亲核共价配体实现了稳定短波红外探测器胶体InSb量子点的同时表面重建和钝化

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Dr. Yangning Zhang, Dr. Muhammad Imran, Dr. Pan Xia, Dr. Yiqing Chen, Ahmet Gulsaran, Yanjiang Liu, Ehsan Nikbin, Dr. Benjamin Rehl, Dr. Lizhou Fan, Dr. Filip Dinic, Dr. Da Bin Kim, Lewei Zeng, Prof. Dr. Mustafa Yavuz, Dr. Sjoerd Hoogland, Prof. Dr. Edward H. Sargent
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引用次数: 0

摘要

摘要锑化铟(InSb)胶体量子点(CQDs)具有较大的玻尔激子半径和在0.6 ~ 1.3 eV范围内可调的带隙,是短波红外(SWIR)光电探测器的理想候选材料。然而,在合成过程中,InSb表面上金属氧化物的形成阻碍了电荷传输,因此需要将CQD重铺策略集成到光电探测器中。先前的报道通过酸-卤化物顺序处理重铺这些cqd,在器件效率方面取得了进展,但器件的工作稳定性仍然令人不满意。本文报道了一种利用硫基亲核共价配体对InSb CQDs进行表面重构和钝化的溶液策略。我们发现短链硫醇分子通过亲核攻击去除表面金属氧化物,并通过强共价键实现In和Sb的强钝化,而金属硫化物在氧化物去除和钝化方面效果较差。因此,与对照相比,硫代酸钝化CQDs的陷阱态密度降低了10倍,并在5个月内保持结构和光学稳定。我们展示了InSb CQD SWIR光电探测器,在1450 nm处实现了28%的高外量子效率(EQE),在已有的CQD SWIR光电探测器中具有最高的工作稳定性,在偏置和照明操作300小时后保持了95%的性能。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Nucleophilic Covalent Ligands Enable Simultaneous Surface Reconstruction and Passivation of Colloidal InSb Quantum Dots for Stable Short-Wave Infrared Photodetectors

Nucleophilic Covalent Ligands Enable Simultaneous Surface Reconstruction and Passivation of Colloidal InSb Quantum Dots for Stable Short-Wave Infrared Photodetectors

Indium antimonide (InSb) colloidal quantum dots (CQDs) are promising candidates for short-wave infrared (SWIR) photodetectors due to their large Bohr exciton radius and tunable bandgap in the 0.6–1.3 eV range. However, the formation of metal oxides on InSb surfaces during synthesis impedes charge transport, necessitating CQD resurfacing strategies for integration into photodetectors. Previous reports achieved progress in device efficiency by resurfacing these CQDs with acid-halide sequential treatments, but the device operating stability remains unsatisfactory. Herein, we report a solution-phase strategy for surface reconstruction and passivation of InSb CQDs using sulfur-based nucleophilic covalent ligands. We find that short-chain thiol molecules remove surface metal oxides through nucleophilic attack and enable robust passivation of In and Sb via strong covalent bonds, whereas metal sulfides are less effective at oxide removal and passivation. Consequently, the thiolate-passivated CQDs exhibit a tenfold decrease in trap state density compared to controls and remain structurally and optically stable for 5 months. We demonstrate InSb CQD SWIR photodetectors that realize a high external quantum efficiency (EQE) of 28% at 1450 nm, with the highest operating stability among reported CQD SWIR photodetectors, retaining 95% of performance following 300 h of biased and illuminated operation.

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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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