Perylene Tetracarboxylic Acid Crosslinked to Silica Matrix that Enables Ultrahigh Solid‐State Quantum Yield and Efficient Photon Recycling for Holographic Luminescent Solar Concentrators

Perylene derivatives possess large absorptivity and high quantum yields (QYs) and thus are promising luminophores for luminescent solar concentrators (LSCs). Unfortunately, severe aggregation‐caused quenching, poor solubility, and large reabsorption significantly reduce their solid‐state photoluminescence. To address these issues, perylene tetracarboxylic acid (PTCA) is prepared by hydrolyzing perylene tetracarboxylic dianhydride in sodium hydroxide, which is highly compatible with amino‐silane precursors for in situ sol–gel synthesis of the silica matrix. In this case, highly luminescent and transparent PTCA@silica composites are formed, in which PTCA mainly exists in the monomer species due to covalent crosslinking to silica network structures. Therefore, a near‐unity solid‐state QY of ≈90% is obtained even at elevated loadings and existence of reabsorption due to the preservation of monomer states and efficient photon recycling. To demonstrate their potentials in LSCs, large‐area LSCs () with laminated configuration are fabricated, yielding a high power conversion efficiency of 1.1%. To mitigate the escape‐cone losses, the LSCs can be integrated with holographic grating, reaching an ultrahigh edge‐emission efficiency of 90%.