Systematic Finite-Temperature Reduction of Crystal Energy Landscapes

التفاصيل البيبلوغرافية
العنوان: Systematic Finite-Temperature Reduction of Crystal Energy Landscapes
المؤلفون: Jonas Nyman, Louise S. Price, Matteo Salvalaglio, Nicholas F. Francia, Sarah L. Price
بيانات النشر: American Chemical Society (ACS), 2020.
سنة النشر: 2020
مصطلحات موضوعية: Lattice energy, Work (thermodynamics), Materials science, 010405 organic chemistry, Stacking, Thermodynamics, General Chemistry, Crystal structure, 010402 general chemistry, Condensed Matter Physics, 01 natural sciences, 0104 chemical sciences, Organic molecules, Crystal structure prediction, Crystal, Maxima and minima, Molecular dynamics, Cluster (physics), General Materials Science, Statistical physics, Reduction (mathematics), Energy (signal processing)
الوصف: 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 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.
DOI: 10.26434/chemrxiv.12609833.v1
URL الوصول: https://explore.openaire.eu/search/publication?articleId=doi_dedup___::d8805aea4c335f3b879b7807116dee0a
https://doi.org/10.26434/chemrxiv.12609833.v1
Rights: OPEN
رقم الانضمام: edsair.doi.dedup.....d8805aea4c335f3b879b7807116dee0a
قاعدة البيانات: OpenAIRE
الوصف
DOI:10.26434/chemrxiv.12609833.v1