Achieve Phosphorescence Activation Through the Modulation of Intermolecular Forces within the Matrix

Abstract Carbon dots (CDs)‐based phosphorescent materials have attracted significant attention due to their widespread applications in anti‐counterfeiting technologies, bioimaging, optoelectronic devices, and other fields. However, synthesizing high‐efficiency phosphorescent CDs materials and elucidating their emission mechanisms remain critical challenges. In this study, phosphorescence in CDs is successfully activated by modulating intermolecular forces within the crystalline matrix. Experimental results demonstrate that precise spatial matching between matrix vacancies and guest carbon dots, achieved through silica introduction to regulate matrix‐driven interactions, is critical for this phenomenon. Notably, a phosphorescence quantum yield as high as 8.79% is achieved. This work provides mechanistic insights into phosphorescence generation in crystalline carbon dots and establishes a novel strategy for designing high‐performance phosphorescent carbon dot materials.