Interchain coupling effects on photoinduced phase transitions between neutral and ionic phases in an extended Hubbard model with alternating potentials and an electron-lattice coupling

TL;DR

This study investigates how interchain couplings influence photoinduced phase transitions in a quasi-one-dimensional extended Hubbard model, revealing nonlinear charge transfer behavior and conditions for coherent domain boundary motion.

Contribution

It demonstrates the significant role of interchain couplings in enabling coherent neutral-ionic domain boundary motion during photoinduced phase transitions.

Findings

Strong interchain couplings lead to synchronized neutral domain growth.

Threshold behavior observed in ionic-to-neutral transition.

Neutral-to-ionic transition shows almost linear charge transfer response.

Abstract

Dynamics of ionic-to-neutral and neutral-to-ionic phase transitions induced by intrachain charge-transfer photoexcitations are studied in a quasi-one-dimensional extended Hubbard model with alternating potentials and an electron-lattice coupling for mixed-stack charge-transfer complexes. For interchain couplings, we use electron-electron interactions previously estimated for TTF-CA (TTF=tetrathiafulvalene, CA=chloranil). Photoexcitation is introduced by a pulse of oscillating electric field. The time-dependent Hartree-Fock approximation is used for the electronic part, and the classical approximation for the lattice part. In the ionic-to-neutral transition, the transferred charge density is a strongly nonlinear function of the photoexcitation density, which is characterized by the presence of a threshold. With substantial interchain couplings comparable to those in TTF-CA, the interchain correlation is strong during the transition. Neutral domains in nearby chains simultaneously grow even if their nucleation is delayed by reducing the amplitude of the electric field. With weaker interchain couplings, the growing processes are in phase only when the amplitude of the electric field is large. Thus, the experimentally observed, coherent motion of a macroscopic neutral-ionic domain boundary is allowed to emerge by such substantial interchain couplings. In the neutral-to-ionic transition, by contrast, the transferred charge density is almost a linear function of the photoexcitation density. Interchain electron-electron interactions make the function slightly nonlinear, but the uncooperative situation is almost unchanged and consistent with the experimental findings.