Leonid Kahle^1*, Benoit Minisini¹, Tai Bui², Jeremy First³, Corneliu Buda², Thomas Goldman², Erich Wimmer¹

1 Materials Design SARL, 42 avenue Verdier, 92120 Montrouge, France

2 bp Exploration Operating Co. Ltd, Chertsey Road, Sunbury-on-Thames TW16 7LN, UK

3 bp, Center for High Performance Computing, 225 Westlake Park Blvd, Houston, TX 77079, USA

* Corresponding authors emails: leonidkahle@gmail.com

DOI10.24435/materialscloud:ed-gp [version v1]

Publication date: Aug 12, 2024

How to cite this record

Leonid Kahle, Benoit Minisini, Tai Bui, Jeremy First, Corneliu Buda, Thomas Goldman, Erich Wimmer, A dual-cutoff machine-learned potential for condensed organic systems obtained via uncertainty-guided active learning, Materials Cloud Archive 2024.121 (2024), https://doi.org/10.24435/materialscloud:ed-gp

Description

Machine-learned potentials (MLPs) trained on ab initio data combine the computational efficiency of classical interatomic potentials with the accuracy and generality of the first-principles method used in the creation of the respective training set. In this work, we implement and train a MLP to obtain an accurate description of the potential energy surface and property predictions for organic compounds, as both single molecules and in the condensed phase. We devise a dual descriptor, based on the atomic cluster expansion (ACE), that couples an information-rich short-range description with a coarser long-range description that captures weak intermolecular interactions. We employ uncertainty-guided active learning for the training set generation, creating a dataset that is comparatively small for the breadth of application and consists of alcohols, alkanes, and an adipate. Utilizing that MLP, we calculate densities of those systems of varying chain lengths as a function of temperature, obtaining a discrepancy of less than 4% compared with experiment. Vibrational frequencies calculated with the MLP have a root mean square error of less than 1 THz compared to DFT. The heat capacities of condensed systems are within 11% of experimental findings, which is strong evidence that the dual descriptor provides an accurate framework for the prediction of both short-range intramolecular and long-range intermolecular interactions.

Materials Cloud sections using this data

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Keywords

molecular dynamics machine learning diffusion radial distribution functions heat capacity VASP training data