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Adsorption and thermal decomposition of acetic acid on Si (111) 7×7 studied by vibrational electron energy loss spectroscopy

机译:振动电子能量损失谱研究乙酸在Si(111)7×7上的吸附和热分解

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Vibrational electron energy loss spectroscopy (EELS) has been used to characterize the adsorption of acetic acid on Si (111) 7×7 at room temperature and as a function of annealing temperature. At room temperature, acetic acid is found to undergo OH dissociative adsorption to form predominantly unidentate adstructure. The equilibrium geometry and the corresponding characteristic vibrational wavenumbers of the adstructures were obtained by density functional theory calculations and are found to be in good accord with the vibrational EELS data. Annealing the sample near 473 K marked the onset of CO dissociation of the acetate adstructure with the emergence of SiOSi vibrational modes at 720 and 1020 cm-1. Further annealing to 673 K caused a marked intensity reduction in the CC stretch at 930 cm-1 and in the CH _3 vibrational features at 1360 and 2990 cm-1, suggesting further dissociation of the adstructures. The complete removal of the blueshifted SiH stretching mode at 2275 cm-1 upon further annealing to 773 K is consistent with the recombinative desorption of H_2 from Si monohydrides expected in this temperature range. The emergence of the SiC stretching mode at 830 cm-1 at 873 K is in good accord with the formation of SiC. Similar thermal evolution of the vibrational features have also been observed for acetic acid adsorption on a sputtered Si(111) surface.
机译:振动电子能量损失谱(EELS)已用于表征乙酸在室温和退火温度下在Si(111)7×7上的吸附性能。在室温下,发现乙酸会经历OH离解吸附,从而形成主要的身份不明的结构。通过密度泛函理论计算获得了结构的平衡几何形状和相应的特征振动波数,并发现它们与振动EELS数据非常吻合。在473 K附近对样品进行退火,标志着720和1020 cm-1处SiOSi振动模的出现,开始乙酸酯结构的CO离解。进一步退火至673 K,导致930 cm-1处的CC拉伸强度以及1360和2990 cm-1处的CH _3振动特征明显降低强度,表明基体结构进一步解离。在进一步退火至773 K时,在2275 cm-1处完全消除了蓝移SiH拉伸模式,这与在该温度范围内预期的H_2从单硅氢中解吸结合是一致的。 873 K下830 cm-1处SiC拉伸模式的出现与SiC的形成非常吻合。对于乙酸在溅射的Si(111)表面上的吸附,也观察到了振动特征的类似热演化。

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