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 (glum) 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 glum value up to 1.38. Remarkably, the glum 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 glum in CP‐OURTP. We propose an effective strategy for achieving circularly polarized organic ultralong room‐temperature phosphorescence (CP‐OURTP) with a high dissymmetry factor based on a bilayered soft helical superstructure doped with a light‐driven molecular motor and room‐temperature polymer layer. This enables the significant modulation of reflection across a wide spectral range and the dynamic controlling the dissymmetry factor of CP‐OURTP from 1.38 to 0.60.