Spectrally Narrow Blue-Light Emission from Nonstoichiometric AgGaS2 Quantum Dots for Application to Light-Emitting Diodes

IF 8.3 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Materials & Interfaces Pub Date : 2024-11-25 DOI:10.1021/acsami.4c13987

Makoto Tozawa, Shuto Ofuji, Mizuki Tanaka, Kazutaka Akiyoshi, Tatsuya Kameyama, Takahisa Yamamoto, Genichi Motomura, Yoshihide Fujisaki, Taro Uematsu, Susumu Kuwabata, Tsukasa Torimoto

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Abstract

Luminescence color tuning of less toxic I–III–VI-based quantum dots (QDs) has been intensively investigated for application in wide-color-gamut displays. However, the emission peaks of these multinary QDs are relatively broad in the blue-light region compared to those in the green and red regions. Here, we report the synthesis of AgGaS₂ (AGS) QDs that show a narrow blue emission peak through nonstoichiometry control and surface defect engineering. While as-prepared AGS QDs with angular shapes primarily exhibited a weak green photoluminescence (PL) peak at 520 nm assigned to defect-site emission, treatment with chloride ions resulted in the appearance of a sharp band-edge PL peak at 442 nm, with the number of surface defect sites decreasing as a result of rounding off the angles of the QD shape. Further coating of the QDs with a gallium sulfide (GaS_x) shell selectively enhanced the band-edge PL peak at 446 nm with a narrow full width at half-maximum of 22 nm, where the defect-site emission was almost eliminated due to the removal of surface defect sites. The PL quantum yield (QY) significantly increased from 5.5% for chloride-treated AGS QDs to 12% for AGS core-GaS_x shell QDs (AGS@GaS_x). QD light-emitting diodes fabricated with AGS@GaS_x QDs exhibited a sharp emission peak at 450 nm, slightly red-shifted from that of the PL spectrum of the QD films, accompanied by the reappearance of a weak broad defect-site emission peak at around 560 nm.

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应用于发光二极管的非化学计量 AgGaS2 量子点发出光谱窄的蓝光

为了将毒性较低的 I-III-VI 基量子点 (QD) 应用于宽色域显示器，人们对其发光颜色调谐进行了深入研究。然而，与绿光和红光区域相比，这些二元量子点在蓝光区域的发射峰相对较宽。在此，我们报告了通过非化学计量控制和表面缺陷工程合成的 AgGaS2 (AGS) QDs，这种 QDs 显示出较窄的蓝色发射峰。制备的具有一定角度形状的 AGS QDs 在 520 纳米波长处主要表现出微弱的绿色光致发光（PL）峰，这属于缺陷位点发射；而用氯离子处理后，则在 442 纳米波长处出现了尖锐的带边 PL 峰，由于 QD 形状的角度变圆，表面缺陷位点的数量也随之减少。在 QD 上进一步涂覆硫化镓（GaSx）外壳可选择性地增强 446 nm 处的带边聚光峰，其窄半最大值全宽为 22 nm，由于表面缺陷位点的去除，缺陷位点发射几乎被消除。经氯化物处理的 AGS QDs 的 PL 量子产率（QY）从 5.5% 显著提高到 AGS 内核-GaSx 外壳 QDs（AGS@GaSx）的 12%。用 AGS@GaSx QD 制作的 QD 发光二极管在 450 纳米波长处显示出尖锐的发射峰，与 QD 薄膜的 PL 光谱相比略有红移，同时在 560 纳米波长处再次出现微弱的宽缺陷点发射峰。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Applied Materials & Interfaces 工程技术-材料科学：综合

CiteScore

16.00

自引率

6.30%

发文量

4978

审稿时长

1.8 months

期刊介绍： ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.