Direct observation of light-driven, concerted electron–proton transfer

Gagliardi, Christopher J.; Wang, Li; Dongare, Prateek; Brennaman, M. Kyle; Papanikolas, John M.; Meyer, Thomas J.; Thompson, David W.

doi:10.1073/pnas.1611496113

Title: Direct observation of light-driven, concerted electron–proton transfer

Journal Article · Thu Sep 22 00:00:00 EDT 2016 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1611496113· OSTI ID:1326239

Gagliardi, Christopher J. ^[1]; Wang, Li ^[2]; Dongare, Prateek ^[1]; Brennaman, M. Kyle ^[1]; Papanikolas, John M. ^[1]; Meyer, Thomas J. ^[1]; Thompson, David W. ^[3]

Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599-3290,
Institute of Environmental Science, Shanxi University, Taiyuan, Shanxi, China 030006,
Department of Chemistry, Memorial University of Newfoundland, St. John’s, NL, A1B 3X7, Canada

Here, the phenols 4-methylphenol, 4-methoxyphenol, and N-acetyl-tyrosine form hydrogen-bonded adducts with N-methyl-4, 4'-bipyridinium cation (MQ⁺) in aqueous solution as evidenced by the appearance of low-energy, low-absorptivity features in UV-visible spectra. They are assigned to the known examples of optically induced, concerted electron–proton transfer, photoEPT. The results of ultrafast transient absorption measurements on the assembly MeOPhO-H---MQ⁺ are consistent with concerted EPT by the instantaneous appearance of spectral features for MeOPhO·---H-MQ⁺ in the transient spectra at the first observation time of 0.1 ps. The transient decays to MeOPhO-H---MQ⁺ in 2.5 ps, accompanied by the appearance of oscillations in the decay traces with a period of ~1 ps, consistent with a vibrational coherence and relaxation from a higher υ(N-H) vibrational level or levels on the timescale for back EPT.

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Research Organization:: Univ. of North Carolina at Chapel Hill, Chapel Hill, NC (United States)

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

Grant/Contract Number:: SC0001011

OSTI ID:: 1326239

Alternate ID(s):: OSTI ID: 1464947

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Vol. 113 Journal Issue: 40; ISSN 0027-8424

Publisher:: Proceedings of the National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 24 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
light driven
electron
proton
transfer
photoEPT

Title: Direct observation of light-driven, concerted electron–proton transfer

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