Generalized Growth of Halide Perovskite Single Crystals Promoted by Light‐Inhibited Nucleation

Abstract Significant advances have been achieved in thermally‐driven growth of halide perovskite single crystals (HPSCs). However, unmanageable crystal nucleation presents long‐term challenges to artificial regulation of the growth of HPSCs. Here a generalized growth strategy of HPSCs by light‐thermally synergistic modulation nucleation is reported. The light‐excited carriers of perovskite pre‐nucleation clusters form strong electrostatic layers, leading to stronger repulsion between the clusters and finally inhibiting nucleation driven by thermal energy. The crystal nuclei concentration in the precursor is greatly decreased by as much as 2 orders of magnitudes, which enables the growth of an individual single crystal in one synthesis with a 96.8% high yield. The synthesized and processed perovskites exhibited good stability underwater or long‐term light irradiation. The crystals can be both size‐, type‐ and shape‐controlled by manipulating the different crystallization parameters. This light modulated nucleation route would help optimize the solution‐based HPSCs growth and promote their applications.