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Title: Communication: Accurate higher-order van der Waals coefficients between molecules from a model dynamic multipole polarizability

Abstract

Due to the absence of the long-range van der Waals (vdW) interaction, conventional density functional theory (DFT) often fails in the description of molecular complexes and solids. In recent years, considerable progress has been made in the development of the vdW correction. However, the vdW correction based on the leading-order coefficient C6 alone can only achieve limited accuracy, while accurate modeling of higher-order coefficients remains a formidable task, due to the strong non-additivity effect. Here, we apply a model dynamic multipole polarizability within a modified single-frequency approximation to calculate C8 and C10 between small molecules. We find that the higher-order vdW coefficients from this model can achieve remarkable accuracy, with mean absolute relative deviations of 5% for C8 and 7% for C10. As a result, inclusion of accurate higher-order contributions in the vdW correction will effectively enhance the predictive power of DFT in condensed matter physics and quantum chemistry.

Authors:
 [1];  [2]
+ Show Author Affiliations
  1. Temple Univ., Philadelphia, PA (United States)
  2. Univ. of Pennsylvania, Philadelphia, PA (United States)
Publication Date:
Research Org.:
Univ. of Pennsylvania, Philadelphia, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1434893
Alternate Identifier(s):
OSTI ID: 1235377
Grant/Contract Number:  
FG02-07ER15920
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 144; Journal Issue: 3; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Complex solids; Polarizability; Intermolecular forces; Interpolation; Electrons Ab initio calculations; Density functional theory; Plasmons; Semiconductor device modeling

Citation Formats

Tao, Jianmin, and Rappe, Andrew M. Communication: Accurate higher-order van der Waals coefficients between molecules from a model dynamic multipole polarizability. United States: N. p., 2016. Web. doi:10.1063/1.4940397.
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Tao, Jianmin, & Rappe, Andrew M. Communication: Accurate higher-order van der Waals coefficients between molecules from a model dynamic multipole polarizability. United States. https://doi.org/10.1063/1.4940397
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Tao, Jianmin, and Rappe, Andrew M. Wed . "Communication: Accurate higher-order van der Waals coefficients between molecules from a model dynamic multipole polarizability". United States. https://doi.org/10.1063/1.4940397. https://www.osti.gov/servlets/purl/1434893.
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@article{osti_1434893,
title = {Communication: Accurate higher-order van der Waals coefficients between molecules from a model dynamic multipole polarizability},
author = {Tao, Jianmin and Rappe, Andrew M.},
abstractNote = {Due to the absence of the long-range van der Waals (vdW) interaction, conventional density functional theory (DFT) often fails in the description of molecular complexes and solids. In recent years, considerable progress has been made in the development of the vdW correction. However, the vdW correction based on the leading-order coefficient C6 alone can only achieve limited accuracy, while accurate modeling of higher-order coefficients remains a formidable task, due to the strong non-additivity effect. Here, we apply a model dynamic multipole polarizability within a modified single-frequency approximation to calculate C8 and C10 between small molecules. We find that the higher-order vdW coefficients from this model can achieve remarkable accuracy, with mean absolute relative deviations of 5% for C8 and 7% for C10. As a result, inclusion of accurate higher-order contributions in the vdW correction will effectively enhance the predictive power of DFT in condensed matter physics and quantum chemistry.},
doi = {10.1063/1.4940397},
journal = {Journal of Chemical Physics},
number = 3,
volume = 144,
place = {United States},
year = {Wed Jan 20 00:00:00 EST 2016},
month = {Wed Jan 20 00:00:00 EST 2016}
}
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