scholarly journals A closer look at Arctic ozone loss and polar stratospheric clouds

2010 ◽  
Vol 10 (17) ◽  
pp. 8499-8510 ◽  
Author(s):  
N. R. P. Harris ◽  
R. Lehmann ◽  
M. Rex ◽  
P. von der Gathen

Abstract. The empirical relationship found between column-integrated Arctic ozone loss and the potential volume of polar stratospheric clouds inferred from meteorological analyses is recalculated in a self-consistent manner using the ERA Interim reanalyses. The relationship is found to hold at different altitudes as well as in the column. The use of a PSC formation threshold based on temperature dependent cold aerosol formation makes little difference to the original, empirical relationship. Analysis of the photochemistry leading to the ozone loss shows that activation is limited by the photolysis of nitric acid. This step produces nitrogen dioxide which is converted to chlorine nitrate which in turn reacts with hydrogen chloride on any polar stratospheric clouds to form active chlorine. The rate-limiting step is the photolysis of nitric acid: this occurs at the same rate every year and so the interannual variation in the ozone loss is caused by the extent and persistence of the polar stratospheric clouds. In early spring the ozone loss rate increases as the solar insolation increases the photolysis of the chlorine monoxide dimer in the near ultraviolet. However the length of the ozone loss period is determined by the photolysis of nitric acid which also occurs in the near ultraviolet. As a result of these compensating effects, the amount of the ozone loss is principally limited by the extent of original activation rather than its timing. In addition a number of factors, including the vertical changes in pressure and total inorganic chlorine as well as denitrification and renitrification, offset each other. As a result the extent of original activation is the most important factor influencing ozone loss. These results indicate that relatively simple parameterisations of Arctic ozone loss could be developed for use in coupled chemistry climate models.

2010 ◽  
Vol 10 (3) ◽  
pp. 6681-6712 ◽  
Author(s):  
N. R. P. Harris ◽  
R. Lehmann ◽  
M. Rex ◽  
P. von der Gathen

Abstract. The empirical relationship found between column-integrated Arctic ozone loss and the volume of polar stratospheric clouds inferred from meteorological analyses is updated and examined in more detail. The relationship is found to hold at different altitudes as well as in the column. Analysis of the photochemistry leading to the ozone loss shows that the early winter activation is limited by the photolysis of nitric acid. This step produces nitrogen dioxide which is converted to chlorine nitrate which in turn reacts with hydrogen chloride on any polar stratospheric clouds to form active chlorine. The rate-limiting step is the photolysis of nitric acid: this occurs at the same rate every year and so the interannual variation in the ozone loss is caused by the extent and persistence of the polar stratospheric clouds. In early spring the ozone loss rate increases as the solar insolation increases the photolysis of the chlorine monoxide dimer. However the length of the ozone loss period is determined by the photolysis of nitric acid which also occurs in the near ultraviolet. As a result of these compensating effects, the amount of the ozone loss is principally limited by the extent of original activation rather than its timing. In addition a number of factors, including the vertical changes in pressure and total inorganic chlorine as well as denitrification and renitrification, offset each other. As a result the extent of original activation is the most important factor influencing ozone loss. These results indicate that relatively simple parameterisations of Arctic ozone loss could be developed for use in coupled chemistry climate models.


2007 ◽  
Vol 7 (9) ◽  
pp. 2151-2163 ◽  
Author(s):  
J. Alfred ◽  
M. Fromm ◽  
R. Bevilacqua ◽  
G. Nedoluha ◽  
A. Strawa ◽  
...  

Abstract. The Polar Ozone and Aerosol Measurement and Stratospheric Aerosol and Gas Experiment instruments both observed high numbers of polar stratospheric clouds (PSCs) in the polar region during the second SAGE Ozone Loss and Validation (SOLVE II) and Validation of INTERnational Satellites and Study of Ozone Loss (VINTERSOL) campaign, conducted during the 2002/2003 Northern Hemisphere winter. Between 15 November 2002 (14 November 2002) and 18 March 2003 (21 March 2003) SAGE (POAM) observed 122 (151) aerosol extinction profiles containing PSCs. PSCs were observed on an almost daily basis, from early December through 15 January, in both instruments. No PSCs were observed from either instrument from 15 January until 4 February, and from then only sparingly in three periods in mid- and late February and mid-March. In early December, PSCs were observed in the potential temperature range from roughly 375 K to 750 K. Throughout December the top of this range decreases to near 600 K. In February and March, PSC observations were primarily constrained to potential temperatures below 500 K. The PSC observation frequency as a function of ambient temperature relative to the nitric acid-trihydrate saturation point (using a nitric acid profile prior to denitrification) was used to infer irreversible denitrification. By late December 38% denitrification was inferred at both the 400–475 K and 475–550 K potential temperature ranges. By early January extensive levels of denitrification near 80% were inferred at both potential temperature ranges, and the air remained denitrified at least through early March.


2021 ◽  
Author(s):  
Ramina Alwarda ◽  
Kristof Bognar ◽  
Kimberly Strong ◽  
Martyn Chipperfield ◽  
Sandip Dhomse ◽  
...  

<p>The Arctic winter of 2019-2020 was characterized by an unusually persistent polar vortex and temperatures in the lower stratosphere that were consistently below the threshold for the formation of polar stratospheric clouds (PSCs). These conditions led to ozone loss that is comparable to the Antarctic ozone hole. Ground-based measurements from a suite of instruments at the Polar Environment Atmospheric Research Laboratory (PEARL) in Eureka, Canada (80.05°N, 86.42°W) were used to investigate chemical ozone depletion. The vortex was located above Eureka longer than in any previous year in the 20-year dataset and lidar measurements provided evidence of polar stratospheric clouds (PSCs) above Eureka. Additionally, UV-visible zenith-sky Differential Optical Absorption Spectroscopy (DOAS) measurements showed record ozone loss in the 20-year dataset, evidence of denitrification along with the slowest increase of NO<sub>2</sub> during spring, as well as enhanced reactive halogen species (OClO and BrO). Complementary measurements of HCl and ClONO<sub>2</sub> (chlorine reservoir species) from a Fourier transform infrared (FTIR) spectrometer showed unusually low columns that were comparable to 2011, the previous year with significant chemical ozone depletion. Record low values of HNO<sub>3</sub> in the FTIR dataset are in accordance with the evidence of PSCs and a denitrified atmosphere. Estimates of chemical ozone loss were derived using passive ozone from the SLIMCAT offline chemical transport model to account for dynamical contributions to the stratospheric ozone budget.</p>


2017 ◽  
Author(s):  
Farahnaz Khosrawi ◽  
Oliver Kirner ◽  
Björn-Martin Sinnhuber ◽  
Sören Johansson ◽  
Michael Höpfner ◽  
...  

Abstract. The Arctic winter 2015/2016 was one of the coldest stratospheric winters in recent years. A stable vortex formed by early December and the early winter was exceptionally cold. Cold pool temperatures dropped below the Nitric Acid Trihydrate (NAT) existence temperature of about 195 K, thus allowing Polar Stratospheric Clouds (PSCs) to form. The low temperatures in the polar stratosphere persisted until early March allowing chlorine activation and catalytic ozone destruction. Satellite observations indicate that sedimentation of PSC particles led to denitrification as well as dehydration of stratospheric layers. Model simulations of the Arctic winter 2015/2016 nudged toward European Center for Medium-Range Weather Forecasts (ECMWF) analyses data were performed with the atmospheric chemistry–climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC) for the Polar Stratosphere in a Changing Climate (POLSTRACC) campaign. POLSTRACC is a High Altitude and LOng Range Research Aircraft (HALO) mission aimed at the investigation of the structure, composition and evolution of the Arctic Upper Troposphere and Lower Stratosphere (UTLS). The chemical and physical processes involved in Arctic stratospheric ozone depletion, transport and mixing processes in the UTLS at high latitudes, polar stratospheric clouds as well as cirrus clouds are investigated. In this study an overview of the chemistry and dynamics of the Arctic winter 2015/2016 as simulated with EMAC is given. Further, chemical-dynamical processes such as denitrification, dehydration and ozone loss during the Arctic winter 2015/2016 are investigated. Comparisons to satellite observations by the Aura Microwave Limb Sounder (Aura/MLS) as well as to airborne measurements with the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) performed on board of HALO during the POLSTRACC campaign show that the EMAC simulations are in fairly good agreement with observations. We derive a maximum polar stratospheric O3 loss of ~ 2 ppmv or 100 DU in terms of column in mid March. The stratosphere was denitrified by about 8 ppbv HNO3 and dehydrated by about 1 ppmv H2O in mid to end of February. While ozone loss was quite strong, but not as strong as in 2010/2011, denitrification and dehydration were so far the strongest observed in the Arctic stratosphere in the at least past 10 years.


2017 ◽  
Author(s):  
Alexander D. James ◽  
James S. A. Brooke ◽  
Thomas P. Mangan ◽  
Thomas F. Whale ◽  
John M. C. Plane ◽  
...  

Abstract. Heterogeneous nucleation of crystalline nitric acid hydrates in Polar Stratospheric Clouds (PSCs) enhances ozone depletion. However, the identity and mode of action of the particles responsible for nucleation remains unknown. It has been suggested that meteoric material may trigger nucleation of nitric acid trihydrate (NAT), but this has never been directly demonstrated in the laboratory. Meteoric material is present in two forms in the stratosphere, smoke which results from the ablation and re-condensation of vapours, and fragments which result from the disruption of meteoroids entering the atmosphere. Here we show that analogues of both materials have a capacity to nucleate nitric acid hydrates. In combination with estimates from a global model of the amount of meteoric smoke and fragments in the polar stratosphere we show that meteoric material probably accounts for NAT observations in early season polar stratospheric clouds in the absence of water ice.


2006 ◽  
Vol 426 (1-3) ◽  
pp. 20-25 ◽  
Author(s):  
Anas Al Natsheh ◽  
Alexey B. Nadykto ◽  
Kurt V. Mikkelsen ◽  
Fangqun Yu ◽  
Juhani Ruuskanen

2018 ◽  
Vol 18 (7) ◽  
pp. 4519-4531 ◽  
Author(s):  
Alexander D. James ◽  
James S. A. Brooke ◽  
Thomas P. Mangan ◽  
Thomas F. Whale ◽  
John M. C. Plane ◽  
...  

Abstract. Heterogeneous nucleation of crystalline nitric acid hydrates in polar stratospheric clouds (PSCs) enhances ozone depletion. However, the identity and mode of action of the particles responsible for nucleation remains unknown. It has been suggested that meteoric material may trigger nucleation of nitric acid trihydrate (NAT, or other nitric acid phases), but this has never been quantitatively demonstrated in the laboratory. Meteoric material is present in two forms in the stratosphere: smoke that results from the ablation and re-condensation of vapours, and fragments that result from the break-up of meteoroids entering the atmosphere. Here we show that analogues of both materials have a capacity to nucleate nitric acid hydrates. In combination with estimates from a global model of the amount of meteoric smoke and fragments in the polar stratosphere we show that meteoric material probably accounts for NAT observations in early season polar stratospheric clouds in the absence of water ice.


1994 ◽  
Vol 12 (4) ◽  
pp. 342-354 ◽  
Author(s):  
M. P. Chipperfield

Abstract. A three-dimensional transport model has been used to compare and contrast the extent of processing by polar stratospheric clouds during the northern hemisphere winters of 1991/1992 and 1992/1993. The model has also been used to compare the potential for ozone loss between these two winters. The TOMCAT off-line model is forced using meteorological analyses from the ECMWF. During winter 1992/1993 polar stratospheric clouds (PSCs) in the model persisted into late February/early March, which is much later than in 1991/1992. This persistence of PSCs should have resulted in much more ozone loss in the later winter. Interestingly, however, the extent of PSC processing and ozone loss was greater in January 1992 than January 1993. In January 1992 PSCs occurred at the edge of a distorted polar vortex whilst in January 1993 the PSCs were located at the centre of a much more zonally symmetrical vortex. In March 1993, distortions of the vortex led to the tearing off of vortex air and its mixing into midlatitudes.


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