Photoinduced intradomain dynamics and nonthermal switching of metastable states in the one-dimensional extended Peierls-Hubbard model

Abstract

We investigate the microscopic dynamics at the initial stage of photoinduced phase transitions in tetrathiafulvalene-$p$-chloranil by exact diagonalization. We first show that the one-dimensional extended Peierls-Hubbard model exhibits a neutral phase with small ionicity and negligible dimerization and an ionic phase with moderate ionicity and dimerization. Aside from these phases, we find a doubly ionized phase with strong dimerization that we call the "dipole" phase. These ground-state phases are characterized by various order parameters and the Zak phase, which is relevant to electronic polarization. We further explore the microscopic dynamics of the three phases triggered by short monocycle optical pulses. The electronic order parameters and lattice displacement suggest that the neutral-ionic, ionic-neutral, and dipole-ionic transitions are induced. Furthermore, clear spectroscopic changes are observed in the time-dependent spectral density and pump-probe conductivity. A detailed analysis of the spectroscopy demonstrates the generation of coherent charge-transfer strings via multiphoton absorption and the crucial roles of the excited states and the metastable ground state at the new lattice position for the ultrafast dynamics.

arXiv comment20 pages, 14 figures

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