一种实现单层MoS2光致发光显著增强的有效缺陷工程策略

An effective defect engineering strategy for giant photoluminescence enhancement of MoS2 monolayers

陈荧 ¹黄卓睿 ¹刘华伟 ¹喻国粮 ²张金鼎 ¹徐哲元 ¹陈明星 ³李东 ¹马超 ¹黄明 ¹朱小莉 ¹陈舒拉 ¹蒋英 ¹潘安练⁴

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作者信息

1. Key Laboratory for Micro-Nano Physics and Technology of Hunan Province,Hunan Institute of Optoelectronic Integration,School of Physics and Electronics,College of Materials Science and Engineering,Hunan University,Changsha 410082,China
2. School of Physics and Electronics,Hunan Normal University,Changsha 410081,China
3. School of Physics and Electronics,Hunan Normal University,Changsha 410081,China;State Key Laboratory of Powder Metallurgy,Central South University,Changsha 410083,China
4. Key Laboratory for Micro-Nano Physics and Technology of Hunan Province,Hunan Institute of Optoelectronic Integration,School of Physics and Electronics,College of Materials Science and Engineering,Hunan University,Changsha 410082,China;School of Physics and Electronics,Hunan Normal University,Changsha 410081,China
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摘要

二维过渡金属硫族化合物(TMDCs)材料被认为是拓展摩尔定律的极具前景的候选材料.然而,该材料的低光致发光效率严重限制了其实际应用,其本质源于材料制备中不可避免引入的缺陷.在本文中,我们报道了一种Sr掺杂单层MoS2的有效缺陷工程策略,该策略在实验上通过简便的化学气相沉积(CVD)一步法成功实现.所制备的具有亚毫米(～324 μm)级的大尺寸样品的光致发光可实现高达两个数量级的增强,并伴随着载流子寿命的显著增强.这一现象主要归因于Sr掺杂后MoS2体系中其三激子向激子转换.与此同时,掺杂样品的辐射质量和稳定性也显著提升.第一性原理计算进一步阐明了其调控机制,即在MoS2中引入适当互补缺陷能级与其自身的缺陷能级协同,从而可调节其载流子组分,以实现光致发光的显著增强.此外,我们的缺陷工程策略也适用于其他掺杂剂,如钙掺杂剂.我们的工作报告了一种可以显著提升单层MoS2的荧光性能的有效缺陷工程策略,这为设计和调控二维TMDCs的光电特性提供一种极具前途的方法.

Abstract

Two-dimensional(2D)transition metal di-chalcogenide(TMDC)materials are considered as promising candidates to extend Moore's Law.However,the low photo-luminescence(PL)quantum yield due to the inevitable defects during material preparation severely restricts its practical applications.Here,we report an effective defect engineering strategy for Sr-doped MoS2 that has been successfully achieved by a facile one-step chemical vapor deposition(CVD)method.PL enhancement up to two orders of magnitude,along with prolonged carrier lifetime,is obtained by doping the sample with a lateral size up to sub-millimeter level(～324 μm).Such an observed phenomenon is attributed to the transformation of negative trions to neutral excitons.Meanwhile,the radia-tion quality and stability of the doped samples are sig-nificantly improved.First-principles calculations further elucidate the underlying mechanism,that is,the introduction of appropriate complementary defect energy levels in MoS2 synergizes with its own defect energy levels to enhance the PL emission,rather than a simple doping effect.In addition,our defect strategy can also be applied to other dopant like calcium atoms.Our work demonstrates an effective defect engineering strategy to improve the PL performance of 2D TMDCs,which provides a promising approach for designing and engineering their optoelectronic properties for potential applications.

关键词

MoS2/substitutional doping/photoluminescence in-tensity enhancement/first-principles calculations

Key words

MoS2/substitutional doping/photoluminescence in-tensity enhancement/first-principles calculations

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基金项目

National Natural Science Foundation of China(62375079)

National Natural Science Foundation of China(52072117)

National Natural Science Foundation of China(62375081)

National Natural Science Foundation of China(52221001)

National Natural Science Foundation of China(51972105)

National Natural Science Foundation of China(62090035)

National Natural Science Foundation of China(U19A2090)

National Natural Science Foundation of China(61905071)

National Key R&D Program of China(2022YFA1204300)

Key Program of Science and Technology Department of Hunan Province(2019XK2001)

Key Program of Science and Technology Department of Hunan Province(2020XK2001)

Key Research and Development Plan of Hunan Province(2023GK2012)

Open Project Program of Key Laboratory of Nanodevices and Applications,Suzhou Institute of Nano-Tech and Nano-Bionics,Chines(22ZS01)

Hunan Provincial Natural Science Foundation of China(2021JJ30132)

China Scholarship Council()

出版年

2024

中国科学:材料科学(英文)

CSTPCD

ISSN：

段落导航