Light‐Dynamic Chirality Inversion of Circularly Polarized Organic Ultralong Room‐Temperature Phosphorescence Enabled by Soft Helical Superstructure

Abstract Dynamic and reversible manipulation of circularly polarized luminescence (CPL) in soft materials is highly desirable for advanced chiroptical devices, information encryption, and labeling technology. However, this remains a formidable challenge in circularly polarized organic ultralong room‐temperature phosphorescence (CP‐OURTP) materials. Herein, a bilayered chiral‐switchable CP‐OURTP system is presented, composed of a light‐driven hydrazone photoswitch (M1)‐doped soft helical superstructure layer and a room temperature phosphorescence (RTP) polymer layer, enabling dynamic chirality inversion in a reversible manner under alternating stimulation of 460 and 340 nm light irradiation. The obtained bilayered film exhibits CP‐OURTP with a maximum absolute luminescence dissymmetry factor ( g lum ) value of 0.39 and a long‐lived emission lifetime of 823 ms. Notably, the g lum values of the bilayered CP‐OURTP film can be dynamically and reversibly modulated between +0.30 and−0.35 under the irradiation of light with different wavelengths over 50 cycles without fatigue, owing to the photoinduced configuration changes of M1, making the first example of dynamically and reversibly regulating the chirality inversion in CP‐OURTP materials.