Degenerate Lattice-Instability-Driven Amorphization under Compression in Metal Halide Perovskite CsPbI 3

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Halide perovskites have been intensively investigated for photovoltaic applications because of their good optoelectronic properties and low cost. Various high-pressure experiments have shown that these materials generally undergo reversible phase transitions between different crystalline phases as well as between crystalline and amorphous phases under external pressure. Herein, using first-principles density functional theory (DFT) and ab initio molecular dynamics (AIMD) calculations, we investigate the origin of the pressure-induced amorphization in CsPbI 3 . We find that the amorphous-like structures obtained from AIMD calculations become more stable than the orthorhombic Pbnm phase above 6.66 GPa, in good agreement with the experimental value (4.44 GPa). We further find that an imaginary flat band appears in the phonon dispersion of the orthorhombic CsPbI 3 phase across the Brillouin zone at 10 GPa, leading to degenerate lattice instabilities. These energetically degenerate phonon modes are related to PbI 6 octahedral tilting modes and provide random local distortions, leading to amorphization.