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Tuning emission color of molecular fluorophores is of fundamental interest as it directly reflects the manipulation of excited states at the quantum mechanical level. Despite recent progress in molecular design and engineering on single fluorophores, a systematic methodology to obtain multicolor emission in aggregated or solid states, which gives rise to practical implications, remains scarce. In this study, we present a general strategy to continuously tune the emission color of a single-fluorophore aggregate by polymerization-mediated through-space charge transfer (TSCT). Using a library of well-defined styrenic donor (D) polymers grown from an acceptor (A) fluorophore by controlled radical polymerization, we found that the solid-state emission color can be fine-tuned by varying three molecular parameters: (i) the monomer substituent, (ii) the end groups of the polymer, and (iii) the polymer chain length. Experimental and theoretical investigations reveal that the color tunability originates from the structurally dependent TSCT process that regulates charge transfer energy.

Continuous color tuning of single-fluorophore emission via polymerization-mediated through-space charge transfer