The increasing demand for white light‐emitting diode (WLED) has prompted the development of phosphors, in which Ce3+‐activated garnet has been representative and widely investigated. The optimization and improvement of performance have long been a focus in the phosphor area. However, the trade‐off of phosphor performance always exists and is difficult to satisfy simultaneously, thereby necessitating a better understanding of the design principles that tune spectra performance comprehensively. Herein, the defect‐induced spectral tuning mechanism in a Ce‐doped garnet solid‐solution phosphor Ca1.5‐xY1.5+xAl3.5+xSi1.5‐xO12:Ce3+ (CYAS:Ce3+) is promoted. The enhancement of luminescence intensity and thermal stability together with red‐shift of emission can be achieved by chemical unit co‐substitution of [Y3+‐Al3+] for [Ca2+‐Si4+], which originated from the increasing anti‐site vacancy. The related mechanism is fully elucidated by combining structural and spectral analysis with density functional theory (DFT) calculations. This study provides a subtle control for the performance‐tuning of phosphors, which can deepen the understanding of the design principle inside‐out and the subsequent development and exploration of novel optoelectronic functional materials.

中文翻译：

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揭示掺杂 Ce 的石榴石固溶体荧光粉中缺陷引起的光谱调谐

对白光发光二极管（WLED）日益增长的需求促进了荧光粉的发展，其中Ce3+‐活化石榴石具有代表性并得到广泛研究。性能的优化和提升一直是荧光粉领域关注的焦点。然而，荧光粉性能的权衡始终存在，并且很难同时满足，因此需要更好地理解综合调节光谱性能的设计原理。本文研究了 Ce 掺杂石榴石固溶体荧光粉 Ca 中缺陷引起的光谱调谐机制1.5‐X是1.5+X铝3.5+X硅1.5‐X氧12:Ce3+(CYAS:Ce3+) 得到提升。通过化学单元共取代[Y]可以实现发光强度和热稳定性的增强以及发射红移3+‐铝3+] 为 [钙2+‐硅4+]，这源于反位点空缺的增加。通过将结构和谱分析与密度泛函理论（DFT）计算相结合，充分阐明了相关机制。该研究为荧光粉的性能调节提供了微妙的控制，可以加深对由内而外的设计原理的理解以及后续新型光电功能材料的开发和探索。