Spicing up continuum solvation models with SaLSA: The spherically averaged liquid susceptibility ansatz

Sundararaman, Ravishankar; Schwarz, Kathleen A.; Letchworth-Weaver, Kendra; Arias, T. A.

doi:10.1063/1.4906828

Title: Spicing up continuum solvation models with SaLSA: The spherically averaged liquid susceptibility ansatz

Journal Article · Tue Feb 03 00:00:00 EST 2015 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4906828· OSTI ID:1370450

^[1]; Schwarz, Kathleen A. ^[1]; Letchworth-Weaver, Kendra ^[1]; Arias, T. A. ^[1]

Cornell Univ., Ithaca, NY (United States). Dept. of Physics

Continuum solvation models enable electronic structure calculations of systems in liquid environments, but because of the large number of empirical parameters, they are limited to the class of systems in their fit set (typically organic molecules). Here, we derive a solvation model with no empirical parameters for the dielectric response by taking the linear response limit of a classical density functional for molecular liquids. This model directly incorporates the nonlocal dielectric response of the liquid using an angular momentum expansion, and with a single fit parameter for dispersion contributions it predicts solvation energies of neutral molecules with a RMS error of 1.3 kcal/mol in water and 0.8 kcal/mol in chloroform and carbon tetrachloride. We show that this model is more accurate for strongly polar and charged systems than previous solvation models because of the parameter-free electric response, and demonstrate its suitability for ab initio solvation, including self-consistent solvation in quantum Monte Carlo calculations.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Energy Materials Center at Cornell (EMC2)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001086

OSTI ID:: 1370450

Alternate ID(s):: OSTI ID: 1228514

Journal Information:: Journal of Chemical Physics, Vol. 142, Issue 5; Related Information: Emc2 partners with Cornell University (lead); Lawrence Berkeley National Laboratory; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 41 works

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