Bond-Dependent Thole Model for Polarizability and Spectroscopy

DelloStritto, Mark; Klein, Michael L.; Borguet, Eric

doi:10.1021/acs.jpca.8b12011

Title: Bond-Dependent Thole Model for Polarizability and Spectroscopy

Journal Article · 12 June 2019 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI: https://doi.org/10.1021/acs.jpca.8b12011 · OSTI ID:1608290

^[1]; Klein, Michael L. ^[2]; Borguet, Eric ^[2]

Temple Univ., Philadelphia, PA (United States); Temple University
Temple Univ., Philadelphia, PA (United States)

We present a new model for the calculation of molecular polarizabilities from effec- tive atomic polarizabilities. This model is based on the Thole modified dipole inter- action model for molecular polarizabilities, where the total polarizability is computed as a sum of effective atomic polarizabilities modified by dipole-dipole interactions. We extend this model by making the atomic polarizabilities explicit functions of the in- teratomic distances, scaling them by the radius of the volume an atom occupies in a molecule. We use the SCAN functional to show that this model, denoted TholeL, yields accurate molecular polarizabilities with little dependence on the training set. We also demonstrate that the TholeL model yields accurate polarizabilities for configurations far from the ground state structure for a wide range of molecules. Finally, we show that the TholeL model can be used to generate accurate Raman spectra for water, crystalline urea, and urea in water from ab-initio molecular dynamics simulations.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Complex Materials from First Principles (CCM); Temple Univ., Philadelphia, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012575

OSTI ID:: 1608290

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Journal Name: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory Journal Issue: 25 Vol. 123; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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