Full-color tuning of emissive materials is attracting great interest in a wide range of applications. While polymers offer flexible structural design and excellent material processability, a general methodology to easily generate full-color solid-state fluorescent polymers with simple chemical structures is lacking. Here, guided by predictive machine learning models, we proposed a versatile polymer platform with full-color emission tuning via manipulation of through-space charge transfer (TSCT). Using a single-acceptor fluorophore as the initiator for atom transfer radical polymerization (ATRP), a series of electron-donor groups containing simple polycyclic aromatic moieties were introduced by one-step copolymerization using commercial monomers or monomers modified in a single step. Upon fine-manipulation of donor-acceptor interplay via simple controlled polymer synthesis, the resulted TSCT polymer library showed continuously tunable emission colors from sky-blue to deep red (Figure 1a). The experimental results rendered a good external validation of the developed machine learning model (R<sup>2</sup> = 0.871 in emission wavelength). The structure-property relationship was investigated via theoretical calculations, confirming the TSCT-induced emission redshifts. We further demonstrated the developed TSCT polymers can be used to design solid-state stimuli-responsive materials with high-contrast photochromic fluorescence, which were applied to light-controlled information encryption (Figure 1b).

Full-color tunable polymers with high-contrast photochromic fluorescence via though-space charge transfer

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ACS Fall 2022

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