Lee, Jung-Hoon Jaffe, Adam Lin, Yu Karunadasa, Hemamala, I Neaton, Jeffrey B. 2024-01-19T17:03:18Z 2024-01-19T17:03:18Z 2021-09-05 2020-07-10 2380-8195 https://pubs.kist.re.kr/handle/201004/118388 Hybrid halide perovskites are promising for applications because of their favorable optoelectronic properties and low cost. Here we investigate the effects of hydrostatic pressure on the structural and electronic properties of (MA)PbI3 (MA = CH3NH3+) using first-principles density functional theory calculations. Our calculations predict that at a pressure of 0.23 GPa, the orthorhombic Fmmm phase becomes unstable with respect to a cubic Im (3) over bar phase, in good agreement with room-temperature experiments (similar to 0.3 GPa). At higher pressures, about 6 GPa, we predict the onset of pronounced intra- and interoctahedral distortions. This symmetry lowering leads to the introduction of I 5p-I 5p* antibonding and Pb 6p-Pb 6p bonding character into the valence band maximum (VBM) and the conduction band minimum (CBM) states, respectively. We find this change in bond character explains the evolution of the VBM and CBM states under compression, trends that ultimately lead to metallization at significantly higher pressures. English AMER CHEMICAL SOC DENSITY-FUNCTIONAL THEORY INDUCED AMORPHIZATION ENERGY 3D Origins of the Pressure-Induced Phase Transition and Metallization in the Halide Perovskite (CH3NH3)PbI3 Article 10.1021/acsenergylett.0c00772 1 ACS ENERGY LETTERS, v.5, no.7, pp.2174 - 2181 ACS ENERGY LETTERS 5 7 2174 2181 scie scopus 000552668000006 2-s2.0-85093847098 Chemistry, Physical Electrochemistry Energy & Fuels Nanoscience & Nanotechnology Materials Science, Multidisciplinary Chemistry Electrochemistry Energy & Fuels Science & Technology - Other Topics Materials Science Article DENSITY-FUNCTIONAL THEORY INDUCED AMORPHIZATION ENERGY 3D