Crystallization of CH₃NH₃PbI₃ perovskite films was performed in supercritical carbon dioxide with and without organic cosolvents. Post deposition crystallization of the films was performed in a binary, single phase supercritical fluid at constant conditions (45$℃$, 1200 psi) but with varying cosolvent volume fractions up to 2 %. Organic cosolvents with varying polarity, propensity for hydrogen bonding and strength of solvation were used and the resulting perovskite film morphology, crystal structure and optical absorption spectra were measured. It was determined that the cosolvents can provide selective interactions with one or both of the perovskite precursor compounds resulting in different film morphologies ranging from uniform films containing large grains to films exhibiting large cubic or hexagonal crystals or preferential crystallographic orientations. The use of supercritical fluids to enhance or tune crystallization in solid-state thin films could have broad applications toward the realization of high efficiency photovoltaic devices.

CH ₃ NH ₃ PbI ₃钙钛矿薄膜的结晶是在有或没有有机助溶剂的超临界二氧化碳中进行的。薄膜的沉积后结晶是在恒定条件下在二元，单相超临界流体中进行的（45$℃$（例如1200 psi），但助溶剂的体积分数变化高达2％。使用具有不同极性，氢键结合倾向和溶剂化强度的有机助溶剂，并测量所得钙钛矿膜的形貌，晶体结构和光吸收光谱。已确定助溶剂可与钙钛矿前体化合物中的一种或两种提供选择性相互作用，从而导致不同的膜形态，范围从包含大晶粒的均匀膜到呈现大的立方或六方晶体或优先晶体学取向的膜。使用超临界流体来增强或调节固态薄膜中的结晶可能对实现高效光伏器件具有广泛的应用。