量子点
光致发光
光漂白
超快激光光谱学
钙钛矿(结构)
光化学
材料科学
接受者
吸收(声学)
猝灭(荧光)
化学物理
光谱学
纳米技术
化学
荧光
光电子学
物理
量子力学
结晶学
凝聚态物理
复合材料
作者
Leon G. Feld,Simon C. Boehme,Viktoriia Morad,Yeşim Şahin,Christoph J. Kaul,Dmitry N. Dirin,Gabriele Rainò,Maksym V. Kovalenko
出处
期刊:ACS Nano
[American Chemical Society]
日期:2024-03-28
卷期号:18 (14): 9997-10007
标识
DOI:10.1021/acsnano.3c11359
摘要
Colloidal quantum dots (QDs) are promising regenerable photoredox catalysts offering broadly tunable redox potentials along with high absorption coefficients. QDs have thus far been examined for various organic transformations, water splitting, and CO2 reduction. Vast opportunities emerge from coupling QDs with other homogeneous catalysts, such as transition metal complexes or organic dyes, into hybrid nanoassemblies exploiting energy transfer (ET), leveraging a large absorption cross-section of QDs and long-lived triplet states of cocatalysts. However, a thorough understanding and further engineering of the complex operational mechanisms of hybrid nanoassemblies require simultaneously controlling the surface chemistry of the QDs and probing dynamics at sufficient spatiotemporal resolution. Here, we probe the ET from single lead halide perovskite QDs, capped by alkylphospholipid ligands, to organic dye molecules employing single-particle photoluminescence spectroscopy with single-photon resolution. We identify a Förster-type ET by spatial, temporal, and photon–photon correlations in the QD and dye emission. Discrete quenching steps in the acceptor emission reveal stochastic photobleaching events of individual organic dyes, allowing a precise quantification of the transfer efficiency, which is >70% for QD–dye complexes with strong donor–acceptor spectral overlap. Our work explores the processes occurring at the QD/molecule interface and demonstrates the feasibility of sensitizing organic photocatalysts with QDs.
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