A study of stratospheric chlorine partitioning based on new satellite measurements and modeling
A study of stratospheric chlorine partitioning based on new satellite measurements and modeling
复制标题
基于新卫星测量和建模的平流层氯分配研究
DOI：
10.1029/2007jd009057
复制
发表时间：
2008
影响因子：
--
通讯作者：
J. Waters
中科院分区：
文献类型：
--
作者：
M. Santee;I. MacKenzie;G. Manney;M. Chipperfield;P. Bernath;K. Walker;C. Boone;L. Froidevaux;N. Livesey;J. Waters
[1] 最近的两个卫星仪器，Aura 上的微波临边探测器 (MLS) 和 SCISAT-1 上的大气化学实验傅立叶变换光谱仪 (ACE-FTS)，为研究平流层氯分配提供了无与伦比的机会。我们利用 MLS 和 ACE-FTS 对 ClO、HCl、ClONO2 和其他物种的测量来研究两个北极和两个南极冬季期间整个平流层下部活性氯和储存氯的演变，这些冬季表征了每个半球相对寒冷和相对温暖和扰动的条件。在中纬度地区和初冬时的高纬度地区，HCl 大大超过 ClONO2，占估计总无机氯的 ∼0.7-0.8。在冬季极地涡旋内可以看到几乎完全的氯活化。在北极，氯的回收在两个冬季遵循不同的路径：2004/2005年，最初通过ClONO2的重整而失活，然后两个储层同时生产，但ClONO2继续显着超过HCl，最后ClONO2和HCl之间发生缓慢的重新分配； 2005/2006 年，一些地区的 HCl 和 ClONO2 增长速度相当。在南极洲，两个冬季氯的失活过程都以类似的方式进行，HCl 快速上升，ClO 下降。将测量结果与 SLIMCAT 三维化学传输模型的定制运行进行比较。在冬季极地地区之外，测量值和模拟值通常非常吻合。相比之下，部分由于用于参数化极地平流层云的平衡方案，该模型高估了极地涡旋内氯激活的幅度、空间范围和持续时间。
[1] Two recent satellite instruments, the Microwave Limb Sounder (MLS) on Aura and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on SCISAT-1, provide an unparalleled opportunity to investigate stratospheric chlorine partitioning. We use measurements of ClO, HCl, ClONO2, and other species from MLS and ACE-FTS to study the evolution of reactive and reservoir chlorine throughout the lower stratosphere during two Arctic and two Antarctic winters characterizing both relatively cold and relatively warm and disturbed conditions in each hemisphere. At middle latitudes, and at high latitudes at the beginning of winter, HCl greatly exceeds ClONO2, representing ∼0.7–0.8 of estimated total inorganic chlorine. Nearly complete chlorine activation is seen inside the winter polar vortices. In the Arctic, chlorine recovery follows different paths in the two winters: In 2004/2005, deactivation initially takes place through reformation of ClONO2, then both reservoirs are produced concurrently but ClONO2 continues to significantly exceed HCl, and finally slow repartitioning between ClONO2 and HCl occurs; in 2005/2006, HCl and ClONO2 rise at comparable rates in some regions. In the Antarctic, chlorine deactivation proceeds in a similar manner in both winters, with a rapid rise in HCl accompanying the decrease in ClO. The measurements are compared to customized runs of the SLIMCAT three-dimensional chemical transport model. Measured and modeled values typically agree well outside the winter polar regions. In contrast, partly because of the equilibrium scheme used to parameterize polar stratospheric clouds, the model overestimates the magnitude, spatial extent, and duration of chlorine activation inside the polar vortices.