Electron transfer reactions: generalized spin-boson approach

We introduce a mathematically rigorous analysis of a generalized spin-boson system for the treatment of a donor–acceptor (reactant-product) quantum system coupled to a thermal quantum noise. The donor/acceptor probability dynamics describes transport reactions in chemical processes in presence of a...

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Bibliographic Details
Published in:Journal of mathematical chemistry 2013-03, Vol.51 (3), p.890-913
Main Authors: Merkli, M., Berman, G. P., Sayre, R.
Format: Article
Language:English
Subjects:
Chemistry
Chemistry and Materials Science
Math. Applications in Chemistry
Original Paper
Physical Chemistry
Theoretical and Computational Chemistry
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Summary:We introduce a mathematically rigorous analysis of a generalized spin-boson system for the treatment of a donor–acceptor (reactant-product) quantum system coupled to a thermal quantum noise. The donor/acceptor probability dynamics describes transport reactions in chemical processes in presence of a noisy environment – such as the electron transfer in a photosynthetic reaction center. Besides being rigorous, our analysis has the advantages over previous ones that (1) we include a general, non energy-conserving system-environment interaction , and that (2) we allow for the donor or acceptor to consist of multiple energy levels lying closely together. We establish explicit expressions for the rates and the efficiency (final donor–acceptor population difference) of the reaction. In particular, we show that the rate increases for a multi-level acceptor, but the efficiency does not.
ISSN:0259-9791
1572-8897
DOI:10.1007/s10910-012-0124-5