Metastable 1T'-phase group VIB transition metal dichalcogenide crystals

Zhuangchai Lai; Qiyuan He; Thu Ha Tran; D V Maheswar Repaka; Dong-Dong Zhou; Ying Sun; Shibo Xi; Yongxin Li; Apoorva Chaturvedi; Chaoliang Tan; Bo Chen; Gwang-Hyeon Nam; Bing Li; Chongyi Ling; Wei Zhai; Zhenyu Shi; Dianyi Hu; Vinay Sharma; Zhaoning Hu; Ye Chen; Zhicheng Zhang; Yifu Yu; Xiao Renshaw Wang; Raju V Ramanujan; Yanming Ma; Kedar Hippalgaonkar; Hua Zhang

doi:10.1038/s41563-021-00971-y

Metastable 1T'-phase group VIB transition metal dichalcogenide crystals

Nat Mater. 2021 Aug;20(8):1113-1120. doi: 10.1038/s41563-021-00971-y. Epub 2021 Apr 15.

Authors

Zhuangchai Lai^#^{1

2}, Qiyuan He^#³, Thu Ha Tran^#², D V Maheswar Repaka^#⁴, Dong-Dong Zhou⁵, Ying Sun^{6

7}, Shibo Xi⁴, Yongxin Li⁸, Apoorva Chaturvedi², Chaoliang Tan⁹, Bo Chen¹, Gwang-Hyeon Nam², Bing Li¹⁰, Chongyi Ling¹, Wei Zhai¹, Zhenyu Shi^{1

2}, Dianyi Hu², Vinay Sharma², Zhaoning Hu², Ye Chen¹¹, Zhicheng Zhang^{2

12}, Yifu Yu^{2

13}, Xiao Renshaw Wang^{8

14}, Raju V Ramanujan², Yanming Ma^{6

7

15}, Kedar Hippalgaonkar^{16

17}, Hua Zhang^{18

19

20}

Affiliations

¹ Department of Chemistry, City University of Hong Kong, Hong Kong SAR, China.
² Center for Programmable Materials, School of Materials Science and Engineering, Nanyang Technological University, Singapore, Singapore.
³ Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong SAR, China.
⁴ Institute of Materials Research and Engineering (IMRE), A*STAR (Agency for Science, Technology and Research), Singapore, Singapore.
⁵ MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou, China.
⁶ State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun, China.
⁷ International Center for Computational Method & Software, College of Physics, Jilin University, Changchun, China.
⁸ School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore, Singapore.
⁹ Department of Electrical Engineering, City University of Hong Kong, Hong Kong SAR, China.
¹⁰ School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, China.
¹¹ Department of Chemistry, The Chinese University of Hong Kong, Hong Kong SAR, China.
¹² Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University & Collaborative Innovation Center of Chemical Science and Engineering, Tianjin, China.
¹³ Institute of Molecular Plus, Tianjin University, Tianjin, China.
¹⁴ School of Electrical and Electronic Engineering, Nanyang Technological University, Singapore, Singapore.
¹⁵ International Center of Future Science, Jilin University, Changchun, China.
¹⁶ Center for Programmable Materials, School of Materials Science and Engineering, Nanyang Technological University, Singapore, Singapore. kedar@ntu.edu.sg.
¹⁷ Institute of Materials Research and Engineering (IMRE), A*STAR (Agency for Science, Technology and Research), Singapore, Singapore. kedar@ntu.edu.sg.
¹⁸ Department of Chemistry, City University of Hong Kong, Hong Kong SAR, China. hua.zhang@cityu.edu.hk.
¹⁹ Hong Kong Branch of National Precious Metals Material Engineering Research Center (NPMM), City University of Hong Kong, Hong Kong SAR, China. hua.zhang@cityu.edu.hk.
²⁰ Shenzhen Research Institute, City University of Hong Kong, Shenzhen, China. hua.zhang@cityu.edu.hk.

^# Contributed equally.

PMID: 33859384
DOI: 10.1038/s41563-021-00971-y

Abstract

Metastable 1T'-phase transition metal dichalcogenides (1T'-TMDs) with semi-metallic natures have attracted increasing interest owing to their uniquely distorted structures and fascinating phase-dependent physicochemical properties. However, the synthesis of high-quality metastable 1T'-TMD crystals, especially for the group VIB TMDs, remains a challenge. Here, we report a general synthetic method for the large-scale preparation of metastable 1T'-phase group VIB TMDs, including WS₂, WSe₂, MoS₂, MoSe₂, WS_2xSe_2(1-x) and MoS_2xSe_2(1-x). We solve the crystal structures of 1T'-WS₂, -WSe₂, -MoS₂ and -MoSe₂ with single-crystal X-ray diffraction. The as-prepared 1T'-WS₂ exhibits thickness-dependent intrinsic superconductivity, showing critical transition temperatures of 8.6 K for the thickness of 90.1 nm and 5.7 K for the single layer, which we attribute to the high intrinsic carrier concentration and the semi-metallic nature of 1T'-WS₂. This synthesis method will allow a more systematic investigation of the intrinsic properties of metastable TMDs.