Achieving color-tunable emission in single-component organic emitters with multistage stimuli-responsiveness is of vital significance for intelligent optoelectronic applications, but remains enormously challenging. Herein, we present an unprecedented example of a color-tunable single-component smart organic emitter (DDOP) that simultaneously exhibits multistage stimuli-responsiveness and multimode emissions. DDOP based on a highly twisted amide-bridged donor–acceptor–donor structure has been found to facilitate intersystem crossing, form multimode emissions, and generate multiple emissive species with multistage stimuli-responsiveness. DDOP pristine crystalline powders exhibit abnormal excitation-dependent emissions from a monomer-dominated blue emission centered at 470 nm to a dimer-dominated yellow emission centered at 550 nm through decreasing the ultraviolet (UV) excitation wavelengths, whereas DDOP single crystals show a wide emission band with a main emission peak at 585 nm when excited at different wavelengths. The emission behaviors of pristine crystalline powders and single crystals are different, demonstrating emission features that are closely related to the aggregation states. The work has developed color-tunable single-component organic emitters with simultaneous multistage stimuli-responsiveness and multimode emissions, which is vital for expanding intelligent optoelectronic applications, including multilevel information encryption, multicolor emissive patterns, and visual monitoring of UV wavelengths.
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