%0 Journal Article %T Light-Regulated Nucleation for Growing Highly Uniform Single-Crystalline Microrods. %A Sun L %A Gong Y %A Che Y %A Ji H %A Liu B %A Che Y %A Zhao J %J Angew Chem Int Ed Engl %V 63 %N 20 %D 2024 May 13 %M 38497168 %F 16.823 %R 10.1002/anie.202402253 %X We report a light-irradiation method to control the synchronous nucleation of a donor-acceptor (D-A) fluorophore for growing highly uniform single-crystalline microrods, which is in sharp contrast to the prevailing methods of restricting spontaneous nucleation and additionally adding seeds. The D-A fluorophore was observed to undergo photoinduced electron transfer to CrCl3, leading to the generation of HCl and the subsequent protonation of the D-A fluorophore. By intensifying photoirradiation or prolonging its duration, the concentration of protonated D-A fluorophores can be rapidly increased to a high supersaturation level. This results in the formation of a controlled number of nuclei in a synchronous manner, which in turn kickstart the epitaxial growth of protonated D-A fluorophores towards uniform single-crystalline microrods of controlled sizes. The light-regulated synchronous nucleation and uniform growth of microrods are a unique phenomenon that can only be achieved by specific Lewis acids, making it a novel probing method for sensitively detecting strong Lewis acids such as chromium chloride.