Less is more: Sampling chemical space with active learning

• Published in: The Journal of chemical physics Vol. 148; no. 24; pp. 241733 - 241742
• Main Authors: Smith, Justin S., Nebgen, Ben, Lubbers, Nicholas, Isayev, Olexandr, Roitberg, Adrian E.
• Format: Journal Article
• Language: English
• Published: United States American Institute of Physics 28.06.2018; American Institute of Physics (AIP)
• Subjects: Active learning; Benchmarks; Fitness; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Machine learning; Material Science; Organic chemistry; Potential energy; Predictions; Random sampling; Training
• ISSN: 0021-9606; 1089-7690; 1089-7690
• DOI: 10.1063/1.5023802

The development of accurate and transferable machine learning (ML) potentials for predicting molecular energetics is a challenging task. The process of data generation to train such ML potentials is a task neither well understood nor researched in detail. In this work, we present a fully automated approach for the generation of datasets with the intent of training universal ML potentials. It is based on the concept of active learning (AL) via Query by Committee (QBC), which uses the disagreement between an ensemble of ML potentials to infer the reliability of the ensemble’s prediction. QBC allows the presented AL algorithm to automatically sample regions of chemical space where the ML potential fails to accurately predict the potential energy. AL improves the overall fitness of ANAKIN-ME (ANI) deep learning potentials in rigorous test cases by mitigating human biases in deciding what new training data to use. AL also reduces the training set size to a fraction of the data required when using naive random sampling techniques. To provide validation of our AL approach, we develop the COmprehensive Machine-learning Potential (COMP6) benchmark (publicly available on GitHub) which contains a diverse set of organic molecules. Active learning-based ANI potentials outperform the original random sampled ANI-1 potential with only 10% of the data, while the final active learning-based model vastly outperforms ANI-1 on the COMP6 benchmark after training to only 25% of the data. Finally, we show that our proposed AL technique develops a universal ANI potential (ANI-1x) that provides accurate energy and force predictions on the entire COMP6 benchmark. This universal ML potential achieves a level of accuracy on par with the best ML potentials for single molecules or materials, while remaining applicable to the general class of organic molecules composed of the elements CHNO.