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Register a new userPhoto-excited Dynamics in the Excitonic Insulator Ta2NiSe5
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The excitonic insulator is an intriguing correlated electron phase formed of condensed excitons. A promising candidate is the small band gap semiconductor Ta2NiSe5. Here we investigate the quasiparticle and coherent phonon dynamics in Ta2NiSe5 in a time resolved pump probe experiment. Using the models originally developed by Kabanov et al. for superconductors, we show that the materials intrinsic gap can be described as almost temperature independent for temperatures up to about 250 K to 275 K. This behavior supports the existence of the excitonic insulator state in Ta2NiSe5. The onset of an additional temperature dependent component to the gap above these temperatures suggests that the material is located in the BEC-BCS crossover regime. Furthermore, we show that this state is very stable against strong photoexcitation, which reveals that the free charge carriers are unable to effectively screen the attractive Coulomb interaction between electrons and holes, likely due to the quasi one-dimensional structure of Ta2NiSe5.
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We study the photo-induced dynamics of the excitonic insulator in the two-band Hubbard model on the Penrose tiling by means of the time-dependent real-space mean-field approximation. We show that, with a single-cycle electric-field pulse, the bulk (spatially averaged) excitonic order parameter decreases in the BCS regime, while it increases in the BEC regime. To clarify the dynamics peculiar to the Penrose tiling, we examine the coordination number dependence of observables and analyze the perpendicular space. In the BEC regime, characteristic oscillations of the electron number at each site are induced by the pulse, which are not observed in normal crystals. On the other hand, the dynamics in the BCS regime is characterized by drastic change in the spatial pattern of the excitonic order parameter.
The excitonic insulator is an intriguing electronic phase of quasi-condensed excitons. A prominent candidate is the small bandgap semiconductor Ta2NiSe5, in which excitons are believed to undergo a BEC-like transition. But experimental evidence for the existence of a coherent condensate in this material is still missing. A direct fingerprint of such a state would be the observation of its collective modes, which are equivalent to the Higgs- and Goldstone-modes in superconductors. Here we report evidence for the existence of a coherent amplitude response in the excitonic insulator phase of Ta2NiSe5. Using non-linear excitations with short laser pulses we identify a phonon-coupled state of the condensate that can be understood as a coupling of its electronic Higgs-mode to a low frequency phonon. The Higgs-mode contribution substantiates the picture of an electronically driven phase transition and characterizes the transient order parameter of the excitonic insulator as a function of temperature and excitation density.
Using a nonequilibrium implementation of the extended dynamical mean field theory (EDMFT) we simulate the relaxation after photo excitation in a strongly correlated electron system with antiferromagnetic spin interactions. We consider the $t$-$J$ model and focus on the interplay between the charge- and spin-dynamics in different excitation and doping regimes. The appearance of string states after a weak photo excitation manifests itself in a nontrivial scaling of the relaxation time with the exchange coupling and leads to a correlated oscillatory evolution of the kinetic energy and spin-spin correlation function. A strong excitation of the system, on the other hand, suppresses the spin correlations and results in a relaxation that is controlled by hole scattering. We discuss the possibility of detecting string states in optical and cold atom experiments.
We show that finite temperature variational cluster approximation (VCA) calculations on an extended Falicov-Kimball model can reproduce angle-resolved photoemission spectroscopy (ARPES) results on Ta2NiSe5 across a semiconductor-to-semiconductor structural phase transition at 325 K. We demonstrate that the characteristic temperature dependence of the flat-top valence band observed by ARPES is reproduced by the VCA calculation on the realistic model for an excitonic insulator only when the strong excitonic fluctuation is taken into account. The present calculations indicate that Ta2NiSe5 falls in the Bose-Einstein condensation regime of the excitonic insulator state.
We investigate the effect of nonlocal interactions on the photo-doped Mott insulating state of the two-dimensional Hubbard model using a nonequilibrium generalization of the dynamical cluster approximation. In particular, we compare the situation where the excitonic states are lying within the continuum of doublon-holon excitations to a set-up where the excitons appear within the Mott gap. In the first case, the creation of nearest-neighbor doublon-holon pairs by excitations across the Mott gap results in enhanced excitonic correlations, but these excitons quickly decay into uncorrelated doublons and holons. In the second case, photo-excitation results in long-lived excitonic states. While in a low-temperature equilibrium state, excitonic features are usually not evident in single-particle observables such as the photoemission spectrum, we show that the photo-excited nonequilibrium system can exhibit in-gap states associated with the excitons. The comparison with exact-diagonalization results for small clusters allows us to identify the signatures of the excitons in the photo-emission spectrum.
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