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Electron Transfer Reactions: Generalized Spin-Boson Approach

2012/08/31 by Marco Merkli, Merkli, Marco, G. P. Berman +3 · 2 citations
Computer Science · Physics and Astronomy · #Advanced Thermodynamics and Statistical Mechanics #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Mathematical Physics (math-ph) #Quantum Information and Cryptography #Quantum Physics (quant-ph) #Spectroscopy and Quantum Chemical Studies

paper · pdf · doi:10.48550/arxiv.1208.6499

openalex publication_date 2012/08/31 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28

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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