Abstract
By adding molar-controlled SbCl3 in a Cs3Sb2Cl9 precursor, we employed a low-temperature solution-processed approach to prepare high-quality (001)-preferred Cs3Sb2Cl9 thin film, which demonstrates a stable defect-dominated broadband emission at room temperature. Density functional theory calculations reveal that the defect emission originates from the donor-acceptor pair (DAP) recombination between chlorine vacancy (VCl) and cesium vacancy (VCs). Furthermore, VCl + VCs DAP is more stable on the (001) surface. The improved film quality and the more stable VCl + VCs DAP increase the activation energy related to defect states, resulting in an enhancement of the defect emission for the high-quality (001)-preferred film. This work provides deep insight into the key role of the (001) surface in defect emission and a feasible strategy to enhance the defect emission in 2D halide perovskites A3B2X9 (A = CH3NH3, Cs, Rb; B = Bi, Sb; X = Cl, Br, I) by control of the thin film preferred orientation.
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