Peroxy radical behavior during the Transport and Chemical Evolution over the Pacific (TRACE-P) campaign as measured aboard the NASA P-3B aircraft
Peroxy radical behavior during the Transport and Chemical Evolution over the Pacific (TRACE-P) campaign as measured aboard the NASA P-3B aircraft
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在 NASA P-3B 飞机上测量的太平洋运输和化学演化 (TRACE-P) 活动期间的过氧自由基行为
DOI：
10.1029/2003jd003674
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发表时间：
2003
影响因子：
--
通讯作者：
A. Clarke
中科院分区：
文献类型：
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作者：
C. Cantrell;G. Edwards;S. Stephens;R. Mauldin;M. Zondlo;E. Kosciuch;F. Eisele;R. Shetter;B. Lefer;S. Hall;F. Flocke;A. Weinheimer;A. Fried;E. Apel;Y. Kondo;D. Blake;N. Blake;I. Simpson;A. Bandy;D. Thornton;B. Heikes;H. Singh;W. Brune;H. Harder;Mónica Martínez;D. Jacob;M. Avery;J. Barrick;G. Sachse;J. Olson;J. Crawford;A. Clarke
[1] 2001 年春季，在太平洋运输和化学演化 (TRACE-P) 活动期间，在 NASA P-3B 飞机上测量了过氧自由基浓度，其变化取决于自由基生成速率和活性氮浓度。本研究中对 HO2 、H O2 +R O2 和 OH 的测量可以计算自由基比率，检查这些比率对控制变量的函数关系，并与数值模型估计进行比较。自由基产量项显示了低、中和高总生产率下相对贡献的变化，这可以通过控制成分（痕量气体浓度和光解速率系数）的系统变化来理解。臭氧趋势计算表明西太平洋盆地的臭氧净产量，因为关键前体痕量气体（例如氮氧化物、碳氢化合物）的浓度在那里最高。臭氧趋势的依赖性系统地遵循NO浓度。两架飞机上的过氧自由基水平（P-3B 上的 HO2 +R O2 和 DC-8 上的 HO2）在两个相对较短的规定相互比较期间，在一种情况下非常一致，而在另一种情况下，考虑到对 HO2 和 RO2 之间自由基分配的合理假设，过氧自由基水平较差。建议对 CH2O 光解量子产率、HO2 自反应和 O( 1 D) 猝灭动力学进行更改，从而导致 TRACE-P 条件下计算的过氧自由基水平发生微小变化 (<5%)。这次活动的证据表明，过氧自由基通过与气溶胶和云滴的相互作用而损失。索引术语：0317 大气成分和结构：化学动力学和光化学性质； 0322 大气成分和结构：成分源和汇； 0365 大气成分和结构：对流层——成分和化学； 0368 大气成分和结构：对流层——成分输送和化学；关键词: 光化学, 过氧自由基, 臭氧
[1] Peroxy radical concentrations were measured aboard the NASA P-3B aircraft during the Transport and Chemical Evolution over the Pacific (TRACE-P) campaign in the spring of 2001 and varied in ways that depended on radical production rates and reactive nitrogen concentrations. Measurements of HO2 ,H O2 +R O2, and OH during this study allowed calculation of radical ratios, examination of functional relationships of these ratios on controlling variables, and comparison with numerical model estimations. Radical production terms show changes in relative contributions at low, middle, and high total production rates that are understandable in terms of systematic variations in the controlling components (trace gas concentrations and photolysis rate coefficients). Ozone tendency calculations indicate net ozone production in the western Pacific basin because the concentrations of critical precursor trace gases (e.g., NOx, hydrocarbons) are highest there. The dependence of ozone tendency follows the concentration of NO systematically. Peroxy radical levels on the two aircraft (HO2 +R O2 on the P-3B and HO2 on the DC-8) during two relatively short prescribed intercomparison periods were in good agreement in one instance and poorer in another given reasonable assumptions about the apportioning of radicals between HO2 and RO2. Recommended changes to CH2O photolysis quantum yields, HO2 self reaction, and O( 1 D) quenching kinetics lead to small changes (<5%) in calculated peroxy radical levels for TRACE-P conditions. There is evidence from this campaign that peroxy radicals are lost by interaction with aerosols and cloud droplets. INDEX TERMS: 0317 Atmospheric Composition and Structure: Chemical kinetic and photochemical properties; 0322 Atmospheric Composition and Structure: Constituent sources and sinks; 0365 Atmospheric Composition and Structure: Troposphere—composition and chemistry; 0368 Atmospheric Composition and Structure: Troposphere—constituent transport and chemistry; KEYWORDS: photochemistry, peroxy radicals, ozone