Moisture-Triggered Solid-Phase Molecular Self-Assembly with Facial Amphiphiles for Efficient and Full-Color Organic Room-Temperature Phosphorescence

Abstract Although room-temperature phosphorescent (RTP) materials have been extensively investigated, the facile generation of efficient RTP at ambient conditions remains a long-standing challenge. Here, we demonstrate a moisture-triggered solid-phase molecular self-assembly (SPMSA) strategy to construct RTP materials through the coassembly of facially rigid amphiphiles─such as sodium cholate (SC)─and fluorescent dyes. This approach simultaneously achieves particle adhesion, molecular rearrangement, and the effective isolation and rigidification of dyes. Mechanistic studies reveal that dye molecules spontaneously diffuse into the hydrophobic pockets formed by SC, where intermolecular interactions promote spin–orbit coupling (SOC) and facilitate intersystem crossing (ISC). These factors, combined with the rigid environment provided by the facially rigid SC matrix, cooperatively suppress nonradiative transitions of triplet excitons. Consequently, we achieve a long phosphorescence lifetime of up to 830 ms and full-spectrum visible RTP. Leveraging these advantages, we demonstrate water-based RTP inks, RTP coatings and RTP 3D origami, offering a green and sustainable pathway for the development of advanced luminescent materials.