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Interface-engineered Au@MoS2 core-shell heterostructures with superior hot-carrier transfer dynamics for plasmonics and optoelectronics

界面工程实现Au@MoS2核壳异质结在等离激元学和光电子学领域卓越的热载流子输运动力学

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Abstract

Heterostructures constructed by noble metals and two-dimensional (2D) semiconductors offer a unique charge transport path to collect hot carriers from plasmonic nanostructures and thus are promising for various plasmonic and optoelectronic devices. However, the desired charge transfer speed and efficiency of the conventional heterostructures are usually restricted by the limited interface area and inevitable interface distortion and contamination. Herein, we report the ultrafast and high-efficiency hot electron transfer by creating a novel Au@MoS2 core-shell heterostructure with atomically sharp and dramatically enlarged interface. Our femtosecond transient absorption spectroscopy study indicates the hot-electron injection from Au nanoparticles to MoS2 in Au@MoS2 is within 244 fs, compared with the 493 fs of the mechanically-transferred Au/MoS2 control sample. And meanwhile, the injection efficiency is improved from 3.33% of Au/MoS2 to 25.3% of our Au@MoS2. The results are further proved by Kelvin probe force microscopy and discrete dipolar approximation studies, which provide strong evidences that the improved charge transfer is attributed to the atomic-level clean and fully-encapsulated interface of the product. This study provides fundamental understanding of the intrinsic charge transfer within Au@MoS2 heterostructures and thus demonstrates an intriguing material geometry for future plasmonic and optoelectronic devices.

摘要

贵金属和二维半导体构建的异质结为等离激元纳米结构产生的热载流子提供了独特的电荷传输路径, 有望应用于各种等离激元和光电子器件. 然而, 传统异质结构的电荷转移速度和效率通常受限于有限的界面面积和不可避免的界面污染. 本文中, 具有原子级清洁和较大接触界面的新型Au@MoS2核壳异质结构能够实现超快和高效的热电子转移. 飞秒瞬态吸收光谱研究表明, Au@MoS2中从金纳米颗粒到MoS2的热电子注入时间常数小于244 fs, 而机械转移方法制备的Au/MoS2对照样品的热电子注入时间常数为493 fs, 同时, 电荷转移效率从Au/MoS2的3.33%提升至Au@MoS2的25.3%. 开尔文探针力显微镜和离散偶极近似研究进一步证明了上述结果, 明显改善的电荷转移归因于原子级清洁和完全封装的异质结界面. 这项研究提供了贵金属-二维半导体异质结构内固有电荷转移的基本理解, 从而展现了Au@MoS2这一新型异质结结构在等离激元和光电子器件中的应用前景.

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Acknowledgements

This work was supported by the Ministry of Science and Technology of China (2021YFA1200501), the National Natural Science Foundation of China (U22A20137, U21A2069, and 21825103), Guangdong Basic and Applied Basic Research Foundation (2020A1515110330), and Shenzhen Science and Technology Innovation Program (JCYJ20220818102215033, GJHZ20210705142542015, and JCYJ20220530160811027). We also thank the technical support from the Analytical and Testing Center at Huazhong University of Science and Technology, and the support from the Queen Mary–HUST Strategic Partner Fund.

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Author notes

  1. These authors contributed equally to this work.

Authors and Affiliations

  1. State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074, China

    Ran Liu  (刘然), Shenghong Liu  (刘盛洪), Decai Ouyang  (欧阳德才), XiaoXi Ma  (马小茜), Fangfang Xia  (夏芳芳), Yuan Li  (李渊) & Tianyou Zhai  (翟天佑)

  2. Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan, 430074, China

    Xiangyu Zhu  (朱翔宇) & Wenxi Liang  (梁文锡)

  3. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Nanostructure Research Center, Wuhan University of Technology, Wuhan, 430070, China

    Yimeng Yu  (余一梦) & Jinsong Wu  (吴劲松)

  4. School of Engineering and Materials Science, Queen Mary University of London, Mile End Road, London, E1 4NS, UK

    Han Zhang  (张悍)

  5. State Key Laboratory of Digital Manufacturing Equipment and Technology, School of Mechanical Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074, China

    Shiyuan Liu  (刘世元)

  6. Shenzhen Huazhong University of Science and Technology Research Institute, Shenzhen, 518057, China

    Yuan Li  (李渊) & Tianyou Zhai  (翟天佑)

Authors
  1. Ran Liu  (刘然)
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Contributions

Author contributions Liu R and Zhu X conducted the experiments and wrote the paper; Liu S performed the DDA simulation; Ouyang D drew schematic diagrams of the sample interface structure and instruments; Xia F provided instrument usage support; Yu Y and Wu J performed part of the TEM measurement; Ma X, Zhang H and Liu S performed some data analysis and offered helpful suggestions. Zhai T, Li Y and Liang W designed this study, analyzed the data and offered helpful suggestions. All authors contributed to the general discussion.

Corresponding authors

Correspondence to Wenxi Liang  (梁文锡), Yuan Li  (李渊) or Tianyou Zhai  (翟天佑).

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

Additional information

Ran Liu received her BS degree from the School of Resources and Civil Engineering, Northeastern University, China, in 2019, and then received her MS degree from the School of Materials Science and Engineering, Huazhong University of Science and Technology (HUST), in 2022. Her research interest focuses on the synthesis and integration of 2D materials towards electronic and optoelectronic applications.

Xiangyu Zhu is currently a PhD candidate at HUST under the supervision of Prof. Wenxi Liang. He received his BS degree and MS degree from Wuhan University of Technology. His PhD research focuses on the studies of ultrafast carrier dynamics in 2D transition metal dichalcogenides and heterostructures.

Yuan Li received his BS degree and MS degree from the Central South University in 2009 and 2011, respectively. He then received his PhD degree in materials science from The University of Alabama in 2015. Afterward he joined the Northwestern University as a UNANCE Postdoctoral Research Associate. He is currently a professor at the School of Materials Science and Engineering, HUST. His research interests mainly focus on 2D nanofabrication and integrated optoelectronic devices.

Wenxi Liang received his BS degree from Tsinghua University in 1998, and PhD degree from the Institute of Physics, Chinese Academy of Sciences in 2009. He worked as a postdoctoral scholar at Caltech from 2009 to 2015. In June 2015, he was appointed as a professor at Wuhan National Laboratory for Optoelectronics, HUST. His research interests focus on the studies of ultrafast dynamics in novel optoelectronic materials and developing the technology of ultrafast probes of electrons and optics.

Tianyou Zhai received his BS degree in chemistry from Zhengzhou University in 2003 and then received his PhD degree in physical chemistry from the Institute of Chemistry, CAS (ICCAS) under the supervision of Prof. Jiannian Yao in 2008. Afterward he joined the National Institute for Materials Science (NIMS) as a Japan Society For Promotion Science (JSPS) postdoctoral fellow of Prof. Yoshio Bando’s group and then as a researcher of International Center for Young Scientists-Materials Nanoarchitectonics (ICYS-MANA) at NIMS. Currently, he is a Chief Professor of the School of Materials Science and Engineering, HUST. His research interests include the controlled synthesis and exploration of fundamental physical properties of inorganic functional nanomaterials, as well as their promising applications in energy science, electronics, and optoelectronics.

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Interface-Engineered Au@MoS2 Core-Shell Heterostructures with Superior Hot-Carrier Transfer Dynamics for Plasmonics and Optoelectronics

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Liu, R., Zhu, X., Liu, S. et al. Interface-engineered Au@MoS2 core-shell heterostructures with superior hot-carrier transfer dynamics for plasmonics and optoelectronics. Sci. China Mater. 66, 3931–3940 (2023). https://doi.org/10.1007/s40843-023-2543-y

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