Heterogeneous reactions of chlorine nitrate and hydrogen chloride on type I polar stratospheric clouds

1991 ◽  
Vol 95 (20) ◽  
pp. 7763-7771 ◽  
Author(s):  
Ming Taun Leu ◽  
Steven B. Moore ◽  
Leon F. Keyser
Keyword(s):  
Hydrogen Chloride ◽  
Heterogeneous Reactions ◽  
Type I ◽  
Polar Stratospheric Clouds ◽  
Chlorine Nitrate ◽  
Stratospheric Clouds

scholarly journals Development of a chemistry module for GCMs: first results of a multiannual integration

1998 ◽  
Vol 16 (2) ◽  
pp. 205-228 ◽  
Author(s):  
B. Steil ◽  
M. Dameris ◽  
C. Brühl ◽  
P. J. Crutzen ◽  
V. Grewe ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
General Circulation ◽  
Lower Stratosphere ◽  
Photochemical Reactions ◽  
Heterogeneous Reactions ◽  
Atmospheric Composition ◽  
Polar Stratospheric Clouds ◽  
First Results ◽  
Stratospheric Clouds ◽  
Chemistry Module

Abstract. The comprehensive chemistry module CHEM has been developed for application in general circulation models (GCMs) describing tropospheric and stratospheric chemistry, including photochemical reactions and heterogeneous reactions on sulphate aerosols and polar stratospheric clouds. It has been coupled to the spectral atmospheric GCM ECHAM3. The model configuration used in the current study has been run in an "off-line" mode, i.e. the calculated chemical species do not affect the radiative forcing of the dynamic fields. First results of a 15-year model integration indicate that the model ECHAM3/CHEM runs are numerically efficient and stable, i.e. that no model drift can be detected in dynamic and chemical parameters. The model reproduces the main features regarding ozone, in particular intra- and interannual variability. The ozone columns are somewhat higher than observed (approximately 10%), while the amplitude of the annual cycle is in agreement with observations. A comparison with HALOE data reveals, however, a serious model deficiency regarding lower-stratosphere dynamics at high latitudes. Contrary to what is concluded by observations, the lower stratosphere is characterized by slight upward motions in the polar regions, so that some of the mentioned good agreements must be considered as fortuitous. Nevertheless, ECHAM3/CHEM well describes the chemical processes leading to ozone reduction. It has been shown that the mean fraction of the northern hemisphere, which is covered by polar stratospheric clouds (PSCs) as well as the temporal appearance of PSCs in the model, is in fair agreement with observations. The model results show an activation of chlorine inside the polar vortex which is stronger in the southern than in the northern winter hemisphere, yielding an ozone hole over the Antarctic; this hole, however, is also caused to a substantial degree by the dynamics. Interhemispheric differences concerning reformation of chlorine reservoir species HCl and ClONO2 in spring have also been well reproduced by the model.Key words. Atmospheric composition and structure · Middle atmosphere · Meteorology and atmospheric dynamics · Climatology · General circulation

Estimation of heterogeneous reaction rates for stratospheric trace gases with particular reference to the diffusional uptake of HCl and ClONO<sub>2</sub> by polar stratospheric clouds

1995 ◽  
Vol 13 (4) ◽  
pp. 406-412 ◽  
Author(s):  
S. Ghosh ◽  
D. Lary ◽  
J. A. Pyle
Keyword(s):  
Reaction Rate ◽  
Heterogeneous Reaction ◽  
Trace Gases ◽  
Three Dimensional ◽  
Reaction Rates ◽  
Gas Diffusion ◽  
Type I ◽  
Polar Stratospheric Clouds ◽  
Reaction Rate Constants ◽  
Stratospheric Clouds

Abstract. The stratosphere holds a variety of particulates like polar stratospheric clouds (PSCs) and sulphate aerosols which catalyse chemical reactions. These reactions cause changes in the composition of the stratosphere, including the redistribution of active chlorine which might lead to ozone destruction. As a result during recent years a lot of effort has been directed towards the quantification of the uptake of trace gases like ClONO2, HCl, etc. into these particulates. However, it has been observed that many of the two and three dimensional models used in such studies are constrained by the lack of adequate rate constant data. This paper describes a theoretical approach to estimate the reaction rate constants for 23 gases on both types of polar stratospheric clouds (type I and II). It is found that for gases like N2O5, ClONO2 and HCl, diffusional uptake is important and contributes significantly to the heterogeneous reaction rate. A complete Lennard-Jones calculation is used to accurately compute the trace gas diffusion coefficients.

scholarly journals Mountain-wave induced polar stratospheric clouds and their representation in the global chemistry model ICON-ART

2020 ◽  
Author(s):  
Michael Weimer ◽  
Jennifer Buchmüller ◽  
Lars Hoffmann ◽  
Ole Kirner ◽  
Beiping Luo ◽  
...  
Keyword(s):  
Antarctic Peninsula ◽  
Climate Models ◽  
Hot Spot ◽  
Heterogeneous Reactions ◽  
Polar Stratospheric Clouds ◽  
Mountain Wave ◽  
Mountain Waves ◽  
Stratospheric Clouds ◽  
Wave Induced ◽  
The Antarctic

Abstract. Polar stratospheric clouds (PSCs) are a driver for ozone depletion in the lower polar stratosphere. They provide surfaces for heterogeneous reactions activating chlorine and bromine reservoir species during the polar night. PSCs are represented in current global chemistry-climate models, but one process is still a challenge: the representation of PSCs formed locally in conjunction with unresolved mountain waves. In this study, we present simulations with the ICOsahedral Nonhydrostatic modelling framework (ICON) with its extension for Aerosols and Reactive Trace gases (ART) that include local grid refinements (nesting) with two-way interaction. Here, the nesting is set up around the Antarctic Peninsula which is a well-known hot spot for the generation of mountain waves in the southern hemisphere. We compare our model results with satellite measurements from the Cloud-Aerosol LIdar with Orthogonal Polarisation (CALIOP) and the Atmospheric InfraRed Sounder (AIRS). We study a mountain wave event that took place from 19 to 29 July 2008 and find similar structures of PSCs as well as a fairly realistic development of the mountain wave in the Antarctic Peninsula nest. We compare a global simulation without nesting with the nested configuration to show the benefit. Although the mountain waves cannot be resolved adequately in the used global resolution (about 160 km), their effect from the nested regions (about 80 and 40 km) on the global domain is represented. Thus, we show in this study that by using the two-way nesting technique the gap between directly resolved mountain-wave induced PSCs and their representation and effect on chemistry in coarse global resolutions can be bridged by the ICON-ART model.

Synchrotron radiation and long path cryogenic cells: New tools and results for modelling chlorinated compounds absorption in the 8-12µm atmospheric window

2020 ◽  
Author(s):  
Laurent Manceron
Keyword(s):  
High Resolution ◽  
Atmospheric Chemistry ◽  
Broad Band ◽  
Spectroscopic Studies ◽  
Heterogeneous Reactions ◽  
Chlorine Nitrate ◽  
Synchrotron Source ◽  
Fourier Transform Spectrometry ◽  
Vibrational Levels ◽  
Stratospheric Clouds

&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;&lt;strong&gt;Anusanth Anantharajah&lt;sup&gt;a&lt;/sup&gt;, Fridolin Kwabia Tchana&lt;sup&gt;a&lt;/sup&gt;, Jean-Marie Flaud&lt;sup&gt;a&lt;/sup&gt; , Pascale Roy&lt;sup&gt;b&lt;/sup&gt; and Laurent Manceron&lt;sup&gt;b,c&lt;/sup&gt;&lt;/strong&gt;&lt;/p&gt;&lt;ul&gt;&lt;li&gt;a- Laboratoire Interuniversitaire des Syst&amp;#232;mes Atmosph&amp;#233;riques (LISA), UMR CNRS 7583, &lt;br&gt;Universit&amp;#233; de Paris et Universit&amp;#233; Paris-Est Cr&amp;#233;teil, Institut Pierre Simon Laplace, &lt;br&gt;61 Avenue du G&amp;#233;n&amp;#233;ral de Gaulle, 94010 Cr&amp;#233;teil Cedex, France.&lt;/li&gt; &lt;li&gt;b- Synchrotron SOLEIL, AILES Beamline, L&amp;#8217;Orme des Merisiers, Saint-Aubin F-91192, France.&lt;/li&gt; &lt;li&gt;c-&amp;#160; Sorbonne Universit&amp;#233;, CNRS, MONARIS, UMR 8233, 4 place Jussieu, F-75005 Paris, France.&amp;#160;&lt;/li&gt; &lt;/ul&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;Nitryl chloride (ClNO&lt;sub&gt;2&lt;/sub&gt;) and Chlorine Nitrate are molecules of great interest for atmospheric chemistry since these are produced by heterogeneous reactions, in the marine troposphere, between NaCl sea-salt aerosols or ClO and gaseous N&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;5&lt;/sub&gt; [1,2], and on polar stratospheric clouds, between N&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;5&lt;/sub&gt; and solid HCl [3,4].&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;Many high-resolution spectroscopic studies in the microwave and mid-infrared regions are available. However, these molecules present low-lying vibrational levels and thus numerous hot bands in the regions of the NOx stretching and bending mode absorptions in the 8-12 &amp;#181;m atmospheric transparency window which could serve for remote sensing and quantification of these species.&lt;/p&gt;&lt;p&gt;Fourier Transform Spectrometry is a useful technique to observe broad band high resolution spectra (0.001 cm&lt;sup&gt;-1&lt;/sup&gt;) of these molecules and a significant advantage is gained by combining interferometry with the high brightness of a synchrotron source [5]. At SOLEIL we have developed specific instrumentation to study such reactive molecules and a few results concerning chlorine-containing compounds will be presented.&lt;/p&gt;&lt;ol&gt;&lt;li&gt;B. J. Finlayson-Pitts, M. J. Ezell, and J. N. Pitts Jr, Nature &lt;strong&gt;337&lt;/strong&gt;, 241-244 (1989).&lt;/li&gt; &lt;li&gt;W. Behnke, V. Scheer, and C. Zetzsch, J. Aerosol Sci. &lt;strong&gt;24&lt;/strong&gt;, 115-116 (1993).&lt;/li&gt; &lt;li&gt;. M. A. Tolbert, M. J. Rossi, and D. M. Golden, Science &lt;strong&gt;240&lt;/strong&gt;, 1018-1021 (1988).&lt;/li&gt; &lt;li&gt;M. T. Leu, Geophys. Res. Lett. &lt;strong&gt;15&lt;/strong&gt;, 851-854 (1988).&lt;/li&gt; &lt;li&gt;&amp;#160;J-M. Flaud, A. Anantharajah, F. Kwabia Tchana, L. Manceron, J. Orphal, G. Wagner, and M. Birk, J Quant Spectrosc Radiat Transf &lt;strong&gt;224&lt;/strong&gt;, 217-221 (2019).&lt;/li&gt; &lt;/ol&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;

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