High-quality and millimeter-sized perovskite single crystals of CsPbBr and CsPbBr were prepared in organic solvents and studied for correlation between photocurrent generation and photoluminescence (PL) emission. The CsPbBr crystals, which have a 3D perovskite structure, showed a highly sensitive photoresponse and poor PL signal. In contrast, CsPbBr crystals, which have a 0D perovskite structure, exhibited more than 1 order of magnitude higher PL intensity than CsPbBr, which generated an ultralow photoresponse under illumination. Their contrasting optoelectrical characteristics were attributed to different exciton binding energies, induced by coordination geometry of the [PbBr] octahedron sublattices. This work correlated the local structures of lead in the primitive perovskite and its derivatives to PL spectra as well as photoconductivity.
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