Interfacial properties of 2D WS<sub>2</sub> on SiO<sub>2</sub> substrate from X-ray photoelectron spectroscopy and first-principles calculations

doi:10.1007/s11467-022-1167-0

Front. Phys.

2022, Vol. 17

Issue (5) : 53500 https://doi.org/10.1007/s11467-022-1167-0

RESEARCH ARTICLE

Interfacial properties of 2D WS₂ on SiO₂ substrate from X-ray photoelectron spectroscopy and first-principles calculations

Changjie Zhou¹, Huili Zhu¹(

), Weifeng Yang²(

), Qiubao Lin¹, Tongchang Zheng¹, Lan Yang¹, Shuqiong Lan¹

¹. Xiamen Key Laboratory of Ultra-Wide Bandgap Semiconductor Materials and Devices, Department of Physics, School of Science, Jimei University, Xiamen 361021, China
². Department of Microelectronics and Integrated Circuits, Xiamen University, Xiamen 361005, China

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Abstract

Two-dimensional (2D) WS₂ films were deposited on SiO₂ wafers, and the related interfacial properties were investigated by high-resolution X-ray photoelectron spectroscopy (XPS) and first-principles calculations. Using the direct (indirect) method, the valence band offset (VBO) at monolayer WS₂/SiO₂ interface was found to be 3.97 eV (3.86 eV), and the conduction band offset (CBO) was 2.70 eV (2.81 eV). Furthermore, the VBO (CBO) at bulk WS₂/SiO₂ interface is found to be about 0.48 eV (0.33 eV) larger due to the interlayer orbital coupling and splitting of valence and conduction band edges. Therefore, the WS₂/SiO₂ heterostructure has a Type I energy-band alignment. The band offsets obtained experimentally and theoretically are consistent except the narrower theoretical bandgap of SiO₂. The theoretical calculations further reveal a binding energy of 75 meV per S atom and the totally separated partial density of states, indicating a weak interaction and negligible Fermi level pinning effect between WS₂ monolayer and SiO₂ surface. Our combined experimental and theoretical results provide proof of the sufficient VBOs and CBOs and weak interaction in 2D WS₂/SiO₂ heterostructures.

Keywords band offsets WS₂ SiO₂ X-ray photoelectron spectroscopy first-principles calculations

Corresponding Author(s): Huili Zhu,Weifeng Yang

Issue Date: 27 June 2022

Cite this article:

Changjie Zhou,Huili Zhu,Weifeng Yang, et al. Interfacial properties of 2D WS₂ on SiO₂ substrate from X-ray photoelectron spectroscopy and first-principles calculations[J]. Front. Phys. , 2022, 17(5): 53500.

URL:

https://academic.hep.com.cn/fop/EN/10.1007/s11467-022-1167-0
https://academic.hep.com.cn/fop/EN/Y2022/V17/I5/53500

Fig.1 (a) AFM image of the monolayer WS₂ film (5 μm × 5 μm). (b) AFM height profile along with the white dashed line in (a). (c) Raman spectrum of WS₂ monolayer grown on SiO₂ wafer. (d) Photoluminescence of WS₂ monolayer. (e) Typical high-resolution TEM image of the WS₂ film. (f) Enlarged TEM image of a specific area illustrated by a red square in (e). The hexagonal atomic structures consist of W and S atoms are presented.

Fig.2 XPS W 4f and S 2p spectra of 1L and bulk WS₂ deposited on the SiO₂ substrates.

Fig.3 The core-level and valence band spectra for (a) bulk WS₂ and (b) bulk SiO₂ samples. (c) The core-level spectra of S 2p and Si 2p obtained for the 1L WS₂/SiO₂ heterostructure. (d) The bandgap of SiO₂ is measured to be 9.05 eV using O 1s loss energy spectrum.

Fig.4 Si 2p and valence band spectra of (a) bare SiO₂ substrate, (b) 1L, and (c) bulk WS₂ deposited on SiO₂ substrates.

Fig.5 (a) Top and side view of the optimized atomic configuration of 1L WS₂/a-SiO₂ heterostructure. (b) The calculated total DOSs of 1L WS₂/a-SiO₂ interface and partial DOSs of Si, O, W, and S atoms based on the HSE06 method. The Fermi level is shifted to 0 eV. (c) Partial DOSs of W 5d and S 3p orbitals of 1L and bulk WS₂. The low-energy electronic states were taken as references to align the partial DOSs.

Fig.6 (a) Top and side view of the optimized atomic configuration of 1L WS₂/O-terminated (2×2)

α

-SiO₂(0001) heterostructure. (b) The calculated total DOSs of 1L WS₂/O-terminated (2×2)

α

-SiO₂(0001) interface and partial DOSs of W, S, Si, and O atoms based on the HSE06 method. The Fermi level is shifted to 0 eV.

Fig.7 Experimental band alignments of 1L and bulk WS₂/SiO₂ heterostructures derived using the indirect (a) and direct (b) method. (c) Theoretical band alignments of 1L and bulk WS₂/a-SiO₂ heterostructures.

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