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On the mechanism of CH_3 radical formation in hot filament activated CH_4/H_2 and C_2H_2/H_2 gas mixtures

机译:热丝活化CH_4 / H_2和C_2H_2 / H_2混合气体中CH_3自由基形成的机理

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摘要

Resonance enhanced multiphoton ionization spectroscopy has been used to determine relative number densities of CH_3 radicals in a hot filament chemical vapour deposition (HF-CVD) reactor designed for diamond growth, as a function of process gas (i.e. both CH_4/H_2 and C_2H_2/H_2 gas mixtures), position (d), filament temperature (T_f) and local gas temperature (T_g). The similar CH_3 radical number density profiles observed upon activation of the two feedstock gas mixtures suggest that CH_3 radical formation in both cases is dominated by gas phase chemistry, in contradiction of the current consensus which invokes surface catalysed hydrogenation as the means of inducing the necessary C_C bond fission in the case of C_2H_2/H_2 gas mixtures. Three body addition reactions involving C_2H_2 (and C_2H_4), together with H atoms and H_2 molecules, are identified as probable reactions requiring further study in order to provide a proper description of diamond CVD using a C_2H_2/H_2 gas feed.
机译:已经使用共振增强多光子电离光谱法确定了为金刚石生长而设计的热丝化学气相沉积(HF-CVD)反应器中CH_3自由基的相对数​​量密度,该相对密度取决于工艺气体(即CH_4 / H_2和C_2H_2 / H_2气体混合物),位置(d),灯丝温度(T_f)和局部气体温度(T_g)。两种原料气混合物活化后观察到的相似的CH_3自由基数密度分布图表明,在两种情况下CH_3自由基的形成均以气相化学为主,这与目前的共识相反,后者将表面催化氢化作为诱导必要C_C的手段在C_2H_2 / H_2混合气体中发生键裂变。涉及C_2H_2(和C_2H_4)以及H原子和H_2分子的三个身体加成反应被确定为可能的反应,需要进一步研究以提供使用C_2H_2 / H_2气体进料的金刚石CVD的正确描述。

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