同步辐射光电离质谱检测氟原子在二氧化硅表面反应产物

汪程程; 唐小锋; 温作赢; 王涛; 张翠红; 杨玖重; 顾学军; 张为俊

doi:10.7538/zpxb.2019.0001

同步辐射光电离质谱检测氟原子在二氧化硅表面反应产物

1.
中国科学院安徽光学精密机械研究所,安徽合肥230031
2.
中国科学技术大学研究生院,安徽合肥230026
3.
中国科学技术大学国家同步辐射实验室,安徽合肥230029
4.
中国科学技术大学环境科学与光电技术学院,安徽合肥230026

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- 刊出日期: 2020-01-19

Reaction Products of F Atoms on the Surface of Silicon Dioxide Probed by Synchrotron Photoionization Mass Spectrometry

1.
Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China
2.
Graduate School, University of Science and Technology of China, Hefei 230026, China
3.
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China
4.
School of Environmental Science and Optoelectronic Technology, University of Science and Technology of China, Hefei 230026, China

摘要

摘要: 采用微波放电等离子体源产生高密度F原子，结合同步辐射真空紫外光电离质谱全面检测F原子在二氧化硅表面刻蚀反应的产物，并探究其反应机理。通过扫描同步辐射光子能量，获得具有特定质量选择的离子光电离效率谱，测量了反应产物的电离能及碎片离子的出现势等基本参数；同时结合量子化学理论计算质谱中离子的来源，即对光电离和光解离过程进行了区分。结果表明，F原子在二氧化硅表面会反应生成一系列的氟氧硅化合物 (Si_xO_yF_z)，主要包括SiF₄、SiF₃OSiF₃和SiFOSiF₂OF等，质谱中观察到的SiF₃⁺、SiF₃OSiF₂⁺等离子信号来源于其对应母体离子的解离碎片。实验测得SiF₄的电离能为15.85 eV，SiF₃⁺和SiF₃OSiF₂⁺碎片离子的出现势分别为16.20、16.40 eV。该方法实现了高效检测F原子刻蚀反应的产物，由于F原子具有较高的化学反应活性，该实验装置也可用于开展气相自由基反应研究，模拟大气化学和燃烧火焰等体系中的化学反应过程。
- 真空紫外光电离质谱 /
- 同步辐射 /
- 微波放电 /
- 氟原子 /
- 二氧化硅 /
- 电离能
Abstract: F atoms etching reaction as an efficient method has been widely used in the fields of optical manufacture, semiconductor and chemistry. But due to the technical challenges of analysis on-line, the products information, especially for the unstable radicals and intermediates, F atoms etching reaction is limited and hinders to understand its detailed mechanisms. The state-of-the-art method of synchrotron vacuum ultraviolet (VUV) photoionization mass spectrometry with high mass reolution and high sensitivity was utilized to probe reaction products of F atoms etching on the surface of silicon dioxide (SiO₂), where a microwave discharge plasma source was combined to produce F atoms with high density. Photoionization efficiency spectra (PIES) corresponding to each mass were measured by scanning synchrotron photon energy continuously, and the ionization energies of the species and the appearance energies of fragment ions were measured, in comparison well to the results of theoretical calculation. Then the ion signals in photoionization mass spectra (PIMS) from different sources, photoionization or dissociative photoionization, were defined and assigned. It was shown that a series of fluorine oxygen silicon compounds (Si_xO_yF_z) were produced and the reaction products of SiF₄, SiF₃OSiF₃ and SiFOSiF₂OF took a large intensity in the PIMS. However, the ion signals of SiF₃⁺and SiF₃OSiF₂⁺ observed in the PIMS were from dissociative photoionization of their respective precursors. In addition, some fundamental data like the ionization energy of SiF₄ and the appearance energies of SiF₃⁺ and SiF₃OSiF₂⁺ fragment ions from dissociative photoionization of SiF₄ and SiF₃OSiF₃ were measured to be 15.85, 16.20 and 16.40 eV, respectively. This method realizes the efficient detection of products in F atom etching reaction. Because F atom has high chemical reaction activity, the experimental device can also be used to carry out the study of gas phase free radical reaction and simulate the chemical reaction process in atmospheric chemistry and combustion flame system.
- vacuum ultraviolet photoionization mass spectrometry /
- synchrotron radiation /
- microwave discharge /
- F atom /
- SiO₂ /
- ionization energy

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同步辐射光电离质谱检测氟原子在二氧化硅表面反应产物

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Reaction Products of F Atoms on the Surface of Silicon Dioxide Probed by Synchrotron Photoionization Mass Spectrometry

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