Organic room-temperature phosphorescent (RTP) materials exhibiting reversible changes in optical properties upon exposure to external stimuli have shown great potential in diverse optoelectronic fields. Particularly, dynamic manipulation of response behaviors for such materials is of fundamental significance, but it remains a formidable challenge. Herein, a series of RTP polymers were prepared by incorporating phosphorescent rotors into polymer backbone, and these materials show color-tunable persistent luminescence upon excitation at different wavelengths. Experimental results and theoretical calculations revealed that the various molecular conformations of monomers are responsible for the excitation wavelength-dependent (Ex-De) RTP behavior. Impressively, after gaining insights into the underlying mechanism, dynamic control of Ex-De RTP behavior was achieved through thermal energy driven molecular rotations of monomers. Eventually, we demonstrate the practical applications of these amorphous polymers in anti-counterfeiting areas. These findings open new opportunities for the control of response behaviors of smart-responsive RTP materials through external stimuli rather than conventional covalent modification method.

Single molecules with dual persistent luminescence are very rarely explored, in spite of their emerging use in frontier optoelectronic applications. Here, a pure organic phosphor of tris(4‐chlorophenyl)phosphine oxide (CPO) possessing a large energy gap between the lowest excited triplet (T1) and higher excited triplet (T2) states is reported, which can emit dual persistent room‐temperature phosphorescence (RTP) from low‐ and high‐lying triplet excited states. The femtosecond transient absorption experiments and theoretical calculations reveal that the excitons to the T1 and T2 states are populated through different pathways. As a result, the distribution of the triplet excitons can be efficiently manipulated by using different excitation energy, and tunable afterglow colors from green to yellow can be achieved. Furthermore, the CPO molecule is successfully applied in the fabrication of high‐level anti‐counterfeiting tags and flexible 3D objects with curling properties. From these initial discoveries, it is expected that triphenylphosphine derivatives, with their rich chemistry of core‐substitution, can provide infinite opportunities in the expansion of organic molecules with high‐lying persistent RTP.

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Persistent room temperature phosphorescent materials with unique mechanical properties and robust optical properties have great potential in flexible electronics and photonics. However, developing such materials remains a formidable challenge. Here, we present highly stretchable, lightweight, and multicolored persistent luminescence elastomers, produced by incorporating ionic room temperature phosphorescent polymers and polyvinyl alcohol into a polydimethylsiloxane matrix. These prepared elastomers exhibit high optical transparency in daylight and emit bright persistent luminescence after the removal of 365 nm excitation. The homogeneous distribution of polymers within the matrix has been confirmed by confocal fluorescence microscopy, scanning electron microscopy, and atomic force microscopy. Mechanical property investigations revealed that the prepared persistent luminescence elastomers possess satisfactory stretchability. Impressively, these elastomers maintain robust optical properties even under extensive and repeated mechanical deformations, a characteristic previously unprecedented. These fantastic features make these persistent luminescence elastomers ideal candidates for potential applications in wearable devices, flexible displays, and anti-counterfeiting.