Overcoming the Anisotropic Growth Limitations of Free‐Standing Single‐Crystal Halide Perovskite Films

Abstract It is extremely challenging to grow single‐crystal halide perovskite films (SCHPFs) with not only desired transport properties but also large lateral size with much thinner thickness. Here, we report the growth of freestanding single crystal CsPbBr 3 SCHPFs with thickness less than 100 nm and a lateral size close to centimeter for the first time. A new model for growth kinetics (Ψ=Aexp[−(E A −E s )/(k B T)]) is proposed to address the surface energy and temperature effect on the growth rate of ultrathin CsPbBr 3 single‐crystal film. The experimental results and DFT calculations both demonstrated that the surfactant plays a critical role in modifying the surface energy and achieving anisotropic growth. This work opens new opportunities for high‐quality SCHPFs with large lateral size and controllable thickness that may find wide applications for optoelectronic devices.