Welcome to the new version of CaltechAUTHORS. Login is currently restricted to library staff. If you notice any issues, please email coda@library.caltech.edu
Published October 16, 2003 | public
Journal Article

Variable-range hopping electron transfer through disordered bridge states: Application to DNA

Abstract

A theory for electron transfer through a donor−bridge−acceptor system is described that involves tunneling and hopping-like transfers and an intermediate regime. The theory considers how a delocalization of electronic states and static and dynamic disorder in electronic energies influence the charge transfer rate and is used to study experiments on hole transfer through DNA. While an exponential distance dependence of the yield of hole trapping is observed experimentally for small bridges, the yield for long bridges is reported to be almost distance-independent. For long bridge lengths, for which thermally activating hopping dominates over tunneling, the model considers two competing channels, a hopping via localized states and a transfer through partly delocalized states. The variable-range hopping mechanism and the delocalized states aspect of the theory are used to interpret the flat rather than a slow decrease of yield with increasing distance reported in experiments with long bridges.

Additional Information

© 2003 American Chemical Society. Received: August 19, 2002; In Final Form: July 25, 2003. Published on Web September 19, 2003. One of us (T.R.) acknowledges support of a Lynen Research Fellowship from the Alexander von Humboldt Foundation and support by the Deutsche Forschungsgemeinschaft (Emmy Noether Grant RE 1610/1-1). Support by the National Science Foundation and the Office of Naval Research is also acknowledged. We thank C. Treadway and T. Fiebig for providing us the absorption and fluorescence spectra, and we thank S. Gosavi for stimulating discussions. It is a pleasure to acknowledge valuable discussions with A. Okada, S. Tanaka, and H. Sumi. Further discussions with M. E. Michel-Beyerle and S. F. Fischer and a comment by J. Jortner were also very helpful.

Additional details

Created:
August 19, 2023
Modified:
October 20, 2023