{"title":"甲醇、丙酮、甲烷、氧气和氮气对 CH(A)的碰撞淬灭率与温度有关","authors":"Sebastian Pfaff, Erxiong Huang, Jonathan H. Frank","doi":"10.1007/s00340-024-08335-5","DOIUrl":null,"url":null,"abstract":"<div><p>Laser-induced fluorescence is a widely used technique for measuring the concentrations of gaseous species in reactive environments. To determine absolute number densities from laser-induced fluorescence signals, the collisional quenching rate of the excited state molecule needs to be known. The methylidyne (CH) radical is an important species in combustion, catalysis, and plasma applications, the latter two of which require laser-induced fluorescence measurements at lower temperatures. Quantitative detection of CH is also needed for photofragmentation laser-induced fluorescence measurements, where CH is produced by photolysis of a larger molecule, such as the methyl radical (CH<span>\\(_{3}\\)</span>), by a pump laser, and then is excited by a probe laser to induce fluorescence. We have measured the collisional quenching rates of CH(A) by methanol, methane, oxygen, nitrogen, and acetone at temperatures between 300 and 600 K. The CH(A) quenching rate by methanol, which is highly relevant in catalysis, has not previously been studied. The quenching rates for acetone, which is used as a precursor to photolytically produce methyl, and methane have been studied but not at elevated temperatures. We find that methanol and acetone both have high quenching rate coefficients of <span>\\(2.2\\cdot10^{-10}\\)</span> to <span>\\(2.5\\cdot10^{-10}\\)</span> cm<span>\\(^3\\)</span>/s with only a small temperature dependence. We also find that the quenching rate of methane has a significant temperature dependence ranging from <span>\\(2.5\\cdot10^{-11}\\)</span> cm<span>\\(^3\\)</span>/s at 300 K to <span>\\(5.0\\cdot10^{-11}\\)</span> cm<span>\\(^3\\)</span>/s at 600 K. The quenching rates determined in this work are important for laser-induced fluorescence studies of catalysis, plasmas, and combustion processes.</p></div>","PeriodicalId":474,"journal":{"name":"Applied Physics B","volume":"130 11","pages":""},"PeriodicalIF":2.0000,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Temperature dependent collisional quenching rates of CH(A) by methanol, acetone, methane, oxygen, and nitrogen\",\"authors\":\"Sebastian Pfaff, Erxiong Huang, Jonathan H. Frank\",\"doi\":\"10.1007/s00340-024-08335-5\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Laser-induced fluorescence is a widely used technique for measuring the concentrations of gaseous species in reactive environments. To determine absolute number densities from laser-induced fluorescence signals, the collisional quenching rate of the excited state molecule needs to be known. The methylidyne (CH) radical is an important species in combustion, catalysis, and plasma applications, the latter two of which require laser-induced fluorescence measurements at lower temperatures. Quantitative detection of CH is also needed for photofragmentation laser-induced fluorescence measurements, where CH is produced by photolysis of a larger molecule, such as the methyl radical (CH<span>\\\\(_{3}\\\\)</span>), by a pump laser, and then is excited by a probe laser to induce fluorescence. We have measured the collisional quenching rates of CH(A) by methanol, methane, oxygen, nitrogen, and acetone at temperatures between 300 and 600 K. The CH(A) quenching rate by methanol, which is highly relevant in catalysis, has not previously been studied. The quenching rates for acetone, which is used as a precursor to photolytically produce methyl, and methane have been studied but not at elevated temperatures. We find that methanol and acetone both have high quenching rate coefficients of <span>\\\\(2.2\\\\cdot10^{-10}\\\\)</span> to <span>\\\\(2.5\\\\cdot10^{-10}\\\\)</span> cm<span>\\\\(^3\\\\)</span>/s with only a small temperature dependence. We also find that the quenching rate of methane has a significant temperature dependence ranging from <span>\\\\(2.5\\\\cdot10^{-11}\\\\)</span> cm<span>\\\\(^3\\\\)</span>/s at 300 K to <span>\\\\(5.0\\\\cdot10^{-11}\\\\)</span> cm<span>\\\\(^3\\\\)</span>/s at 600 K. 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引用次数: 0
摘要
激光诱导荧光是一种广泛用于测量反应环境中气体物种浓度的技术。要从激光诱导荧光信号中确定绝对数量密度,需要知道激发态分子的碰撞淬灭率。甲基idyne(CH)自由基是燃烧、催化和等离子体应用中的重要物种,后两种应用需要在较低温度下进行激光诱导荧光测量。光碎片激光诱导荧光测量也需要对 CH 进行定量检测,在这种测量中,CH 是通过泵浦激光对较大分子(如甲基自由基 (CH\(_{3}\))的光解而产生的,然后被探针激光激发以诱导荧光。我们测量了甲醇、甲烷、氧气、氮气和丙酮在 300 至 600 K 温度下对 CH(A) 的碰撞淬灭率。丙酮(用于光解产生甲基的前体)和甲烷的淬灭速率也曾被研究过,但没有在高温下研究过。我们发现甲醇和丙酮的淬灭速率系数都很高,从(2.2\cdot10^{-10}\)到(2.5\cdot10^{-10}\)cm\(^3\)/s,而且只有很小的温度依赖性。我们还发现,甲烷的淬灭速率具有显著的温度依赖性,范围从 300 K 时的\(2.5\cdot10^{-11}\) cm\(^3\)/s 到 600 K 时的\(5.0\cdot10^{-11}\) cm\(^3\)/s.
Temperature dependent collisional quenching rates of CH(A) by methanol, acetone, methane, oxygen, and nitrogen
Laser-induced fluorescence is a widely used technique for measuring the concentrations of gaseous species in reactive environments. To determine absolute number densities from laser-induced fluorescence signals, the collisional quenching rate of the excited state molecule needs to be known. The methylidyne (CH) radical is an important species in combustion, catalysis, and plasma applications, the latter two of which require laser-induced fluorescence measurements at lower temperatures. Quantitative detection of CH is also needed for photofragmentation laser-induced fluorescence measurements, where CH is produced by photolysis of a larger molecule, such as the methyl radical (CH\(_{3}\)), by a pump laser, and then is excited by a probe laser to induce fluorescence. We have measured the collisional quenching rates of CH(A) by methanol, methane, oxygen, nitrogen, and acetone at temperatures between 300 and 600 K. The CH(A) quenching rate by methanol, which is highly relevant in catalysis, has not previously been studied. The quenching rates for acetone, which is used as a precursor to photolytically produce methyl, and methane have been studied but not at elevated temperatures. We find that methanol and acetone both have high quenching rate coefficients of \(2.2\cdot10^{-10}\) to \(2.5\cdot10^{-10}\) cm\(^3\)/s with only a small temperature dependence. We also find that the quenching rate of methane has a significant temperature dependence ranging from \(2.5\cdot10^{-11}\) cm\(^3\)/s at 300 K to \(5.0\cdot10^{-11}\) cm\(^3\)/s at 600 K. The quenching rates determined in this work are important for laser-induced fluorescence studies of catalysis, plasmas, and combustion processes.
期刊介绍:
Features publication of experimental and theoretical investigations in applied physics
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Coverage includes laser physics, linear and nonlinear optics, ultrafast phenomena, photonic devices, optical and laser materials, quantum optics, laser spectroscopy of atoms, molecules and clusters, and more
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In addition to regular papers Applied Physics B: Lasers and Optics features invited reviews. Fields of topical interest are covered by feature issues. The journal also includes a rapid communication section for the speedy publication of important and particularly interesting results.