Coherent dynamics of photoinduced nucleation processes

TL;DR

This paper investigates the initial nucleation dynamics in photoinduced structural changes of molecular crystals, emphasizing the role of coherent molecular distortions and multiple intermolecular interactions in the process.

Contribution

It introduces a minimal quantum model capturing nonadiabatic transitions and coherent molecular distortions essential for understanding photoinduced nucleation.

Findings

Coherent molecular distortions are crucial for successive electronic state conversion.

Multiple intermolecular interactions are necessary for nucleation.

The model successfully describes the dynamics of photoinduced structural change.

Abstract

We study the dynamics of initial nucleation processes of photoinduced structural change of molecular crystals. In order to describe the nonadiabatic transition in each molecule, we employ a model of localized electrons coupled with a fully quantized phonon mode, and the time-dependent Schr\"odinger equation for the model is numerically solved. We found a minimal model to describe the nucleation induced by injection of an excited state of a single molecule in which multiple types of intermolecular interactions are required. In this model coherently driven molecular distortion plays an important role in the successive conversion of electronic states which leads to photoinduced cooperative phenomena.