Nucleation of molecular crystals driven by relative information entropy

Gianpaolo Gobbo, Michael A. Bellucci, Gareth Tribello, Giovanni Ciccotti

Research output: Contribution to journalArticle

12 Citations (Scopus)
168 Downloads (Pure)

Abstract

Simulating nucleation of molecular crystals is extremely challenging for all but the simplest cases. The challenge lies in formulating effective order parameters that are capable of driving the transition process. In recent years, order parameters based on molecular pair-functions have been successfully used in combination with enhanced sampling techniques to simulate nucleation of simple molecular crystals. However, despite the success of these approaches, we demonstrate that they can fail when applied to more complex cases. In fact, we show that order parameters based on molecular pair-functions, while successful at nucleating benzene, fail for paracetamol. Hence, we introduce a novel approach to formulate order parameters. In our approach, we construct reduced dimensional distributions of relevant quantities on the fly and then quantify the difference between these distributions and selected reference distributions. By computing the distribution of different quantities and by choosing different reference distributions, it is possible to systematically construct an effective set of order parameters. We then show that our new order parameters are capable of driving the nucleation of ordered states and, in particular, the form I crystal of paracetamol.
Original languageEnglish
Pages (from-to)1-14
JournalJournal of chemical theory and computation
Early online date22 Dec 2017
DOIs
Publication statusEarly online date - 22 Dec 2017

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