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Systematic Finite-Temperature Reduction of Crystal Energy Landscapes

Francia, NF; Price, LS; Nyman, J; Price, SL; Salvalaglio, M; (2020) Systematic Finite-Temperature Reduction of Crystal Energy Landscapes. Crystal Growth & Design 10.1021/acs.cgd.0c00918. (In press). Green open access

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Abstract

Crystal structure prediction methods are prone to overestimate the number of potential polymorphs of organic molecules. In this work, we aim to reduce the overprediction by systematically applying molecular dynamics simulations and biased sampling methods to cluster subsets of structures that can easily interconvert at finite temperature and pressure. Following this approach, we rationally reduce the number of predicted putative polymorphs in crystal structure prediction (CSP)-generated crystal energy landscapes. This uses an unsupervised clustering approach to analyze independent finite-temperature molecular dynamics trajectories and hence identify a representative structure of each cluster of distinct lattice energy minima that are effectively equivalent at finite temperature and pressure. Biased simulations are used to reduce the impact of limited sampling time and to estimate the work associated with polymorphic transformations. We demonstrate the proposed systematic approach by studying the polymorphs of urea and succinic acid, reducing an initial set of over 100 energetically plausible CSP structures to 12 and 27 respectively, including the experimentally known polymorphs. The simulations also indicate the types of disorder and stacking errors that may occur in real structures.

Type: Article
Title: Systematic Finite-Temperature Reduction of Crystal Energy Landscapes
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/acs.cgd.0c00918
Publisher version: https://doi.org/10.1021/acs.cgd.0c00918
Language: English
Additional information: This is an open access article published under a Creative Commons Attribution (CC-BY) License (http://pubs.acs.org/page/policy/authorchoice_ccby_termsofuse.html), which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.
Keywords: Molecular structure, Cluster structure, Cluster chemistry, Crystal structure, Molecules
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10111025
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