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

Ananth, Nandini and Miller, Thomas F., III (2012) Flux-correlation approach to characterizing reaction pathways in quantum systems: a study of condensed-phase proton-coupled electron transfer. Molecular Physics, 110 (9-10). pp. 1009-1015. ISSN 0026-8976. doi:10.1080/00268976.2012.686641.

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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.

Item Type:Article
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URLURL TypeDescription Paper
Miller, Thomas F., III0000-0002-1882-5380
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.
Funding AgencyGrant Number
Department of Energy (DOE)DE-FG02-11ER16247
Alfred P. Sloan FoundationUNSPECIFIED
Subject Keywords:quantum dynamics; reaction paths; proton-coupled electron transfer; energy transfer; path-integral methods
Issue or Number:9-10
Record Number:CaltechAUTHORS:20120627-114459530
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:32143
Deposited By: Aucoeur Ngo
Deposited On:27 Jun 2012 19:12
Last Modified:09 Nov 2021 21:25

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