Quantifying Dynamic Tilting in Halide Perovskites: Chemical Trends and Local Correlations

J. Wiktor, E. Fransson, D. Kubicki, and P. Erhart
doi: 10.48550/arXiv.2304.07402
zenodo: 7889314 (associated data)
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Halide perovskites have emerged as one of the most interesting materials for optoelectronic applications due to their favorable properties, such as defect-tolerance and long charge carrier lifetimes, which are attributed to their dynamic softness. However, this softness has led to apparent disagreements between the local instantaneous and global average structures of these materials. In this work, we assess the local tilt angles of octahedra in the perovskite structure through large-scale molecular dynamics simulations using machine learned potentials based on density functional theory. We compare structural properties given by different density functionals, namely PBE, PBEsol, SCAN, and vdW-DF-cx, and establish trends across a family of CsMX3 with M=Sn or Pb and X=Cl, Br or I perovskites. Notably, we demonstrate a strong short-range ordering that persists even in the cubic phase of halide perovskites. This ordering is reminiscent of the tetragonal phase and bridges the disordered local structure and the global cubic arrangement. Our results provide a deeper understanding of the structural properties of halide perovskites and their local distortions, which is crucial for further understanding their optoelectronic properties.

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