Development of reactive force fields using ab initio molecular dynamics simulation minimally biased to experimental data

The Journal of Chemical Physics
Chen ChenGregory A Voth

Abstract

Incorporation of quantum mechanical electronic structure data is necessary to properly capture the physics of many chemical processes. Proton hopping in water, which involves rearrangement of chemical and hydrogen bonds, is one such example of an inherently quantum mechanical process. Standard ab initio molecular dynamics (AIMD) methods, however, do not yet accurately predict the structure of water and are therefore less than optimal for developing force fields. We have instead utilized a recently developed method which minimally biases AIMD simulations to match limited experimental data to develop novel multiscale reactive molecular dynamics (MS-RMD) force fields by using relative entropy minimization. In this paper, we present two new MS-RMD models using such a parameterization: one which employs water with harmonic internal vibrations and another which uses anharmonic water. We show that the newly developed MS-RMD models very closely reproduce the solvation structure of the hydrated excess proton in the target AIMD data. We also find that the use of anharmonic water increases proton hopping, thereby increasing the proton diffusion constant.

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Citations

Nov 4, 2017·The Journal of Chemical Physics·Jean-Philip Piquemal, Kenneth D Jordan
Oct 13, 2018·Chemical Science·Sean A FischerDaniel Gunlycke
Jan 9, 2021·Science·Mischa Bonn, Johannes Hunger
Jul 10, 2021·The Journal of Chemical Physics·Christopher ArntsenGregory A Voth
Jun 11, 2019·The Journal of Physical Chemistry. B·Sean A Fischer, Daniel Gunlycke
Aug 7, 2019·Journal of the American Chemical Society·Zhi YueJessica M J Swanson
Jun 10, 2020·The Journal of Physical Chemistry. B·Chenghan Li, Jessica M J Swanson
Oct 28, 2019·The Journal of Physical Chemistry. B·Zhen-Hao Xu, Markus Meuwly
Apr 26, 2018·Journal of Chemical Theory and Computation·Emre SevgenJuan J de Pablo

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