Accelerated identification of equilibrium structures of multicomponent inorganic crystals using machine learning potentials

Abstract

Abstract The discovery of multicomponent inorganic compounds can provide direct solutions to scientific and engineering challenges, yet the vast uncharted material space dwarfs synthesis throughput. While the crystal structure prediction (CSP) may mitigate this frustration, the exponential complexity of CSP and expensive density functional theory (DFT) calculations prohibit material exploration at scale. Herein, we introduce SPINNER, a structure-prediction framework based on random and evolutionary searches. Harnessing speed and accuracy of neural network potentials (NNPs), the program navigates configurational spaces 102–103 times faster than DFT-based methods. Furthermore, SPINNER incorporates algorithms tuned for NNPs, achieving performances exceeding conventional algorithms. In blind tests on 60 ternary compositions, SPINNER identifies experimental (or theoretically more stable) phases for ~80% of materials. When benchmarked against data-mining or DFT-based evolutionary predictions, SPINNER identifies more stable phases in many cases. By developing a reliable and fast structure-prediction framework, this work paves the way to large-scale, open exploration of undiscovered inorganic crystals.