Poly(vinyl alcohol) induced chirality inversion and amplification of circularly polarized room-temperature phosphorescence in homopolypeptide aggregates

Organic circularly polarized room-temperature phosphorescence (CPRTP) materials represent an emerging research frontier with broad application prospects. However, achieving efficient and controllable CPRTP remains challenging due to inefficient chirality transfer and the limited ability to regulate chiral environments. Here, we develop a strategy involving self-assembled chiral homopolypeptides to realize manipulable CPRTP. Chiral homopolypeptides functionalized with achiral phosphorescent terminals are first designed, which self-assemble into vesicles exhibiting weak CPRTP. Remarkably, dispersing these vesicles into a poly(vinyl alcohol) matrix induces structural reorganization, leading to inversion and significant amplification of CPRTP. Experimental and computational studies reveal the critical role of matrix-assistance in chirality propagation, inversion, and amplification. Moreover, multicolor afterglow films with tunable emissions are readily achieved by varying the terminal phosphor. This work not only establishes a universal platform for constructing tunable CPRTP materials through homopolypeptide self-assembly but also provides deep mechanistic insights into supramolecular chirality manipulation. The development of materials exhibiting efficient and controllable circularly polarized room-temperature phosphorescence remains challenging, primarily due to inefficient chirality transfer and the limited ability to regulate chiral environments. Here, the authors address this challenge by constructing homopolypeptide vesicles bearing achiral phosphorescent terminals and embedding them within a poly(vinyl alcohol) matrix.