Abstract
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.
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Acknowledgments
M.M. acknowledges the support of the Natural Sciences and Engineering Research Council of Canada (NSERC) through an Individual Discovery Grant. He and G.P.B are grateful for support from the Institut Henri Poincaré (IHP) through the programme “Research in Paris”. The work by G.P.B. and R.S. was carried out under the auspices of the National Nuclear Security Administration of the U.S. Department of Energy at Los Alamos National Laboratory under Contract No. DE-AC52-06NA25396.
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Merkli, M., Berman, G.P. & Sayre, R. Electron transfer reactions: generalized spin-boson approach. J Math Chem 51, 890–913 (2013). https://doi.org/10.1007/s10910-012-0124-5
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DOI: https://doi.org/10.1007/s10910-012-0124-5