Mechanism of the trivalent lanthanides' persistent luminescence in wide bandgap materials.
Mechanism of the trivalent lanthanides' persistent luminescence in wide bandgap materials.
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DOI：
10.1038/s41377-022-00736-5
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发表时间：
2022-03-08
期刊：
影响因子：
--
通讯作者：
Qiu J
中科院分区：
文献类型：
--
作者：
Li L;Li T;Hu Y;Cai C;Li Y;Zhang X;Liang B;Yang Y;Qiu J
三价镧系元素由于具有较宽的发光光谱范围而被广泛用作余辉发光材料的发光中心，引起了人们的广泛关注。然而，三价镧系元素荧光粉的来源问题至今仍是一个悬而未决的问题，这阻碍了稀土荧光粉的开发和应用。本文报道了除La ~（3+）、Lu ~（3+）和Pm ~（3+）外的12种三价镧系元素的掺杂发光，并提出了三价镧系元素在宽带隙基质中的掺杂发光机理。根据该机制，宽带隙材料中的激子将它们的复合能量转移到结合激子的三价镧系元素，随后产生三价镧系元素。在稀土离子的配位过程中，三价镧系元素作为等电子陷阱与激子结合，这种结合能力不仅与镧系元素4f电子的固有排列有关，还与阴离子配位和阳离子取代等外在配位场有关。我们的工作对设计高性能的荧光粉具有指导意义。报道了Gd ~（3+）的长余辉发光，提出了三价镧系元素在宽禁带基质中长余辉发光的可能机制。
The trivalent lanthanides have been broadly utilized as emitting centers in persistent luminescence (PersL) materials due to their wide emitting spectral range, which thus attract considerable attention over decades. However, the origin of the trivalent lanthanides’ PersL is still an open question, hindering the development of excellent PersL phosphors and their broad applications. Here, the PersL of 12 kinds of the trivalent lanthanides with the exception of La3+, Lu3+, and Pm3+ is reported, and a mechanism of the PersL of the trivalent lanthanides in wide bandgap hosts is proposed. According to the mechanism, the excitons in wide bandgap materials transfer their recombination energy to the trivalent lanthanides that bind the excitons, followed by the generation of PersL. During the PersL process, the trivalent lanthanides as isoelectronic traps bind excitons, and the binding ability is not only related to the inherent arrangement of the 4f electrons of the trivalent lanthanides, but also to the extrinsic ligand field including anion coordination and cation substitution. Our work is believed to be a guidance for designing high-performance PersL phosphors. Long persistent luminescence of Gd3+ is reported and a possible mechanism of the trivalent lanthanides’ persistent luminescence in wide bandgap hosts is proposed.
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