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Phase-selective synthesis of 1T′ MoS2 monolayers and heterophase bilayers

Nature Materials volume 17, pages 1108–1114 (2018)Cite this article

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Abstract

Two-dimensional (2D) MoS2, which has great potential for optoelectronic and other applications, is thermodynamically stable and hence easily synthesized in its semiconducting 2H phase. In contrast, growth of its metastable 1T and 1T′ phases is hampered by their higher formation energy. Here we use theoretical calculations to design a potassium (K)-assisted chemical vapour deposition method for the phase-selective growth of 1T′ MoS2 monolayers and 1T′/2H heterophase bilayers. This is realized by tuning the concentration of K in the growth products to invert the stability of the 1T′ and 2H phases. The synthesis of 1T′ MoS2 monolayers with high phase purity allows us to characterize their intrinsic optical and electrical properties, revealing a characteristic in-plane anisotropy. This phase-controlled bottom-up synthesis offers a simple and efficient way of manipulating the relevant device structures, and provides a general approach for producing other metastable-phase 2D materials with unique properties.

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Fig. 1: Schematics for the phase-controlled synthesis strategy.
Fig. 2: Selective CVD growth of 1T′-phase and 2H-phase MoS2 monolayers.
Fig. 3: Vertically stacked 1T′/2H heterophase bilayers.
Fig. 4: In-plane anisotropic spectroscopic characterizations.
Fig. 5: In-plane anisotropic electrical characterizations.
Fig. 6: Electrochemical performance of CVD-grown 1T′ and 2H MoS2 flakes.

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Data availability

The data that support the findings of this study are available from the corresponding author upon request.

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Acknowledgements

L.J. acknowledges the National Natural Science Foundation of China (grant numbers 21573125, 21322303 and 51372134) and the Tsinghua University Initiative Scientific Research Program. L.X. acknowledges the NSFC (grant number 21673058), the Key Research Program of Frontier Sciences of CAS (grant number QYZDB-SSW-SYS031), the Strategic Priority Research Program of Chinese Academy of Sciences (grant number XDB30000000) and the Beijing Nova Program-Joint Project (grant number Z171100001117129). X.J. acknowledges the National Natural Science Foundation of China (grant numbers 11574304 and 11774338) and the Youth Innovation Promotion Association CAS (grant number 2016109). L.G. acknowledges the National Program on Key Basic Research Project (grant number 2014CB921002), The Strategic Priority Research Program of Chinese Academy of Sciences (grant number XDB07030200) and the National Natural Science Foundation of China (grant numbers 51522212, 51421002 and 51672307). P.L. acknowledges the National Natural Science Foundation of China (grant number 61675032), the National Basic Research Program of China (973 Program) under grant number 2014CB643900 and the Open Program of State Key Laboratory of Functional Materials for Informatics. We thank X. Yan for TEM data analysis and X. Ping for HER measurements.

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Authors and Affiliations

  1. Key Laboratory of Organic Optoelectronics and Molecular Engineering of the Ministry of Education, Department of Chemistry, Tsinghua University, Beijing, China

    Lina Liu, Lifei Sun, Jingying Zheng, Lei Xing & Liying Jiao

  2. CAS Key Laboratory of Standardization and Measurement for Nanotechnology, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing, China

    Juanxia Wu & Liming Xie

  3. State Key Laboratory of Information Photonics and Optical Communications, Beijing University of Posts and Telecommunications, Beijing, China

    Liyuan Wu, Qian Wang, Siyao Hou & Pengfei Lu

  4. State Key Laboratory of Superlattices and Microstructures, Institute of Semiconductors, Chinese Academy of Sciences, Beijing, China

    Meng Ye & Xiangwei Jiang

  5. University of Chinese Academy of Sciences, Beijing, China

    Xiaozhi Liu, Lin Gu & Liming Xie

  6. Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, China

    Xiaozhi Liu & Lin Gu

  7. Collaborative Innovation Center of Quantum Matter, Beijing, China

    Lin Gu

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Contributions

L.J. and L.X. cosupervised this project. L.J. and L.L. conceived the ideas. L.L., J.W., L.S., J.Z. and L.X. performed the experiments. L.W., Q.W., S.H., P.L., M.Y. and X.J. carried out the theoretical calculations. X.L. and L.G. performed the STEM characterizations. L.J., L.L., J.W. and L.X. co-wrote the manuscript. All authors read the manuscript and commented on it.

Corresponding authors

Correspondence to Liming Xie or Liying Jiao.

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Supplementary Figures 1–17, Supplementary Tables 1–2, Supplementary References 1–17

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Liu, L., Wu, J., Wu, L. et al. Phase-selective synthesis of 1T′ MoS2 monolayers and heterophase bilayers. Nature Mater 17, 1108–1114 (2018). https://doi.org/10.1038/s41563-018-0187-1

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