We study the electronic phase diagram of the excitonic insulator candidates Ta$_2$Ni(Se$_{1-x}$S$_x$)$_5$ [x=0, ... ,1] using Raman spectroscopy. Critical excitonic fluctuations are observed, that diminish with $x$ and ultimately shift to high energies, characteristic of a quantum phase transition. Nonetheless, a symmetry-breaking transition at finite temperatures is detected for all $x$, exposing a cooperating lattice instability that takes over for large $x$. Our study reveals a failed excitonic quantum phase transition, masked by a preemptive structural order.
Trion gas on the surface of a failed excitonic insulator
Technion（以色列理工学院）；Tel Aviv University（特拉维夫大学）；Center for Light-Matter Interaction, Tel Aviv University（特拉维夫大学光物质相互作用中心）；SOLEIL Synchrotron（索雷尔同步辐射中心）；Helmholtz-Zentrum Berlin für Materialien und Energie（柏林亥姆霍兹材料与能源中心）；IMDEA Nanoscience（IMDEA纳米科学研究所）
We consider a two-orbital Hubbard model with Hund coupling and crystal-field splitting and show that in the vicinity of the high-spin/low-spin transition, crystal-field quenches can induce an excitonic condensation at initial temperatures above the highest ordering temperature in equilibrium. This condensation is the effect of an increase in the spin entropy and an associated cooling of the effective electronic temperature. We identify a dynamical phase transition and show that such quenches can result in long-lived nonthermal excitonic condensates which have no analogue in the equilibrium pha…
We performed ultrasonic measurements on (Ta$_{0.952}$V$_{0.048}$)$_2$NiSe$_5$ to investigate the contribution of acoustic phonons at the zone center to structural and possible excitonic transitions. The transverse elastic constant $C_{55}$ with irreducible representation $B_\mathrm{2g}$ exhibits softening over 90\% above a transition temperature of $T_\mathrm{s} = 280$ K, indicating the soft mode of corresponding TA phonons. Our analysis based on the quadrupole response indicates that the electron-phonon interaction contributes to the excitonic transition in addition to the hybridization betwe…
The origin of the second order phase transition at 328K in Ta$_2$NiSe$_5$, a prominent candidate for direct gap excitonic insulator, remains under fervent debate. The driving force for the transition can be revealed by identification of the soft mode's origin that may be deducted from polarization resolved Raman scattering experiments. Such studies were recently reported in [arXiv:2007.07344 (2020)], [arXiv:2102.07912 (2021)], [arXiv:2007.01723 (2020)] and [arXiv:2007.08212 (2020)]. In this Comment, it is shown that the parameters derived in a recent arXiv by Kwangrae Kim et. al. [arXiv:2007.0…
The layered compound $\mathrm{Ta_2NiSe_5}$ is a quasi-one-dimensional and narrow-gap semiconductor, which is proposed to undergo a transition to an excitonic insulator at $T_\mathrm{c}=326$ K. We found a clear anomaly at $T_\mathrm{c}$ in the in-plane thermal conductivities both parallel ($\parallel$ $a$) and perpendicular ($\parallel$ $c$) to the one-dimensional chains, $κ_\mathrm{a}$ and $κ_\mathrm{c}$. While $κ_\mathrm{a}$ shows a rapid decrease below $T_\mathrm{c}$, $κ_\mathrm{c}$ shows a pronounced V-shaped suppression centered at $T_\mathrm{c}$. We argue that the decrease of $κ_\mathrm{a…
The effects associated with exciton Bose condensate formation in strongly correlated spin crossover systems are considered within the effective Hamiltonian obtained from the two-orbital Hubbard-Kanamori model. The collective excitations spectrum at various points of the temperature-crystal field phase diagram is calculated. The role of the electron-phonon interaction is discussed. The exciton and magnetic order photoenhancement (induction) in strongly correlated spin crossover systems a new mechanism based on the cooperative effect of electron-phonon and interatomic exchange interactions and t…
While excitonic instabilities in multiorbital systems recently have come under scrutiny in a variety of transition-metal compounds, understanding emergence of these instabilities from strong electronic interactions has remained a challenge. Here, we present a sign-problem-free determinant quantum Monte Carlo study of excitonic density orders in a half-filled two-orbital Hubbard-Kanamori model with broken orbital degeneracy, which accounts for the role of Hund's coupling in transition-metal compounds. For strong inverted (negative) Hund's exchange, we find numerical evidence for the emergence o…
We use the density-matrix-renormalization-group (DMRG) method to study the combined effects of nonlocal interactions on valence transitions and the formation of excitonic bound states in the generalized Falicov-Kimball model. In particular, we consider the nearest-neighbour Coulomb interaction $U_{nn}$ between two $d$, two $f$, $d$ and $f$ electrons as well as the so-called correlated hopping term $U_{ch}$ and examine their effects on the density of conduction $n_d$ (valence $n_f$) electrons and the excitonic momentum distribution $N(q)$. It is shown that $U_{nn}$ and $U_{ch}$ exhibit very str…
Excitonic insulator is a coherent electronic phase that results from the formation of a macroscopic population of bound particle-hole pairs - excitons. With only a few candidate materials known, the collective excitonic behavior is challenging to observe, being obscured by crystalline lattice effects. Here we use polarization-resolved Raman spectroscopy to reveal the quadrupolar excitonic mode in the candidate zero-gap semiconductor Ta$_2$NiSe$_5$ disentangling it from the lattice phonons. The excitonic mode pronouncedly softens close to the phase transition, showing its electronic character, …
The excitonic insulator Ta$_2$NiSe$_5$ experiences a first-order structural transition under pressure from rippled to flat layer-structure at Ps = 3 GPa, which drives the system from an almost zero-gap semiconductor to a semimetal. The pressure-induced semimetal, with lowering temperature, experiences a transition to another semimetal with a partial-gap of 0.1-0.2 eV, accompanied with a monoclinic distortion analogous to that occurs at the excitonic transition below Ps. We argue that the partial-gap originates primarily from a symmetry-allowed hybridization of Ta-conduction and Ni-valence band…
In this paper, first, we present a general formulation to investigate the ground-state and elementary excitations of an excitonic insulator (EI) in real materials. In addition, we discuss the out-of-equilibrium state induced (albeit transiently) by high-intensity light illumination of a conventional two-dimensional (2D) insulator. We then, present various band-structure models which allow us to study the transition from a conventional insulator to an EI in 2D materials as a function of the dielectric constant, the conventional insulator gap (and chemical potential), the bandwidths of the condu…
Excitonic condensation of strongly correlated electrons: the case of Pr$_{0.5}$Ca$_{0.5}$CoO$_3$
我们使用动态平均场模型计算和LDA+U材料特定计算相结合的方法研究了（Pr $_{1-y}$ R $_y$）$_x$ Ca $_{1-x}$ CoO $_3$（R=Nd，Sm，Eu，Gd，Tb，Y）系列化合物（PCCO）的低温相变.转变，标志着由一个尖锐的峰值在比热，导致直流电阻率的指数增加和磁化率的下降，但尚未确定序参量。我们表明，凝聚的自旋三重态，原子大小的激子提供了一个一致的解释所观察到的物理。特别是，它解释了交换分裂的Pr网站和同时Pr价跃迁。PCCO中的激子凝聚是在自旋态转变附近的某些系统中预期的一般行为的示例。
Engineering excitonic metal-insulator transitions in ultra-thin doped copper sulfides
Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences（中国科学院上海高等研究院）；Hefei National Laboratory（合肥国家实验室）
Ta$_2$NiSe$_5$ became one of the most investigated candidate materials for hosting an excitonic insulator ground state. Many studies describe the corresponding phase transition as a condensation of excitons breaking a continuous symmetry. This view got challenged recently pointing out the importance of the loss of two mirror symmetries at a structural phase transition that occurs together with the semiconductor-excitonic insulator transition. For such a scenario an unstable optical zone-center phonon at low energy is proposed to drive the transition. Here we report on the experimental observat…
In this paper, the effects of the external transverse magnetic field $B$ (perpendicular to the surface of the layers) on the electronic and excitonic properties are studied in the AA-stacked bilayer graphene (BLG). The effects of the Coulomb interactions and excitonic pairing have been taken into account and analyzed in detail within the bilayer Hubbard model. Both half-filling and partial filling regimes have been taken into account and the magnetic field dependence of a series of physical parameters was found. It is shown that the difference between the average electron concentrations in the…
We investigate the non-equilibrium electronic structure and characteristic time scales in a candidate excitonic insulator, Ta$_2$NiSe$_5$, using time- and angle-resolved photoemission spectroscopy with a temporal resolution of 50 fs. Following a strong photoexcitation, the band gap closes transiently within 100 fs, i.e., on a time scale faster than the typical lattice vibrational period. Furthermore, we find that the characteristic time associated with the rise of the photoemission intensity above the Fermi energy decreases with increasing excitation strength, while the relaxation time of the …
1T-TiSe2 has a semimetallic band structure at room temperature and undergoes phase transition to a triple-q charge density wave (CDW) state with a commensurate superlattice structure (2a * 2a * 2c) below Tc ~ 200 K at ambient pressure. This phase transition is caused by cooperative phenomena involving electron-phonon and electron-hole (excitonic) interactions, and cannot be described by a standard CDW framework. By Cu intercalation or the application of pressure, this phase transition temperature is suppressed and superconductivity (SC) appears. However, it is not clear what kind of order para…
Coulomb attraction between electrons and holes in a narrow-gap semiconductor or a semimetal is predicted to lead to an elusive phase of matter dubbed 'excitonic insulator'. However, direct observation of such electronic instability remains extremely rare. Here, we report the observation of incipient divergence in the static excitonic susceptibility of the candidate material Ta2NiSe5 using Raman spectroscopy. Critical fluctuations of the excitonic order parameter give rise to quasi-elastic scattering of B2g symmetry, whose intensity grows inversely with temperature toward the Weiss temperature …
Utilizing the time-dependent density-matrix renormalization group technique, we numerically prove photoinduced pairing states in the extended Falicov-Kimball model (EFKM) at half filling, both with and without internal SU(2) symmetry. In the time-dependent photoemission spectra an extra band appears above the Fermi energy after pulse irradiation, indicating an insulator-to-metal transition. Even in the absence of the SU(2) structure, the pair correlations are enhanced during the pump, and afterwards decrease over time. This implies the possible metallization of Ta$_2$NiSe$_5$, a strong candida…
We introduce a generalized Gross-Neveu (GN) model to describe the excitonic instabilities in two different systems: a small overlap semi-metal (SM) and a small gap semi-conductor (SMC), both in two (2d) and three-dimensions (3d). We identify the excitonic order parameter (EOP) and obtain the effective potential within the Large $N$ limit approach where the GN model can be exactly solved. We obtain the excitonic insulator (EI) phase diagrams as a function of temperature, chemical potential, overlap between bands and gaps of the system. We show that the EI may undergo first- or second-order ther…
Substrate tuning of the structural and electronic transition in thin flakes of the excitonic insulator candidate Ta$_2$NiSe$_5$
Max Planck Institute for Solid State Research（马克斯·普朗克固体研究所）；Institute for Functional Matter and Quantum Technologies, University of Stuttgart（斯图加特大学功能物质与量子技术研究所）；Department of Physics, University of Tokyo（东京大学物理系）
We study the thermal conductivity in the excitonic insulator using a simple quasi one-dimensional two-band model consisting of electron and hole bands with the Coulomb interactions between these bands. Based on the linear response theory within a mean-field scheme, we develop a method to identify the contributions to thermal conductivity driven by excitonic insulator. It is found that there is an additional heat current operator owing to the excitonic phase transition, and that it gives contributions to thermal conductivity which are not expressed in the form of Sommerfeld-Bethe relations writ…
