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 Fe1-xS as an example,the thickness of the Fe1-xS flakes is down to 3 nm with a lateral size of over 100 μm.Importantly,we find ordered cation Fe vacancies in Fe1-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 Fe1-xS is a stable semiconductor with a narrow bandgap of～60 meV.In addition to Fe1-xS,the method is universal in growing various non-layered 2D TMCs contain-ing ordered cation vacancies,including Fe1-xSe,Co1-xS,Cr1-xS,and V1-xS.This work paves the way to grow and exploit properties of non-layered materials at 2D thickness limit.

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

Shenzhen Geim Graphene Center,Tsinghua-Berkeley Shenzhen Institute and Institute of Materials Research,Shenzhen International Graduate School,Tsinghua University,Shenzhen 518055,China;Department of Physics and Shenzhen Key Laboratory of Advanced Quantum Functional Materials and Devices,Southern University of Science and Technology,Shenzhen 518055,China;School of Electronic Information Engineering,Foshan University,Foshan 528000,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

科学通报（英文版）

[1]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-.Dual-metal precursors for the universal growth of non-layered 2D transition metal chalcogenides with ordered cation vacancies)[J].科学通报（英文版）,2022(16):1649-1658

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