A wave packet model for electron transfer and its implications for the semiconductor-liquid interface

This paper establishes the computational feasibility and examines the impli cations of a particular technique for simulations of time dependent electro n transfer (ET) at semiconductor-liquid interfaces (SLIs). The methodology uses a one electron formalism employing wave packets, pseudopotentials, and molecular dynamics, which we dub WPMD. We describe a detailed mechanism fo r SLI ET by using the methodology. The model is versatile enough to address conventional SLI ET, surface state and adsorption mediated ET, photoexcite d ET, and ET between quantum dots and other microstructures. We contrast th e perspectives of our WPMD model of SLI ET with those in traditional litera ture and find substantial differences. The use of standard Landau-Zener the ory for SLI ET is found particularly problematic.