期刊
ADVANCED SCIENCE
卷 9, 期 32, 页码 -出版社
WILEY
DOI: 10.1002/advs.202203735
关键词
charge transfer; double perovskites; lanthanide ions; local electronic structure; near-infrared luminescence
资金
- National Natural Science Foundation of China [U1805252, 21975257, 12074380, 12004384, 22135008]
- Key Research Program of the Chinese Academy of Sciences [ZDRW-CN-2021-3]
- CAS/SAFEA International Partnership Program for Creative Research Teams
- Natural Science Foundation of Fujian Province [2021L3024, 2019J01403]
The study unveils the strategy of Cl-Yb3+ charge transfer sensitization in Ln(3+)-doped Cs2NaInCl6 DPs, resulting in efficient NIR luminescence of Ln(3+). The localized electrons of [YbCl6](3-) octahedron in Cs2NaInCl6 DPs facilitate the Cl-Yb3+ charge transfer process. The mechanism of Cl-Yb3+ charge transfer sensitization is verified by spectroscopic experiments and theoretical calculations. Furthermore, the efficient NIR emission of Er3+ is also realized using the same strategy. These findings provide fundamental insights for optical manipulation of Ln(3+)-doped halide DPs.
Lanthanide ion (Ln(3+))-doped halide double perovskites (DPs) have evoked tremendous interest due to their unique optical properties. However, Ln(3+) ions in these DPs still suffer from weak emissions due to their parity-forbidden 4f-4f electronic transitions. Herein, the local electronic structure of Ln(3+)-doped Cs2NaInCl6 DPs is unveiled. Benefiting from the localized electrons of [YbCl6](3-) octahedron in Cs2NaInCl6 DPs, an efficient strategy of Cl--Yb3+ charge transfer sensitization is proposed to obtain intense near-infrared (NIR) luminescence of Ln(3+). NIR photoluminescence (PL) quantum yield (QY) up to 39.4% of Yb3+ in Cs2NaInCl6 is achieved, which is more than three orders of magnitude higher than that (0.1%) in the well-established Cs2AgInCl6 via conventional self-trapped excitons sensitization. Density functional theory calculation and Bader charge analysis indicate that the [YbCl6](3-) octahedron is strongly localized in Cs2NaInCl6:Yb3+, which facilitates the Cl--Yb3+ charge transfer process. The Cl--Yb3+ charge transfer sensitization mechanism in Cs2NaInCl6:Yb3+ is further verified by temperature-dependent steady-state and transient PL spectra. Furthermore, efficient NIR emission of Er3+ with the NIR PLQY of 7.9% via the Cl--Yb3+ charge transfer sensitization is realized. These findings provide fundamental insights into the optical manipulation of Ln(3+)-doped halide DPs, thus laying a foundation for the future design of efficient NIR-emitting DPs.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据