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Raman scattering investigation of twisted WS2/MoS2 heterostructures: interlayer mechanical coupling versus charge transfer

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Abstract

Twisted van der Waals homo- and hetero-structures have aroused great attentions due to their unique physical properties, providing a new platform to explore the novel two-dimensional (2D) condensed matter physics. The robust dependence of phonon vibrations and electronic band structures on the twist angle has been intensively observed in transition metal dichalcogenide (TMD) homo-structures. However, the effects of twist angle on the lattice vibrational properties in the TMD heterostructures have not caused enough attention. Here, we report the distinct evolutions of Raman scattering and the underlying interlayer interactions in the twisted WS2/MoS2 heterostructures. The shifts and linewidths of E2g(Γ) and A1g(Γ) phonon modes are found to be twist angle dependent. In particular, analogous to that of the twisted TMD homostructures, the frequency separations between E2g(Γ) and A1g(Γ) modes of MoS2 and WS2 in the twisted heterostructures varying with twist angle correlate with the interlayer mechanical coupling, essentially originating from the spacing-related repulsion between sulfur atoms. Moreover, the opposite shift behaviors and broadening of A1g(Γ) modes caused by charge transfer are also observed in the twisted heterostructures. The calculated interlayer distances and band alignment of twisted WS2/MoS2 through density functional theory further evidence our interpretations on the roles of the interlayer mechanical coupling and charge transfer in variations of Raman features. Such understanding and controlling of interlayer interaction through the stacking orientation are significant for future optoelectronic device design based on the newly emerged 2D heterostructures.

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Acknowledgements

We thank Dr. Jiaxu Yan from Institute of Advanced Materials, Nanjing Tech. University and Dr. Juan Xia from University of Science and Technology, China for their helpful discussions. This work was mainly supported by the National Key R&D Program of China (Grant No. 2018YFA0703700) and the Ministry of Education, Singapore, MOE Tier 1 RG93/19, NRF-CRP-21-2018-0007, MOE2018-T2-2-072, and MOE2019-T2-1-004. C. X. C. also thanks the support of the National Natural Science Foundation of China (Grant No. 61774040), the Shanghai Municipal Science and Technology Commission (Grant No. 18JC1410300), the Fudan University-CIOMP Joint Fund (Grant No. FC2018-002), the National Young 1000 Talent Plan of China, and the Shanghai Municipal Natural Science Foundation (No. 16ZR1402500). J. Z. S. appreciates the support of the Fundamental Research Funds for the Central Universities of China, National Natural Science Foundation of China under Grant No. 61904151, Natural Science Foundation of Shaanxi under Grant No. 2020JM-108, and the Joint Research Funds of Department of Science & Technology of Shaanxi Province and Northwestern Polytechnical University (No. 2020GXLH-Z-020). Z. L. acknowledges the support of MOE Tier 1 grant RG164/15, Tier 2 grant MOE2016-T2-2-153, and MOE2015-T2-2-007, and Singapore National Research Foundation under NRF award No. NRF-NRFF2013-08. W. H. Y. acknowledges the support of the National Natural Science Foundations of China (Grant No. 61704040). This research was also supported by Zhejiang Provincial Natural Science Foundation of China (Grant No. LGG19F040003).

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  1. Lishu Wu and Chunxiao Cong contributed equally to this work.

Authors and Affiliations

  1. Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore, 637371, Singapore

    Lishu Wu, Yu Chen, Shun Feng, Hongbo Zhang & Ting Yu

  2. School of Information Science and Technology, Fudan University, Shanghai, 200433, China

    Chunxiao Cong

  3. Shaanxi Institute of Flexible Electronics, Northwestern Polytechnical University, Xi’an, 710129, China

    Jingzhi Shang & Wei Ai

  4. Engineering Research Center of Smart Microsensors and Microsystems, Ministry of Education, College of Electronics and Information, Hangzhou Dianzi University, Hangzhou, 310018, China

    Weihuang Yang

  5. School of Materials Science and Engineering, Nanyang Technological University, Singapore, 639798, Singapore

    Jiadong Zhou & Zheng Liu

  6. Key Laboratory of Chemical Lasers, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China

    Yanlong Wang

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Correspondence to Chunxiao Cong, Jingzhi Shang or Ting Yu.

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Raman scattering investigation of twisted WS2/MoS2 heterostructures: interlayer mechanical coupling versus charge transfer

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Wu, L., Cong, C., Shang, J. et al. Raman scattering investigation of twisted WS2/MoS2 heterostructures: interlayer mechanical coupling versus charge transfer. Nano Res. 14, 2215–2223 (2021). https://doi.org/10.1007/s12274-020-3193-y

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