Highly Elastic Full Hydrocarbon Ultralong RTP Polymers with Visible Light Excitable S₀→T₁ Population

Abstract Highly elastic ultralong organic room temperature phosphorescence (RTP) polymers are highly desired in wearable optoelectronic fields, but they are hardly realized in rubbers since chain segment motions deactivate triplet excitons. In the current work, it is revealed that polystyrene (PS) can inhibit triplet thermal deactivation of coronene (Cor), and it is the serious oxygen diffusion and quenching that disables RTP emission of Cor/polymers. In view of oxygen barrier function of rubbers, PS−polyisoprene−PS tri‐block elastomers (SIS) are used as Cor's doping matrices. The results show that Cor/SIS sheets show bright and ultralong afterglow with RTP lifetime up to 3.64 s in air after brief 365 nm light excitation. More impressively, Cor/SIS and its red fluorescent dye doped sheets all exhibit ultralong room temperature afterglow under large dynamic elastic deformation. Further, all these sheets exhibit long‐wave blue light excited afterglow despite Cor/SIS having no visible light absorption band, and the unique photoexcitation and emission mechanism is verified. This work not only provides the development strategy of the latest elastic RTP materials, but also will evoke a fresh understanding on organic doped RTP polymers.