用于氢过氧自由基光谱和动力学分析的腔衰荡光谱装置

引用本文: 胡晓, 倪世传, 杨娜娜, 王春晖, 韦娜娜, 方波, 刘栋沅, 赵卫雄, 张为俊. 用于氢过氧自由基光谱和动力学分析的腔衰荡光谱装置[J]. 分析化学, 2023, 51(6): 994-1002. doi: 10.19756/j.issn.0253-3820.231062 shu

Citation: HU Xiao, NI Shi-Chuan, YANG Na-Na, WANG Chun-Hui, WEI Na-Na, FANG Bo, LIU Dong-Yuan, ZHAO Wei-Xiong, ZHANG Wei-Jun. A Cavity Ring-down Spectrum Instrument for Analysis of HO₂ Radical Spectroscopy and Kinetics[J]. Chinese Journal of Analytical Chemistry, 2023, 51(6): 994-1002. doi: 10.19756/j.issn.0253-3820.231062 shu

用于氢过氧自由基光谱和动力学分析的腔衰荡光谱装置

胡晓 ^1,2, ,
倪世传 ^1,2, ,
杨娜娜 ^1, ,
王春晖 ^3, ,
韦娜娜 ^1, ,
方波 ^1, ,
刘栋沅 ^1,2, ,
赵卫雄 ^{1,
,} ,
张为俊 ^1,3,

1.
中国科学院合肥物质科学研究院安徽光学精密机械研究所, 合肥 230031;
2.
中国科学技术大学研究生院科学岛分院, 合肥 230026;
3.
中国科学技术大学环境科学与光电技术学院, 合肥 230026

通讯作者: 赵卫雄,E-mail:wxzhao@aiofm.ac.cn

基金项目:
国家自然科学基金项目(Nos.U21A2028,42022051)、中国科学院青年创新促进会项目(No.Y202089)和合肥研究院院长基金项目(No.YZJJ202101)资助。

摘要: 基于近红外腔衰荡光谱技术（CRDS）结合闪光光解，搭建了一套用于瞬态自由基探测的高灵敏度实验装置。通过扫描自主设计的光学谐振腔腔长，实现激光器与腔的模式耦合，基于线性回归求和（LRS）算法对衰荡曲线进行拟合，获得衰荡时间，在20.3 km有效光程和6.25 s采集时间下，系统可实现5.05×10^-11 cm^-1的探测灵敏度。使用266 nm Nd:YAG激光器光解臭氧（O₃）和乙炔（C₂H₂）的混合物产生氢过氧自由基（HO₂·），测量了HO₂·在6638.203 cm^-1位置处的特征吸收，获得了分辨率为0.002 cm-1的吸收光谱。在2 kPa条件下，通过测量HO₂·自反应的衰变获得了6638.203 cm^-1处HO₂·的吸收截面（σ）为3.3×10^-19 cm²/molecule，对应的吸收谱线强度（S）为6.02×10^-21 cm^-1/（molecule/cm²）。

关键词:

English

A Cavity Ring-down Spectrum Instrument for Analysis of HO₂ Radical Spectroscopy and Kinetics

1.
Anhui Institute of Optics and Fine Mechanics, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei 230031, China;
2.
Science Island Branch, Graduate School, University of Science and Technology of China, Hefei 230026, China;
3.
School of Environmental Science and Optoelectronics Technology, University of Science and Technology of China, Hefei 230026, China

Corresponding author: ZHAO Wei-Xiong, wxzhao@aiofm.ac.cn

Received Date: 21 February 2023
Revised Date: 19 April 2023
Fund Project:
Supported by the National Natural Science Foundation of China (Nos. U21A2028, 42022051), the Youth Innovation Promotion Association, CAS (No. Y202089) and the CASHIPS Director′s Fund (No. YZJJ202101).

Abstract: A new experimental set-up for highly sensitive detection of transient radicals was established based on cavity ring-down spectroscopy (CRDS) combined with flash photolysis. The mode coupling between the laser and the cavity was achieved by scanning the cavity length of the self-designed optical resonant cavity, and the ringdown time was obtained by fitting the decay curve based on the linear regression summation (LRS) algorithm. The minimum detectable absorption of the system of 5.05×10^-11 cm^-1 was achieved with effective optical path of 20.3 km and acquiring time of 6.25 s. HO₂ radicals were generated by using a 266 nm Nd∶YAG laser photolysis of O₃/C₂H₂ mixtures. The characteristic absorption of HO₂ radicals at 6638.203 cm^-1 was measured, and the absorption spectrum with a resolution of 0.002 cm^-1 was obtained. Under the condition of 2 kPa, the absorption cross section of HO₂ radicals at 6638.203 cm^-1 was 3.3×10^-19 cm²/molecule by measuring the decay of the HO₂ radicals self-reaction, and the corresponding absorption line strength was 6.02×10^-21 cm^-1/(molecule/cm²).

Key words:

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通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

用于氢过氧自由基光谱和动力学分析的腔衰荡光谱装置

通讯作者: 赵卫雄,E-mail:wxzhao@aiofm.ac.cn

English

A Cavity Ring-down Spectrum Instrument for Analysis of HO₂ Radical Spectroscopy and Kinetics

Corresponding author: ZHAO Wei-Xiong, wxzhao@aiofm.ac.cn

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通讯作者: 陈斌, bchen63@163.com

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用于氢过氧自由基光谱和动力学分析的腔衰荡光谱装置

通讯作者: 赵卫雄,E-mail:wxzhao@aiofm.ac.cn

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