Amorphous polymers with ultralong room‐temperature phosphorescence (RTP) are highly promising for various applications. Particularly, polymer‐based RTP materials with multiple functions such as color‐tunability or stimulus‐response are highly desirable for multilevel anti‐counterfeiting but are rarely reported. Herein, a facile strategy is presented to achieve a series of polymer‐based RTP materials with ultralong lifetime, multicolor afterglow, and reversible response to UV irradiation by simply embedding pyridine‐substituted triphenylamine derivatives into the polymer matrix poly(vinyl alcohol) (PVA) and poly(methyl methacrylate) (PMMA), respectively. Notably, the pyridine group with the capabilities of promoting intersystem crossing and forming hydrogen‐bonding interactions is essential for triggering ultralong RTP from the doping PVA system, among which the doping film TPA‐2Py@PVA exhibits excellent RTP property with an ultralong lifetime of 798.4 ms and a high quantum yield of 15.2%. By further co‐doping with the commercially available fluorescent dye, multicolor afterglow is obtained via phosphorescence energy transfer. Meanwhile, the doped PMMA system exhibits reversible photoactivated ultralong RTP properties under continuous UV irradiation. Finally, potential applications of these doped PVA and PMMA systems with ultralong lifetime, multicolor afterglow, and photoactivated ultralong RTP in multidimensional anti‐counterfeiting are demonstrated.
Amorphous polymers with ultralong room-temperature phosphorescence (RTP) have received considerable attention due to their potential applications in anti-counterfeiting, bioimaging, and sensing. However, multifunctional polymer-based RTP materials endowed with color-tunability or stimulus-responsiveness are highly desirable but rarely reported. Herein, we have designed three pyridine-substituted triphenylamine derivatives and achieved ultralong RTP properties with both color-tunability and UV irradiation-responsiveness by embedding them into poly(vinyl alcohol) (PVA) and poly(methyl methacrylate) (PMMA) matrices, respectively. Notably, introducing the pyridine groups with the capabilities of promoting intersystem crossing (ISC) and forming hydrogen-bonding networks is essential for triggering efficient and ultralong RTP from doping PVA systems. Consequently, doping film TPA-2Py@PVA exhibits excellent RTP property with an ultralong lifetime of 798.4 ms and a high quantum yield of 15.2%. Moreover, by co-doping with the fluorescent dye rhodamine B, color-tunable persistent luminescence has been realized via phosphorescence energy transfer. More importantly, doping PMMA systems exhibit reversible UV irradiation-responsive ultralong RTP properties. Finally, various patterns are devised to demonstrate the potential applications of these doping PVA and PMMA systems in advanced anti-counterfeiting and information encryption. We believe this feasible and facile strategy to achieve multifunctional organic RTP materials with color-tunability and stimulus-responsiveness will provide new opportunities for high-tech applications.
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