Atomic and electronic structure of monolayer ferroelectric GeS on Cu(111)

Zhu Meng-Long; Yang Jun; Dong Yu-Lan; Zhou Yuan; Shao Yan; Hou Hai-Liang; Chen Zhi-Hui; He Jun

doi:10.7498/aps.73.20231246

Abstract

Two-dimensional (2D) ferroelectric materials are important materials for both fundamental properties and potential applications. Especially, group Ⅳ monochalcogenide possesses highest thermoelectric performance and intrinsic ferroelectric polarization properties and can sever as a model to explore ferroelectric polarization properties. However, due to the relatively large exfoliation energy, the creation of high-quality and large-size monolayer group Ⅳ monochalcogenide is not so easy, which seriously hinders the integration of these materials into the fast-developing field of 2D materials and their heterostructures. Herein, monolayer GeS is successfully fabricated on Cu(111) substrate by molecular beam epitaxy method, and the lattice structure and the electronic band structure of monolayer GeS are systematically characterized by high-resolution scanning tunneling microscopy, low-energy electron diffraction, in-situ X-ray photoelectron spectroscopy, Raman spectra, and angle-resolved photoelectron spectroscopy, and density functional theory calculations. All atomically resolved STM images reveal that the obtained monolayer GeS has an orthogonal lattice structure, which consists with theoretical prediction. Meanwhile, the distinct moiré pattern formed between monolayer GeS and Cu(111) substrate also confirms the orthogonal lattice structure. In order to examine the chemical composition and valence state of as-prepared monolayer GeS, in-situ XPS is utilized without being exposed to air. The measured spectra of XPS core levels suggest that the valence states of Ge and S elements are identified to be +2 and –2, respectively and the atomic ratio of Ge/S is 1∶1.5, which is extremely close to the stoichiometric ratio of 1∶1 for GeS. To further corroborate the quality and lattice structure of the monolayer GeS film, ex-situ Raman measurements are also performed for monolayer GeS on highly oriented pyrolytic graphene (HOPG) and multilayer graphene substrate. Three well-defined typical characteristic Raman peaks of GeS are observed. Finally, in-situ ARPES measurement are conducted to determine the electronic band structure of monolayer GeS on Cu(111). The results demonstrate that the monolayer GeS has a nearly flat band electronic band structure, consistent with our density functional theory calculation. The realization and investigation of the monolayer GeS extend the scope of 2D ferroelectric materials and make it possible to prepare high quality and large size monolayer group Ⅳ monochalcogenides, which is beneficial to the application of this main group material to the rapidly developing 2D ferroelectric materials and heterojunction research.

Keywords:

Authors and contacts

1.
School of Microelectronics and Physics, Hunan University of Technology and Business, Changsha 410205, China
2.
Hunan Key Laboratory of Nanophotonics and Devices, School of Physics and Electronics, Central South University, Changsha 410083, China
3.
MIIT Key Laboratory for Low-Dimensional Quantum Structure and Devices, School of Integrated Circuits and Electronics, Beijing Institute of Technology, Beijing 100081, China

Corresponding author: Hou Hai-Liang, hhlcj1732@126.com ; Chen Zhi-Hui, czh_nlo@csu.edu.cn ;

Funds: Project supported by the Research Foundation of Education Bureau of Hunan Province, China (Grant No. 22B0658), the Natural Science Foundation of Hunan Province, China (Grant Nos. 2023JJ30199, 2021JJ40704), and the National Natural Science Foundation of China (Grant Nos. 12004440, 62275275).

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Cited By

图 1 单层GeS原子分辨STM测量　(a) MBE生长腔结构(左)与STM测量和单层GeS晶体结构(右); (b), (c) 单层GeS在Cu(111)衬底表面形成的摩尔条纹及其快速傅里叶变换, 图像大小为14 nm×14 nm; (d) Cu(111)上单层GeS生长顶示意图; (e), (f) 单层GeS原子分辨STM图像及其快速傅里叶变换, 样品偏压1.2 V和隧穿电流0.60 nA, 图像大小为14 nm×14 nm

Figure 1. Atomically resolved STM measurements of monolayer GeS: (a) Schematic of MBE growth chamber (left) and STM set-up and crystal structure of monolayer GeS (right); (b), (c) moiré pattern formed betweem monolayer GeS and Cu(111) substrate and its fast Fourier transform with the image size of 14 nm × 14 nm; (d) schematic of the monolayer GeS grown on Cu(111); (e), (f) atomically resolved STM images of monolayer GeS and its fast Fourier transform with sample bias voltage of 1.2 V and tunneling current of 0.60 nA, and image size of 14 nm × 14 nm.

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图 2 单层GeS的Ge 3d (a)和S 2p (b)芯能级XPS能谱

Figure 2. XPS spectra of monolayer GeS for (a) Ge 3d and (b) S 2p core levels.

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图 3 Γ→Χ和Γ→Y高对称方向的能带结构　(a), (b) 单层GeS理论计算能带结构; (c), (d) Cu(111)衬底能带结构; (e), (f)单层GeS/Cu(111)异质结理论计算的能带结构(上)与APRES测量的能带结构(下)

Figure 3. Electronic band structures along Γ→Χ and Γ→Y high symmetry directions: (a), (b) Theoretically calculated electronic band structure of monolayer GeS; (c), (d) elelctronic band structure of Cu(111) substrate; (e), (f) theoretically calculated electronic band structure of monolayer GeS/Cu(111) heterojunction (top) and electronic band structure measured by APRES (bottom).

DownLoad: Full-Size Img PowerPoint

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[48]	Ribeiro H B, Ramos S, Seixas L, De Matos C J S, Pimenta M A 2019 Phys. Rev. B 100 094301 Google Scholar
[49]	Ul Haq B, AlFaify S, Laref A 2019 J. Phys. Chem. C 123 18124 Google Scholar
[50]	Zhou Y, Wu D, Zhu Y, Cho Y, He Q, Yang X, Herrera K, Chu Z, Han Y, Downer M C, Peng H, Lai K 2017 Nano Lett. 17 5508 Google Scholar
[51]	王慧, 徐萌, 郑仁奎 2020 物理学报 69 017301 Google Scholar Wang H, Xu M, Zheng R K 2020 Acta Phys. Sin. 69 017301 Google Scholar

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Vol. 73, Issue 1 - 2024-01-05

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