Abstract

Engineering surface structure can precisely and effectively tune optoelectronic properties of halide perovskites, but are incredibly challenging. Herein, we report the design and fabrication of uniform all-inorganic CsPbBr3 cubes/tetrahedrons single-crystals with precise control of (100) and (111) surface anisotropy, respectively. By combining theoretical calculations, we demonstrated that the preferred (100) surface engineering of CsPbBr3 single-crystals enables a lowest surface bandgap energy (2.33eV) and high-rate carrier mobility up to 241 μm2 V-1 s-1 , inherently boosting their light-harvesting and carrier transport capability. Whereas, the polar (111) surface induces ∼0.16eV upward surface-band bending and ultrahigh surface defect density of 1.49 × 1015 cm-3 , which is beneficial for enhancing surface defects-catalyzed reactions. Our work highlights the anisotropic surface engineering for boosting perovskite optoelectronic devices and beyond. This article is protected by copyright. All rights reserved.

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