Resolving Femtosecond Solvent Reorganization Dynamics in an Iron Complex by Nonadiabatic Dynamics Simulations
Diana Bregenholt Zederkof, Klaus B. Møller, M. Nielsen, Kristoffer Haldrup, Leticia González, Sebastian Mai
Abstract
MC) character. We also find that solvent reorganization after excitation is ultrafast, on the order of 50 fs around the cyanides and slower around the bpy ligand. In contrast, the nuclear vibrational dynamics, in the form of Fe-ligand bond changes, takes place on slightly longer time scales. We demonstrate that the surprisingly fast solvent reorganizing should be observable in time-resolved X-ray solution scattering experiments, as simulated signals show strong contributions from the solute-solvent scattering cross term. Altogether, the simulations paint a comprehensive picture of the coupled and concurrent electronic, nuclear, and solvent dynamics and interactions in the first hundreds of femtoseconds after excitation.