Approaches to molecular devices based on controlled intramolecular electronic energy and electron transfer. Electron transfer rates through flexible molecular bridges by a time-dependent super exchange model

摘要

In this paper we propose to use intramolecular electron and electronic energy transfer as a way of connecting between logical operations that are implemented on different molecules. We have already shown that the rate of through-bond-mediated intramolecular singlet-singlet electronic energy transfer (EET) in certain rigid bichromophoric molecules is five orders of magnitude higher than that observed in flexibly linked systems containing the same donor-acceptor chromophores, for which through space EET via exchange interaction is dominant. This is the first direct evidence that the rigidity of the interchromophore bridge is significant for promoting through-bond bridge-mediated intramolecular EET. Preliminary results of a theoretical model for explaining this striking observation are discussed.