A closer look at Arctic ozone loss and polar stratospheric clouds

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.

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A closer look at Arctic ozone loss and polar stratospheric clouds

Atmospheric Chemistry and Physics ◽

10.5194/acp-10-8499-2010 ◽

2010 ◽

Vol 10 (17) ◽

pp. 8499-8510 ◽

Cited By ~ 35

Author(s):

N. R. P. Harris ◽

R. Lehmann ◽

M. Rex ◽

P. von der Gathen

Keyword(s):

Nitric Acid ◽

Climate Models ◽

Empirical Relationship ◽

Early Spring ◽

Aerosol Formation ◽

Polar Stratospheric Clouds ◽

Ozone Loss ◽

Relationship Analysis ◽

Near Ultraviolet ◽

Stratospheric Clouds

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.

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Observations and analysis of polar stratospheric clouds detected by POAM III and SAGE III during the SOLVE II/VINTERSOL campaign in the 2002/2003 Northern Hemisphere winter

Atmospheric Chemistry and Physics ◽

10.5194/acp-7-2151-2007 ◽

2007 ◽

Vol 7 (9) ◽

pp. 2151-2163 ◽

Cited By ~ 10

Author(s):

J. Alfred ◽

M. Fromm ◽

R. Bevilacqua ◽

G. Nedoluha ◽

A. Strawa ◽

...

Keyword(s):

Nitric Acid ◽

Northern Hemisphere ◽

Potential Temperature ◽

Stratospheric Aerosol ◽

Polar Stratospheric Clouds ◽

Ozone Loss ◽

Temperature Ranges ◽

Hemisphere Winter ◽

Stratospheric Clouds ◽

Northern Hemisphere Winter

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.

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Record springtime stratospheric ozone depletion at 80°N in 2020

10.5194/egusphere-egu21-8892 ◽

2021 ◽

Author(s):

Ramina Alwarda ◽

Kristof Bognar ◽

Kimberly Strong ◽

Martyn Chipperfield ◽

Sandip Dhomse ◽

...

Keyword(s):

Ozone Depletion ◽

Transport Model ◽

Stratospheric Ozone ◽

Polar Vortex ◽

The Arctic ◽

Optical Absorption Spectroscopy ◽

Chemical Transport Model ◽

Polar Stratospheric Clouds ◽

Ozone Loss ◽

Stratospheric Clouds

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&#176;N, 86.42&#176;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 NO2 during spring, as well as enhanced reactive halogen species (OClO and BrO). Complementary measurements of HCl and ClONO2 (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 HNO3 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.

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Denitrification, dehydration and ozone loss during the Arctic winter 2015/2016

10.5194/acp-2017-503 ◽

2017 ◽

Cited By ~ 3

Author(s):

Farahnaz Khosrawi ◽

Oliver Kirner ◽

Björn-Martin Sinnhuber ◽

Sören Johansson ◽

Michael Höpfner ◽

...

Keyword(s):

Atmospheric Chemistry ◽

Stratospheric Ozone ◽

Satellite Observations ◽

The Arctic ◽

Cold Pool ◽

Polar Stratospheric Clouds ◽

Airborne Measurements ◽

Ozone Loss ◽

Polar Stratosphere ◽

Stratospheric Clouds

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.

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Nucleation of nitric acid hydrates in Polar Stratospheric Clouds by meteoric material

10.5194/acp-2017-816 ◽

2017 ◽

Cited By ~ 1

Author(s):

Alexander D. James ◽

James S. A. Brooke ◽

Thomas P. Mangan ◽

Thomas F. Whale ◽

John M. C. Plane ◽

...

Keyword(s):

Nitric Acid ◽

Heterogeneous Nucleation ◽

Ozone Depletion ◽

Mode Of Action ◽

Polar Stratospheric Clouds ◽

Water Ice ◽

Meteoric Smoke ◽

Polar Stratosphere ◽

Stratospheric Clouds ◽

Meteoric Material

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.

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Polar processing in a split vortex: early winter Arctic ozone loss in 2012/13

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-15-4973-2015 ◽

2015 ◽

Vol 15 (4) ◽

pp. 4973-5029 ◽

Cited By ~ 3

Author(s):

G. L. Manney ◽

Z. D. Lawrence ◽

M. L. Santee ◽

N. J. Livesey ◽

A. Lambert ◽

...

Keyword(s):

Nitric Acid ◽

Lower Stratosphere ◽

Polar Vortex ◽

The Arctic ◽

Early Winter ◽

Sudden Stratospheric Warming ◽

Ozone Loss ◽

Chlorine Monoxide ◽

Polar Stratospheric Cloud ◽

Vortex Split

Abstract. A sudden stratospheric warming (SSW) in early January 2013 caused the polar vortex to split. After the lower stratospheric vortex split on 8 January, the two offspring vortices – one over Canada and the other over Siberia – remained intact, well-confined, and largely at latitudes that received sunlight until they reunited at the end of January. As the SSW began, temperatures abruptly rose above chlorine activation thresholds throughout the lower stratosphere. The vortex was very disturbed prior to the SSW, and was exposed to much more sunlight than usual in December 2012 and January 2013. Aura Microwave Limb Sounder (MLS) nitric acid (HNO3) data and observations from CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) indicate extensive polar stratospheric cloud (PSC) activity, with evidence of PSCs containing solid nitric acid trihydrate particles during much of December 2012. Consistent with the sunlight exposure and PSC activity, MLS observations show that chlorine monoxide (ClO) became enhanced early in December. Despite the cessation of PSC activity with the onset of the SSW, enhanced vortex ClO persisted until mid-February, indicating lingering chlorine activation. The smaller Canadian offspring vortex had lower temperatures, lower HNO3, lower hydrogen chloride (HCl), and higher ClO in late January than the Siberian vortex. Chlorine deactivation began later in the Canadian than in the Siberian vortex. HNO3 remained depressed within the vortices after temperatures rose above the PSC existence threshold, and passive transport calculations indicate vortex-averaged denitrification of about 4 ppbv; the resulting low HNO3 values persisted until the vortex dissipated in mid-February. Consistent with the strong chlorine activation and exposure to sunlight, MLS measurements show rapid ozone loss commencing in mid-December and continuing through January. Lagrangian transport estimates suggest ~ 0.7–0.8 ppmv (parts per million by volume) vortex-averaged chemical ozone loss by late January near 500 K (~ 21 km), with substantial loss occurring from ~ 450 to 550 K. The surface area of PSCs in December 2012 was larger than that in any other December observed by CALIPSO. As a result of denitrification, HNO3 abundances in 2012/13 were among the lowest in the MLS record for the Arctic. ClO enhancement was much greater in December 2012 through mid-January 2013 than that at the corresponding time in any other Arctic winter observed by MLS. Furthermore, reformation of HCl appeared to play a greater role in chlorine deactivation than in more typical Arctic winters. Ozone loss in December 2012 and January 2013 was larger than any previously observed in those months. This pattern of exceptional early winter polar processing and ozone loss resulted from the unique combination of dynamical conditions associated with the early January 2013 SSW, namely unusually low temperatures in December 2012 and offspring vortices that remained well-confined and largely in sunlit regions for about a month after the vortex split.

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