Formation mechanism of hydrogenated silicon clusters during thermal decomposition of disilane
Formation mechanism of hydrogenated silicon clusters during thermal decomposition of disilane
复制标题
乙硅烷热分解过程中氢化硅团簇的形成机理
DOI：
10.1021/jp015523n
复制
发表时间：
2002
影响因子：
3.3
通讯作者：
M. Koshi
中科院分区：
文献类型：
--
作者：
K. Tonokura;and Tetsuya Murasaki;M. Koshi
采用飞行时间（TOF）质谱联用真空紫外（VUV）光电离，在680 ~ 860 K的温度范围和20 ~ 40 Torr的总压力下，对二硅烷热分解过程中的氢化硅团簇（SinHm）进行了检测。在10.2 eV （121.6 nm）的紫外辐射下，SinHm团簇被光电离。在二硅烷热解过程中，观察到SinH2n+2 （n≥2）、SinH2n （n≥2）、SinH2n-2 （n≥5）和SinH2n-4 （n≥5）为气相产物，而未检测到Si、SiH、SiH2和SiH3等Si1组分的离子信号。在高斯-3 (G3)//B3LYP理论水平上计算了二硅烷单分子分解的能量学。基于Swihart和Girshick提出的动力学模型[J]。理论物理。化学。[1999, 103, 64]，通过气相动力学模拟分析了二硅烷热分解过程中氢化硅团簇的形成机理。Temperatu……
Hydrogenated silicon clusters (SinHm) were detected during the thermal decomposition of disilane in a flow reactor by using time-of-flight (TOF) mass spectrometry coupled with vacuum ultraviolet (VUV) photoionization at a temperature range of 680−860 K and total pressures of 20−40 Torr. SinHm clusters were photoionized by the VUV radiation at 10.2 eV (121.6 nm). The SinH2n+2 (n ≥ 2), SinH2n (n ≥ 2), SinH2n-2 (n ≥ 5), and SinH2n-4 (n ≥ 5) containing up to 10 silicon atoms were observed as gas-phase products during the disilane pyrolysis, while no ion signal due to Si1 species such as Si, SiH, SiH2, and SiH3 was detected. Energetics for the disilane unimolecular decomposition has been calculated at the Gaussian-3 (G3)//B3LYP level of theory. On the basis of a kinetic model proposed by Swihart and Girshick [J. Phys. Chem. B 1999, 103, 64], the gas-phase kinetic simulation has been performed to analyze the formation mechanism of hydrogenated silicon clusters in the thermal decomposition of disilane. Temperatu...