Continuous tuning of persistent luminescence wavelength by intermediate-phase engineering in inorganic crystals

Multicolor tuning of persistent luminescence has been extensively studied by deliberately integrating various luminescent units, known as activators or chromophores, into certain host compounds. However, it remains a formidable challenge to fine-tune the persistent luminescence spectra either in organic materials, such as small molecules, polymers, metal-organic complexes and carbon dots, or in doped inorganic crystals. Herein, we present a strategy to delicately control the persistent luminescence wavelength by engineering sub-bandgap donor-acceptor states in a series of single-phase Ca(Sr)ZnOS crystals. The persistent luminescence emission peak can be quasi-linearly tuned across a broad wavelength range (500-630 nm) as a function of Sr/Ca ratio, achieving a precision down to ~5 nm. Theoretical calculations reveal that the persistent luminescence wavelength fine-tuning stems from constantly lowered donor levels accompanying the modified band structure by Sr alloying. Besides, our experimental results show that these crystals exhibit a high initial luminance of 5.36 cd m^-² at 5 sec after charging and a maximum persistent luminescence duration of 6 h. The superior, color-tunable persistent luminescence enables a rapid, programable patterning technique for high-throughput optical encryption.