Rescaling Classical Electron Transfer Energy as a Reaction Coordinate and Understanding the Influence of the Electrolyte Environment on the Reorganization Energy

This research elucidates a rescaling approach for calculating quantum energies associated with charge transfer reactions, significantly reducing the need for expensive Density Functional Theory (DFT) calculations. Our strategy involves estimating quantum electron-transfer (ET) energies through a comprehensive analysis of computationally economical classical MD data. Consequently, DFT calculations are now only necessary for rescaling the classical ET energies on a much smaller dataset. Notably, our research also highlights that quantum effects, such as charge delocalization, can provide additional stabilization following redox reactions, which is not accounted for in the classical ET energy distribution due to its inability to consider charge delocalization. Moreover, this work examines how variations in the electrolyte environment can alter the reorganization energy and, consequently, influence ET dynamics.