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arXiv · 2506.21504

Correlated reaction coordinate motion produces non-additive rate enhancement for electron and energy transfer in multi-acceptor structures

Hanggai Nuomin·Feng-Feng Song·Peng Zhang·David N. Beratan
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Abstract

Molecular structures with multiple donor, bridge, or acceptor units can display quantum interference effects that influence electron and energy transfer (ET and EnT) rates. Recent experiments found a 4- to 5-fold increase in ET rates for donor-acceptor structures with two acceptors compared to one. This result is surprising: simple classical or quantum analysis suggests a factor of two rate enhancement. We analyze the coupling interactions in multiple acceptor systems and find that rate enhancements beyond additive effects arise from acceptor-acceptor interactions that: 1) shift the reaction free energy, 2) change the donor-acceptor couplings, and 3) alter the reaction-coordinate motion. Consideration of these effects explains the observed rates in multi-acceptor systems and suggests strategies to tailor energy and electron transfer kinetics.

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Hanggai Nuomin, Feng-Feng Song, Peng Zhang, David N. Beratan. 2025-06-26. Correlated reaction coordinate motion produces non-additive rate enhancement for electron and energy transfer in multi-acceptor structures. https://arxiv.org/abs/2506.21504

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