Dual adaptive sampling and machine learning interatomic potentials for modeling materials with chemical bond hierarchy

HL Yang and YF Zhu and ET Dong and YB Wu and J Yang and WQ Zhang, PHYSICAL REVIEW B, 104, 094310 (2021).

DOI: 10.1103/PhysRevB.104.094310

The development of reliable and flexible machine learning based interatomic potentials (ML-IPs) is becoming increasingly important in studying the physical properties of complex condensed matter systems. Besides the structure descriptor model for total energy decomposition, the trial-and-error approach used in the design of the training dataset makes the ML-IP hardly improvable and reliable for modeling materials with chemical bond hierarchy. In this work, a dual adaptive sampling (DAS) method with an on the fly ambiguity threshold was developed to automatically generate an effective training dataset covering a wide temperature range or a wide spectrum of thermodynamic conditions. The DAS method consists of an inner loop for exploring the local configuration space and an outer loop for covering a wide temperature range. We validated the developed DAS method by simulating thermal transport of complex materials. The simulation results show that even with a substantially small dataset, our approach not only accurately reproduces the energies and forces but also predicts reliably effective high-order force constants to at least fourth order. The lattice thermal conductivity and its temperature dependence were evaluated using the Green-Kubo simulations with ML-IP for CoSb3 with up to third-order phonon scattering, and those for Mg3Sb2 with up to fourth-order phonon scattering, and all show good agreements with experiments. Our work provides an avenue to effectively construct a training dataset for ML-IP of complex materials with chemical bond hierarchy.

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