Evolution of inorganic chlorine partitioning in the Arctic polar vortex
Evolution of inorganic chlorine partitioning in the Arctic polar vortex
复制标题
北极极地涡旋中无机氯分配的演变
DOI：
10.1029/2005jd006951
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发表时间：
2006
影响因子：
--
通讯作者：
L. Lait
中科院分区：
文献类型：
--
作者：
D. M. Wilmouth;R. Stimpfle;James G. Anderson;J. Elkins;D. Hurst;R. Salawitch;L. Lait
[1] 在 SOLVE/THESEO 任务期间，使用从瑞典基律纳部署的 NASA ER-2 飞机对 ClO、ClOOCl、ClONO2 和 HCl（它们几乎构成总无机氯 Cly）进行了首次同步原位大气测量。这些氯测量以及从有机氯源气体的原位测量中推断出的 Cly，为观察极地冬季平流层中氯的活化和恢复以及评估无机氯预算提供了前所未有的机会，即测试 ClOx (ClO + 2 × ClOOCl)、ClONO2 和 HCl 与 Cly 之和之间的定量一致性。在北极涡旋内部，无机氯很少被完全激活，ClOx/Cly 的范围约为 0.25 至 0.90。仲冬大部分时间无机氯收支的明显差异与回轨迹太阳天顶角最小值密切相关，并且与无法观测到的 Cl2 的存在相一致。对仲冬无机氯预算的评估（排除存在 Cl2 的数据）得出 (ClOx + ClONO2 + HCl)/Cly = 0.94 ± 0.07。相比之下，冬末无机氯预算的短缺是由于 HCl 测量值明显偏低造成的。为分析氯回收率而构建的昼夜箱模型不仅强调了 Cl + CH4 反应在 HCl 形成中的重要性，而且还强调了 OH + ClO 以及潜在的 HO2 + ClO。我们发现，在今年北极冬季的无机氯回收阶段，随着净 ClONO2 的产生，大量的 HCl 产生。
[1] The first simultaneous, in situ atmospheric measurements of ClO, ClOOCl, ClONO2, and HCl, which together nearly compose total inorganic chlorine, Cly, were obtained using the NASA ER-2 aircraft, deployed from Kiruna, Sweden, during the SOLVE/THESEO mission. These chlorine measurements, along with Cly inferred from in situ measurements of organic chlorine source gases, offer an unprecedented opportunity to observe chlorine activation and recovery in the polar winter stratosphere and evaluate the inorganic chlorine budget, i.e., a test of the quantitative agreement between the sum of ClOx (ClO + 2 × ClOOCl), ClONO2, and HCl with Cly. Inside the Arctic vortex, inorganic chlorine is rarely fully activated with ClOx/Cly ranging from approximately 0.25 to 0.90. An apparent discrepancy in the inorganic chlorine budget for much of the midwinter correlates well with back trajectory solar zenith angle minimum and is consistent with the presence of Cl2, which was not observable. Evaluation of the midwinter inorganic chlorine budget, excluding data where Cl2 is present, yields (ClOx + ClONO2 + HCl)/Cly = 0.94 ± 0.07. In contrast, a shortfall in the late winter inorganic chlorine budget is the result of an apparent low bias in the HCl measurements. A diurnal box model constructed to analyze chlorine recovery rates highlights the importance of not only the Cl + CH4 reaction in HCl formation, but also OH + ClO and potentially HO2 + ClO. We find that significant HCl production accompanied net ClONO2 production in the inorganic chlorine recovery phase of this Arctic winter.