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Reliable crystal structure predictions from first principles

An inexpensive and reliable method for molecular crystal structure predictions (CSPs) has been developed. The new CSP protocol starts from a two-dimensional graph of crystal’s monomer(s) and utilizes no experimental information. Using results of quantum mechanical calculations for molecular dimers,...

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Autores principales: Nikhar, Rahul, Szalewicz, Krzysztof
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9163189/
https://www.ncbi.nlm.nih.gov/pubmed/35654882
http://dx.doi.org/10.1038/s41467-022-30692-y
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author Nikhar, Rahul
Szalewicz, Krzysztof
author_facet Nikhar, Rahul
Szalewicz, Krzysztof
author_sort Nikhar, Rahul
collection PubMed
description An inexpensive and reliable method for molecular crystal structure predictions (CSPs) has been developed. The new CSP protocol starts from a two-dimensional graph of crystal’s monomer(s) and utilizes no experimental information. Using results of quantum mechanical calculations for molecular dimers, an accurate two-body, rigid-monomer ab initio-based force field (aiFF) for the crystal is developed. Since CSPs with aiFFs are essentially as expensive as with empirical FFs, tens of thousands of plausible polymorphs generated by the crystal packing procedures can be optimized. Here we show the robustness of this protocol which found the experimental crystal within the 20 most stable predicted polymorphs for each of the 15 investigated molecules. The ranking was further refined by performing periodic density-functional theory (DFT) plus dispersion correction (pDFT+D) calculations for these 20 top-ranked polymorphs, resulting in the experimental crystal ranked as number one for all the systems studied (and the second polymorph, if known, ranked in the top few). Alternatively, the polymorphs generated can be used to improve aiFFs, which also leads to rank one predictions. The proposed CSP protocol should result in aiFFs replacing empirical FFs in CSP research.
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spelling pubmed-91631892022-06-05 Reliable crystal structure predictions from first principles Nikhar, Rahul Szalewicz, Krzysztof Nat Commun Article An inexpensive and reliable method for molecular crystal structure predictions (CSPs) has been developed. The new CSP protocol starts from a two-dimensional graph of crystal’s monomer(s) and utilizes no experimental information. Using results of quantum mechanical calculations for molecular dimers, an accurate two-body, rigid-monomer ab initio-based force field (aiFF) for the crystal is developed. Since CSPs with aiFFs are essentially as expensive as with empirical FFs, tens of thousands of plausible polymorphs generated by the crystal packing procedures can be optimized. Here we show the robustness of this protocol which found the experimental crystal within the 20 most stable predicted polymorphs for each of the 15 investigated molecules. The ranking was further refined by performing periodic density-functional theory (DFT) plus dispersion correction (pDFT+D) calculations for these 20 top-ranked polymorphs, resulting in the experimental crystal ranked as number one for all the systems studied (and the second polymorph, if known, ranked in the top few). Alternatively, the polymorphs generated can be used to improve aiFFs, which also leads to rank one predictions. The proposed CSP protocol should result in aiFFs replacing empirical FFs in CSP research. Nature Publishing Group UK 2022-06-02 /pmc/articles/PMC9163189/ /pubmed/35654882 http://dx.doi.org/10.1038/s41467-022-30692-y Text en © The Author(s) 2022 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Nikhar, Rahul
Szalewicz, Krzysztof
Reliable crystal structure predictions from first principles
title Reliable crystal structure predictions from first principles
title_full Reliable crystal structure predictions from first principles
title_fullStr Reliable crystal structure predictions from first principles
title_full_unstemmed Reliable crystal structure predictions from first principles
title_short Reliable crystal structure predictions from first principles
title_sort reliable crystal structure predictions from first principles
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9163189/
https://www.ncbi.nlm.nih.gov/pubmed/35654882
http://dx.doi.org/10.1038/s41467-022-30692-y
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