Inverted Region in Bimolecular Electron Transfer in Solution Enabled by Delocalization

Takeda, Norihiko; Miller, John R.

doi:10.1021/jacs.0c04780

Title: Inverted Region in Bimolecular Electron Transfer in Solution Enabled by Delocalization

Journal Article · 13 October 2020 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.0c04780 · OSTI ID:1670665

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Brookhaven National Lab. (BNL), Upton, NY (United States)

Rate constants for bimolecular electron transfer (ET) increased with driving force, -ΔG°, reached a plateau, and then decreased in an inverted region. This rate data was described well by electron transfer theory subject to a diffusion-controlled limit. These were for ET from radical anions of polydecylthiophene (P3DT) to a series of acceptors in THF solution. When the donor was the smaller anion of quaterthiophene (T4^•-) the inverted region was much less prominent, and still less so for when the donor was the anion of bithiophene (T2^•-). Description of the data using ET theory identifies smaller electronic couplings for the highly-delocalized P3DT anions as enabling the inverted behavior: The presence of a Marcus inverted region is a consequence of delocalized electronic states. The results of this study further imply that electronic couplings smaller than usually found for molecules in contact could boost efficiency of energy storage by electron transfer, and identifies size-mismatch as an important concept in control of electronic couplings.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704; AC02-98CH10886

OSTI ID:: 1670665

Report Number(s):: BNL-219915-2020--JAAM

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 42 Vol. 142; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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