Generating Minimal Training Sets for Machine Learned Potentials.

Abstract

This Letter presents a novel approach for identifying uncorrelated atomic configurations from extensive datasets with a nonstandard neural network workflow known as random network distillation (RND) for training machine-learned interatomic potentials (MLPs). This method is coupled with a DFT workflow wherein initial data are generated with cheaper classical methods before only the minimal subset is passed to a more computationally expensive abinitio calculation. This benefits training not only by reducing the number of expensive DFT calculations required but also by providing a pathway to the use of more accurate quantum mechanical calculations. The method's efficacy is demonstrated by constructing machine-learned interatomic potentials for the molten salts KCl and NaCl. Our RND method allows accurate models to be fit on minimal datasets, as small as 32 configurations, reducing the required structures by at least 1 order of magnitude compared to alternative methods. This reduction in dataset sizes not only substantially reduces computational overhead for training data generation but also provides a more comprehensive starting point for active-learning procedures.