Concerted Hydrogen-Bond Dynamics in the Transport Mechanism of the Hydrated Proton: A First-Principles Molecular Dynamics Study

Timothy C. Berkelbach, Hee Seung Lee, Mark E. Tuckerman

Research output: Contribution to journalArticle

Abstract

First-principles molecular dynamics calculations performed in a fully converged basis set are used to reveal new details about the mechanism of the anomalous proton-transport process in water, a fundamental question dating back over 200 years. By separating actual structural diffusion from simple rattling events, wherein a proton shuttles forth and back in a hydrogen bond, it is found that the former are driven by a concerted mechanism in which hydronium begins to accept a hydrogen bond from a donor water molecule while the proton-receiving water molecule simultaneously loses one of its acceptor hydrogen bonds. The kinetics of the process are found to be in good agreement with recent experiments.

Original languageEnglish (US)
Article number238302
JournalPhysical Review Letters
Volume103
Issue number23
DOIs
StatePublished - Nov 30 2009

ASJC Scopus subject areas

  • Physics and Astronomy(all)

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