<i>In-situ</i> diagnosis of Ar/CH<sub>4</sub> helicon wave plasma for synthesis of carbon nanomaterials

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Abstract

A variety of carbon-based thin films are prepared by self-developed helicon wave plasma chemical vapor deposition (HMHX, HWP-CVD) through changing the parameters of plasma discharge. The Ar/CH ₄plasma discharge is diagnosed in situby Langmuir probe, emission spectroscopy and mass spectrometry. The carbon thin films are characterized by scanning electron microscopy (SEM) and Raman spectroscopy (Raman). The results show that under the given parameters, the plasma discharge modes are all helicon wave discharge modes. Under a given CH ₄flow rate, the energy distribution in the plasma is enough to dissociate the methane molecules and form carbon free radicals. The preparation of different carbon-based films is realized by adjusting the CH ₄fluence. The research result shows that when the plasma is rich in CH and H radicals, it is suitable for growing diamond-like carbon films. When the plasma is rich in C ₂radicals and less H, it is favorable for growing vertical graphene nanosheets. According to the results of plasma diagnosis and material characterization, the decomposition mechanism of methane molecules under the action of Ar helicon wave plasma (HWP) is proposed, and the growth model of carbon-based materials is established, the feasibility of Ar/CH ₄-HWP in the preparation of carbon-based nanomaterials is verified, which provides a reference for preparing the carbon-based materials by HWP-CVD technology.

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Corresponding author:Zhuge Lan-Jian,ljzhuge@suda.edu.cn; Wu Xue-Mei,xmwu@suda.edu.cn

Funds:Project supported by the National Natural Science Foundation of China (Grant No. 11975163), the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD), China, and the Postgraduate Research & Practice Innovation Program of Jiangsu Province, China (Grant No. KYCX20_2649)

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等离子体中主要物质	产生过程	参考文献
Ar^+/*	${\rm{A} }{\rm{r} }\stackrel{ {{E} }\;{\rm{a} }{\rm{n} }{\rm{d} }\;{{H} } }{\longrightarrow }{\rm{Ar} }^{*}+{\rm{e} }^{-}$	[22,24]
	$ {\rm{Ar}}^{*}+{\rm{e}}^{-}\Rightarrow {\rm{Ar}}^{+}+{2{\rm{e}}}^{-} $
	$ {\rm{A}}{\rm{r}}+{\rm{e}}^{-}\Rightarrow {\rm{Ar}}^{*}+{\rm{e}}^{-} $
H	$ {\rm{Ar}}^{}+{{\rm{H}}}_{2}\Rightarrow {{\rm{A}}{\rm{r}}{\rm{H}}}^{}+{\rm{H}} $	[20,22,24]
	$ {\rm{CH}}_{4}+{\rm{e}}\Rightarrow {{\rm{CH}}_{3}}^{+}+{\rm{H}}+2{\rm{e}} $
	$ \Rightarrow {{\rm{CH}}_{2}}^{+}+{{\rm{H}}}_{2} $
	$ \Rightarrow {\rm{C}}{\rm{H}}+{\rm{H}}+{{\rm{H}}}_{2} $
	$ \Rightarrow {\rm{C}}+{2{\rm{H}}}_{2} $
CH	$ {\rm{C}}+{\rm{CH}}_{4}\rightleftharpoons {\rm{C}}{\rm{H}}+{\rm{CH}}_{3} $	[26]
CH	$ {\rm{CH}}_{2}^{*}+{\rm{H}}\leftrightarrows {\rm{C}}{\rm{H}}+{{\rm{H}}}_{2} $	[26]
C₂	$ {\rm{A}}{\rm{r}}+{{\rm{C}}}_{2}{{\rm{H}}}_{2}\Rightarrow {{\rm{C}}}_{2}+{{\rm{H}}}_{2}+{\rm{A}}{\rm{r}} $	[24]
	$ {\rm{C}}+{\rm{C}}{\rm{H}}\rightleftharpoons {{\rm{C}}}_{2}+{\rm{H}} $
	$ {{\rm{C}}}_{2}{\rm{H}}+{\rm{H}}\rightleftharpoons {{\rm{C}}}_{2}+{{\rm{H}}}_{2} $
	$ {{\rm{C}}}_{2}{\rm{H}}+{\rm{M}}\rightleftharpoons {{\rm{C}}}_{2}+{\rm{H}}+{\rm{M}} $
C₂H₂	$ {\rm{C}}{\rm{H}}+{\rm{CH}}_{2}\rightleftharpoons {{\rm{C}}}_{2}{{\rm{H}}}_{2}+{\rm{H}} $	[24,26]
	$ {\rm{CH}}_{2}+{\rm{CH}}_{2}\rightleftharpoons {{\rm{C}}}_{2}{{\rm{H}}}_{2}+{{\rm{H}}}_{2} $
	$ {\rm{CH}}_{2}+{\rm{CH}}_{2}\rightleftharpoons {{\rm{C}}}_{2}{{\rm{H}}}_{2}+2{\rm{H}} $
CH_n	$ {\rm{Ar}}^{+}+{\rm{CH}}_{4}\rightleftharpoons {\rm{CH}}_{n}+\left(4-n\right){\rm{H}}+{\rm{A}}{\rm{r}} $	[24]
CH_n	$ {\rm{e}}+{\rm{CH}}_{4}\rightleftharpoons {\rm{CH}}_{n}+\left(4-n\right){\rm{H}}+{\rm{e}} $	[24]

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Vol. 70, Issue 9 - 2021-05-05

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