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In this study, different electronic structure evolutions of perovskite singlecrystals are found via angle-resolved photoelectron spectroscopy (ARPES): (i)unchanged top valence band (VB) dispersions under different temperatures can befound in the CH3NH3PbI3, (ii) phase transitions induced the evolution of top VBdispersions, and even a top VB splitting with Rashba effects can be observed inthe CH3NH3PbBr3. Combined with low-energy electron diffraction (LEED),metastable atom electron spectroscopy (MAES), and DFT calculation, we confirmdifferent band structure evolutions observed in these two perovskite singlecrystals are originated from the cleaved top surface layers, where thedifferent surface geometries with CH3NH3+-I in CH3NH3PbI3 and Pb-Br inCH3NH3PbBr3 are responsible for finding band dispersion change and appearing ofthe Rashba-type splitting. Such findings suggest that the top surface layer inorganic halide perovskites should be carefully considered to create functionalinterfaces for developing perovskite devices.

Surface geometry determined temperature-dependent band structure evolutions in organic halide perovskite single crystals