Communication: Regularizing binding energy distributions and thermodynamics of hydration: Theory and application to water modeled with classical and ab initio simulations

Valéry Weber; Safir Merchant; D. Asthagiri

doi:10.1063/1.3660205

Communication: Regularizing binding energy distributions and thermodynamics of hydration: Theory and application to water modeled with classical and ab initio simulations

Valéry Weber, Safir Merchant, D. Asthagiri

Research output: Contribution to journal › Article › peer-review

19 Scopus citations

Abstract

The high-energy tail of the distribution of solute-solvent interaction energies is poorly characterized for condensed systems, but this tail region is of principal interest in determining the excess free energy of the solute. We introduce external fields centered on the solute to modulate the short-range repulsive interaction between the solute and solvent. This regularizes the binding energy distribution and makes it easy to calculate the free energy of the solute with the field. Together with the work done to apply the field in the presence and absence of the solute, we calculate the excess chemical potential of the solute. We present the formal development of this idea and apply it to study liquid water.

Original language	English
Article number	181101
Journal	Journal of Chemical Physics
Volume	135
Issue number	18
DOIs	https://doi.org/10.1063/1.3660205
State	Published - Nov 14 2011
Externally published	Yes

Funding

The authors warmly thank Claude Daul (University of Fribourg) for computer resources. We thank Hank Ashbaugh (Tulane) for helpful insights about the deviation between our calculations and the scaled particle results. D.A. thanks the donors of the American Chemical Society Petroleum Research Fund for financial support. This research used resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE- AC02-05CH11231.

Funders	Funder number
U.S. Department of Energy	DE- AC02-05CH11231
Office of Science
American Chemical Society Petroleum Research Fund

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Communication: Regularizing binding energy distributions and thermodynamics of hydration: Theory and application to water modeled with classical and ab initio simulations

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