Abstract
Doping is crucial for improving the properties of transition metal dichalcogenide (TMD) monolayers. However, most existing studies have focused on doping ability, and the research on doping distribution is rare. Recently, differences in the spatial distribution of dopants using chemical vapor deposition based on the spin-coating method have been investigated. Most of these doped TMDs are grown through a vapor–liquid–solid (VLS) growth mechanism. The doping distribution of TMD generated by the vapor–solid–solid (VSS) growth mechanism has not been studied extensively. Herein, various precursors such as Na2WO4, NaVO3, NaOH (Na-Pre), (NH4)2WO4, and NH4VO3 (NH4-Pre) are used to synthesize V–WS2. An entirely reversed doping distribution of the central and marginal regions is observed. Moreover, an interface where the concentration changes substantially is also observed. The spatial concentration of dopants is accurately confirmed through transmission electron microscope. According to the results from density functional theory, the difference in the doping distribution is caused by the initial state, which is related to the VLS and VSS growth mechanisms. This research provides a new method to control the distribution of dopants and is important for applications of doped TMD in microelectronic and nanoelectronic devices.
摘要
掺杂是改善过渡金属二硫族化合物(TMD)单层薄膜性能的重要 方法. 然而, 现有的研究大多集中在掺杂能力上, 对掺杂分布的研究还 处于起步阶段. 近年来, 基于旋涂化学气相沉积法研究了掺杂原子空间 掺杂分布的差异. 这些掺杂的TMD大多是通过气-液-固(VLS)生长机制 生长的. 采用气-固-固(VSS)生长机制生长的TMD尚未被用来深入研究 掺杂分布. 本文采用Na2WO4, NaVO3, NaOH (Na-Pre), (NH4)2WO4, NH4VO3 (NH4-Pre)等前驱体合成V–WS2. 观察到中心和边缘区域完全 相反的掺杂分布. 还观察到浓度变化较大的界面的出现. 通过透射电子 显微镜精确地表征了掺杂原子的空间浓度. 根据密度泛函理论的计算 结果, 掺杂分布的差异是由初始态引起的, 这与VLS和VSS的生长机制 有关. 这项工作为控制掺杂原子的分布提供了一种新的方法, 对掺杂 TMD在微电子和纳米电子器件中的应用具有重要意义.
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Acknowledgements This work was financially supported by the Science and Technology Commission of Shanghai Municipality (20501130200), the National Natural Science Foundation of China (51402342 and 61775201), and the National Defense Technology Innovation Special Zone Project.
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Author contributions Tian C and Xiao R conceived and designed the study and conducted the main experiments. Sui Y, Wang H and Feng Y helped to conduct the STEM and AFM measurements. Zhao S, Liu J, Sun H and Gao X assisted with the Raman and PL measurements. Peng S, Jin Z and Liu X analyzed the experimental data. Li P conducted the DFT calculation. Wang S and Yu G helped to revise the article. All authors contributed to the general discussion.
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Chuang Tian is a Master’s student under the guidance of Prof. Guanghui Yu at Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, China. She received her BSc degree from the School of Materials Science and Engineering, Huazhong University of Science and Technology in 2021. Her current research interest focuses on the growth and application of high-quality 2D materials.
Runhan Xiao received his Master’s degree under the guidance of Prof. Guanghui Yu from Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, China. He received his BSc degree from the School of Materials Science and Engineering, Tianjin University in 2020. His current research interest focuses on the growth and application of high-quality 2D materials.
Shuang Wang received his PhD degree from Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, China, under the supervision of Prof. Guanghui Yu. His research focuses on the growth and preparation of 2D materials.
Pai Li received his PhD degree from the University of Science and Technology of China (USTC) in 2018. Then, he took a postdoctoral research position at USTC and the Institute for Basic Science in Korea until the end of 2022. His research interest lies in the growth mechanism of novel materials using first-principles calculation and machine-learning force fields.
Guanghui Yu received his BSc degree from Jilin University. He obtained his PhD degree from Changchun Institute of Physics, Chinese Academy of Sciences, in 1999. Then, he worked as a postdoctoral fellow at Chiba University, Japan (1999–2002). He has been a professor and a group leader at Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, since 2002. His current research interest includes the controlled growth and applications of 2D crystals.
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Tian, C., Xiao, R., Sui, Y. et al. Opposite doping distribution in TMD monolayer regulated by VLS and VSS growth mechanism. Sci. China Mater. 66, 4723–4732 (2023). https://doi.org/10.1007/s40843-023-2615-1
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DOI: https://doi.org/10.1007/s40843-023-2615-1