Texture Formation in Polycrystalline Thin Films of All-Inorganic Lead Halide Perovskite.

Abstract

Controlling grain orientations within polycrystalline all-inorganic halide perovskite solar cells can help increase conversion efficiencies toward their thermodynamic limits; however, the forces governing texture formation are ambiguous. Using synchrotron X-ray diffraction, mesostructure formation within polycrystalline CsPbI_2.85 Br_0.15 powders as they cool from a high-temperature cubic perovskite (α-phase) is reported. Tetragonal distortions (β-phase) trigger preferential crystallographic alignment within polycrystalline ensembles, a feature that is suggested here to be coordinated across multiple neighboring grains via interfacial forces that select for certain lattice distortions over others. External anisotropy is then imposed on polycrystalline thin films of orthorhombic (γ-phase) CsPbI_3- _x Br_x perovskite via substrate clamping, revealing two fundamental uniaxial texture formations; i) I-rich films possess orthorhombic-like texture (<100> out-of-plane; <010> and <001> in-plane), while ii) Br-rich films form tetragonal-like texture (<110> out-of-plane; <110> and <001> in-plane). In contrast to relatively uninfluential factors like the choice of substrate, film thickness, and annealing temperature, Br incorporation modifies the γ-CsPbI_3- _x Br_x crystal structure by reducing the orthorhombic lattice distortion (making it more tetragonal-like) and governs the formation of the different, energetically favored textures within polycrystalline thin films.