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Time-Resolved Laser-Flash Photolysis Faraday Rotation Spectrometer: A New Tool for Total OH Reactivity Measurement and Free Radical Kinetics Research

Abstract : The total OH reactivity (kOH′) is an important parameter for quantitative assessment of the atmospheric oxidation capacity. Although laboratory measurement of kOH′ has been achieved 20 years ago, the instruments required are often costly and complex. Long-term atmospheric observations remain challenging and elusive. In this work, a novel instrument combining laser-flash photolysis with a mid-infrared Faraday rotation spectrometer (LFP-FRS) has been developed for the measurement of kOH′ and for studying gas phase free radical kinetics. The reactor is composed of a Herriott-type optical multipass cell, and OH radicals were generated by flash photolysis of ozone with a 266 nm pulsed Nd:YAG laser. The decay of the OH signal was directly measured with a time-resolved FRS spectrometer at 2.8 μm. The overlapping path length between the pump beam and probe beam was 25 m. High performance was achieved by subtracting the signals before and after flash photolysis to eliminate interferences caused by H2O absorption and background drift. The optimum precisions (1σ) of OH concentration and kOH′ measurement were 4 × 106 molecules cm–3 and 0.09 s–1 over data acquisition times of 56 and 112 s, respectively. The performance of the system was evaluated by the reaction of OH with CO and NO. The measured rate coefficients (kOH+CO and kOH+NO) were in good agreement with values reported in the literature. The developed LFP-FRS provides a new, high precision, and highly selective tool for atmospheric chemistry research of OH radicals and other transient paramagnetic free radicals such as HO2 radicals.
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https://hal.univ-lille.fr/hal-02968041
Contributeur : Lilloa Université de Lille <>
Soumis le : jeudi 15 octobre 2020 - 12:55:18
Dernière modification le : mardi 3 novembre 2020 - 15:44:02

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Nana Wei, Bo Fang, Weixiong Zhao, Chunhui Wang, Nana Yang, et al.. Time-Resolved Laser-Flash Photolysis Faraday Rotation Spectrometer: A New Tool for Total OH Reactivity Measurement and Free Radical Kinetics Research. Analytical Chemistry, 2020, Analytical Chemistry, 92 (6), pp.4334-4339. ⟨10.1021/acs.analchem.9b05117⟩. ⟨hal-02968041⟩

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