Water network-mediated, electron-induced proton transfer in [C5H5N • (H2O)n]– clusters

DeBlase, Andrew F.; Wolke, Conrad T.; Weddle, Gary H.; Archer, Kaye A.; Jordan, Kenneth D.; Kelly, John T.; Tschumper, Gregory S.; Hammer, Nathan I.; Johnson, Mark A.

doi:10.1063/1.4931928

Title: Water network-mediated, electron-induced proton transfer in [C₅H₅N • (H₂O)n]^– clusters

Journal Article · Fri Oct 09 00:00:00 EDT 2015 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4931928· OSTI ID:1469362

DeBlase, Andrew F. ^[1]; Wolke, Conrad T. ^[1]; Weddle, Gary H. ^[2]; Archer, Kaye A. ^[3];

^[3];

^[4];

^[4]; Hammer, Nathan I. ^[4];

^[1]

Yale Univ., New Haven, CT (United States)
Yale Univ., New Haven, CT (United States); Fairfield Univ., Fairfield, CT (United States)
Univ. of Pittsburgh, Pittsburgh, PA (United States)
Univ. of Mississippi, University, MS (United States)

The role of proton-assisted charge accommodation in electron capture by a heterocyclic electron scavenger is investigated through theoretical analysis of the vibrational spectra of cold, gas phase [Py·(H₂O)_n=3–5]– clusters. These radical anions are formed when an excess electron is attached to water clusters containing a single pyridine (Py) molecule in a supersonic jet ion source. Under these conditions, the cluster ion distribution starts promptly at n = 3, and the photoelectron spectra, combined with vibrational predissociation spectra of the Ar-tagged anions, establish that for n > 3, these species are best described as hydrated hydroxide ions with the neutral pyridinium radical, PyH⁽⁰⁾, occupying one of the primary solvation sites of the OH^–. The n = 3 cluster appears to be a special case where charge localization on Py and hydroxide is nearly isoenergetic, and the nature of this species is explored with ab initio molecular dynamics calculations of the trajectories that start from metastable arrangements of the anion based on a diffuse, essentially dipole-bound electron. These calculations indicate that the reaction proceeds via a relatively slow rearrangement of the water network to create a favorable hydration configuration around the water molecule that eventually donates a proton to the Py nitrogen atom to yield the product hydroxide ion. In conclusion, the correlation between the degree of excess charge localization and the evolving shape of the water network revealed by this approach thus provides a microscopic picture of the “solvent coordinate” at the heart of a prototypical proton-coupled electron transfer reaction

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Research Organization:: Yale Univ., New Haven, CT (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: FG02-06ER15800; FG02-00ER15066

OSTI ID:: 1469362

Alternate ID(s):: OSTI ID: 1223330

Journal Information:: Journal of Chemical Physics, Vol. 143, Issue 14; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 7 works

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