Stability and Dynamics of Sn-based Halide Perovskites: Insights from MACE-MP-0 and Molecular Dynamics Simulations

TL;DR

This study evaluates the MACE-MP-0 machine learning model's ability to predict the temperature-dependent structural stability and phase transitions of Sn-based halide perovskites using molecular dynamics simulations.

Contribution

It demonstrates that MACE-MP-0 can qualitatively reproduce key thermal and structural features of CsSnBr3 and Cs2SnBr6, serving as a useful initial predictive tool.

Findings

CsSnBr3 undergoes a low-temperature orthorhombic-to-cubic phase transition.

Cs2SnBr6 remains cubic and structurally rigid across 100 K to 500 K.

MACE-MP-0 captures major thermal and structural behaviors but misses some subtle phases.

Abstract

Tin-based halide perovskites have emerged as promising lead-free alternatives for optoelectronic applications, yet their structural stability and phase behavior at finite temperatures remain challenging to predict. Here, we assess the predictive capabilities of the foundational machine learning model MACE-MP-0 - trained on a broad chemical space and applied without system-specific fine-tuning - for the temperature-dependent behavior of CsSnBr3 and Cs2SnBr6. Molecular Dynamics simulations in the NpT ensemble were performed from 100 K to 500 K, and thermodynamic and structural descriptors including enthalpy, specific heat, radial distribution functions, translational order, bond angle distributions, and vibrational spectra were analyzed. Our results show that CsSnBr3 undergoes a low-temperature orthorhombic-to-cubic phase transition, evidenced by both the evolution of lattice parameters and subtle anomalies in enthalpy and specific heat, although the experimentally observed intermediate tetragonal phase is not captured. In contrast, Cs2SnBr6 remains cubic and maintains a more rigid octahedral framework across the entire temperature range. Overall, MACE-MP-0 qualitatively reproduces key thermal and structural features of these materials, highlighting its usefulness as a first step for studying new materials. For cases where capturing more subtle phase behavior is required, system-specific fine-tuning with Density Functional Theory data should be considered.