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通过使用基于非金属的廉价HCl/HI进行卤化物交换,在室温、露天大气的溶液相中瞬时合成钙钛矿量子点:系综和单粒子光谱。

Instantaneous, room-temperature, open-air atmosphere, solution-phase synthesis of perovskite quantum dots through halide exchange employing non-metal based inexpensive HCl/HI: ensemble and single particle spectroscopy.

作者信息

Mandal Saptarshi, Roy Debjit, De Chayan K, Ghosh Swarnali, Mandal Mrinal, Das Ananya, Mandal Prasun K

机构信息

Department of Chemical Sciences, Indian Institute of Science Education and Research (IISER) Kolkata Mohanpur West Bengal 741246 India

Centre of Advanced Functional Materials, Indian Institute of Science Education and Research (IISER) Kolkata Mohanpur West Bengal 741246 India.

出版信息

Nanoscale Adv. 2019 Jul 9;1(9):3506-3513. doi: 10.1039/c9na00406h. eCollection 2019 Sep 11.

DOI:10.1039/c9na00406h
PMID:36133552
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9419528/
Abstract

Herein, the instantaneous synthesis of highly crystalline, uniform-sized ( 11.3 ± 0.1 nm), blue-to-green to yellow to red-emitting all-inorganic perovskite quantum dots (CsPbBr and mixed halide PQDs) was achieved at room temperature under an open-air atmosphere (no glove box) through halide exchange in the solution phase employing easily available, inexpensive non-metal-based halide sources such as HCl and HI. No complicated pre-treatment of the halide source was required. Moreover, these PQDs were stable for a few weeks under an open-air atmosphere. The PL emission spectra are quite narrow, and the PLQYs are quite high (80% for even Br/I mixed PQDs). At the single particle level, the 〈ON fraction〉 has been noted to vary from 75% to 85% for different PQDs, the values are close to 1.0, and the values are >1.5. The latter indicates that long ON durations are more probable. The increase in the ON event truncation time (from 2.7 to 4.0 s) and the concomitant decrease in the OFF event truncation time (from 6.6 to 4.3 s) could be correlated with the increase in the PLQY (from 0.55 to 0.75). In addition, an interesting memory effect could be observed in both the ON and the OFF event durations.

摘要

在此,通过在溶液相中使用易于获得的、廉价的非金属基卤化物源(如HCl和HI)进行卤化物交换,在室温下的露天大气环境(无手套箱)中实现了高结晶度、尺寸均匀(11.3±0.1纳米)、发射蓝光至绿光再到黄光至红光的全无机钙钛矿量子点(CsPbBr和混合卤化物量子点)的瞬时合成。卤化物源无需复杂的预处理。此外,这些量子点在露天大气环境下可稳定存在数周。其光致发光发射光谱相当窄,光致发光量子产率相当高(即使是Br/I混合量子点也高达80%)。在单粒子水平上,不同量子点的〈开启分数〉在75%至85%之间变化, 值接近1.0, 值大于1.5。后者表明开启持续时间更长的可能性更大。开启事件截断时间的增加(从2.7秒至4.0秒)以及伴随的关闭事件截断时间的减少(从6.6秒至4.3秒)可能与光致发光量子产率的增加(从0.55至0.75)相关。此外,在开启和关闭事件持续时间中均可观察到有趣的记忆效应。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b1a5/9419528/6ffb686858bd/c9na00406h-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b1a5/9419528/bbcd42e5e35a/c9na00406h-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b1a5/9419528/afd99bbf5078/c9na00406h-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b1a5/9419528/2f42fd63c3e1/c9na00406h-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b1a5/9419528/f8c79abebda3/c9na00406h-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b1a5/9419528/6ffb686858bd/c9na00406h-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b1a5/9419528/bbcd42e5e35a/c9na00406h-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b1a5/9419528/afd99bbf5078/c9na00406h-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b1a5/9419528/2f42fd63c3e1/c9na00406h-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b1a5/9419528/f8c79abebda3/c9na00406h-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b1a5/9419528/6ffb686858bd/c9na00406h-f4.jpg

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本文引用的文献

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Ce-Doping to Modulate Photoluminescence Kinetics for Efficient CsPbBr Nanocrystals Based Light-Emitting Diodes.Ce 掺杂调制基于 CsPbBr 纳米晶的高效发光二极管的光致发光动力学。
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Bright triplet excitons in caesium lead halide perovskites.
钙钛矿卤化物中的亮三重激子。
Nature. 2018 Jan 10;553(7687):189-193. doi: 10.1038/nature25147.
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Highly Luminescent CsPbX (X=Cl, Br, I) Nanocrystals Achieved by a Rapid Anion Exchange at Room Temperature.通过室温下快速阴离子交换制备的高发光性CsPbX(X = Cl、Br、I)纳米晶体。
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