Machine learning the density functional theory potential energy surface for the inorganic halide perovskite CsPbBr3

Abstract

Structural phase transitions as a function of temperature dictate the structure--functionality relationships in many technologically important materials. Harmonic Hamiltonians have proven successful in predicting the vibrational properties of many materials. However, they are inadequate for modeling structural phase transitions in crystals with potential energy surfaces that are either strongly anharmonic or no\ n-convex with respect to collective atomic displacements or homogeneous strains. In this paper we develop a framework to express highly anharmonic first-principles potential energy surfaces as polynomials of collective cluster deformati\ ons. We further adapt the approach to a nonlinear extension of the cluster expansion formalism through the use of an artificial neural net model. The machine learning models are trained on a large database of first-principles calculations and are shown to reproduce the potential energy surface with l\ ow error.