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Electron Transfer Rates in Bridged Molecular Systems: A Phenomenological Approach to Relaxation
Abstract
A model for bridge-assisted, long-range electron transfer in a molecule interacting with a dissipative external bath is presented. The effects of the system−bath interaction are included phenomenologically in the evolution of the system density matrix as energy dephasings on the bridge sites. When the bridge dephasings are small, the steady state ET rate in this model is found to be the sum of two competing terms; the first is a McConnell-type rate arising from direct tunneling from donor to acceptor, and the second is a dephasing-dependent, length-independent scattering channel through the bridge sites. In the limit of large dephasings, an incoherent channel dominates the dynamics and leads to ET rates that can become only weakly dependent ( k ET ∝ 1/ N ) on the number of bridge sites in the system, for multisite bridges.
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Citations
Cites
On the generators of quantum dynamical semigroups
Lindblad, G. (1976) · Communications in Mathematical Physics · doi:10.1007/bf01608499 · Cited by 7,548
Completely positive dynamical semigroups of N -level systems
Gorini, V., Kossakowski, A., & Sudarshan, E. C. G. (1976) · Journal of Mathematical Physics · doi:10.1063/1.522979 · Cited by 3,998
Description of States in Quantum Mechanics by Density Matrix and Operator Techniques
Fano, U. (1957) · Reviews of Modern Physics · doi:10.1103/revmodphys.29.74 · Cited by 1,975
Density Matrix Theory and Applications
Blum, K. (2012) · Springer Series on Atomic, Optical, and Plasma Physics · doi:10.1007/978-3-642-20561-3 · Cited by 1,936
Quantum Dynamical Semigroups and Applications
(2007) · Lecture Notes in Physics · doi:10.1007/3-540-70861-8 · Cited by 1,182
Cited by
Unimolecular Electrical Rectifiers
Metzger, R. M. (2003) · Chemical Reviews · doi:10.1021/cr020413d · Cited by 518
Berlin, Y. A., Burin, A. L., & Ratner, M. A. (2001) · Journal of the American Chemical Society · doi:10.1021/ja001496n · Cited by 326
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Metadata
- Authors
- Davis, W. B., Wasielewski, M. R., Ratner, M. A., Mujica, V., & Nitzan, A.
- Venue
- The Journal of Physical Chemistry A
- Publisher
- American Chemical Society (ACS)
- Published
- 1997-08-01
- Volume
- 101
- Issue
- 35
- Pages
- 6158-6164
- ISSN
- 1089-5639 (ISSN-L)
- 1520-5215
- OpenAlex
- W2136705067
- Cited by
- 191
- References
- 5
- FWCI
- 8.31
- Type
- journal article
- Language
- en
- Open access
- closed
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- Davis, W. B., Wasielewski, M. R., Ratner, M. A., Mujica, V., & Nitzan, A. (1997). Electron Transfer Rates in Bridged Molecular Systems: A Phenomenological Approach to Relaxation. The Journal of Physical Chemistry A. https://doi.org/10.1021/jp970909c
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Bibliographic data: Semantic Scholar, OpenAlex, Crossref.
Contains information from the Semantic Scholar Academic Graph Datasets, made available under the ODC Attribution License (ODC-BY 1.0).
Semantic Scholar’s data is described in: Kinney, R., et al. (2023). The Semantic Scholar Open Data Platform. arXiv:2301.10140.
