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Efficient control of emission and carrier polarity in WS2 monolayer by indium doping

通过铟掺杂有效控制单层WS2的发射和载流子极性

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Abstract

Substitutional doping of two-dimensional (2D) transition metal dichalcogenides (TMDs) has been recognized as a promising strategy to tune their optoelectronic properties for a wide array of applications. However, controllable doping of TMDs remains a challenging issue due to the natural doping of these materials. Here, we demonstrate the controllable growth of indium-doped p-type WS2 monolayers with various doping concentrations via chemical vapor deposition (CVD) of a host tungsten (W) source and indium (In) dopant. Scanning transmission electron microscopy confirmed that In atoms successfully substitute the W atoms in the WS2 lattice. Intriguingly, the photoluminescence of the doped sample experiences strong intensity modulation by the doping concentration, which first increases remarkably with an enhancement factor up to ~35 and then decreases gradually when further increasing the doping concentration. Such a phenomenon is attributed to the progressive change of the exciton to trion ratio as well as the defect concentration in the doped samples. The assignment was further verified by the electric behavior of the fabricated In-doped WS2 field effect transistors, which changes regularly from n-type to bipolar and finally to p-type behavior with increasing doping concentration. The successful growth of p-type monolayer WS2 and the dual control of its optical and electrical properties by In doping may provide a promising method to engineer the opto-electronic properties of 2D materials.

摘要

二维(2D)过渡金属硫族化合物(TMDs)的掺杂被认为是调控其光电特性的一种有效途径. 但是TMDs材料在制备过程中会引入自身掺杂, 使其可控掺杂仍具有较大的挑战. 本文中我们通过含有钨(W)源和铟(In)源掺杂剂的化学气相沉积法(CVD)实现了不同铟掺杂浓度的单层WS2的可控制备. 扫描透射电镜结果表明In原子成功取代了WS2晶体中的W原子. 掺杂样品的发光特性受到了In掺杂浓度的明显调制, 其发光强度随掺杂浓度呈现出先增强后衰减的趋势, 最大增强倍数可达约35倍. 这一现象主要归因于In掺杂后WS2体系中激子与三激子的比例随掺杂浓度逐渐变化. 基于In掺杂的WS2场效应晶体管的电学特性表明, 随着In掺杂浓度的增加, 单层WS2实现了从本征n型到双极性, 最终到p型半导体的转变, 表明掺杂样品的载流子极性也受到了掺杂浓度的有效调控. 通过In掺杂可实现p型单层WS2的成功制备, 并且可对WS2体系光学和电学特性进行双重调制, 为实现2D材料光电特性的有效调控提供了一种潜在的可行方法.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (51525202, 61635001, 52072117 and 21703059), the Key Program of the Hunan Provincial Science and Technology Department (2019XK2001), and the International Science and Technology Innovation Cooperation Base of Hunan Province (2018WK4004).

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. Department of Key Laboratory for Micro-Nano Physics and Technology of Hunan Province, State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Materials Science and Engineering, Hunan University, Changsha, 410082, China

    Ying Chen  (陈荧), Chen Yi  (易琛), Shula Chen  (陈舒拉), Xingxia Sun  (孙兴霞), Chao Ma  (马超), Dong Li  (李东), Chenglin He  (何承林), Ziyu Luo  (骆子煜), Boyi Xu  (徐博一), Zheyuan Xu  (徐哲元) & Anlian Pan  (潘安练)

  2. Department of School of Physics and Electronics, Hunan University, Changsha, 410082, China

    Ying Jiang  (蒋英), Huawei Liu  (刘华伟), Feng Jiang  (姜峰), Weihao Zheng  (郑玮豪) & Biyuan Zheng  (郑弼元)

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  1. Ying Chen  (陈荧)
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  8. Dong Li  (李东)
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  10. Ziyu Luo  (骆子煜)
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  11. Feng Jiang  (姜峰)
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  12. Weihao Zheng  (郑玮豪)
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  15. Zheyuan Xu  (徐哲元)
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  16. Anlian Pan  (潘安练)
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Contributions

Chen Y, Jiang Y and Pan A conceived and designed the project, and wrote the manuscript. Liu H, Sun X and Li D performed the device fabrication and characterizations. Yi C, Ma C, Chen S, He C, Luo Z, Jiang F, Zheng W, Zheng B, Xu B and Xu Z conducted the SEM, STEM, AFM, PL, TRPL and Raman measurements, and advised on data analysis. Pan A supervised the experiments and provided theoretical guidance. All authors contributed to the general discussion.

Corresponding author

Correspondence to Anlian Pan  (潘安练).

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Conflict of interest

The authors declare no conflict of interest.

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 photoelectric devices.

Ying Jiang received her MSc degree in electronics and systems from Jilin University in 2010 and PhD degree (“Pass with Distinction and Honour”) in physical chemistry from Instituto Superior Tecnico, University of Lisbon, in 2015. She is currently an associate professor at the School of Physics and Electronics, Hunan University. Her current research interests focus on the ultrafast spectroscopic study of 2D transition metal dichalcogenide 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 the Max Planck Institute of Microstructure Physics, and then joined Arizona State University as a Postdoctoral Fellow, where he became a research assistant professor. He joined Hunan University in 2010 and has been working as the distinguished professor of “Furong Scholar” in Hunan province since then. His research interests include the micro-nano optical, electronics of semiconductor nanostructures.

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Chen, Y., Jiang, Y., Yi, C. et al. Efficient control of emission and carrier polarity in WS2 monolayer by indium doping. Sci. China Mater. 64, 1449–1456 (2021). https://doi.org/10.1007/s40843-020-1594-2

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