Constructing a Supramolecular Photosensitizer to Enhance Solid‐State Emission and Promote Fabrication Volume Grating

Abstract Visible‐light‐driven photopolymerization is a promising approach for fabricating high‐quality volume holographic gratings, with applications spanning high‐density data storage, augmented reality displays, and diffractive optical elements. However, a major limitation in this field is the aggregation‐caused quenching (ACQ) of organic dye‐based photosensitizers, which reduces their solid‐state emission efficiency and hinders energy transfer to co‐initiators. To overcome this challenge, a supramolecular strategy, integrated with density functional theory (DFT) calculations, is employed for the rapid screening and precise identification of the most compatible cyclodextrin host molecules. Methyl‐ β ‐cyclodextrin (Me‐ β ‐CD) is identified as the optimal host and utilized to encapsulate the dye 2,4‐Bis(4‐(diethylamino)benzylidene)cyclobutanone (C4) by a hydrothermal method. The resulting inclusion complex, stabilized by hydrogen bonding and van der Waals forces interactions, exhibit a twofold increase in fluorescence quantum yield, reaching 32% and significantly enhanced diffraction efficiency. This work highlights a novel strategy combining supramolecular chemistry to overcome ACQ and optimize photopolymerization systems, paving the way for advanced functional photopolymers in optical applications.