Repository: Freie Universität Berlin, Math Department

Markov state modeling reveals competing collective hydrogen bond rearrangements in liquid water

Schulz, R. and Hansen, Y. von and Daldrop, J.O. and Kappler, J. and Noé, F. and Netz, R.R. (2018) Markov state modeling reveals competing collective hydrogen bond rearrangements in liquid water. SFB 1114 Preprint 02/2018 . (Unpublished)

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Abstract

We construct a Markov state model for the dynamic rearrangement of the local hydrogen bond network in liquid water. The model is based on trajectories from classical molecular dynamics simulations and accounts for the dynamics of relative angular and separation coordinates of water molecules. We analyze first the conformational subspace of three water molecules and find five well separated dynamic modes with reaction times in the 2 - 5 ps range, which correspond to different interchanges of hydrogen bond donor and acceptors, followed by an entire continuum spectrum of modes. We then analyze the switching of one hydrogen bond between two water molecules and derive the complete transition network. The most probable pathway corresponds to a direct switch without an intermediate, in agreement with previous studies. However, a considerable fraction of paths proceeds along different intermediate states that involve alternative hydrogen bonds or unbound states.

Item Type:Article
Subjects:Physical Sciences
Mathematical and Computer Sciences > Mathematics > Applied Mathematics
ID Code:2236
Deposited By: Silvia Hoemke
Deposited On:23 Feb 2018 13:20
Last Modified:23 Feb 2018 13:20

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