Direct dynamics simulations of photoexcited charge-transfer-to-solvent states of the I−(H2O)6 cluster

Direct molecular dynamics simulations have been carried out to understand the relaxation dynamics of photoexcited charge-transfer-to-solvent (CTTS) states for the I−(H2O)6 cluster and the subsequent excess electron stabilization dynamics by solvent molecules. Due to a small singlet–triplet splitting, the lowest triplet potential energy surface at the B3LYP-level calculations was used to model the CTTS singlet excited-state surface. Two book-type structures, which correspond to the lowest ground-state minimum-energy geometries, were vertically excited with the initial kinetic energy being zero. Although these two structures have a very similar geometry, it was found that the excess electron localization dynamics was totally different.