Microscopic Mechanism of the Heat-Induced Blueshift in Phosphors and a Logarithmic Energy Dependence on the Nearest Dopant– Vacancy Distance
Microscopic Mechanism of the Heat-Induced Blueshift in Phosphors and a Logarithmic Energy Dependence on the Nearest Dopant– Vacancy Distance
复制标题
荧光粉中热致蓝移的微观机制以及对最近掺杂剂空位距离的对数能量依赖性
DOI：
10.1002/anie.202116404
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Deng Shuiquan
中科院分区：
文献类型：
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作者：
Xu Jing;Huang Xueli;Cheng Xiyue;Whangbo Myung-Hwan;Deng Shuiquan
在许多发光材料中观察到的热致蓝移（HIB）是一种令人困惑的现象，几十年来一直无法解释。通过使用高通量的第一性原理计算和能量屏蔽技术，我们生成了五种荧光粉的一些模型结构，RbLi[Li 3SiO 4]2：Eu 2+，Na[Li 3SiO 4]：Eu 2+，K[Li 3SiO 4]：Eu 2+，Sr[LiAl 3 N4]：Eu 2+和Ca[LiAl 3 N4]：Eu 2+。我们的分析表明，在第一近似下，对数能量依赖于掺杂剂和金属阳离子空位之间的最近距离。通过识别 从屏蔽模型结构计算的电子结构的跃迁能，我们表明，Eu ~（2+）离子的振动躺在一个不对称和非谐势阱与电子态耦合，导致其HIB现象。
Heat‐induced blueshift (HIB) observed in many luminescent materials is a puzzling phenomenon that has remained unexplained for decades. By using the high‐throughput first‐principles calculations and energy‐screening techniques, we generated a number of model structures for five phosphors, RbLi[Li3SiO4]2:Eu2+, Na[Li3SiO4]:Eu2+, K[Li3SiO4]:Eu2+, Sr[LiAl3N4]:Eu2+, and Ca[LiAl3N4]:Eu2+. Our analyses suggest, to a first approximation, a logarithmic energy dependence on the nearest distance between the dopant and the metal‐cation vacancy. By identifying the transition energies from the electronic structures calculated for the screened model structures, we show that the vibration of the Eu2+ion lying in an asymmetric and anharmonic potential well couples with the electronic states, leading to their HIB phenomena.