Ab-initio investigation of the structural, electronic and optical properties of CsPbBr3 perovskite under pressure using the DFT-1/2 method

Abstract

Pressure-induced phase transitions in metal halide perovskites lead to significantly different material properties and offer great potential for diverse applications. The electronic, structural, and optical properties of Cesium lead bromide (CsPbBr3) crystals are investigated using density functional theory (DFT) to draw an integrated picture of orbital morphology, absorption spectra, and band gap values. Spin-orbit coupling and DFT-1/2 correction are used to gain a better insight into electronic properties and band splitting in the cubic phase. Calculations of pressure-induced phase transitions, electronic band gap engineering, and manipulation of optical absorption edges of CsPbBr3 are conducted. In the cubic and tetragonal crystal lattices, a band gap closure and opening occurs demonstrating a Dirac cone upon application and increase of pressure. Indeed, in the tetragonal lattice of CsPbBr3, a topological band occurs. Orthorhombic perovskite crystal lattice undergoes successive direct-indirect and indirect-direct band gap transitions, followed by a space group change at extreme pressures. However, under pressure, orthorhombic non-perovskite lattice experiences a sudden band gap breakdown. Phase and band gap transitions are explained by orbital hybridizations and structural symmetry evolution (e.g., bond length contraction/dilation and octahedral cage rotation/distortion). These results provide comprehensive guidelines for further experimental studies on pressure engineering, advanced photovoltaic and optoelectronic applications, discovering and understanding new topological band structures of perovskite materials.