Issue 33, 2024

Active sparse Bayesian committee machine potential for isothermal–isobaric molecular dynamics simulations

Abstract

Recent advancements in machine learning potentials (MLPs) have significantly impacted the fields of chemistry, physics, and biology by enabling large-scale first-principles simulations. Among different machine learning approaches, kernel-based MLPs distinguish themselves through their ability to handle small datasets, quantify uncertainties, and minimize over-fitting. Nevertheless, their extensive computational requirements present considerable challenges. To alleviate these, sparsification methods have been developed, aiming to reduce computational scaling without compromising accuracy. In the context of isothermal and isobaric ML molecular dynamics (MD) simulations, achieving precise pressure estimation is crucial for reproducing reliable system behavior under constant pressure. Despite progress, sparse kernel MLPs struggle with precise pressure prediction. Here, we introduce a virial kernel function that significantly enhances the pressure estimation accuracy of MLPs. Additionally, we propose the active sparse Bayesian committee machine (BCM) potential, an on-the-fly MLP architecture that aggregates local sparse Gaussian process regression (SGPR) MLPs. The sparse BCM potential overcomes the steep computational scaling with the kernel size, and a predefined restriction on the size of kernel allows for fast and efficient on-the-fly training. Our advancements facilitate accurate and computationally efficient machine learning-enhanced MD (MLMD) simulations across diverse systems, including ice–liquid coexisting phases, Li10Ge(PS6)2 lithium solid electrolyte, and high-pressure liquid boron nitride.

Graphical abstract: Active sparse Bayesian committee machine potential for isothermal–isobaric molecular dynamics simulations

Supplementary files

Article information

Article type
Paper
Submitted
30 4 2024
Accepted
30 7 2024
First published
31 7 2024

Phys. Chem. Chem. Phys., 2024,26, 22073-22082

Active sparse Bayesian committee machine potential for isothermal–isobaric molecular dynamics simulations

S. Y. Willow, D. G. Kim, R. Sundheep, A. Hajibabaei, K. S. Kim and C. W. Myung, Phys. Chem. Chem. Phys., 2024, 26, 22073 DOI: 10.1039/D4CP01801J

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