Effect of Cs vacancy on thermal conductivity in CsPbBr3 perovskites unveiled by deep potential molecular dynamics†

In addition to its excellent photoelectronic properties, the CsPbBr₃ perovskite has been reported as a low thermal conductivity (k) material. However, few studies investigated the microscopic mechanisms underlying its low k. Studying its thermal transport behavior is crucial for understanding its thermal properties and thus improving its thermal stability. Here, we train a DFT-level deep-learning potential (DP) of CsPbBr₃ and explore its ultra-low k using nonequilibrium molecular dynamics (NEMD). The k calculated using NEMD is 0.43 ± 0.01 W m⁻¹ K⁻¹, which is consistent with experimental results. Furthermore, the Cs vacancy contributes to the decrease in k due to the distortion of the Pb–Br cage, which enhances phonon scattering and reduces the phonon lifetime. Our research reveals the significant potential of machine learning force fields in thermal and phonon behavior research and the valuable insights gained from defect-regulated thermal conductivity.