醋酸锌对 InP/ZnSe 量子点表面钝化的增强作用

IF 7.2 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Chemistry of Materials Pub Date : 2024-06-07 DOI:10.1021/acs.chemmater.4c00492
Pieter Schiettecatte*, Luca Giordano, Ben Cruyssaert, Guillaume Bonifas, Norick De Vlamynck, Hannes Van Avermaet, Qiang Zhao, André Vantomme, Celine Nayral, Fabien Delpech and Zeger Hens*, 
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摘要

在照明和显示应用中,磷化铟(InP)量子点(QDs)是受限制的镉基 QDs 的主要替代品。通常情况下,InP QD 的光致发光(PL)是通过叠层生长由 ZnSe 和/或 ZnS 组成的铬化锌外壳来提高的。在这里,我们展示了使用基于氨基膦的化学方法合成的 InP/ZnSe QD 外表面被油胺和氯化锌钝化,而作为外壳生长前体的油酸锌则不在表面。因此,锌盐的表面浓度较低,导致配位不足的表面钙化物无法完全钝化,而钙化物是已知的陷阱态来源。我们证明,随后将 QDs 暴露于醋酸锌(一种温和的路易斯酸),可大幅提高 PL 量子产率(PLQY),从暴露前的约 40% 提高到暴露后的 90%。这一结果具有很高的可重复性,既可以通过在反应混合物中加入醋酸锌进行原位暴露,也可以通过在纯化的 InP 基 QDs 上进行异位暴露来实现。鉴于铬化锌经常被用作 QD 的外壳,这种钝化配位不足的铬化锌的方法有望提高各种核/壳 QD 系统的 PLQY。
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Enhanced Surface Passivation of InP/ZnSe Quantum Dots by Zinc Acetate Exposure

Indium phosphide (InP) quantum dots (QDs) represent the main alternative to restricted Cd-based QDs in lighting and display applications. Typically, the photoluminescence (PL) of InP QDs is increased by overgrowth of a zinc chalcogenide shell, consisting of ZnSe and/or ZnS. Here, we show that the outer surface of InP/ZnSe QDs synthesized using aminophosphine-based chemistry is passivated by oleylamine and zinc chloride, while zinc oleate, used as a precursor for shell growth, is absent from the surface. The resulting low surface concentration of zinc salts leads to an incomplete passivation of undercoordinated surface chalcogenides, a known source of trap states. We demonstrate that a subsequent exposure of the QDs to zinc acetate, a mild Lewis acid, drastically enhances the PL quantum yield (PLQY) from approximately 40% before to 90% after exposure. This outcome is highly reproducible and can be realized either through an in situ exposure by adding zinc acetate to the reaction mixture or an ex situ exposure on purified InP-based QDs. Given that zinc chalcogenides are frequently used as an outer shell for QDs, this method of passivating undercoordinated chalcogenides holds significant promise for enhancing the PLQY across a wide array of core/shell QD systems.

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来源期刊
Chemistry of Materials
Chemistry of Materials 工程技术-材料科学:综合
CiteScore
14.10
自引率
5.80%
发文量
929
审稿时长
1.5 months
期刊介绍: The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.
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