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New scaling relations to compute atom-in-material polarizabilities and dispersion coefficients: part 1. Theory and accuracy
Polarizabilities and London dispersion forces are important to many chemical processes. Force fields for classical atomistic simulations can be constructed using atom-in-material polarizabilities and C(n) (n = 6, 8, 9, 10…) dispersion coefficients. This article addresses the key question of how to e...
Autores principales: | , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
The Royal Society of Chemistry
2019
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9064874/ https://www.ncbi.nlm.nih.gov/pubmed/35519408 http://dx.doi.org/10.1039/c9ra03003d |
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author | Manz, Thomas A. Chen, Taoyi Cole, Daniel J. Limas, Nidia Gabaldon Fiszbein, Benjamin |
author_facet | Manz, Thomas A. Chen, Taoyi Cole, Daniel J. Limas, Nidia Gabaldon Fiszbein, Benjamin |
author_sort | Manz, Thomas A. |
collection | PubMed |
description | Polarizabilities and London dispersion forces are important to many chemical processes. Force fields for classical atomistic simulations can be constructed using atom-in-material polarizabilities and C(n) (n = 6, 8, 9, 10…) dispersion coefficients. This article addresses the key question of how to efficiently assign these parameters to constituent atoms in a material so that properties of the whole material are better reproduced. We develop a new set of scaling laws and computational algorithms (called MCLF) to do this in an accurate and computationally efficient manner across diverse material types. We introduce a conduction limit upper bound and m-scaling to describe the different behaviors of surface and buried atoms. We validate MCLF by comparing results to high-level benchmarks for isolated neutral and charged atoms, diverse diatomic molecules, various polyatomic molecules (e.g., polyacenes, fullerenes, and small organic and inorganic molecules), and dense solids (including metallic, covalent, and ionic). We also present results for the HIV reverse transcriptase enzyme complexed with an inhibitor molecule. MCLF provides the non-directionally screened polarizabilities required to construct force fields, the directionally-screened static polarizability tensor components and eigenvalues, and environmentally screened C(6) coefficients. Overall, MCLF has improved accuracy compared to the TS-SCS method. For TS-SCS, we compared charge partitioning methods and show DDEC6 partitioning yields more accurate results than Hirshfeld partitioning. MCLF also gives approximations for C(8), C(9), and C(10) dispersion coefficients and quantum Drude oscillator parameters. This method should find widespread applications to parameterize classical force fields and density functional theory (DFT) + dispersion methods. |
format | Online Article Text |
id | pubmed-9064874 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2019 |
publisher | The Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
spelling | pubmed-90648742022-05-04 New scaling relations to compute atom-in-material polarizabilities and dispersion coefficients: part 1. Theory and accuracy Manz, Thomas A. Chen, Taoyi Cole, Daniel J. Limas, Nidia Gabaldon Fiszbein, Benjamin RSC Adv Chemistry Polarizabilities and London dispersion forces are important to many chemical processes. Force fields for classical atomistic simulations can be constructed using atom-in-material polarizabilities and C(n) (n = 6, 8, 9, 10…) dispersion coefficients. This article addresses the key question of how to efficiently assign these parameters to constituent atoms in a material so that properties of the whole material are better reproduced. We develop a new set of scaling laws and computational algorithms (called MCLF) to do this in an accurate and computationally efficient manner across diverse material types. We introduce a conduction limit upper bound and m-scaling to describe the different behaviors of surface and buried atoms. We validate MCLF by comparing results to high-level benchmarks for isolated neutral and charged atoms, diverse diatomic molecules, various polyatomic molecules (e.g., polyacenes, fullerenes, and small organic and inorganic molecules), and dense solids (including metallic, covalent, and ionic). We also present results for the HIV reverse transcriptase enzyme complexed with an inhibitor molecule. MCLF provides the non-directionally screened polarizabilities required to construct force fields, the directionally-screened static polarizability tensor components and eigenvalues, and environmentally screened C(6) coefficients. Overall, MCLF has improved accuracy compared to the TS-SCS method. For TS-SCS, we compared charge partitioning methods and show DDEC6 partitioning yields more accurate results than Hirshfeld partitioning. MCLF also gives approximations for C(8), C(9), and C(10) dispersion coefficients and quantum Drude oscillator parameters. This method should find widespread applications to parameterize classical force fields and density functional theory (DFT) + dispersion methods. The Royal Society of Chemistry 2019-06-19 /pmc/articles/PMC9064874/ /pubmed/35519408 http://dx.doi.org/10.1039/c9ra03003d Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by/3.0/ |
spellingShingle | Chemistry Manz, Thomas A. Chen, Taoyi Cole, Daniel J. Limas, Nidia Gabaldon Fiszbein, Benjamin New scaling relations to compute atom-in-material polarizabilities and dispersion coefficients: part 1. Theory and accuracy |
title | New scaling relations to compute atom-in-material polarizabilities and dispersion coefficients: part 1. Theory and accuracy |
title_full | New scaling relations to compute atom-in-material polarizabilities and dispersion coefficients: part 1. Theory and accuracy |
title_fullStr | New scaling relations to compute atom-in-material polarizabilities and dispersion coefficients: part 1. Theory and accuracy |
title_full_unstemmed | New scaling relations to compute atom-in-material polarizabilities and dispersion coefficients: part 1. Theory and accuracy |
title_short | New scaling relations to compute atom-in-material polarizabilities and dispersion coefficients: part 1. Theory and accuracy |
title_sort | new scaling relations to compute atom-in-material polarizabilities and dispersion coefficients: part 1. theory and accuracy |
topic | Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9064874/ https://www.ncbi.nlm.nih.gov/pubmed/35519408 http://dx.doi.org/10.1039/c9ra03003d |
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