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Physical Review B

Photoinduced Hubbard band mixing due to ultrafast laser irradiation of a one-dimensional Mott insulator

J. D. Lee, Jun‐ichi Inoue

Published Nov 28, 2007• 16 citations
Publisher

Abstract

Based on the nonperturbative many-body time-dependent approach, photoinduced Hubbard band mixing by ultrashort laser pulse is found in a one-dimensional half-filled Hubbard model through the optical conductivity. The nonlinear development of Drude-like (metallic) weight in the resonant optical pumping (${\ensuremath{\omega}}_{\mathrm{pu}}\ensuremath{\approx}{E}_{g}$; ${\ensuremath{\omega}}_{\mathrm{pu}}$ is the pumping laser energy and ${E}_{g}$ is the gap energy) indicates reconstruction and mixing of the upper and lower Hubbard bands, in contrast to the case of linear development in off-resonant pumping $({\ensuremath{\omega}}_{\mathrm{pu}}⪢{E}_{g})$ where the rigid band picture is valid. The photoemission response after the ultrashort pulse confirms our finding.

DOI
10.1103/physrevb.76.205121

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Based on the nonperturbative many-body time-dependent approach, photoinduced Hubbard band mixing by ultrashort laser pulse is found in a one-dimensional half-filled Hubbard model through the optical conductivity. The nonlinear development of Drude-like (metallic) weight in the resonant optical pumping (\ensuremathωpu\ensuremath≈Eg{\ensuremath{\omega}}_{\mathrm{pu}}\ensuremath{\approx}{E}_{g}\ensuremathωpu​\ensuremath≈Eg​; \ensuremathωpu{\ensuremath{\omega}}_{\mathrm{pu}}\ensuremathωpu​ is the pumping laser energy and Eg{E}_{g}Eg​ is the gap energy) indicates reconstruction and mixing of the upper and lower Hubbard bands, in contrast to the case of linear development in off-resonant pumping (\ensuremathωpu⪢Eg)({\ensuremath{\omega}}_{\mathrm{pu}}⪢{E}_{g})(\ensuremathωpu​⪢Eg​) where the rigid band picture is valid. The photoemission response after the ultrashort pulse confirms our finding.
We study photoinduced optical responses of one-dimensional strongly correlated electron systems. The optical conductivity spectra are calculated for the ground state and a photoexcited state in the one-dimensional Hubbard model at half filling by using the exact diagonalization method. It is found that, in the Mott insulator phase, the photoexcited state has large spectral weights including the Drude weight below the optical gap. As a consequence, the spectral weight above the optical gap is largely reduced. These results imply that a metallic state is induced by photoexcitation. Comparison between the photoexcited and hole-doped states shows that the photoexcitation is similar to chemical doping.
Abstract Utilizing the time-dependent Lanczos method, we investigate the photoexcitation dynamics of the one-dimensional (1D) extended Peierls–Hubbard model at quarter filling. In equilibrium, it is well established that introducing the nearest-neighbour interaction V into the 1D Peierls–Hubbard model can lead to the formation of Mott–Hubbard excitons, which exhibit a characteristic frequency in the optical conductivity that is lower than the Mott gap. Ultrafast photoexcitation of this model gives rise to a transient metallic state for V < 2, characterized by several features, including a zero-frequency Drude peak in the post-pump optical conductivity, an increase in the density of charge carriers, and enhanced electron hopping between dimers. In contrast, when V ≥ 2, this metallic state is no longer observed, as photoinduced carriers bind to form excitons, thereby inhibiting metallic behavior. These results highlight a parallel between the optical excitation of the 1D extended Peierls–Hubbard model at quarter filling and that of the 1D extended Hubbard model at half filling, suggesting a universal mechanism governing their photoinduced responses.
Utilizing the exact diagonalization method, we investigate the one-dimensional Peierls-Hubbard model at quarter filling, where it manifests as an antiferromagnetic Mott insulator in units of dimers. By increasing the on-site Coulomb repulsion UUU, we observe a significant suppression of the Drude peak, based on a nonequilibrium linear-response theory capable of capturing the zero-frequency (Drude) weight of the optical conductivity under periodic boundary conditions. However, after the ultrafast photoirradiation of this model with large UUU, we detect a distinct enhancement of the Drude peak, signifying the onset of a photoinduced insulator-metal transition. Comparing these dynamics with the half-filled Hubbard model and a noninteracting spinless half-filled Su-Schrieffer-Heeger model (corresponding to the quarter-filled Peierls-Hubbard model with infinite UUU), we propose a mechanism for the photoinduced metallic state: The empty-occupied and double-occupied dimers serve as the photoinduced charge carriers, akin to the holons and doublons in the Hubbard model.
Abstract Motivated by the recent progress in time-resolved nonequilibrium spectroscopy in condensed matter, we study an optically excited one-dimensional ionic Hubbard model by exact diagonalization. The model is relevant to organic crystals, transition metal oxides, or ultracold atoms in optical lattices. We implement numerical pump-probe measurements to calculate time-dependent conductivity and single-particle spectral functions. In general, short optical excitation induces a metallic behavior imprinted as a Drude peak in conductivity or an in-gap density of states. In a Mott insulator, we find that the induced Drude peak oscillates at the pump frequency and its second harmonic. The former comes from the oscillation of currents, and the latter from the interference of single- and three-photon excited states. In a band insulator, the Drude peak oscillates only at the pump frequency, and quantities such as the double occupancy do not oscillate. The absence of the second harmonic oscillation is due to the degeneracy of multi-photon excited states. The in-gap density of states in both insulators correlates with the Drude weight and the energy absorption for weak pumping. Strong pumping leads to saturation of the in-gap density of states and to suppression of the Drude weight in the Mott regime. We have also checked that the above features are robust for insulators in the intermediate parameter range. Our study demonstrates the distinct natures of the multi-photon excited states in two different insulators.
We use time-evolution techniques for (infinite) matrix product states to calculate, directly in the thermodynamic limit, the time-dependent photoemission spectra and dynamic structure factors of the half-filled Hubbard chain after pulse irradiation.These quantities exhibit clear signatures of the photoinduced phase transition from insulator to metal that occurs because of the formation of so-called η pairs.In addition, the spin dynamic structure factor loses spectral weight in the whole momentum space, reflecting the suppression of antiferromagnetic correlations due to the buildup of η-pairing states.The numerical method demonstrated in this work can be readily applied to other one-dimensional models driven out of equilibrium by optical pumping.
We define, compute, and analyze the nonequilibrium differential optical conductivity of the one-dimensional extended Hubbard model at half-filling after applying a pump pulse, using the time-dependent density matrix renormalization group method. The melting of the Mott insulator is accompanied by a suppression of the local magnetic moment and ensuing photogeneration of doublon-holon pairs. The differential optical conductivity reveals (i) mid-gap states related to parity-forbidden optical states and (ii) strong renormalization and hybridization of the excitonic resonance and the absorption band, yielding a Fano resonance. We offer evidence and interpret such a resonance as a signature of nonequilibrium optical excitations resembling excitonic strings, (bi)excitons, and unbound doublon-holon pairs, depending on the magnitude of the intersite Coulomb repulsion. We discuss our results in the context of pump and probe spectroscopy experiments on organic Mott insulators.