材料科学
钙钛矿(结构)
光致发光
量子效率
镱
吸收(声学)
纳米晶
兴奋剂
发光
分析化学(期刊)
光电子学
纳米技术
化学
结晶学
色谱法
复合材料
作者
Joo Yeon D. Roh,Tyler J. Milstein,Daniel R. Gamelin
出处
期刊:ACS Nano
[American Chemical Society]
日期:2023-08-22
卷期号:17 (17): 17190-17198
被引量:4
标识
DOI:10.1021/acsnano.3c05053
摘要
Ytterbium-doped all-inorganic lead-halide perovskites (Yb3+:CsPb(Cl1–xBrx)3) show broadband absorption and exceptionally high near-infrared photoluminescence quantum yields, providing opportunities for solar spectral shaping to improve photovoltaic power conversion efficiencies. Here, we report that Yb3+:CsPb(Cl1–xBrx)3 NCs also show extremely strong negative thermal quenching of the Yb3+ luminescence, with intensities at room temperature >100 times those at 5 K for some compositions. Analysis of this temperature dependence as a function of x shows that it stems from thermally activated quantum cutting related to the temperature dependence of the spectral overlap between the PL of the perovskite (donor) and the simultaneous-pair absorption of two Yb3+ ions (acceptor). In the Yb3+:CsPbBr3 limit, this spectral overlap goes to zero at 5 K, such that only single-Yb3+ sensitization requiring massive phonon emission occurs. At room temperature, Yb3+ PL in this composition is enhanced ∼135-fold by thermally activated quantum cutting, highlighting the extreme efficiency of quantum cutting relative to single-Yb3+ sensitization. These results advance the fundamental mechanistic understanding of quantum cutting in doped perovskites, with potential ramifications for solar and photonics technologies.
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