<br>强限域 CsPbBr3 量子点作为量子发射器和菱形超晶格的构建块,ACS Nano

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强限域 CsPbBr3 量子点作为量子发射器和菱形超晶格的构建块
ACS Nano ( IF 15.8 ) Pub Date : 2023-01-31 , DOI: 10.1021/acsnano.2c07677
Simon C Boehme _{1,

2} , Maryna I Bodnarchuk _{1,

2} , Max Burian ₃ , Federica Bertolotti ₄ , Ihor Cherniukh _{1,

2} , Caterina Bernasconi _{1,

2} , Chenglian Zhu _{1,

2} , Rolf Erni ₅ , Heinz Amenitsch ₆ , Denys Naumenko ₆ , Hordii Andrusiv _{1,

2} , Nazar Semkiv _{1,

2} , Rohit Abraham John _{1,

2} , Alan Baldwin _{7,

8} , Krzysztof Galkowski ₇ , Norberto Masciocchi ₄ , Samuel D Stranks _{7,

8} , Gabriele Rainò _{1,

2} , Antonietta Guagliardi ₉ , Maksym V Kovalenko _{1,

2}

Affiliation

Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, 8093 Zürich, Switzerland.
Laboratory for Thin Films and Photovoltaics, Empa, Swiss Federal Laboratories for Materials Science and Technology, 8600 Dübendorf, Switzerland.
Swiss Light Source, Paul Scherrer Institute, 5232 Villigen, Switzerland.
Department of Science and High Technology and To.Sca.Lab., University of Insubria, via Valleggio 11, 22100 Como, Italy.
Electron Microscopy Center, Empa, Swiss Federal Laboratories for Materials Science and Technology, 8600 Dübendorf, Switzerland.
Institute of Inorganic Chemistry, Graz University of Technology, 8010 Graz, Austria.
Cavendish Laboratory, University of Cambridge, JJ Thomson Avenue, Cambridge CB3 0HE, U.K.
Department of Chemical Engineering & Biotechnology, University of Cambridge, Philippa Fawcett Drive, Cambridge CB3 0AS, U.K.
Istituto di Cristallografia and To.Sca.Lab, Consiglio Nazionale delle Ricerche, via Valleggio 11, 22100 Como, Italy.

胶体半导体量子点 (QD) 领域的成功植根于对 QD 尺寸、形状和成分的精确合成控制，从而实现电子明确的功能纳米材料，从而促进基础科学并推动不同领域的应用。虽然强约束机制的利用一直在推动 InP 或 CdSe QD 的商业和科学兴趣，但这种机制尚未在卤化铅钙钛矿 QD 中得到彻底的探索和利用，这主要是由于迄今为止化学稳定性和尺寸不足钙钛矿量子点的单分散性小于约7 nm。在这里，我们通过使用双十二烷基二甲基溴化铵配体的后合成处理证明了化学稳定的强限制的 5 nm CsPbBr ₃胶体量子点。所实现的高尺寸单分散性 (7.5% ± 2.0%) 和形状均匀性使得 QD 超晶格的自组装具有特殊的长程有序、均匀的厚度、钝角为 104° 的不寻常菱形堆积和窄带青色发射。增强的化学稳定性表明强约束钙钛矿量子点有望用于溶液处理的单光子源，单量子点在室温下表现出 73% 的高单光子纯度和最小的闪烁（78%“开启”分数）。

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Strongly Confined CsPbBr3 Quantum Dots as Quantum Emitters and Building Blocks for Rhombic Superlattices

The success of the colloidal semiconductor quantum dots (QDs) field is rooted in the precise synthetic control of QD size, shape, and composition, enabling electronically well-defined functional nanomaterials that foster fundamental science and motivate diverse fields of applications. While the exploitation of the strong confinement regime has been driving commercial and scientific interest in InP or CdSe QDs, such a regime has still not been thoroughly explored and exploited for lead-halide perovskite QDs, mainly due to a so far insufficient chemical stability and size monodispersity of perovskite QDs smaller than about 7 nm. Here, we demonstrate chemically stable strongly confined 5 nm CsPbBr₃ colloidal QDs via a postsynthetic treatment employing didodecyldimethylammonium bromide ligands. The achieved high size monodispersity (7.5% ± 2.0%) and shape-uniformity enables the self-assembly of QD superlattices with exceptional long-range order, uniform thickness, an unusual rhombic packing with an obtuse angle of 104°, and narrow-band cyan emission. The enhanced chemical stability indicates the promise of strongly confined perovskite QDs for solution-processed single-photon sources, with single QDs showcasing a high single-photon purity of 73% and minimal blinking (78% “on” fraction), both at room temperature.

更新日期：2023-01-31

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