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arXiv:1907.01770 · Physical review. B./Physical review. B

Photoinduced electron-electron pairing in the extended Falicov-Kimball model

Ryo Fujiuchi, Tatsuya Kaneko, Y. Ohta, Seiji Yunoki

Published Jul 15, 2019• 17 citations
arXivHTMLPDF

Abstract

By employing the time-dependent exact diagonalization method, we investigate the photoexcited states of the excitonic insulator in the extended Falicov-Kimball model (EFKM). We here show that the pulse irradiation can induce the interband electron-electron pair correlation in the photoexcited states, while the excitonic electron-hole pair correlation in the initial ground state is strongly suppressed. We also show that the photoexcited states contain the eigenstates of the EFKM with a finite number of interband electron-electron pairs, which are responsible for the enhancement of the electron-electron pair correlation. The mechanism found here is due to the presence of the internal SU(2) pairing structure in the EFKM and thus it is essentially the same as that for the photoinduced $\ensuremath{\eta}$ pairing in the repulsive Hubbard model reported recently [T. Kaneko et al., Phys. Rev. Lett. 122, 077002 (2019)]. This also explains why the nonlinear optical response is effective to induce the electron-electron pairs in the photoexcited states of the EFKM. Furthermore, we show that, unlike the $\ensuremath{\eta}$ pairing in the Hubbard model, the internal SU(2) structure is preserved even for a nonbipartite lattice when the EFKM has the direct-type band structure, in which the pulse irradiation can induce the electron-electron pair correlation with momentum $\mathbit{q}=\mathbit{0}$ in the photoexcited states. We also discuss briefly the effect of a perturbation that breaks the internal SU(2) structure.

DOI
10.1103/physrevb.100.045121

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By employing the time-dependent exact diagonalization method, we investigate the photoexcited states of the excitonic insulator in the extended Falicov-Kimball model (EFKM). We here show that the pulse irradiation can induce the interband electron-electron pair correlation in the photoexcited states, while the excitonic electron-hole pair correlation in the initial ground state is strongly suppressed. We also show that the photoexcited states contain the eigenstates of the EFKM with a finite number of interband electron-electron pairs, which are responsible for the enhancement of the electron-electron pair correlation. The mechanism found here is due to the presence of the internal SU(2) pairing structure in the EFKM and thus it is essentially the same as that for the photoinduced \ensuremathη\ensuremath{\eta}\ensuremathη pairing in the repulsive Hubbard model reported recently [T. Kaneko et al., Phys. Rev. Lett. 122, 077002 (2019)]. This also explains why the nonlinear optical response is effective to induce the electron-electron pairs in the photoexcited states of the EFKM. Furthermore, we show that, unlike the \ensuremathη\ensuremath{\eta}\ensuremathη pairing in the Hubbard model, the internal SU(2) structure is preserved even for a nonbipartite lattice when the EFKM has the direct-type band structure, in which the pulse irradiation can induce the electron-electron pair correlation with momentum \mathbitq=\mathbit0\mathbit{q}=\mathbit{0}\mathbitq=\mathbit0 in the photoexcited states. We also discuss briefly the effect of a perturbation that breaks the internal SU(2) structure.
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 they decrease over time. This implies the possible metallization of Ta2NiSe5{\mathrm{Ta}}_{2}\mathrm{Ni}{\mathrm{Se}}_{5}Ta2​NiSe5​, a strong candidate for an excitonic insulator material, for which the EFKM is considered to be the minimal theoretical model. Simulating the photoemission with optimized pulse parameters, we demonstrate a photoinduced quantum phase transition, in accord with recent findings in time- and angle-resolved photoemission spectroscopy experiments on Ta2NiSe5{\mathrm{Ta}}_{2}\mathrm{Ni}{\mathrm{Se}}_{5}Ta2​NiSe5​.
By employing unbiased numerical methods, we show that pulse irradiation can induce unconventional superconductivity even in the Mott insulator of the Hubbard model. The superconductivity found here in the photoexcited state is due to the η-pairing mechanism, characterized by staggered pair-density-wave oscillations in the off-diagonal long-range correlation, and is absent in the ground-state phase diagram; i.e., it is induced neither by a change of the effective interaction of the Hubbard model nor by simple photocarrier doping. Because of the selection rule, we show that the nonlinear optical response is essential to increase the number of η pairs and thus enhance the superconducting correlation in the photoexcited state. Our finding demonstrates that nonequilibrium many-body dynamics is an alternative pathway to access a new exotic quantum state that is absent in the ground-state phase diagram, and also provides an alternative mechanism for enhancing superconductivity.
We study the excitonic phase transition in a system of the conduction band electrons and valence band holes described by the three-dimensional (3D) extended Falicov–Kimball (EFKM) model with the tunable Coulomb interaction UUU between both species. By lowering the temperature, the electron–hole system may become unstable with respect to the formation of the excitons, i.e, electron–hole pairs at temperature T=TΔT=T_{\Delta }T=TΔ​ , exhibiting a gap Δ\Delta Δ in the particle excitation spectrum. To this end we implement the functional integral formulation of the EFKM, where the Coulomb interaction term is expressed in terms of U(1) phase variables conjugate to the local particle number, providing a useful representation of strongly correlated system. The effective action formalism allows us to formulate a problem in the phase-only action in the form of the quantum rotor model and to obtain analytical formulas for the critical lines and other quantities of physical interest like charge gap, chemical potential and the correlation length.
We investigate the condition for the photoinduced enhancement of an excitonic order in a two-orbital Hubbard model, which has been theoretically proposed in our previous work [Phys. Rev. B 97, 115105 (2018)], and analyze it from the viewpoint of the Rabi oscillation. Within the mean-field approximation, we simulate real-time dynamics of an excitonic insulator with a direct gap, where the pair condensation in the initial state is of BEC nature and the photoexcitation is introduced by electric dipole transitions. We first discuss that in the atomic limit our model is reduced to a two-level system that undergoes the Rabi oscillation, so that for single cycle pulses physical quantities after the photoirradiation are essentially determined by the ratio of the Rabi frequency to the pump-light frequency. Then, it is shown that this picture holds even in the case of nonzero transfer integrals where each one-particle state exhibits the Rabi oscillation leading to the enhancement of the excitonic order. We demonstrate that effects of electron-phonon interactions do not alter the results qualitatively. We also examine many-body dynamics by the exact diagonalization method on small clusters, which strongly suggests that our mechanism for the enhancement of the excitonic order survives even when quantum fluctuations are taken into account.
We study the electron-hole pair (or excitonic) condensation in the extended Falicov-Kimball model at finite temperatures based on the cluster mean-field-theory approach, where we make the grand canonical exact-diagonalization analysis of small clusters using the sine-square deformation function. We thus calculate the ground-state and finite-temperature phase diagrams of the model, as well as its optical conductivity and single-particle spectra, thereby clarifying how the preformed pair states appear in the strong-coupling regime of excitonic insulators. We compare our results with experiment on Ta2_22​NiSe5_55​.
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 hybridization. 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 hybridization with a fully localized band) is approached. The instability is due to the presence of another, lower-lying ground state and not to the degeneracy of the excitonic phase in the pure FKM. The excitonic phase, however, may be stabilized further away from the pure FKM limit. In this case, the low-energy excitation spectrum contains important information about the properties of the excitonic condensate (including the strongly suppressed critical temperature).