Abstract
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.
Highlights
Among various light-emitting materials, organic/polymeric fluorescent materials are receiving increasing attention recently
End group library of well-defined styrenic donor (D) polymers grown from an acceptor (A) fluorophore by atom transfer radical polymerization (ATRP), we reveal that the solid-state emission color can be tuned in three different ways: (i) varying the monomer substituent, (ii) transforming the polymer end groups, and (iii) changing the polymer chain length
As a functional ATRP initiator with bidirectional initiating groups, Naphthalene diimide (NDI)-diBr was synthesized under mild conditions in high yield (>75% yield over two steps), enabling controlled growth of polymer chains from a single NDI molecule in the center
Summary
Among various light-emitting materials, organic/polymeric fluorescent materials are receiving increasing attention recently They offer flexibility and diversity due to highly varied molecular design and material processing options [1,2,3,4,5,6]. By incorporating different donor (D)/acceptor (A) fluorophore pairs in one polymer, blue-to-red emission color can be achieved for the resulted through-space charge transfer (TSCT) polymers, owing to the varied D-A charge transfer (CT) strength [12,13,14]. These strategies often require tedious and costly multistep organic syntheses. Supramolecular chemistry approaches [15,16,17] were used to design color-tunable fluorescent materials, but their usability is limited as they require the combination of multiple chemical species that causes instability and complicates the fabrication of devices
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