Theoretical study on the nucleation control of WS<sub>2 </sub>on Au(111) surfaces

Hu Yi-Shan; Yuan Qing-Hong

doi:10.7498/aps.73.20240417

Abstract

Two-dimensional tungsten disulfide (WS₂), as a semiconductor material with unique layer-dependent electronic and optoelectronic characteristics, demonstrates a promising application prospect in the field of optoelectronic devices. The fabrication of wafer-scale monolayer WS₂ films is currently a critical challenge that propels their application in advanced transistors and integrated circuits. Chemical vapor deposition (CVD) is a feasible technique for fabricating large-area, high-quality monolayer WS₂ films, yet the complexity of its growth process results in low growth efficiency and inconsistent film quality of WS₂. In order to guide experimental efforts to diminish grain boundaries in WS₂, thereby improving film quality to enhance electronic performance and mechanical stability, this study investigates the nucleation mechanisms of WS₂ during CVD growth through first-principles theoretical calculations. By considering chemical potential as a crucial variable, we analyze the growth energy curves of WS₂ under diverse experimental conditions. Our findings demonstrate that modulating the temperature or pressure of the tungsten and sulfur precursors can decisively influence the nucleation rate of WS₂. Notably, the nucleation rate reaches a peak at a tungsten source temperature of 1250 K, while an increase in sulfur source temperature or a decrease in pressure can suppress the nucleation rate, thereby enhancing the crystallinity and uniformity of monolayer WS₂. These insights not only furnish a robust theoretical foundation for experimentally fine-tuning the nucleation rate as needed but also provide strategic guidance for optimizing experimental parameters to refine the crystallinity and uniformity of monolayer WS₂ films. Such advancements are expected to accelerate the deployment of WS₂ materials in a range of high-performance electronic devices, marking a significant stride in the field of materials science and industrial applications.

Keywords:

Authors and contacts

State Key Laboratory of Precision Spectroscopy School of Physics and Electronic Science, East China Normal University, Shanghai 200241, China

Corresponding author: Yuan Qing-Hong, qhyuan@phy.ecnu.edu.cn

Funds: Project supported by the National Key Research and Development Program of China (Grant No. 2021YFA1200801) and the National Natural Science Foundation of China (Grant No. 22173031).

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Cited By

图 1 (a)以W或S边终结的三角形WS₂团簇的形成能(E_f)与其尺寸大小(N)的关系, $ {E_{\text{f}}} = {E_{{\text{tot}}}} - {N_{\text{W}}} \cdot {\mu _{{\text{W(ref)}}}} - {N_{\text{S}}} \cdot {\mu _{{\text{S(ref)}}}} $, 其中$ {E_{{\text{tot}}}} $为WS₂整体能量, $ {N_{\text{W}}} $和$ {N_{\text{S}}} $分别为W, S原子数, $ {\mu _{{\text{W(ref)}}}} $, $ {\mu _{{\text{S(ref)}}}} $分别为W, S前驱体的参考化学势. (b), (c) Au(111)表面S边终结的WS₂团簇的形成能及其线性拟合

Figure 1. (a) Forming energy (E_f) versus size (N) of triangular WS₂ clusters terminated with W or S edge, $ {E_{\text{f}}} = {E_{{\text{tot}}}} - {N_{\text{W}}} \cdot {\mu _{{\text{W(ref)}}}} - $$ {N_{\text{S}}} \cdot {\mu _{{\text{S(ref)}}}} $, where $ {E_{{\text{tot}}}} $ is the overall energy of WS₂, $ {N_{\text{W}}} $ and $ {N_{\text{S}}} $ are the number of atoms W and S respectively, $ {\mu _{{\text{W(ref)}}}} $ and $ {\mu _{{\text{S(ref)}}}} $ are the reference chemical potential of W and S precursors respectively. (b), (c) Formation energy and linear fitting of WS₂ clusters terminated with S edge on Au(111) surface.

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图 2 前驱体(a)钨源、(b)硫源化学势随温度的变化; (c) 500 K的硫源化学势随硫源压强的变化

Figure 2. Changes of chemical potential of precursor (a) tungsten source and (b) sulfur source with temperature; (c) chemical potential of sulfur source changes with the pressure of sulfur source at 500 K.

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图 3 不同钨源温度(a)、硫源温度(b)以及硫源压强(c)条件下Au(111)表面WS₂的吉布斯自由能与团簇大小的关系

Figure 3. Gibbs free energy versus cluster size of WS₂ on Au(111) surface under different (a) tungsten source temperature, (b) sulfur source temperature and (c) sulfur source pressure.

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图 4 Au(111)表面 WS₂团簇的成核速率与不同实验条件的关系　(a) T(W); (b) T(S); (c) P(S)/P₀. 纵坐标为log10刻度类型, 红色虚线标注为T(W) = 1300 K, T(S) = 500 K, P(S) = 763.10 Pa实验条件下WS₂团簇的成核速率

Figure 4. Nucleation rates of WS₂ clusters on Au(111) surface under different experimental conditions: (a) T(W); (b) T(S); (c) P(S)/P₀. Scale of the vertical axis in the graph is non-linear and is of the log10 type, and the red dotted lines indicate the nucleation rates of WS₂ clusters under experimental conditions of T(W) = 1300 K, T(S) = 500 K and P(S) = 763.10 Pa.

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[1]	Zhao W J, Ghorannevis Z, Chu L Q, Toh M L, Kloc C, Tan P H, Eda G 2013 ACS Nano 7 791 Google Scholar
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Theoretical study on the nucleation control of WS₂on Au(111) surfaces

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Theoretical study on the nucleation control of WS2 on Au(111) surfaces

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Theoretical study on the nucleation control of WS₂on Au(111) surfaces