A Bond-order Analysis of the Mechanism for Hydrated Proton Mobility in Liquid Water

TitleA Bond-order Analysis of the Mechanism for Hydrated Proton Mobility in Liquid Water
Publication TypeJournal Article
Year of Publication2005
AuthorsLapid, H, Agmon, N, Petersen, MK, Voth, GA
JournalJ Chem Phys
Volume122
Pagination14506
Abstract

Bond-order analysis is introduced to facilitate the study of cooperative many-molecule effects on proton mobility in liquid water, as simulated using the multistate empirical valence-bond methodology. We calculate the temperature dependence for proton mobility and the total effective bond orders in the first two solvation shells surrounding the H(5)O(2) (+) proton-transferring complex. We find that proton-hopping between adjacent water molecules proceeds via this intermediate, but couples to hydrogen-bond dynamics in larger water clusters than previously anticipated. A two-color classification of these hydrogen bonds leads to an extended mechanism for proton mobility.

DOI10.1063/1.1814973