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Boosting STE and Nd3+ NIR Luminescence in Cs2AgInCl6 Double Perovskite via Na+/Bi3+-Induced Local Structure Engineering
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-08-21 , DOI: 10.1002/adfm.202304577
Shilin Jin 1 , He Yuan 1 , Tao Pang 2 , Manjia Zhang 1 , Youwu He 3 , Bin Zhuang 1 , Tianmin Wu 3 , Yuanhui Zheng 4, 5 , Daqin Chen 1, 4, 6, 7
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-08-21 , DOI: 10.1002/adfm.202304577
Shilin Jin 1 , He Yuan 1 , Tao Pang 2 , Manjia Zhang 1 , Youwu He 3 , Bin Zhuang 1 , Tianmin Wu 3 , Yuanhui Zheng 4, 5 , Daqin Chen 1, 4, 6, 7
Affiliation
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Currently, lanthanide (Ln3+) doped Pb-free double perovskites (DPs) suffer from competitive emissions of the self-trapped exciton (STE) and Ln3+. Herein, a new type of Nd3+-doped Cs2AgInCl6 DPs with Na+/Bi3+ co-alloying is developed. Benefiting from Na+/Bi3+-induced local structural modification, both STE broadband visible luminescence and Nd3+ near-infrared (NIR) emissions are boosted via free exciton sensitization. Specifically, a total 648-fold enhancement in emitting intensities compared to the Na+/Bi3+-free counterpart is realized, with a significantly improved NIR photoluminescence quantum yield (PLQY) from 0.16% to 30.3%. First-principles density functional theory calculations, Raman spectra, and steady/transient-state PL spectra verify the modification of local site symmetry, breakdown of parity-forbidden absorption, and reduction of electron-phonon coupling via Na+/Bi3+ doping. Finally, a compact vis–NIR broadband light-emitting diode (LED) is designed by coupling the Na/Bi/Nd: Cs2AgInCl6 DP with a commercial ultraviolet LED chip, which shows promising applications in spectroscopic analyses and multifunctional lighting.
中文翻译：
通过 Na+/Bi3+ 诱导局部结构工程增强 Cs2AgInCl6 双钙钛矿中的 STE 和 Nd3+ 近红外发光
目前，镧系元素（Ln 3+）掺杂的无铅双钙钛矿（DP）受到自陷激子（STE）和Ln 3+的竞争性发射的影响。本文开发了一种新型的Nd 3+掺杂Cs 2 AgInCl 6 DPs，其具有Na + /Bi 3+共合金化。受益于Na + /Bi 3+诱导的局部结构修饰，STE 宽带可见光发光和Nd 3+近红外（NIR）发射均通过自由激子敏化而增强。具体而言，与不含Na + /Bi 3+的对应物相比，发射强度总共提高了648倍，近红外光致发光量子产率（PLQY）从0.16%显着提高到30.3%。第一性原理密度泛函理论计算、拉曼光谱和稳态/瞬态PL光谱验证了局部位点对称性的修改、宇称禁止吸收的破坏以及通过Na + / Bi 3+掺杂减少电子-声子耦合。最后，通过将Na/Bi/Nd: Cs 2 AgInCl 6 DP与商用紫外LED芯片耦合设计了紧凑型可见光-近红外宽带发光二极管（LED），该器件在光谱分析和多功能照明方面显示出良好的应用前景。
更新日期：2023-08-21
中文翻译：
通过 Na+/Bi3+ 诱导局部结构工程增强 Cs2AgInCl6 双钙钛矿中的 STE 和 Nd3+ 近红外发光
目前，镧系元素（Ln 3+）掺杂的无铅双钙钛矿（DP）受到自陷激子（STE）和Ln 3+的竞争性发射的影响。本文开发了一种新型的Nd 3+掺杂Cs 2 AgInCl 6 DPs，其具有Na + /Bi 3+共合金化。受益于Na + /Bi 3+诱导的局部结构修饰，STE 宽带可见光发光和Nd 3+近红外（NIR）发射均通过自由激子敏化而增强。具体而言，与不含Na + /Bi 3+的对应物相比，发射强度总共提高了648倍，近红外光致发光量子产率（PLQY）从0.16%显着提高到30.3%。第一性原理密度泛函理论计算、拉曼光谱和稳态/瞬态PL光谱验证了局部位点对称性的修改、宇称禁止吸收的破坏以及通过Na + / Bi 3+掺杂减少电子-声子耦合。最后，通过将Na/Bi/Nd: Cs 2 AgInCl 6 DP与商用紫外LED芯片耦合设计了紧凑型可见光-近红外宽带发光二极管（LED），该器件在光谱分析和多功能照明方面显示出良好的应用前景。
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