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A complete description of thermodynamic stabilities of molecular crystals

Venkat Kapil, Edgar A. Engel

2022Proceedings of the National Academy of Sciences73 citationsDOIOpen Access PDF

Abstract

molecular compounds, which simultaneously account for all effects, have hitherto not been computationally viable. Here we present an efficient "end to end" framework that seamlessly combines state-of-the art electronic structure calculations, machine-learning potentials, and advanced free energy methods to calculate ab initio Gibbs free energies for general organic molecular materials. The facile generation of machine-learning potentials for a diverse set of polymorphic compounds-benzene, glycine, and succinic acid-and predictions of thermodynamic stabilities in qualitative and quantitative agreement with experiments highlight that predictive thermodynamic studies of industrially relevant molecular materials are no longer a daunting task.

Topics & Concepts

ThermodynamicsMaterials scienceStatistical physicsPhysicsChemical Thermodynamics and Molecular StructureCrystallography and molecular interactionsThermal and Kinetic Analysis
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