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

一种实现单层MoS2光致发光显著增**的有效缺陷工 程策略

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Abstract

Two-dimensional (2D) transition metal dichalcogenide (TMDC) materials are considered as promising candidates to extend Moore’s Law. However, the low photoluminescence (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 do** 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 radiation quality and stability of the doped samples are significantly 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 do** 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.

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 **, 并伴随着载流子寿命的显著增**. 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**. 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.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (62375079, 52072117, 62375081, 52221001, 51972105, 62090035, U19A2090, and 61905071), the National Key R&D Program of China (2022YFA1204300), the Key Program of Science and Technology Department of Hunan Province (2019XK2001 and 2020XK2001), the Key Research and Development Plan of Hunan Province (2023GK2012), the Open Project Program of Key Laboratory of Nanodevices and Applications, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences (22ZS01), the Hunan Provincial Natural Science Foundation of China (2021JJ30132), and the China Scholarship Council.

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Author notes

  1. These authors contributed equally to this work.

Authors and Affiliations

  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

    Ying Chen  (陈荧), Zhuorui Huang  (黄卓睿), Huawei Liu  (刘华伟), **ding Zhang  (张金鼎), Zheyuan Xu  (徐哲元), Dong Li  (**东), Chao Ma  (马超), Ming Huang  (黄明), **aoli Zhu  (朱小莉), Shula Chen  (陈舒拉), Ying Jiang  (蒋英) & Anlian Pan  (潘安练)

  2. School of Physics and Electronics, Hunan Normal University, Changsha, 410081, China

    Guoliang Yu  (喻国粮), Mingxing Chen  (陈明星) & Anlian Pan  (潘安练)

  3. State Key Laboratory of Powder Metallurgy, Central South University, Changsha, 410083, China

    Mingxing Chen  (陈明星)

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  1. Ying Chen  (陈荧)
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Contributions

Author contributions Chen Y, Huang Z, Jiang Y, Chen S and Pan A conceived and designed this project, and wrote and revised the manuscript. Yu G and Chen M carried out DFT theoretical calculations. Zhang J, Xu Z, Li D, Ma C and Zhu X performed AFM, SEM, STEM, PL, Raman and TRPL measurements and provided recommendations for data analysis. Jiang Y, Chen S and Pan A supervised the experiments and provided theoretical guidance. All authors contributed to the general discussion.

Corresponding authors

Correspondence to Shula Chen  (陈舒拉), Ying Jiang  (蒋英) or Anlian Pan  (潘安练).

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Conflict of interest The authors declare that they have no conflict of interest.

Additional information

Supplementary information Experimental details and supporting data are available in the online version of the paper.

Ying Chen is currently a PhD candidate at the College of Materials Science and Engineering, Hunan University. His main research interests include the synthesis of nanomaterials with controlled CVD route and their applications in optoelectric devices

Zhuorui Huang is currently a Master student at the College of Materials Science and Engineering, Hunan University. His main research interests include the synthesis of 2D materials and their applications in optoelectric devices.

Shula Chen received his PhD degree from the Department of Physics, Linkö** University, Sweden, in 2014. After that, he worked as a postdoctoral researcher at the Graduate School of Information Science and Technology, Hokkaido University, Japan. Later on, in 2016, he returned to Linkö** University and became a lecturer. In 2019, He joined the College of Materials Science and Engineering, Hunan University as a professor. Currently, his main research interests cover nano-photonics of III-V-based semiconductors, opto-spintronic properties and device applications of emerging 2D semiconductors and low-dimensional perovskite materials.

Ying Jiang received the MS degree in electronics and systems from Jilin University in 2010 and her PhD degree in physical chemistry from Instituto Superior Tecnico, University of Lisbon, in 2015. She is currently an associate professor in School of Physics and Electronics, Hunan University. Her current research interests focus on the ultrafast spectroscopic study of 2D transition metal dichalcogenides materials and perovskite nanostructures.

Anlian Pan received his PhD degree from the Institute of Physics, Chinese Academy of Sciences in 2006. Afterwards, he worked for one year as a Humboldt Research Fellow with Prof. Ulrich Goesele at Max Planck Institute of Microstructure Physics, and then joined Arizona State University as a Postdoctoral Fellow, where he became a research assistant professor. He came back to Hunan University in 2010 and had been working as the distinguished professor of “Furong” scholar in Hunan province since then. His research interests include the micronano optical, and electronics of semiconductor nanostructures.

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Chen, Y., Huang, Z., Liu, H. et al. An effective defect engineering strategy for giant photoluminescence enhancement of MoS2 monolayers. Sci. China Mater. (2024). https://doi.org/10.1007/s40843-024-2974-7

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