Two-step model for ultrafast interfacial electron transfer: limitations of Fermi's golden rule revealed by quantum dynamics simulations.

ABSTRACT: Interfacial electron transfer (IET) is one of the crucial steps in the light-harvesting process that occurs in various assemblies for solar energy conversion, such as dye-sensitized solar cells or dye-sensitized photoelectrosynthesis cells. Computational studies of IET in dye-semiconductor assemblies employ a variety of approaches, ranging from phenomenological models such as Fermi's golden rule to more complex methods relying on explicit solutions of the time-dependent Schrödinger equation. This work investigates IET in a model pyridine-TiO₂ assembly, with the goals of assessing the validity of Fermi's golden rule for calculation of the IET rates, understanding the importance of conformational sampling in modeling the IET process, and establishing an approach to rapid computati

SUBMITTER: Liu C 

PROVIDER: S-EPMC5621017 | biostudies-literature | 2017 Sep

REPOSITORIES: biostudies-literature