We investigate the bulk photovoltaic effect, which rectifies light into electric current, in a collective quantum state with correlation driven electronic ferroelectricity. We show via explicit real-time dynamical calculations that the effect of the applied electric field on the electronic order parameter leads to a strong enhancement of the bulk photovoltaic effect relative to the values obtained in a conventional insulator. The enhancements include both resonant enhancements at sub-band-gap frequencies, arising from excitation of optically active collective modes, and broadband enhancements arising from nonresonant deformations of the electronic order. The deformable electronic order parameter produces an injection current contribution to the bulk photovoltaic effect that is entirely absent in a rigid-band approximation to a time-reversal symmetric material. Our findings establish that correlation effects can lead to the bulk photovoltaic effect and demonstrate that the collective behavior of ordered states can yield large nonlinear optical responses.
We discuss the photovoltaic effect at a p-n heterojunction, in which the illuminated side is a doped Mott insulator, using the simplest description of a Mott insulator within the Hubbard model. We find that the internal quantum efficiency of such a device, if we choose an appropriate narrow-gap Mott insulator, can be significantly enhanced due to impact ionization caused by the photoexcited ``hot'' electron/hole pairs. Namely, the photoexcited electron and/or hole can convert its excess energy beyond the Mott-Hubbard gap to additional electrical energy by creating multiple electron/hole pairs …
Oxygen vacancy is intrinsically coupled with magnetic, electronic and transport properties of transition-metal oxide materials and directly determines their multifunctionality. Here, we demonstrate reversible control of oxygen content by post-annealing at temperature lower than 300 degree centigrade and realize the reversible metal-insulator transition in epitaxial NdNiO3 films. Importantly, over six orders of magnitude in the resistance modulation and a large change in optical band gap are demonstrated at room temperature without destroying the parent framework and changing the p-type conduct…
Photovoltaic effect, e.g., solar cells, converts light into DC electric current. This phenomenon takes place in various setups such as in noncentrosymmetric crystals and semiconductor pn junctions. Recently, we proposed a theory for producing DC spin current in magnets using electromagnetic waves, i.e., the spin-current counterpart of the solar cells. Our calculation shows that the nonlinear conductivity for the spin current is nonzero in a variety of noncentrosymmetric magnets, implying that the phenomenon is ubiquitous in inversion-asymmetric materials with magnetic excitations. Intuitively,…
Excitonic insulators host a condensate of electron-hole pairs at equilibrium, giving rise to collective many-body effects. Although several materials have emerged as excitonic insulator candidates, evidence of long-range coherence is lacking and the origin of the ordered phase in these systems remains controversial. Here, using ultrafast pump-probe microscopy, we investigate the possible excitonic insulator Ta$_2$NiSe$_5$. Below 328 K, we observe the anomalous micrometer-scale propagation of coherent modes at velocities of the order of $\sim10^5$ m/s, which we attribute to the hybridization be…
We consider a two-band spinless model describing an excitonic insulator (EI) on the two-dimensional square lattice with anisotropic hopping parameters and electron-phonon (el-ph) coupling, inspired by the EI candidate Ta$_2$NiSe$_5$. We systematically study the nature of the collective excitations in the ordered phase which originates from the interband Coulomb interaction and the el-ph coupling. When the ordered phase is stabilized only by the Coulomb interaction (pure EI phase), its collective response exhibits a massless phase mode in addition to the amplitude mode. We show that in the BEC …
We study a model for photovoltaic energy collection consisting of a Mott insulating layer in presence of acoustic phonons, coupled to two wide-band fermion leads at different chemical potentials and driven into a nonequilibrium steady state by a periodic electric field. We treat electron correlations with nonequilibrium dynamical mean-field theory (DMFT) using the so-called auxiliary master equation approach as impurity solver and include dissipation by acoustic phonons via the Migdal approximation. For a small hybridization to the leads, we obtain a peak in the photocurrent as a function of t…
Based on the Hubbard model description of the doped Mott insulator, we prove that there must exist a spinless collective excitation of charge $2e$ and of energy $U-2μ$ peaked at momentum $(π/a,π/a)$ in the non-superconducting state due to doping. Such a collective excitation arises from the electron pair correlation. Its existence is related to the breakdown of an approximate SU(2) particle-hole symmetry, from which an effective field theory of the new excitations is constructed.
The layered chalcogenide Ta$_{2}$NiSe$_{5}$ has been proposed to host an excitonic condensate in its ground state, a phase that could offer a unique platform to study and manipulate many-body states at room temperature. However, identifying the dominant microscopic contribution to the observed spontaneous symmetry breaking remains challenging, perpetuating the debate over the ground state properties. Here, using broadband ultrafast spectroscopy we investigate the out-of-equilibrium dynamics of Ta$_{2}$NiSe$_{5}$ and demonstrate that the transient reflectivity in the near-infrared range is conn…
The charge response in the barium vanadium sulfide (BaVS3) single crystals is characterized by dc resistivity and low frequency dielectric spectroscopy. A broad relaxation mode in MHz range with huge dielectric constant ~= 10^6 emerges at the metal-to-insulator phase transition TMI ~= 67 K, weakens with lowering temperature and eventually levels off below the magnetic transition Tchi ~= 30 K. The mean relaxation time is thermally activated in a manner similar to the dc resistivity. These features are interpreted as signatures of the collective charge excitations characteristic for the orbital …
The terahertz (THz) response in 10-100 cm^-1 was investigated in an organic dimer-Mott (DM) insulator kappa-(ET)_2Cu_2(CN)_3 that exhibits a relaxor-like dielectric anomaly. 30 cm^-1 band in the optical conductivity was attributable to collective excitation of the intra-dimer electric dipoles which are formed by an electron correlation. We succeeded in observing photoinduced enhancement of this 30 cm^-1 band, reflecting the growth of the electric dipole cluster in the DM phase. Such optical responses in kappa-(ET)_2Cu_2(CN)_3 reflect instability near the boundary between the DM-ferroelectric c…
We study a Haldane model with nearest neighbor interactions. We find one-dimensional like collective modes arising due to the interplay of pseudo-spin and valley degrees of freedom. In the large band gap or moderate interaction limit, these excitations are low energy modes lying in the band gap. The dispersion relations are qualitatively different in trivial insulator phase and Chern insulator phase, thus can be used to identify the topology of the Haldane model with the bulk property. We also discuss how to detect these modes in cold atom systems. An abelian gauge theory will emerge when a ph…
Solar cells based on conventional semiconductors have low efficiency in converting solar energy into electricity because the excess energy beyond the gap of an incident solar photon is converted into heat by phonons. Here we show by ab initio methods that the presence of strong Coulomb interactions in strongly correlated insulators (SCI) causes the highly photo-excited electron-hole pair to decay fast into multiple electron-hole pairs via impact ionization (II). We show that the II rate in the insulating $M_1$ phase of vanadium dioxide (chosen for this study as it is considered a prototypical …
We introduce the notion of the strongly correlated band insulator (SCI), where the lowest energy excitations are collective modes (excitons) rather than the single particles. We construct controllable 1/N expansion for SCI to describe their observables properties. A remarkable example of the SCI is bilayer graphene which is shown to be tunable between the SCI and usual weak coupling regime.
We investigate the equilibrium state and the collective modes of an excitonic insulator (EI) in a Fabry-Pérot cavity. In an EI, two bands of a semiconductor or semimetal spontaneously hybridize due to the Coulomb interaction between electrons and holes, leading to the opening of a gap. The coupling to the electromagnetic field reduces the symmetry of the system with respect to phase rotations of the excitonic order parameter from $U(1)$ to $Z_2$. While the reduction to a discrete symmetry would in general lead to a gapped phase mode and enhance the stability of the ordered phase, the coupling …
Collective and separate metal-insulator transitions in correlated vanadium dioxide
Key Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education & School of Materials Science and Engineering, Shanxi Normal University（山西师范大学材料科学与工程学院）；Research Institute of Materials Science, Shanxi Key Laboratory of Advanced Magnetic Materials and Devices, Shanxi Normal University（山西师范大学材料科学研究院）
The nonlinear optical response of an excitonic insulator coupled to lattice degrees of freedom is shown to depend in strong and characteristic ways on whether the insulating behavior originates primarily from electron-electron or electron-lattice interactions. Linear response optical signatures of the massive phase mode and the amplitude (Higgs) mode are identified. Upon nonlinear excitation resonant to the phase mode, a new in-gap mode at twice the phase mode frequency is induced, leading to a huge second harmonic response. Excitation of in-gap phonon modes leads to different and much smaller…
Momentum resolved inelastic resonant x-ray scattering is used to map the evolution of charge excitations over a large range of energies, momenta and doping levels in the electron doped Mott insulator class Nd$_{2-x}$Ce$_x$CuO$_4$. As the doping induced AFM-SC (antiferromagnetic-superconducting) transition is approached, we observe an anisotropic softening of collective charge modes over a large energy scale along the Gamma to (π,π)-direction, whereas the modes exhibit broadening ($\sim$ 1 eV) with relatively little softening along Gamma to (π,0) with respect to the parent Mott insulator (x=0).…
Exciton-roton mode in moiré fractional Chern insulators
Tsinghua University（清华大学）；Institute for Advanced Study, Tsinghua University（清华大学高等研究院）；Frontier Science Center for Quantum Information, Beijing（北京量子前沿科学中心）
We consider the zero-filled quantum-Hall ferromagnetic state of bilayer graphene subject to a kink-like perpendicular electric field, which generates domain walls in the electronic state and low-energy collective modes confined to move along them. In particular, it is shown that two pairs of collective helical modes are formed at opposite sides of the kink, each pair consisting of modes with identical helicities. We derive an effective field-theoretical model of these modes in terms of two weakly coupled anisotropic quantum spin-ladders, with parameters tunable through control of the electric …
Samarium hexaboride (SmB$_6$) is the first strongly correlated material with a recognized non-trivial band-structure topology. Its electron correlations are seen by inelastic neutron scattering as a coherent collective excitation at the energy of 14 meV. Here we calculate the spectrum of this mode using a perturbative slave boson method. Our starting point is the recently constructed Anderson model that properly captures the band-structure topology of SmB$_6$. Most self-consistent renormalization effects are captured by a few phenomenological parameters whose values are fitted to match the cal…
In this article, we discuss the non-trivial collective charge excitations (plasmons) of the extended square-lattice Hubbard model. Using a fully non-perturbative approach, we employ the hybrid Monte Carlo algorithm to simulate the system at half-filling. A modified Backus-Gilbert method is introduced to obtain the spectral functions via numerical analytic continuation. We directly compute the single-particle density of states which demonstrates the formation of Hubbard bands in the strongly-correlated phase. The momentum-resolved charge susceptibility is also computed on the basis of the Eucli…
Long-range interactions drive some of the rich phenomenology of quasiparticle collective states in the fractional quantum Hall (FQH) regime. We test for analogues in models of fractional Chern insulators (FCIs) derived from a screened Coulomb interaction. We find that the uniform FCI liquid is surprisingly robust to long-range interactions but gives way to a unidirectional charge density wave (CDW) of fractionally charged quasiparticles with increased screening length. Our results show that FCIs offer a robust and important platform for studying quasiparticles collective states.
We study third-harmonic generation (THG) in an excitonic insulator (EI) described in a two-band correlated electron model. Employing the perturbative expansion with respect to the external electric field, we derive the THG susceptibility taking into account the collective dynamics of the excitonic order parameter. In the inversion-symmetric EI, the collective order parameter motion is activated at second order of the external field and its effects arise in THG. We find three peaks in the THG susceptibility at energies $\hbar Ω= Δ_g/3$, $Δ_g/2$, and $Δ_g$, where $Δ_g$ is the band gap. While the…
Symmetric Mode Ansatz: Theory of Magnon Collective Modes in Chern Insulators
Princeton Center for Theoretical Science, Princeton University（普林斯顿大学理论科学中心）；Department of Physics, Princeton University（普林斯顿大学物理系）；Institut für Theoretische Physik und Astrophysik and Würzburg-Dresden Cluster of Excellence ctd.qmat, Julius-Maximilians-Universität Würzburg（维尔茨堡大学理论与天体物理研究所及维尔茨堡-德累斯顿卓越集群ctd.qmat）；Donostia International Physics Center（圣塞巴斯蒂安国际物理中心）；IKERBASQUE, Basque Foundation for Science（伊卡巴斯科，巴斯克科学基金会）；Center for Computational Quantum Physics, Flatiron Institute（平顿研究院计算量子物理中心）；Laboratoire de Physique de l’Ecole normale supérieure, ENS, Université PSL, CNRS, Sorbonne Université, Université Paris-Diderot, Sorbonne Paris Cité（巴黎高等师范学院物理实验室，ENS，PSL大学，CNRS，索邦大学，巴黎第七大学，索邦巴黎城）
Employing elastic and inelastic neutron scattering (INS) techniques, we report on detailed microscopic properties of the ferromagnetism in he magnetic topological insulator (Bi$_{0.95}$Mn$_{0.05}$)$_{2}$Te$_{3}$. Neutron diffraction of polycrystalline samples show the ferromagnetic (FM) ordering is long-range within the basal plane, and mainly 2D in character with short-range correlations between layers below $T_{\mathrm{C}} \approx 13$ K. Despite the random distribution of the dliute Mn atoms, we find that the 2D-like magnetic peaks are commensurate with the chemical structure, and the absenc…
The periodic Anderson model is extended by switching on a Hubbard U for the conduction electrons. We use the Gutzwiller variational method to study the nearly integral valent limit. The lattice Kondo energy contains the U-dependent chemical potential of the Hubbard subsystem in the exponent, and the correlation-induced band narrowing in the prefactor. Both effects tend to suppress the Kondo scale, which can be understood to result from the blocking of hybridization. At half-filling, we find a Brinkman-Rice-type transition from a Kondo insulator to a Mott insulator.
An excitonic insulator (EI) is an unconventional quantum phase of matter in which excitons, bound pairs of electrons and holes, undergo Bose--Einstein condensation, forming a macroscopic coherent state. While its existence was first hypothesized half a century ago, the EI has eluded experimental observation in bulk materials for decades. In the last few years, a resurgence of interest in the subject has been driven by the identification of several candidate materials suspected to support an excitonic condensate. However, one obstacle in verifying the nature of these systems has been to find si…
Excitonic insulating system is studied from the viewpoints of the orbital physics in strongly correlated electron systems. An effective model Hamiltonian for low-energy electronic states is derived from the two-orbital Hubbard model with a finite energy difference corresponding to the crystalline field splitting. The effective model is represented by the spin operators and the pseudo-spin operators for the spin-state degrees of freedom. The ground state phase diagram is analyzed by the mean-field approximation. In addition to the low-spin state and high-spin state phases, two kinds of the exci…
The generation of a current by light is a key process in optoelectronic and photovoltaic devices. In band semiconductors, depletion fields associated with interfaces separate long-lived photo-induced carriers. However, in systems with strong electron-electron and electron-phonon correlations it is unclear what physics will dominate the photoresponse. Here we investigate photocurrent in a vanadium dioxide, an exemplary strongly correlated material known for its dramatic metal-insulator transition (MIT) at Tc = 68 C which could be useful for optoelectronic detection and switching up to ultraviol…
We consider a model for a metal-insulator transition of correlated electrons in an external magnetic field. We find a broad region in interaction and magnetic field where metallic and insulating (fully magnetized) solutions coexist and the system undergoes a first-order metal-insulator transition. A global instability of the magnetically saturated solution precedes the local ones and is caused by collective fluctuations due to poles in electron-hole vertex functions.
The development of long-range ferromagnetic (FM) order in dilute magnetic topological insulators can induce dissipationless electronic surface transport via the quantum anomalous Hall effect. We measure the magnetic excitations in a prototypical magnetic topological crystalline insulator, Sn$_{0.95}$Mn$_{0.05}$Te, using inelastic neutron scattering. Neutron diffraction and magnetization data indicate that our Sn$_{0.95}$Mn$_{0.05}$Te sample has no FM long-range order above a temperature of 2 K. However, we observe slow, collective FM fluctuations ($<$~70 $μ$eV), indicating proximity to FM orde…
We study electronic transport in Anderson insulators with strong Coulomb interactions in dimensions d>=2. Close to the metal insulator transition where the single particle localization length is much larger than interparticle-distance, the interactions lead to a strongly correlated quantum glass phase. Even though single particle excitations are localized and the system is insulating, there are collective electronic modes which remain delocalized down to parametrically small energies. These collective excitations serve as a continuous bath which can provide the activation energy for variable r…
Graphene subject to a strong, tilted magnetic field exhibits an insulator-metal transition tunable by tilt-angle, attributed to the transition from a canted antiferromagnetic (CAF) to a ferromagnetic (FM) bulk state at filling factor zero. We develop a theoretical description for the spin and valley edge textures in the two phases, and the implied evolution in the nature of edge modes through the transition. In particular, we show that the CAF has gapless neutral modes in the bulk, but supports gapped charged edge modes. At the transition to the FM state the charged edge modes become gapless a…
We theoretically discover purely electronic polarization modes in THz frequency region in dimer Mott insulators $κ$-(BEDT-TTF)$_2$X. The unusual low-frequency modes arise from the coupling between the oscillation of intradimer electric dipole moments and that of alternating interdimer bond orders. These collective motions play an important role in the dynamical dielectric properties of the dimer Mott insulators. Near the phase boundary of the dimer Mott transition, the ferroelectric ground state is realized by introducing electron-lattice coupling.
Manipulating the orbital state in a strongly correlated electron system is of fundamental and technological importance for exploring and developing novel electronic phases. Here, we report an unambiguous demonstration of orbital occupancy control between t2g and eg multiplets in quasi-twodimensional transition metal oxide superlattices (SLs) composed of a Mott insulator LaCoO3 and a band insulator LaAlO3. As the LaCoO3 sublayer thickness approaches its fundamental limit (i.e. one unit-cell-thick), the electronic state of the SLs changed from a Mott insulator, in which both t2g and eg orbitals …
Vanadium dioxide is of broad interest as a spin-1/2 electron system that realizes a metal-insulator transition near room temperature, due to a combination of strongly correlated and itinerant electron physics. Here, resonant inelastic X-ray scattering is used to measure the excitation spectrum of charge, spin, and lattice degrees of freedom at the vanadium L-edge under different polarization and temperature conditions. These spectra reveal the evolution of energetics across the metal-insulator transition, including the low temperature appearance of a strong candidate for the singlet-triplet ex…
Collective excitations contain rich information about photoinduced transient states in correlated systems. In a Mott insulator, charge degrees of freedom are frozen, but can be activated by photodoping. The energy-momentum distribution of the charge excitation spectrum reflects the propagation of charge degrees of freedom, and provides information about the interplay among various intertwined instabilities on the time scale set by the pump. To reveal charge excitations out of equilibrium, we simulate time-resolved x-ray absorption and resonant inelastic x-ray scattering using a Hubbard model. …
We consider the excitonic insulator state (often associated with electronic ferroelectricity), which arises on the phase diagram of an extended spinless Falicov--Kimball model (FKM) at half-filling. Within the Hartree--Fock approach, we calculate the spectrum of low-energy collective excitations in this state up to second order in the narrow-band hopping and/or hybridisation. This allows to probe the mean-field stability of the excitonic insulator. The latter is found to be unstable when the case of the pure FKM (no hybridisation with a fully localised band) is approached. The instability is d…
In this work we investigate charge transport in one-dimensional (1D) insulators via semi-classical and perturbative renormalization group (RG) methods. We consider the problem of electron-electron, electron-phonon and electron-two-level system interactions. We show that non-linear collective modes such as polarons and solitons are reponsible for transport. We find a new excitation in the Mott insulator: the polaronic soliton. We discuss the differences between band and Mott insulators in terms of their spin spectrum and obtain the charge and spin gaps in each one of these systems. We show that…
We study the equilibrium dynamics of magnetic moments in the Mott insulating phase of the Hubbard model on the square and triangular lattice. We rewrite the Hubbard interaction in terms of an auxiliary vector field and use a recently developed Langevin scheme to study its dynamics. A thermal `noise', derivable approximately from the Keldysh formalism, allows us to study the effect of finite temperature. At strong coupling, $U \gg t$, where $U$ is the local repulsion and $t$ the nearest neighbour hopping, our results reproduce the well known dynamics of the nearest neighbour Heisenberg model wi…
Particle-hole continuum (PHC) for massive Dirac fermions in presence of short range interactions, provides an unprecedented opportunity for formation of two collective split-off states, one in the singlet and the other in the triplet (spin-1) channel in undoped system. Both poles are close in energy and are separated from thec continuum of free particle-hole excitations by an energy scale of the order of gap parameter $Δ$. They both disperse linearly with two different velocities reminiscent of spin-charge separation in Luttinger liquids. When the strength of Hubbard interactions is stronger t…
We show that doped Mott insulators exhibit a collective degree of freedom, not made out of the elemental excitations, because the number of single-particle addition states at low energy per electron per spin is greater than one. The presence of such a collective degree of freedom which is not a consequence of proximity to a phase transition is a consequence of dynamical spectral weight transfer from high to low energies. This physics is captured by the charge $2e$ boson that emerges by explicitly integrating out the high-energy scale in the Hubbard model. The charge $2e$ boson binds to a hole,…
To investigate the non-Fermi liquid behavior we consider the extended two-dimensional t-J model which includes additional hopping t''. In the regime t,J << t'' we were able to solve the model analytically. It has a very rich phase diagram including antiferromagnetic (AF) insulator and AF strange metal with different kinds of pseudospin-singlet superconducting pairings (p,d,g-waves). We also demonstrate a collective triplet excitation with energy below the superconducting gap
We propose a mechanism of the spin Seebeck effect attributed to excitonic condensation in a nonmagnetic insulator. We analyze a half-filled two-orbital Hubbard model with a crystalline field splitting in the strong coupling limit. In this model, the competition between the crystalline field and electron correlations brings about an excitonic insulating state, where the two orbitals are spontaneously hybridized. Using the generalized spin-wave theory and Boltzmann transport equation, we find that a spin current generated by a thermal gradient is observed in the excitonic insulating state withou…
Within the framework of periodic asymmetric Anderson model for Kondo isoulators an effective singlet-triplet Hamiltonian with indirect antiferromagnetic f-f exchange interaction is introduced which allows to study analytically the dynamic magnetic susceptibilities of f-electrons. The approach allows to describe the three-level spin excitation spectrum with a specific dispersion in $YbB_{12}$. Distinctive feature of the consideration is the introduction of small radius singlet and triplet collective f-d excitations which at movement on a lattice form low - and high-energy spin bands.
Condensed matter systems admit topological collective excitations above a trivial ground state, an example being Chern insulators formed by Dirac bosons with a gap at finite energies. However, in contrast to electrons, there is no particle-number conservation law for collective excitations. This gives rise to particle number-nonconserving many-body interactions whose influence on single-particle topology is an open issue of fundamental interest in the field of topological quantum materials. Taking magnons in ferromagnets as an example, we uncover topological magnon insulators that are stabiliz…
