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Published May 25, 2012 | Submitted
Journal Article Open

Flux-correlation approach to characterizing reaction pathways in quantum systems: a study of condensed-phase proton-coupled electron transfer

Abstract

We introduce a simple method for characterizing reactive pathways in quantum systems. Flux auto-correlation and cross-correlation functions are employed to develop a quantitative measure of dynamical coupling in quantum transition events, such as reactive tunnelling and resonant energy transfer. We utilize the method to study condensed-phase proton-coupled electron transfer (PCET) reactions and to determine the relative importance of competing concerted and sequential reaction pathways. Results presented here include numerically exact quantum dynamics simulations for model condensed-phase PCET reactions. This work demonstrates the applicability of the new method for the analysis of both approximate and exact quantum dynamics simulations.

Additional Information

© 2012 Taylor & Francis. Received 6 February 2012; final version received 12 April 2012. Accepted author version posted online: 27 Apr 2012; Version of record first published: 25 May 2012. This work was supported by the US Department of Energy (DOE), Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences under Grant No. DE-FG02-11ERI6247 and the National Science Foundation (NSF) CAREER Award under Grant No. CHE-1057112. Additionally, T.F.M. acknowledges support from an Alfred P. Sloan Foundation Research Fellowship. Computational resources were provided by the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the US Department of Energy under Contract No. DE-AC02-05CH11231.

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August 22, 2023
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