Dynamically Modulating the Dissymmetry Factor of Circularly Polarized Organic Ultralong Room‐Temperature Phosphorescence from Soft Helical Superstructures

Achieving circularly polarized organic ultralong room-temperature phosphorescence (CP-OURTP) with a high luminescent dissymmetry factor (g_lum ) is crucial for diverse optoelectronic applications. In particular, dynamically controlling the dissymmetry factor of CP-OURTP can profoundly advance these applications, but it is still unprecedented. This study introduces an effective strategy to achieve photoirradiation-driven chirality regulation in a bilayered structure film, which consists of a layer of soft helical superstructure incorporated with a light-driven molecular motor and a layer of room-temperature phosphorescent (RTP) polymer. The prepared bilayered film exhibits CP-OURTP with an emission lifetime of 805 ms and a g_lum value up to 1.38. Remarkably, the g_lum value of the resulting CP-OURTP film can be reversibly controlled between 0.6 and 1.38 over 20 cycles by light irradiation, representing the first example of dynamically controlling the g_lum in CP-OURTP.