We have utilized time-domain magneto-terahertz spectroscopy to investigate the low frequency optical response of topological insulator Cu$_{0.02}$Bi$_2$Se$_3$ and Bi$_2$Se$_3$ films. With both field and frequency dependence, such experiments give sufficient information to measure the mobility and carrier density of multiple conduction channels simultaneously. We observe sharp cyclotron resonances (CRs) in both materials. The small amount of Cu incorporated into the Cu$_{0.02}$Bi$_2$Se$_3$ induces a true bulk insulator with only a \textit{single} type of conduction with total sheet carrier density $\sim4.9\times10^{12}/$cm$^{2}$ and mobility as high as 4000 cm$^{2}/$V$\cdot$s. This is consistent with conduction from two virtually identical topological surface states (TSSs) on top and bottom of the film with a chemical potential $\sim$145 meV above the Dirac point and in the bulk gap. The CR broadens at high fields, an effect that we attribute to an electron-phonon interaction. This assignment is supported by an extended Drude model analysis of the zero field Drude conductance. In contrast, in normal Bi$_2$Se$_3$ films two conduction channels were observed and we developed a self-consistent analysis method to distinguish the dominant TSSs and coexisting trivial bulk/2DEG states. Our high-resolution Faraday rotation spectroscopy on Cu$_{0.02}$Bi$_2$Se$_3$ paves the way for the observation of quantized Faraday rotation under experimentally achievable conditions to push chemical potential in the lowest Landau Level.
Faraday's experiment measures -- within a modern view -- the charge adiabatically transported over a macroscopic distance by a given nuclear species in insulating liquids: the reason why it is integer is deeply rooted in topology. Whole numbers enter chemistry in a different form: atomic oxidation states. They are not directly measurable, and are determined instead from an agreed set of rules. Insulating liquids are a remarkable exception: Faraday's experiment indeed measures the oxidation numbers of each dissociated component in the liquid phase, whose topological values are unambiguous. Ioni…
We discuss the rich vibrational dynamics of nanometer-scale semiconducting and insulating crystals as probed by localized electronic impurity states, with an emphasis on nanoparticles that are only weakly coupled to their environment. Two principal regimes of electron-phonon dynamics are distinguished, and a brief survey of vibrational-mode broadening mechanisms is presented. Recent work on the effects of mechanical interaction with the environment is discussed.
Using first-principles density functional calculations, we study the electronic and magnetic properties of ferromagnetic insulating double-perovskite compound La2NiMnO6, which has been reported to exhibit interesting magnetic field sensitive dielectric anomaly as a function of temperature. Our study reveals existence of very soft infra-red active phonons that couple strongly with spins at the Ni and Mn sites through modification of the super-exchange interaction. We suggest that these modes are the origin for observed dielectric anomaly in La2NiMnO6.
Development of topological insulating phases in IV-VI compounds under dynamic lattice deformations is studied using first-principles methods. Unlike the static state of topological phases at equilibrium conditions, we show that non-trivial topological phases are induced in the compounds by the dynamic lattice deformations from selective phonon modes. Calculations of the time-reversal polarization show that the Z2 invariant of the compounds is flipped by the atomic displacements of selective phonon modes and that the compounds exhibit oscillating topological phases upon dynamic lattice deformat…
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 study the structural, electronic and vibrational properties of single-layer 1TNbSe$_2$ from first principles. Within the generalized gradient approximation, the 1T polytype is highly unstable with respect to the 2H. The DFT+U method improves the stability of the 1T phase, explaining its detection in experiments. A charge density wave occurs with a $\sqrt{13}\times\sqrt{13}~R30^{\circ}$ periodicity, in agreement with STM data. At $U=0$, the David-star reconstruction displays a flat band below the Fermi level with a marked d$_{z^2-r^2}$ orbital character of the central Nb. The Hubbard interac…
The tetradymite compound BiSbTeSe$_2$, is one of the most bulk-insulating three-dimensional topological insulators, which makes it important in the topological insulator research. It is a member of the solid-solution system Bi$_{2-x}$Sb$_x$Te$_{3-y}$Se$_y$, for which the local crystal structure, such as the occupation probabilities of each atomic site, is not well understood. We have investigated the temperature and polarization dependent spontaneous Raman scattering in BiSbTeSe$_2$, revealing a much higher number of lattice vibrational modes than predicted by group theoretical considerations …
The universal value of Faraday rotation angle close to the fine structure constant is experimentally observed in thin HgTe quantum wells with thickness on the border between trivial insulating and the topologically non-trivial Dirac phases. The quantized value of the Faraday angle remains robust in the broad range of magnetic fields and gate voltages. Dynamic Hall conductivity of the hole-like carriers extracted from the analysis of the transmission data shows theoretically predicted universal value of consistent with the doubly degenerate Dirac state. On shifting the Fermi level by the gate v…
We consider theoretically a superlattice formed by thin conducting layers separated spatially between insulating layers. The dispersion of two coupled phonon-plasmon modes of the system is analyzed by using Maxwell's equations, with the influence of retardation included. Both transmission for the finite plate as well as absorption for the semi-infinite superlattice in the infrared are calculated. Reflectance minima are determined by the longitudinal and transverse phonon frequencies in the insulating layers and by the density-state singularities of the coupled modes. We evaluate also the Raman…
Two-dimensional (2D) van der Waals (vdW) magnets have been a fertile playground for the discovery and exploration of physical phenomena and new physics. In this Letter, we report the observation of an anomalous thermal Hall effect (THE) with \k{appa}_xy ~ 1x10^(-2) W K^(-1) m^(-1) in an insulating van der Waals ferromagnet VI3. The thermal Hall signal persists in the absence of an external magnetic field and flips sign upon the switching of the magnetization. In combination with theoretical calculations, we show that VI3 exhibits a dual nature of the THE, i.e., dominated by topological magnons…
The monoclinic crystal structure of $β$-$\mathrm{Ga_2O_3}$ leads to significant anisotropy of the thermal properties. The 2$ω$-method is used to measure the thermal diffusivity $D$ in [010] and [001] direction respectively and to determine the thermal conductivity values $λ$ of the [100], [010] and [001] direction from the same insulating Mg doped $β$-$\mathrm{Ga_2O_3}$ single crystal. We detect a temperature independent anisotropy factor of both the thermal diffusivity and conductivity values of $D_{[010]}/D_{[001]}=λ_{[010]}/λ_{[001]}=1.4\pm 0.1$. The temperature-dependence is in accord with…
By combining genetic algorithm optimizations, first-principles calculations and the double-exchange model studies, we have unveiled that the exotic insulating ferromagnetism in LaMnO3 thin film originates from the previously unreported G-type d_{3z^2-r^2}/d_{x^2-y^2} orbital ordering. An insulating gap opens as a result of both the orbital ordering and the strong electron-phonon coupling. Therefore, there exist two strain induced phase transitions in the LaMnO3 thin film, from the insulating A-type antiferromagnetic phase to the insulating ferromagnetic phase and then to the metallic ferromagn…
We calculate the vibrational density-of-states in an insulating nanoparticle that is in weak mechanical contact with a semi-infinite substrate. The work is motivated by a recent experiment by Yang et al., where the low-energy phonon density-of-states of Y2O3 nanoparticles doped with Eu was measured. Preliminary results presented here, based on the conventional quasiparticle-pole approximation for the phonon propagator, are in reasonable agreement with experiment.
The spin relaxation dynamics of Ce$^{3+}$ ions in heavily cerium-doped YAG crystals is studied using pulse-electron paramagnetic resonance and time-resolved pump-probe Faraday rotation. Both techniques address the 4$f$ ground state, while pump-probe Faraday rotation provides also access to the excited 5$d$ state. We measure a millisecond spin-lattice relaxation time $T_1$, a microsecond spin coherence time $T_2$ and a $\sim 10$ ns inhomogeneous spin dephasing time $T_2^*$ for the Ce$^{3+}$ ground state at low temperatures. The spin-lattice relaxation of Ce$^{3+}$ ions is due to modified Raman …
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…
Vanadium dioxide (VO2) undergoes a phase transition at a temperature of 340 K between an insulating monoclinic M1 phase and a conducting rutile phase. Accurate measurements of possible anisotropy of the electronic properties and phonon features of VO2 in the insulating monoclinic M1 and metallic rutile phases are a prerequisite for understanding the phase transition in this correlated system. Recently, it has become possible to grow single domain untwinned VO2 microcrystals which makes it possible to investigate the true anisotropy of VO2. We performed polarized transmission infrared micro-spe…
We investigate the electron population dynamics in an ensemble of nearly isolated insulating nanoparticles, each nanoparticle modeled as an electronic two-level system coupled to a single vibrational mode. We find that at short times the ensemble-averaged excited-state population oscillates but has a decaying envelope. At long times, the oscillations become purely sinusoidal about a ``plateau'' population, with a frequency determined by the electron-phonon interaction strength, and with an envelope that decays algebraically as t^-{1/2} We use this theory to predict electron-phonon dynamics in …
The effects of doping on the spectral properties of low doped systems are investigated by means of Coherent Potential Approximation to describe the distributed disorder induced by the impurities and Phonon-Phonon Non-Crossing Approximation to characterize a wide class of electron-phonon interactions which dominate the low-energy spectral features. When disorder and electron-phonon interaction work on comparable energy scales, a strong interplay between them arises, the effect of disorder can no more be described as a mere broadening of the spectral features and the phonon signatures are still …
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…
We present a mechanism by which optically driven chiral phonon modes in rare-earth trihalides generate giant effective magnetic fields acting on the paramagnetic $4f$ spins. With cerium trichloride (CeCl$_3$) as our example system, we calculate the coherent phonon dynamics in response to the excitation by an ultrashort terahertz pulse using a combination of phenomenological modeling and first-principles calculations. We find that effective magnetic fields of over 100 tesla can possibly be generated that polarize the spins for experimentally accessible pulse energies. The direction of induced m…
We present a microscopic picture rationalizing the surprisingly steep decrease of the band gap with temperature in insulators, crystalline or otherwise. The gap narrowing largely results from fluctuations of long-wavelength optical phonons---when the latter are present---or their disordered analogs, if the material is amorphous. We elaborate on this notion to show that possibly with the exception of weakly bound solids made of closed-shell atoms, the existence of an insulating gap or pseudo-gap in a periodic solid implies that optical phonons must be present, too. This means that in an insulat…
Electron-phonon-driven charge density waves can in some circumstances allow electronic correlations to become predominant, driving a system into a Mott insulating state. New insights into both the Mott state and preceding charge density wave may result from observations of the coupled dynamics of their underlying degrees of freedom. Here, tunneling injection of single electrons into the upper Hubbard band of the Mott charge-density-wave material 1T-TaS2 reveals extraordinarily narrow electronic excitations which couple to amplitude mode phonons associated with the charge density wave's periodi…
Here we examine the role of the amorphous insulating substrate in the thermal relaxation in thin NbN, InO$_x$, and Au/Ni films at temperatures above 5 K. The studied samples are made up of metal bridges on an amorphous insulating layer lying on or suspended above a crystalline substrate. Noise thermometry was used to measure the electron temperature $T_e$ of the films as a function of Joule power per unit of area $P_{2D}$. In all samples, we observe the dependence $P_{2D}\propto T_e^n$ with the exponent $n\simeq 2$, which is inconsistent with both electron-phonon coupling and Kapitza thermal r…
We present electronic transport measurements of GaAs nanowires grown by catalyst-free metal-organic chemical vapor deposition. Despite the nanowires being doped with a relatively high concentration of substitutional impurities, we find them inordinately resistive. By measuring sufficiently high aspect-ratio nanowires individually in situ, we decouple the role of the contacts and show that this semi-insulating electrical behavior is the result of trap-mediated carrier transport. We observe Poole-Frenkel transport that crosses over to phonon-assisted tunneling at higher fields, with a tunneling …
We study the half-breathing phonon in the three-band model of a high temperature superconductor, allowing for vibrations of atoms and resulting changes of hopping parameters. Two different approaches are compared. From the three-band model a t-J model with phonons can be derived, and phonon properties can be calculated. To make contact to density functional calculations, we also study the three-band model in the Hartree-Fock (HF) approximation. The paramagnetic HF solution, appropriate for the doped cuprates, has similarities to the local-density approximation (LDA). However, in contrast to th…
Nickel substitution at the cobalt site in NaxCoO2 induces a Metal Insulator Transition (MIT) and the temperature at which this occurs (TMIT) increases with Ni content. Low temperature far infrared measurements on polycrystalline samples of Na0.75CoO2 and Na0.75Co0.95Ni0.05O2 (TMIT = ~ 150K) were carried out to look for signatures of this transition. While both the samples show an evident splitting of the high frequency Co-O mode on lowering the temperature, dramatic changes are observed in the low frequency sodium mode in Na0.75Co0.95Ni0.05O2 clearly pointing out to an ordering of the sodium i…
Electronic structure near Fermi level of Pr2CoFeO6 (at 300 K) was investigated by X-ray photoemission spectroscopy (XPS) technique. All three cations, i.e., Pr, Co and Fe were found to be trivalent in nature. XPS analysis also suggested the system to be insulating in nature. Moreover, Raman spectroscopy study indicated the random distribution of the B-site ions (Co/Fe) triggered by same charge states. In temperature-dependent Raman study, the relative heights of the two observed phonon modes exhibited anomalous behaviour near magnetic transition temperature TN~270 K, thus indicating towards in…
To gain control over magnetic order on ultrafast time scales, a fundamental understanding of the way electron spins interact with the surrounding crystal lattice is required. However, measurement and analysis even of basic collective processes such as spin-phonon equilibration have remained challenging. Here, we directly probe the flow of energy and angular momentum in the model insulating ferrimagnet yttrium iron garnet. Following ultrafast resonant lattice excitation, we observe that magnetic order reduces on distinct time scales of 1 ps and 100 ns. Temperature-dependent measurements, a spin…
The temperature dependence of electron spin coherence in singly negatively charged (In,Ga)As/GaAs quantum dots is studied by time-resolved Faraday rotation. The decoherence time T2 is constant on a microsecond scale for temperatures below 20 K, for higher temperatures it shows a surprisingly sharp drop into the nanoseconds range. The decrease cannot be explained through inelastic scattering with phonons, and may be related with elastic scattering due to phonon-mediated fluctuations of the hyperfine interaction.
We demonstrate a thermodynamic formulation to quantify defect formation energetics in an insulator under high electric field. As a model system, we analyzed neutral oxygen vacancies (color centers) in alkaline-earth-metal binary oxides using density functional theory, Berry phase calculations, and maximally localized Wannier functions. Work of polarization lowers the field dependent electric Gibbs energy of formation of this defect. This is attributed mainly to the ease of polarizing the two electrons trapped in the vacant site, and secondarily to the defect induced reduction in bond stiffness…
We present a magneto-infrared spectroscopic study of thin Bi2Se3 single crystal flakes. Magneto-infrared transmittance and reflectance measurements are performed in the Faraday geometry at 4.2K in a magnetic field up to 17.5T. Thin Bi2Se3 flakes (much less than 1μm thick) are stabilized on the Scotch tape, and the reduced thickness enables us to obtain appreciable far-infrared transmission through the highly reflective Bi2Se3 single crystals. A pronounced electron-phonon coupling is manifested as a Fano resonance at the α optical phonon mode in Bi2Se3, resulting from the quantum interference b…
Recent attempts at topological materials have revealed a large class of materials that show gapless surface states protected by time-reversal symmetry and crystal symmetries. Among them, topological insulating states protected by crystal symmetries, rather than time-reversal symmetry are classified as topological crystalline insulators. We computationally predict the signature of new three-dimensional topological crystalline insulating compounds of space group 139(I/4mmm). After conducting a full volume optimization process by allowing to rearrange of atomic positions and lattice parameters, t…
Optical, vibrational, and electronic properties of semiconducting YbN
Robinson Research Institute, Victoria University of Wellington（罗宾逊研究所，惠灵顿维多利亚大学）；The MacDiarmid Institute for Advanced Materials and Nanotechnology, Victoria University of Wellington（麦克迪亚米德先进材料与纳米技术研究所，惠灵顿维多利亚大学）
A modeling of the normal state of the p-doped high-temperature superconductors (HTSC's) is presented. This is achieved starting from a more conventional metallic phase for optimal- and overdoping and passing via the underdoped to the insulating state by consecutive orbital selective compressibility-incompressibility transitions in terms of sum rules for the charge response. The modeling is substantiated by corresponding phonon calculations. Extending investigations of the full dispersion and in particular of the strongly doping dependent anomalous phonon modes in LaCuO, which so far underpin o…
Monolayers of two-dimensional van der Waals materials exhibit novel electronic phases distinct from their bulk due to the symmetry breaking and reduced screening in the absence of the interlayer coupling. In this work, we combine angle-resolved photoemission spectroscopy and scanning tunneling microscopy/spectroscopy to demonstrate the emergence of a unique insulating 2 x 1 dimer ground state in monolayer 1T-IrTe2 that has a large band gap in contrast to the metallic bilayer-to-bulk forms of this material. First-principles calculations reveal that phonon and charge instabilities as well as loc…
Ab Initio Theory of Phonon Magnetic Moment Induced by Electron-Phonon Coupling in Magnetic Materials
National Laboratory of Solid State Microstructures, School of Physics, Nanjing University（南京大学固体微结构物理学院）；Center for Quantum Transport and Thermal Energy Science, Institute of Physics Frontiers and Interdisciplinary Sciences, School of Physics and Technology, Nanjing Normal University（南京师范大学物理科学与技术学院前沿交叉科学研究院量子输运与热能科学中心）；Department of Physics, Tokyo Institute of Technology（东京工业大学物理学系）；Collaborative Innovation Center of Advanced Microstructures, Nanjing University（南京大学先进微结构协同创新中心）；Jiangsu Physical Science Research Center, Nanjing（江苏物理科学研究中心）
We investigate the interplay of the electron-electron and electron-phonon interactions in the electronic structure of an exotic insulating state in the layered dichalcogenide 1T-TaS2, where the charge-density-wave (CDW) order coexists with a Mott correlation gap. Scanning tunneling microscopy and spectroscopy measurements with high spatial and energy resolution determine unambiguously the CDW and the Mott gap as 0.20-0.24 eV and 0.32 eV, respectively, through the real space electron phases measured across the multiply formed energy gaps. An unusual local reduction of the Mott gap is observed o…
The concept of topological energy bands and their manifestations have been demonstrated in condensed matter systems as a fantastic paradigm toward unprecedented physical phenomena and properties that are robust against disorders. Recent years, this paradigm was extended to phononic metamaterials (including mechanical and acoustic metamaterials), giving rise to the discovery of remarkable phenomena that were not observed elsewhere thanks to the extraordinary controllability and tunability of phononic metamaterials as well as versatile measuring techniques. These phenomena include, but not limit…
The electron-phonon coupling of a theoretically devised carbon phase made by assembling the smallest fullerenes C$_{20}$ is calculated from first principles. The structure consists of C$_{20}$ cages in an {\it fcc} lattice interlinked by two bridging carbon atoms in the interstitial tetrahedral sites ({\it fcc}-C$_{22}$). The crystal is insulating but can be made metallic by doping with interstitial alkali atoms. In the compound NaC$_{22}$ the calculated coupling constant $λ/N(0)$ is 0.28 eV, a value much larger than in C$_{60}$, as expected from the larger curvature of C$_{20}$. On the basis …
The disadvantage of BaBiO$_3$ of not being a topological insulator despite having symmetry protected Dirac state is overcome by shifting the Fermi level (E$_F$) via fluorination. The DFT calculations reveal that the fluorination neither affects the spin-orbit coupling nor the parity of the states, but it acts as a perfect electron donor to shift the E$_F$. We find that 33 % fluorination is sufficient to shift the E$_F$ by $\sim$ 2 eV so that the invariant Dirac state lies on it to make BaBiO$_2$F a topological insulator. The fluorinated cubic compound can be experimentally synthesized as the p…
Topological insulators are non-trivial quantum states of matter which exhibit a gap in the electronic structure of their bulk form, but a gapless metallic electronic spectrum at the surface. Here, we predict a uniaxial strain induced electronic topological transition (ETT) from a band to topological insulating state in the rhombohedral phase (space group: R$\bar{3}$m) of As$_2$Te$_3$ ($β$-As$_2$Te$_3$) through \textit{first-principles} calculations including spin-orbit coupling within density functional theory. The ETT in $β$-As$_2$Te$_3$ is shown to occur at the uniaxial strain $ε_{zz}$ = -0.…
Addressing the role of quantum coherence in the interplay between the different matter constituents (electrons, phonons and spin) is a critical step towards understanding transition metal oxides and design complex materials with new functionalities. Here we use coherent vibrational control of onsite d-d electronic transitions in a model edge-sharing insulating transition metal oxide (CuGeO3) to single-out the effects of vibrational coherence in electron-phonon coupling. By comparing time domain experiments based on high and low frequency ultrashort pumps with a fully quantum description of pho…
In ionic Raman scattering, infrared-active phonons mediate a scattering process that results in the creation or destruction of a Raman-active phonon. This mechanism relies on nonlinear interactions between phonons and has in recent years been associated with a variety of emergent lattice-driven phenomena in complex transition-metal oxides, but the underlying mechanism is often obscured by the presence of multiple coupled order parameters in play. Here, we use time-resolved spectroscopy to compare coherent phonons generated by ionic Raman scattering with those created by more conventional elect…
The coupling between localized spins and phonons can lead to shifts in the dielectric constant of insulating materials at magnetic ordering transitions. Studies on isostructural SeCuO3 (ferromagnetic) and TeCuO3 (antiferromagnetic) illustrate how the q-dependent spin-spin correlation function couples to phonon frequencies leading to a shift in the dielectric constant. A model is discussed for this spin-phonon coupling. The magnetodielectric coupling in multiferroic materials can be very large at a ferroelectric transition temperature. This coupling is investigated in the recently identified mu…
The lattice dynamics of low-frequency rigid-plane modes in metallic (graphene multilayers, GML) and in insulating (hexagonal boron-nitride multilayers, BNML) layered crystals is investigated. The frequencies of shearing and compression (stretching) modes depend on the layer number ${\EuScript N}$ and are presented in the form of fan diagrams. The results for GML and BNML are very similar. In both cases only the interactions (van der Waals and Coulomb) between nearest-neighbor planes are effective, while the interactions between more distant planes are screened. A comparison with recent Raman s…
The great potential of Dirac electrons for plasmonics and photonics has been readily recognized after their discovery in graphene, followed by applications to smart optical devices. Dirac carriers are also found in topological insulators (TI) --quantum systems having an insulating gap in the bulk and intrinsic Dirac metallic states at the surface--. Here, we investigate the plasmonic response of ring structures patterned in Bi$_2$Se$_3$ TI films, which we investigate through terahertz (THz) spectroscopy. The rings are observed to exhibit a bonding and an antibonding plasmon modes, which we tun…
