Ligand-Driven Facet Control of InAs-Based Quantum Dots for Enhanced Near- and Shortwave Infrared Emission

IF 6.1 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR
Hyunjin Cho, Yujin Kim, Whi Dong Kim, Young-Shin Park, Ju Young Woo, Hyung-Kyu Lim, Doh C. Lee
{"title":"Ligand-Driven Facet Control of InAs-Based Quantum Dots for Enhanced Near- and Shortwave Infrared Emission","authors":"Hyunjin Cho, Yujin Kim, Whi Dong Kim, Young-Shin Park, Ju Young Woo, Hyung-Kyu Lim, Doh C. Lee","doi":"10.1039/d5qi00142k","DOIUrl":null,"url":null,"abstract":"InAs-based quantum dots (QDs) are promising heavy-metal-free semiconductors for infrared emission technologies, offering tunable bandgaps via quantum confinement and excellent charge-carrier transport properties. Building on these advantages, we report the synthesis of QDs tailored for emission in the near-infrared (NIR) and short-wave infrared (SWIR) regions, emphasizing the critical role of capping ligands in controlling surface facet populations and nanocrystal morphology. Specifically, we demonstrate that the choice of ligand plays a critical role in determining the morphology and surface characteristics of InAs QDs. Using dioctylamine as a ligand results in InAs QDs with a spherical or tetrapod morphology, where nonpolar (110) facets are predominantly exposed on the surface. In contrast, oleic acid as a ligand promotes the formation of tetrahedral-shaped QDs with polar (111) crystalline planes being more prominently exposed. Using a one-pot synthesis approach, we successfully synthesized InAs/InZnP/ZnSe/ZnS core-multi-shell structures that effectively minimize interfacial defects. QDs with dioctylamine-capped core exhibit significantly higher photoluminescence quantum yield (PLQY) compared to those with oleic acid-capped cores. We achieved a PLQY of 39% at 1260 nm and 7.3% at 1420 nm with QDs using dioctylamine, representing efficiency values among the best reported in both the NIR and SWIR regions. Transient absorption (TA) spectroscopy reveals that dioctylamine-capped QDs exhibit reduced ground-state bleaching differences across excitation wavelengths compared to oleic acid-capped QDs, indicating significantly reduced interfacial trap states. These findings highlight the importance of ligand-driven facet control in the context of minimizing interfacial defect formation.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"57 1","pages":""},"PeriodicalIF":6.1000,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Inorganic Chemistry Frontiers","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1039/d5qi00142k","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}
引用次数: 0

Abstract

InAs-based quantum dots (QDs) are promising heavy-metal-free semiconductors for infrared emission technologies, offering tunable bandgaps via quantum confinement and excellent charge-carrier transport properties. Building on these advantages, we report the synthesis of QDs tailored for emission in the near-infrared (NIR) and short-wave infrared (SWIR) regions, emphasizing the critical role of capping ligands in controlling surface facet populations and nanocrystal morphology. Specifically, we demonstrate that the choice of ligand plays a critical role in determining the morphology and surface characteristics of InAs QDs. Using dioctylamine as a ligand results in InAs QDs with a spherical or tetrapod morphology, where nonpolar (110) facets are predominantly exposed on the surface. In contrast, oleic acid as a ligand promotes the formation of tetrahedral-shaped QDs with polar (111) crystalline planes being more prominently exposed. Using a one-pot synthesis approach, we successfully synthesized InAs/InZnP/ZnSe/ZnS core-multi-shell structures that effectively minimize interfacial defects. QDs with dioctylamine-capped core exhibit significantly higher photoluminescence quantum yield (PLQY) compared to those with oleic acid-capped cores. We achieved a PLQY of 39% at 1260 nm and 7.3% at 1420 nm with QDs using dioctylamine, representing efficiency values among the best reported in both the NIR and SWIR regions. Transient absorption (TA) spectroscopy reveals that dioctylamine-capped QDs exhibit reduced ground-state bleaching differences across excitation wavelengths compared to oleic acid-capped QDs, indicating significantly reduced interfacial trap states. These findings highlight the importance of ligand-driven facet control in the context of minimizing interfacial defect formation.
配体驱动的 InAs 基量子点表面控制用于增强近红外和短波红外发射
砷化铟基量子点(QDs)是红外发射技术领域前景广阔的无重金属半导体,通过量子约束提供可调带隙,并具有优异的电荷载流子传输特性。基于这些优势,我们报告了为近红外(NIR)和短波红外(SWIR)区域发射而定制的 QDs 的合成,强调了封接配体在控制表面面群和纳米晶体形态方面的关键作用。具体来说,我们证明了配体的选择在决定 InAs QDs 的形态和表面特征方面起着关键作用。使用二辛胺作为配体会产生具有球形或四足形态的 InAs QDs,其中非极性(110)面主要暴露在表面。与此相反,油酸作为配体可促进四面体形 QD 的形成,极性(111)晶面暴露得更明显。我们采用一锅合成法成功合成了 InAs/InZnP/ZnSe/ZnS 核心多壳结构,有效地减少了界面缺陷。与油酸封端的 QD 相比,二辛胺封端的 QD 具有更高的光致发光量子产率(PLQY)。使用二辛胺的 QD 在 1260 纳米波长的光量子产率为 39%,在 1420 纳米波长的光量子产率为 7.3%,其效率值在近红外和西南红外区域均名列前茅。瞬态吸收(TA)光谱显示,与油酸封接的 QD 相比,二辛胺封接的 QD 在不同激发波长下的基态漂白差异减小,这表明界面陷阱态显著减少。这些发现凸显了配体驱动的面控制在尽量减少界面缺陷形成方面的重要性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 求助全文
来源期刊
Inorganic Chemistry Frontiers
Inorganic Chemistry Frontiers CHEMISTRY, INORGANIC & NUCLEAR-
CiteScore
10.40
自引率
7.10%
发文量
587
审稿时长
1.2 months
期刊介绍: The international, high quality journal for interdisciplinary research between inorganic chemistry and related subjects
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信