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首页> 外文期刊>Atmospheric chemistry and physics >HOCl chemistry in the Antarctic stratospheric vortex 2002, as observed with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS)
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HOCl chemistry in the Antarctic stratospheric vortex 2002, as observed with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS)

机译:用无源大气探测的迈克尔逊干涉仪(MIPAS)观测到的南极平流层涡旋2002中的HOCl化学

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In the 2002 Antarctic polar vortex enhanced HOCl mixing ratios were detected by the Michelson Interferometer for Passive Atmospheric Sounding both at altitudes of around 35 km (1000 K potential temperature), where HOCl abundances are ruled by gas phase chemistry and at around 18-24 km (475-625 K), which belongs to the altitude domain where heterogeneous chlorine chemistry is relevant. At altitudes of 33 to 40 km polar vortex HOCl mixing ratios were found to be around 0.14 ppbv as long as the polar vortex was intact, centered at the pole, and thus received relatively little sunlight. This is the altitude region where in midlatitudinal and tropic atmospheres peak HOCl mixing ratios significantly above 0.2 ppbv (in terms of daily mean values) are observed. After deformation and displacement of the polar vortex in the course of a major warming, ClO-rich vortex air was more exposed to sunlight, where enhanced HO_x abundances led to largely increased HOCl mixing ratios (up to 0.3 ppbv), exceeding typical midlatitudinal and tropical amounts significantly. The HOCl increase was preceded by an increase of ClO. Model runs could reproduce these measurements only when the Stimpfle et al. (1979) rate constant for the reaction ClO+HO_2→HOCl+O_2 was used but not with the current JPL recommendation. At an altitude of 24 km, HOCl mixing ratios of up to 0.15 ppbv were detected. This HOCl enhancement, which is already visible in 18 September data, is attributed to heterogeneous chemistry, which is in agreement with observations of polar stratospheric clouds. The measurements were compared to a model run where no polar stratospheric clouds appeared during the observation period. The fact that HOCl still was produced in the model run suggests that a significant part of HOCl was generated from ClO rather than directly via heterogeneous reaction. Excess ClO, lower CIONO_2 and earlier loss of HOCl in the measurements are attributed to ongoing heterogeneous chemistry which is not reproduced by the model. On 11 October, polar vortex mean daytime mixing ratios were only 0.03 ppbv.
机译:在2002年,迈克尔逊干涉仪通过被动大气探测法检测到了南极极涡的增强HOCl混合比,这两个高度都在大约35 km(1000 K的潜在温度)的高度上,其中HOCl的丰度由气相化学法控制并且在大约18-24 km (475-625 K),属于与异质氯化学有关的海拔区域。在33至40 km的高度,发现极涡旋HOCl的混合比约为0.14 ppbv,只要极涡旋完好无损,以极点为中心,因此受到的阳光相对较少。这是在中纬度和热带大气中观察到的HOCl混合比峰值明显高于0.2 ppbv(按日平均值)的海拔区域。在主要变暖过程中极性涡旋发生变形和位移之后,富含ClO的涡旋空气更多地暴露于阳光下,其中HO_x丰度的提高导致HOCl混合比大大提高(最高0.3 ppbv),超过了典型的中纬度和热带数量明显。 HOCl增加之前是ClO增加。只有在Stimpfle等人(2002年)的模型运行中才能重现这些测量结果。 (1979)使用了反应速率常数ClO + HO_2→HOCl + O_2,但当前的JPL建议中没有使用。在24 km的海拔高度,检测到的HOCl混合比高达0.15 ppbv。 HOCl的这种增强作用已经在9月18日的数据中可见,这归因于化学性质的异质性,这与极地平流层云的观测结果一致。将测量结果与模型运行进行比较,在模型运行期间观察期间没有出现极地平流层云。在模型运行中仍然产生HOCl的事实表明,HOCl的很大一部分是从ClO生成的,而不是直接通过异质反应生成的。测量中过量的ClO,较低的CIONO_2和较早的HOCl损失归因于模型未再现的正在进行的异质化学反应。 10月11日,极地涡旋平均日混合比仅为0.03 ppbv。

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