequency shifts of optical phonon modes near the $Γ$ point are sensitive to the cutoff radius of the fo…
We study the magnetically-induced phonon splitting in cubic ACr$_2$O$_4$ (A=Mg, Zn, Cd, Hg) spinels from first principles, and demonstrate that the sign of the splitting, which is experimentally observed to be opposite in CdCr$_2$O$_4$ compared to ZnCr$_2$O$_4$ and MgCr$_2$O$_4$, is determined solely by the particular magnetic ordering pattern observed in these compounds. We further show that this interaction between magnetism and phonon frequencies can be fully described by the previously proposed spin-phonon coupling model that includes only the nearest neighbor exchange. Finally, using this…
Opposite impact of thermal expansion and phonon anharmonicity on the phonon-limited resistivity of elemental metals from first principles
European Theoretical Spectroscopy Facility, Institute of Condensed Matter and Nanosciences, Université catholique de Louvain（欧洲理论光谱设施，凝聚态物质与纳米科学研究所，天主教鲁汶大学）；Scientific Computing Department, Science and Technology Facilities Council, UK Research and Innovation, Daresbury Laboratory（科学与工程设施理事会英国研究与创新达尔斯伯里实验室科学计算部）；Département de Physique et Institut Courtois, Université de Montréal（蒙特利尔大学物理系与库瓦托瓦研究所）；Department of Molecular Chemistry and Materials Science, Weizmann Institute of Science（魏茨曼科学研究所分子化学与材料科学系）；WEL Research Institute（WEL研究所）
We have studied the dielectric properties of the ferromagnetic spinel CdCr$_2$S$_4$ from first principles. Zone-center phonons and Born effective charges were calculated by frozen-phonon and Berry phase techniques within LSDA+U. We find that all infrared-active phonons are quite stable within the cubic space group. The calculated static dielectric constant agrees well with previous measurements. These results suggest that the recently observed anomalous dielectric behavior in CdCr$_2$S$_4$ is not due to the softening of a polar mode. We suggest further experiments to clarify this point.
We develop a method for calculating the electron-phonon vertex in polar semiconductors and insulators from first principles. The present formalism generalizes the Fröhlich vertex to the case of anisotropic materials and multiple phonon branches, and can be used either as a post-processing correction to standard electron-phonon calculations, or in conjunction with {\it ab initio} interpolation based on maximally localized Wannier functions. We demonstrate this formalism by investigating the electron-phonon interactions in anatase TiO$_2$, and show that the polar vertex significantly reduces the…
