Ultrafast Charge Migration in Molecules in Liquid Environment

Whereas most theoretical and experimental studies of attosecond charge migration (CM) have been in the gas phase, CM in the condensed phase remains poorly understood. In this study, we investigate the influence of a liquid-phase environment on CM, by comparing the dynamics induced in a bromoaniline molecule in isolation vs that in a molecule solvated in methanol. The solute-solvent environment is analyzed through molecular dynamics simulations, providing a range of environments for the bromoaniline molecule. Subsequently, the CM is initiated by placing a localized hole on the bromine atom using constrained density functional theory, and the ensuing dynamics are calculated using real-time time-dependent density functional theory. Our results reveal that CM is modulated by solvation, due to the polarizability of the first shell of methanol molecules.