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.