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Mass Imbalance Effects in the Excitonic Condensation of the Extended Falicov–Kimball Model

Quoc-Huy Ninh, Van‐Nham Phan

Published Mar 19, 2021• 3 citations
Publisher

Abstract

The ground‐state properties of the excitonic condensation state in the effects of the mass imbalance are discussed in the framework of the spinless extended Falicov–Kimball model, in which the hopping of the f electrons is involved. Using the unrestricted Hartree–Fock approximation, a set of self‐consistent equations are obtained so the excitonic condensate order parameter is determined. In this sense, the real part of the optical conductivity is analytically calculated based on the Kubo formula. Phase diagram releases a complex phase structure of the excitonic condensation state with a strong depression of its Bardeen–Cooper–Schrieffer (BCS)–Bose–Einstein condensation (BEC) crossover in the influence of the mass imbalance. The impression of the mass imbalance affecting the excitonic condensate is also addressed in the signature of the optical conductivity. The finding delivers the natural scenario of the excitonic condensation state applied for a wide range of materials, from transition‐metal dichalcogenides to double‐layer systems such as a semiconductor double quantum well, double‐bilayer graphene, or double‐layer graphene.

DOI
10.1002/pssb.202000564

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The ground‐state properties of the excitonic condensation state in the effects of the mass imbalance are discussed in the framework of the spinless extended Falicov–Kimball model, in which the hopping of the f electrons is involved. Using the unrestricted Hartree–Fock approximation, a set of self‐consistent equations are obtained so the excitonic condensate order parameter is determined. In this sense, the real part of the optical conductivity is analytically calculated based on the Kubo formula. Phase diagram releases a complex phase structure of the excitonic condensation state with a strong depression of its Bardeen–Cooper–Schrieffer (BCS)–Bose–Einstein condensation (BEC) crossover in the influence of the mass imbalance. The impression of the mass imbalance affecting the excitonic condensate is also addressed in the signature of the optical conductivity. The finding delivers the natural scenario of the excitonic condensation state applied for a wide range of materials, from transition‐metal dichalcogenides to double‐layer systems such as a semiconductor double quantum well, double‐bilayer graphene, or double‐layer graphene.
Low-energy excitations of the excitonic states in the semimetal and semiconducting materials described by the extended Falicov-Kimball model with phonon correlation are investigated. In the framework of the unrestricted Hartree-Fock approximation, we derive a set of self-consistent equations to find the quasiparticle energies and excitonic condensate order parameters. The real part of the optical conductivity and then the dynamical excitonic susceptibility function are analytically evaluated by means of the linear response theory. Numerical results reveal the significant expansion of the excitonic condensation window in the temperature--Coulomb interaction plane by lowering the mass imbalance. Under the influence of the mass imbalance and thermal fluctuations, the BCS-BEC crossover of the excitonic condensation states has been also addressed in the collective mode signatures of the optical conductivity. Out of the condensation state, the collective excitation of the excitonic bound state is examined by analyzing the imaginary part of the dynamical excitonic susceptibility function. At large mass imbalance and low thermal fluctuations, we find an extremely sharp peak with high intensity at low frequency in the imaginary part of the dynamical excitonic susceptibility spectrum, specifying the long-lifetime exciton existence before it becomes condensed.
Using exact numerical techniques, we investigate the nature of excitonic (electron-hole) bound states and the development of exciton coherence in the one-dimensional half-filled extended Falicov-Kimball model. The ground-state phase diagram of the model exhibits, besides band-insulator and staggered orbital ordered phases, an excitonic insulator (EI) with power-law correlations. The criticality of the EI state shows up in the von Neumann entropy. The anomalous spectral function and condensation amplitude provide the binding energy and coherence length of the electron-hole pairs which, on their part, point towards a Coulomb interaction driven crossover from BCS-like electron-hole pairing fluctuations to tightly bound excitons. We show that while a mass imbalance between electrons and holes does not affect the location of the BCS-BEC crossover regime, it favors staggered orbital ordering to the disadvantage of the EI. Within the Bose-Einstein condensation (BEC) regime, the quasiparticle dispersion develops a flat valence-band top, in accord with the experimental finding for Ta2NiSe5.
We report on small-cluster exact-diagonalization calculations which prove the formation of electron-hole pairs (excitons) as a prerequisite for spontaneous interlayer phase coherence in double-layer systems described by the extended Falicov-Kimball model. Evaluating the anomalous Green's function and momentum distribution function of the pairs, and thereby analyzing the dependence of the exciton binding energy, condensation amplitude, and coherence length on the Coulomb interaction strength, we demonstrate a crossover between a BCS-like electron-hole pairing transition and a Bose-Einstein condensation of tightly bound preformed excitons. We furthermore show that a mass imbalance between electrons and holes tends to suppress the condensation of excitons.
We investigate single-particle properties of a mass-imbalanced Fermi gas in the BCS (Bardeen-Cooper-Schrieffer)--BEC (Bose-Einstein condensation) crossover region. In the presence of mass imbalance, we point out that the ordinary TTT-matrix approximation, which has been extensively used to clarify various BCS-BEC crossover physics in the mass-balanced case, unphysically gives a double-valued solution in terms of the superfluid phase transition temperature Tc{T}_{\mathrm{c}}Tc​ in the crossover region. To overcome this serious problem, we include higher order strong-coupling corrections beyond the TTT-matrix level. Using this extended TTT-matrix theory, we calculate single-particle excitations in the normal state above Tc{T}_{\mathrm{c}}Tc​. The so-called pseudogap phenomena originating from pairing fluctuations are shown to be different between the light-mass component and heavy-mass component, which becomes more remarkable at higher temperatures. Since Fermi condensates with hetero-Cooper pairs have recently been discussed in various fields, such as exciton (polariton) condensates as well as color superconductivity, our results would be useful for the further development of Fermi superfluid physics, beyond the conventional superfluid state with homo-Cooper pairs.
We study the spontaneous symmetry breaking of the excitonic insulator state induced by the Coulomb interaction UUU in the two-dimensional extended Falicov-Kimball model. Using the variational cluster approximation (VCA) and Hartree-Fock approximation (HFA), we evaluate the order parameter, single-particle excitation gap, momentum distribution functions, coherence length of excitons, and single-particle and anomalous excitation spectra as functions of UUU at zero temperature. We find that in the weak-to-intermediate coupling regime, the Fermi surface plays an essential role and calculated results can be understood in close correspondence with the BCS theory, whereas in the strong-coupling regime, the Fermi surface plays no role and results are consistent with the picture of a Bose-Einstein condensate (BEC). Moreover, we find that HFA works well in both the weak- and strong-coupling regimes, and that the difference between the results of VCA and HFA mostly appears in the intermediate-coupling regime. The reason for this is discussed from a viewpoint of the self-energy. We thereby clarify the excitonic insulator state that typifies either a BCS condensate of electron-hole pairs (weak-coupling regime) or a BEC of preformed excitons (strong-coupling regime).
Based on the SO(2)\mathrm{SO}(2)SO(2)-invariant slave-boson scheme, the static charge, orbital, and excitonic susceptibilities in the extended Falicov--Kimball model are calculated. Analyzing the phase without long-range order, we find instabilities toward charge order, orbital order, and the excitonic insulator (EI) phase. The instability toward the EI is in agreement with the saddle-point phase diagram. We also evaluate the dynamic excitonic susceptibility, which allows the investigation of uncondensed excitons. We find qualitatively different features of the exciton dispersion at the semimetal-EI and at the semiconductor-EI transition supporting a crossover scenario between a BCS-type electron-hole condensation and a Bose--Einstein condensation of preformed bound electron-hole pairs.