No Arabic abstract
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 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.
We study the dynamics of excitonic insulators coupled to phonons. Without phonon couplings, the linear response is given by the damped amplitude oscillations of the order parameter with frequency equal to the minimum band gap. A phonon coupling to the interband transfer integral induces two types of long-lived collective oscillations of the amplitude, one originating from the phonon dynamics and the other from the phase mode, which becomes massive. We show that even for small phonon coupling, a photo-induced enhancement of the exciton condensation and the gap can be realized. Using the Anderson pseudo-spin picture, we argue that the origin of the enhancement is a cooperative effect of the massive phase mode and the Hartree shift induced by the photo excitation. We also discuss how the enhancement of the order and the collective modes can be observed with time-resolved photo-emission spectroscopy.
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 electron population towards equilibrium shows an opposite behaviour. We argue that these experimental observations can be consistently explained by an excitonic origin of the band gap in the material. The excitonic picture is supported by microscopic calculations based on the non-equilibrium Greens function formalism for an interacting two-band system. We interpret the speedup of the rise time with fluence in terms of an enhanced scattering probability between photo-excited electrons and excitons, leading to an initially faster decay of the order parameter. We show that the inclusion of electron-phonon coupling at a semi-classical level changes only the quantitative aspects of the proposed dynamics, while the qualitative features remain the same. The experimental observations and microscopic calculations allow us to develop a simple and intuitive phenomenological model that captures the main dynamics after photoexcitation in Ta$_2$NiSe$_5$.
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.
Ultrafast light pulses can modify the electronic properties of quantum materials by perturbing the underlying, intertwined degrees of freedom. In particular, iron-based superconductors exhibit a strong coupling among electronic nematic fluctuations, spins, and the lattice, serving as a playground for ultrafast manipulation. Here we use time-resolved x-ray scattering to measure the lattice dynamics of photo-excited BaFe2As2. Upon optical excitation, no signature of an ultrafast change of the crystal symmetry is observed, but the lattice oscillates rapidly in time due to the coherent excitation of an A1g mode that modulates the Fe-As-Fe bond angle. We directly quantify the coherent lattice dynamics and show that even a small photo-induced lattice distortion can induce notable changes in the electronic and magnetic properties. Our analysis implies that transient structural modification can generally be an effective tool for manipulating the electronic properties of multi-orbital systems, where electronic instabilities are sensitive to the orbital character of bands near the Fermi level.