Efficient Single-Phase Tunable Dual-Color Luminescence with High Quantum Yield Greater than 100% for Information Encryption and LED Applications.

In modern society, the investigation of highly efficient photoluminescent bulk materials with excitation-induced tunable multicolor luminescence and multiexciton generation (MEG) is of great significance to information security and the application of optoelectronic devices. In this study, two bulk Cu-based halide crystals of (CHNO)CuBr·Br and (CHNO)CuI·I·HO, respectively, with one-dimensional structures were grown by a solvent evaporation method. Unexpectedly, (CHNO)CuI·I·HO displayed excitation-induced tunable dual-color luminescence; one band is a brilliant green-yellow emission centered at 547 nm with a high photoluminescence quantum yield (PLQY) of up to 169.67%, and the other is a red emission at 695 nm with a PLQY of 75.76%. Just as importantly, (CHNO)CuBr·Br exhibits a strong broadband green-yellow emission at 561 nm under broad band excitation ranging from 252 to 350 nm, a long PL decay lifetime of 106.9 μs, and an ultrahigh PLQY of 198.22%. These materials represent the first two examples of 1D bulk crystals and Cu(I)-based halides that have a PLQY exceeding 100%. Combining the unusual luminescence characteristics with theoretical calculations reveals that MEG contributes to the green-yellow emission with ultrahigh PLQY > 100%, and that the red emission can be ascribed to [CuI] cluster-centered emission. Additionally, an information encryption method was designed based on the Morse Code. The high luminescence characteristics of LED devices fabricated using the (CHNO)CuBr·Br and (CHNO)CuI·I·HO crystals appear to lead to promising applications in solid-state lighting. This work extends the catalog of high-performance luminescent materials and also promotes application prospects of low-dimensional copper-based halides in optoelectronics.