Volume 216, 2019

Quantum interferences among Dexter energy transfer pathways

Abstract

Dexter energy transfer in chemical systems moves an exciton (i.e., an electron–hole pair) from a donor chromophore to an acceptor chromophore through a bridge by a combination of bonded and non-bonded interactions. The transition is enabled by both one-electron/one-particle and two-electron/two-particle interaction mechanisms. Assuming that there is no real intermediate state population of an electron, hole, or exciton in the bridge, the transport involves two states that are coupled non-adiabatically. As such, coherent quantum interferences arise among the Dexter energy coupling pathways. These interferences, while related to well understood interferences in single-electron transfer, are much richer because of their two particle nature: the transfer of a triplet exciton involves the net transfer of both an electron and a hole. Despite this additional complexity, simple rules can govern Dexter coupling pathway interferences in special cases. As in the case of single-electron transfer, identical parallel coupling pathways can be constructively interfering and may enhance the Dexter transfer rate. Because of the virtual particle combinatorics associated with two-particle superexchange, two parallel Dexter coupling routes may be expected to enhance Dexter couplings by more than a factor of two. We explore Dexter coupling pathway interferences in non-covalent assemblies, employing a method that enables the assessment of Dexter coupling pathway strengths and interferences, in the context of one-particle and two-particle coupling interactions.

Graphical abstract: Quantum interferences among Dexter energy transfer pathways

Associated articles

Supplementary files

Article information

Article type
Paper
Submitted
14 Jan 2019
Accepted
21 Jan 2019
First published
08 Mey 2019

Faraday Discuss., 2019,216, 301-318

Author version available

Quantum interferences among Dexter energy transfer pathways

S. Bai, P. Zhang, P. Antoniou, S. S. Skourtis and David N. Beratan, Faraday Discuss., 2019, 216, 301 DOI: 10.1039/C9FD00007K

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