Dual-metal precursors for the universal growth of non-layered 2D transition metal chalcogenides with ordered cation vacancies

Junyang Tan; Zongteng Zhang; Shengfeng Zeng; Shengnan Li; Jingwei Wang; Rongxu Zheng; Fuchen Hou; Yinping Wei; Yujie Sun; Rongjie Zhang; Shilong Zhao; Huiyu Nong; Wenjun Chen; Lin Gan; Xiaolong Zou; Yue Zhao; Junhao Lin; Bilu Liu; Hui-Ming Cheng

doi:10.1016/j.scib.2022.06.022

Dual-metal precursors for the universal growth of non-layered 2D transition metal chalcogenides with ordered cation vacancies

Sci Bull (Beijing). 2022 Aug 31;67(16):1649-1658. doi: 10.1016/j.scib.2022.06.022. Epub 2022 Jun 27.

Authors

Junyang Tan¹, Zongteng Zhang², Shengfeng Zeng¹, Shengnan Li¹, Jingwei Wang¹, Rongxu Zheng¹, Fuchen Hou², Yinping Wei¹, Yujie Sun¹, Rongjie Zhang¹, Shilong Zhao¹, Huiyu Nong¹, Wenjun Chen³, Lin Gan¹, Xiaolong Zou¹, Yue Zhao⁴, Junhao Lin⁵, Bilu Liu⁶, Hui-Ming Cheng⁷

Affiliations

¹ Shenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute and Institute of Materials Research, Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China.
² Department of Physics and Shenzhen Key Laboratory of Advanced Quantum Functional Materials and Devices, Southern University of Science and Technology, Shenzhen 518055, China.
³ Shenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute and Institute of Materials Research, Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China; School of Electronic Information Engineering, Foshan University, Foshan 528000, China.
⁴ Department of Physics and Shenzhen Key Laboratory of Advanced Quantum Functional Materials and Devices, Southern University of Science and Technology, Shenzhen 518055, China. Electronic address: zhaoy@sustech.edu.cn.
⁵ Department of Physics and Shenzhen Key Laboratory of Advanced Quantum Functional Materials and Devices, Southern University of Science and Technology, Shenzhen 518055, China. Electronic address: linjh@sustech.edu.cn.
⁶ Shenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute and Institute of Materials Research, Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China. Electronic address: bilu.liu@sz.tsinghua.edu.cn.
⁷ Shenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute and Institute of Materials Research, Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China; Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China; Faculty of Materials Science and Engineering/Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen 518055, China. Electronic address: hmcheng@sz.tsinghua.edu.cn.

PMID: 36546044
DOI: 10.1016/j.scib.2022.06.022

Abstract

Two-dimensional (2D) transition metal chalcogenides (TMCs) are promising for nanoelectronics and energy applications. Among them, the emerging non-layered TMCs are unique due to their unsaturated dangling bonds on the surface and strong intralayer and interlayer bonding. However, the synthesis of non-layered 2D TMCs is challenging and this has made it difficult to study their structures and properties at thin thickness limit. Here, we develop a universal dual-metal precursors method to grow non-layered TMCs in which a mixture of a metal and its chloride serves as the metal source. Taking hexagonal Fe_1-_xS as an example, the thickness of the Fe_1-_xS flakes is down to 3 nm with a lateral size of over 100 μm. Importantly, we find ordered cation Fe vacancies in Fe_1-_xS, which is distinct from layered TMCs like MoS₂ where anion vacancies are commonly observed. Low-temperature transport measurements and theoretical calculations show that 2D Fe_1-_xS is a stable semiconductor with a narrow bandgap of ∼60 meV. In addition to Fe_1-_xS, the method is universal in growing various non-layered 2D TMCs containing ordered cation vacancies, including Fe_1-_xSe, Co_1-_xS, Cr_1-_xS, and V_1-_xS. This work paves the way to grow and exploit properties of non-layered materials at 2D thickness limit.

Keywords: Chemical vapor deposition; Dual-metal precursors; Non-layered two-dimensional materials; Ordered cation vacancies; Transition metal chalcogenides.