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Susan Solomon - One of the best experts on this subject based on the ideXlab platform.
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simulation of Polar ozone depletion an update
Journal of Geophysical Research, 2015Co-Authors: Susan Solomon, D E Kinnison, Justin Bandoro, Rolando R GarciaAbstract:We evaluate Polar ozone depletion chemistry using the specified dynamics version of the Whole Atmosphere Community Climate Model for the year 2011. We find that total ozone depletion in both hemispheres is dependent on cold temperatures (below 192 K) and associated heterogeneous chemistry on Polar Stratospheric Cloud particles. Reactions limited to warmer temperatures above 192 K, or on binary liquid aerosols, yield little modeled Polar ozone depletion in either hemisphere. An imposed factor of three enhancement in Stratospheric sulfate increases ozone loss by up to 20 Dobson unit (DU) in the Antarctic and 15 DU in the Arctic in this model. Such enhanced sulfate loads are similar to those observed following recent relatively small volcanic eruptions since 2005 and imply impacts on the search for Polar ozone recovery. Ozone losses are strongly sensitive to temperature, with a test case cooler by 2 K producing as much as 30 DU additional ozone loss in the Antarctic and 40 DU in the Arctic. A new finding of this paper is the use of the temporal behavior and variability of ClONO2 and HCl as indicators of the efficacy of heterogeneous chemistry. Transport of ClONO2 from the southern subPolar regions near 55–65°S to higher latitudes near 65–75°S provides a flux of NOx from more sunlit latitudes to the edge of the vortex and is important for ozone loss in this model. Comparisons between modeled and observed total column and profile ozone perturbations, ClONO2 abundances, and the rate of change of HCl bolster confidence in these conclusions.
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fundamental differences between arctic and antarctic ozone depletion
Proceedings of the National Academy of Sciences of the United States of America, 2014Co-Authors: Susan Solomon, Diane J. Ivy, J Haskins, Flora MinAbstract:Antarctic ozone depletion is associated with enhanced chlorine from anthropogenic chlorofluorocarbons and heterogeneous chemistry under cold conditions. The deep Antarctic “hole” contrasts with the generally weaker depletions observed in the warmer Arctic. An unusually cold Arctic Stratospheric season occurred in 2011, raising the question of how the Arctic ozone chemistry in that year compares with others. We show that the averaged depletions near 20 km across the cold part of each pole are deeper in Antarctica than in the Arctic for all years, although 2011 Arctic values do rival those seen in less-depleted years in Antarctica. We focus not only on averages but also on extremes, to address whether or not Arctic ozone depletion can be as extreme as that observed in the Antarctic. This information provides unique insights into the contrasts between Arctic and Antarctic ozone chemistry. We show that extreme Antarctic ozone minima fall to or below 0.1 parts per million by volume (ppmv) at 18 and 20 km (about 70 and 50 mbar) whereas the lowest Arctic ozone values are about 0.5 ppmv at these altitudes. At a higher altitude of 24 km (30-mbar level), no Arctic data below about 2 ppmv have been observed, including in 2011, in contrast to values more than an order of magnitude lower in Antarctica. The data show that the lowest ozone values are associated with temperatures below −80 °C to −85 °C depending upon altitude, and are closely associated with reduced gaseous nitric acid concentrations due to uptake and/or sedimentation in Polar Stratospheric Cloud particles.
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heterogeneous reactions on Stratospheric background aerosols volcanic sulfuric acid droplets and type i Polar Stratospheric Clouds effects of temperature fluctuations and differences in particle phase
Journal of Geophysical Research, 1997Co-Authors: Stephan Borrmann, Susan Solomon, K K Kelly, James E Dye, D Baumgardner, Roland K ChanAbstract:Northern hemispheric ER-2 (NASA) data from Stratospheric aerosol measurements during background conditions, periods disturbed by the influence of Mount Pinatubo, and Polar Stratospheric Cloud (PSC) type I events are used to study the heterogeneous reactions of ClONO2 with H2O and of HOCl and ClONO2 with HCl in comparison to the gas phase reaction rate of OH with HCl. To calculate the reaction rates, the measured data of pressure, temperature, water vapor, and aerosol surface are utilized together with recent laboratory results for the heterogeneous reactive uptake coefficients. Because observations are limited, the mixing ratios of the gas phase species entering these rate calculations (i.e., ClONO2, HOCl, HCl, and N2O5) are taken from a two-dimensional model. It is found that in dense volcanic Clouds at temperatures below 200 K the resulting heterogeneous reaction rates of chlorine activation can be of similar magnitude as the gas phase reaction rate. The heterogeneous rates in PSCs can exceed the gas phase rates by more than 2 orders of magnitude. For the ClONO2 and HOCl reactions the measured aerosol surfaces during the PSC events are treated both as liquid (e.g., ternary solution) droplets and as solid NAT to compare the effects of the different phases. The reaction rates on NAT are significantly lower than on liquid droplets. Indeed, this study shows that a transition from liquid ternary solutions to NAT is expected to reduce the rate of chlorine activation based on present chemical understanding and on observed aerosol surface areas. Additionally, the effect of temperature and surface area fluctuations on the heterogeneous reaction rates is discussed.
M. C. Pitts - One of the best experts on this subject based on the ideXlab platform.
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Polar Stratospheric Cloud climatology based on CALIPSO spaceborne lidar measurements from 2006 to 2017
Copernicus Publications, 2018Co-Authors: M. C. Pitts, L. R. Poole, R. GonzalezAbstract:The Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) on the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) satellite has been observing Polar Stratospheric Clouds (PSCs) from mid-June 2006 until the present. The spaceborne lidar profiles PSCs with unprecedented spatial (5 km horizontal × 180 m vertical) resolution and its dual-Polarization capability enables classification of PSCs according to composition. Nearly coincident Aura Microwave Limb Sounder (MLS) measurements of the primary PSC condensables (HNO3 and H2O) provide additional constraints on particle composition. A new CALIOP version 2 (v2) PSC detection and composition classification algorithm has been implemented that corrects known deficiencies in previous algorithms and includes additional refinements to improve composition discrimination. Major v2 enhancements include dynamic adjustment of composition boundaries to account for effects of denitrification and dehydration, explicit use of measurement uncertainties, addition of composition confidence indices, and retrieval of particulate backscatter, which enables simplified estimates of particulate surface area density (SAD) and volume density (VD). The over 11 years of CALIOP PSC observations in each v2 composition class conform to their expected thermodynamic existence regimes, which is consistent with previous analyses of data from 2006 to 2011 and underscores the robustness of the v2 composition discrimination approach.The v2 algorithm has been applied to the CALIOP dataset to produce a PSC reference data record spanning the 2006–2017 time period, which is the foundation for a new comprehensive, high-resolution climatology of PSC occurrence and composition for both the Antarctic and Arctic. Time series of daily-averaged, vortex-wide PSC areal coverage versus altitude illustrate that Antarctic PSC seasons are similar from year to year, with about 25 % relative standard deviation in Antarctic PSC spatial volume at the peak of the season in July and August. Multi-year average, monthly zonal mean cross sections depict the climatological patterns of Antarctic PSC occurrence in latitude–altitude and also equivalent-latitude–potential-temperature coordinate systems, with the latter system better capturing the microphysical processes controlling PSC existence. Polar maps of the multi-year mean geographical patterns in PSC occurrence frequency show a climatological maximum between longitudes 90° W and 0°, which is the preferential region for forcing by orography and upper tropospheric anticyclones. The climatological mean distributions of particulate SAD and VD also show maxima in this region due to the large enhancements from the frequent ice Clouds.Stronger wave activity in the Northern Hemisphere leads to a more disturbed Arctic Polar vortex, whose evolution and lifetime vary significantly from year to year. Accordingly, Arctic PSC areal coverage is distinct from year to year with no typical year, and the relative standard deviation in Arctic PSC spatial volume is > 100 % throughout most of the season. When PSCs are present in the Arctic, they most likely occur between longitudes 60° W and 90° E, which is consistent with the preferential location of the Arctic vortex.Comparisons of CALIOP v2 and Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) Antarctic PSC observations show excellent correspondence in the overall spatial and temporal evolution, as well as for different PSC composition classes. Climatological patterns of CALIOP v2 PSC occurrence frequency in the vicinity of McMurdo Station, Antarctica, and Ny-Ålesund, Spitsbergen, are similar in nature to those derived from local ground-based lidar measurements. To investigate the possibility of longer-term trends, appropriately subsampled and averaged CALIOP v2 PSC observations from 2006 to 2017 were compared with PSC data during the 1978–1989 period obtained by the spaceborne solar occultation instrument SAM II (Stratospheric Aerosol Measurement II). There was good consistency between the two instruments in column Antarctic PSC occurrence frequency, suggesting that there has been no long-term trend. There was less overall consistency between the Arctic records, but it is very likely due to the high degree of interannual variability in PSCs rather than a long-term trend.
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development of a Polar Stratospheric Cloud model within the community earth system model assessment of 2010 antarctic winter
Journal of Geophysical Research, 2017Co-Authors: Yunqian Zhu, Owen B Toon, A Lambert, Douglas E Kinnison, Charles G Bardeen, M. C. PittsAbstract:To simulate Polar Stratospheric Clouds (PSCs) during the Antarctic winter of 2010, we have developed a PSC model within the Community Earth System Model framework that includes detailed microphysics of sulfuric aerosols and three types of PSCs: supercooled ternary solution (STS), nitric acid trihydrate (NAT) and ice. Our model includes two major NAT formation mechanisms both of which are essential to reproduce the PSC and gas phase chemical features in the 2010 Antarctic winter. Homogeneous nucleation of NAT from STS produces NAT particles with sizes near 8 μm, which are important to properly simulate denitrification and the gas phase HNO3 observed by the Microwave Limb Sounder (MLS). Heterogeneous nucleation of NAT on ice particles or ice particles on NAT and subsequent evaporation of the ice produces NAT particles with sizes from sub-micrometers to a few micrometers. These particles account for the large backscattering ratio from NAT observed by the CALIPSO satellite, especially in the mid-winter season. Adding temperature fluctuations from gravity waves is important to produce larger number density and higher backscattering ratio from ice and NAT particles. However, our model needs a better representation of waves to improve the backscattering ratio and gas phase HNO3 compared with observations. Our model also includes homogeneous nucleation of ice from STS and heterogeneous nucleation of ice on NAT. The model reproduces the gas phase H2O during the winter within the uncertainty of the MLS observations.
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The effect of orographic gravity waves on Antarctic Polar Stratospheric Cloud occurrence and composition
Journal of Geophysical Research Atmospheres, 2011Co-Authors: S. P. Alexander, Ar Klekociuk, M. C. Pitts, A J Mcdonald, A. Arevalo-torresAbstract:A seasonal analysis of the relationship between mesoscale orographic gravity wave activity and Polar Stratospheric Cloud (PSC) composition occurrence around the whole of Antarctica is presented. Gravity wave variances are derived from temperature measurements made with the Constellation Observing System for Meteorology, Ionosphere and Climate (COSMIC) Global Positioning System Radio Occultation (GPS-RO) satellites. Data from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument onboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite are used to determine the PSC composition class distribution and spatial volume. The results show intermittent large wave activity above the Antarctic Peninsula which is coincident with large volumes of H2O ice PSCs. These ice PSC volumes advect downstream, where increases in nitric acid trihydrate (NAT) PSC volumes occur, supporting the mountain wave seeding hypothesis. During winter 2007 in the latitude range 60°S–70°S, near the edge of the vortex and where temperatures are close to PSC formation thresholds, 30% of all PSCs are attributable to orographic gravity waves. In the separate composition classes, around 50% of both H2O ice PSCs and a high NAT number density liquid–NAT mixture class of PSCs are due to these waves. While we show that planetary waves are the major determinant of PSC presence at temperatures close to the NAT formation threshold, we also demonstrate the important role of mesoscale, intermittent orographic gravity wave activity in accounting for the composition and distribution of PSCs around Antarctica.
Michael C Pitts - One of the best experts on this subject based on the ideXlab platform.
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Polar processing in a split vortex arctic ozone loss in early winter 2012 2013
Atmospheric Chemistry and Physics, 2015Co-Authors: Gloria L Manney, A Lambert, M L Santee, Zachary D Lawrence, N J Livesey, Michael C PittsAbstract:Abstract. A sudden Stratospheric warming (SSW) in early January 2013 caused the Arctic Polar vortex to split and temperatures to rapidly rise above the threshold for chlorine activation. However, ozone in the lower Stratospheric Polar vortex from late December 2012 through early February 2013 reached the lowest values on record for that time of year. Analysis of Aura Microwave Limb Sounder (MLS) trace gas measurements and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) Polar Stratospheric Cloud (PSC) data shows that exceptional chemical ozone loss early in the 2012/13 Arctic winter resulted from a unique combination of meteorological conditions associated with the early-January 2013 SSW: unusually low temperatures in December 2012, offspring vortices within which air remained well isolated for nearly 1 month after the vortex split, and greater-than-usual vortex sunlight exposure throughout December 2012 and January 2013. Conditions in the two offspring vortices differed substantially, with the one overlying Canada having lower temperatures, lower nitric acid (HNO3), lower hydrogen chloride, more sunlight exposure/higher ClO in late January, and a later onset of chlorine deactivation than the one overlying Siberia. MLS HNO3 and CALIPSO data indicate that PSC activity in December 2012 was more extensive and persistent than at that time in any other Arctic winter in the past decade. Chlorine monoxide (ClO, measured by MLS) rose earlier than previously observed and was the largest on record through mid-January 2013. Enhanced vortex ClO persisted until mid-February despite the cessation of PSC activity when the SSW started. Vortex HNO3 remained depressed after PSCs had disappeared; passive transport calculations indicate vortex-averaged denitrification of about 4 parts per billion by volume. The estimated vortex-averaged chemical ozone loss, ~ 0.7–0.8 parts per million by volume near 500 K (~21 km), was the largest December/January loss in the MLS record from 2004/05 to 2014/15.
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the 2009 2010 arctic Polar Stratospheric Cloud season a calipso perspective
Atmospheric Chemistry and Physics, 2011Co-Authors: Michael C Pitts, Lamont R Poole, Andreas Dornbrack, L W ThomasonAbstract:Abstract. Spaceborne lidar measurements from CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) are used to provide a vortex-wide perspective of the 2009–2010 Arctic PSC (Polar Stratospheric Cloud) season to complement more focused measurements from the European Union RECONCILE (reconciliation of essential process parameters for an enhanced predictability of Arctic Stratospheric ozone loss and its climate interactions) field campaign. The 2009–2010 Arctic winter was unusually cold at Stratospheric levels from mid-December 2009 until the end of January 2010, and was one of only a few winters from the past fifty-two years with synoptic-scale regions of temperatures below the frost point. More PSCs were observed by CALIPSO during the 2009–2010 Arctic winter than in the previous three Arctic seasons combined. In particular, there were significantly more observations of high number density NAT (nitric acid trihydrate) mixtures (referred to as Mix 2-enh) and ice PSCs. We found that the 2009–2010 season could roughly be divided into four periods with distinctly different PSC optical characteristics. The early season (15–30 December 2009) was characterized by patchy, tenuous PSCs, primarily low number density liquid/NAT mixtures. No ice Clouds were observed by CALIPSO during this early phase, suggesting that these early season NAT Clouds were formed through a non-ice nucleation mechanism. The second phase of the season (31 December 2009–14 January 2010) was characterized by frequent mountain wave ice Clouds that nucleated widespread NAT particles throughout the vortex, including Mix 2-enh. The third phase of the season (15–21 January 2010) was characterized by synoptic-scale temperatures below the frost point which led to a rare outbreak of widespread ice Clouds. The fourth phase of the season (22–28 January) was characterized by a major Stratospheric warming that distorted the vortex, displacing the cold pool from the vortex center. This final phase was dominated by STS (supercooled ternary solution) PSCs, although NAT particles may have been present in low number densities, but were masked by the more abundant STS droplets at colder temperatures. We also found distinct variations in the relative proportion of PSCs in each composition class with altitude over the course of the 2009–2010 Arctic season. Lower number density liquid/NAT mixtures were most frequently observed in the lower altitude regions of the Clouds (below ~18–20 km), which is consistent with CALIPSO observations in the Antarctic. Higher number density liquid/NAT mixtures, especially Mix 2-enh, were most frequently observed at altitudes above 18–20 km, primarily downstream of wave ice Clouds. This pattern is consistent with the conceptual model whereby low number density, large NAT particles are precipitated from higher number density NAT Clouds (i.e. mother Clouds) that are nucleated downstream of mountain wave ice Clouds.
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calipso Polar Stratospheric Cloud observations second generation detection algorithm and composition discrimination
Atmospheric Chemistry and Physics, 2009Co-Authors: Michael C Pitts, Lamont R Poole, L W ThomasonAbstract:Abstract. This paper focuses on Polar Stratospheric Cloud (PSC) measurements by the CALIOP (Cloud-Aerosol LIdar with Orthogonal Polarization) lidar system onboard the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) spacecraft, which has been operating since June 2006. We describe a second-generation PSC detection algorithm that utilizes both the CALIOP 532-nm scattering ratio (ratio of total-to-molecular backscatter coefficients) and 532-nm perpendicular backscatter coefficient measurements for Cloud detection. The inclusion of the perpendicular backscatter measurements enhances the detection of tenuous PSC mixtures containing low number densities of solid (likely nitric acid trihydrate, NAT) particles and leads to about a 15% increase in PSC areal coverage compared with our original algorithm. Although these low number density NAT mixtures would have a minimal impact on chlorine activation due to their relatively small particle surface area, these particles may play a significant role in denitrification and therefore are an important component of our PSC detection. In addition, the new algorithm allows discrimination of PSCs by composition in terms of their ensemble backscatter and dePolarization in a manner analogous to that used in previous ground-based and airborne lidar PSC studies. Based on theoretical optical calculations, we define four CALIPSO-based composition classes which we call supercooled ternary solution (STS), ice, and Mix1 and Mix2, denoting mixtures of STS with NAT particles in lower or higher number densities/volumes, respectively. We examine the evolution of PSCs for three Antarctic and two Arctic seasons and illustrate the unique attributes of the CALIPSO PSC database. These analyses show substantial interannual variability in PSC areal coverage and also the well-known contrast between the Antarctic and Arctic. The CALIPSO data also reveal seasonal and altitudinal variations in Antarctic PSC composition, which are related to changes in HNO3 and H2O observed by the Microwave Limb Sounder on the Aura satellite.
A Lambert - One of the best experts on this subject based on the ideXlab platform.
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development of a Polar Stratospheric Cloud model within the community earth system model assessment of 2010 antarctic winter
Journal of Geophysical Research, 2017Co-Authors: Yunqian Zhu, Owen B Toon, A Lambert, Douglas E Kinnison, Charles G Bardeen, M. C. PittsAbstract:To simulate Polar Stratospheric Clouds (PSCs) during the Antarctic winter of 2010, we have developed a PSC model within the Community Earth System Model framework that includes detailed microphysics of sulfuric aerosols and three types of PSCs: supercooled ternary solution (STS), nitric acid trihydrate (NAT) and ice. Our model includes two major NAT formation mechanisms both of which are essential to reproduce the PSC and gas phase chemical features in the 2010 Antarctic winter. Homogeneous nucleation of NAT from STS produces NAT particles with sizes near 8 μm, which are important to properly simulate denitrification and the gas phase HNO3 observed by the Microwave Limb Sounder (MLS). Heterogeneous nucleation of NAT on ice particles or ice particles on NAT and subsequent evaporation of the ice produces NAT particles with sizes from sub-micrometers to a few micrometers. These particles account for the large backscattering ratio from NAT observed by the CALIPSO satellite, especially in the mid-winter season. Adding temperature fluctuations from gravity waves is important to produce larger number density and higher backscattering ratio from ice and NAT particles. However, our model needs a better representation of waves to improve the backscattering ratio and gas phase HNO3 compared with observations. Our model also includes homogeneous nucleation of ice from STS and heterogeneous nucleation of ice on NAT. The model reproduces the gas phase H2O during the winter within the uncertainty of the MLS observations.
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development of a Polar Stratospheric Cloud model within the community earth system model using constraints on type i pscs from the 2010 2011 arctic winter
Journal of Advances in Modeling Earth Systems, 2015Co-Authors: Yunqian Zhu, Owen B Toon, A Lambert, Douglas E Kinnison, Charles G Bardeen, Matthias Brakebusch, Michael J Mills, Jason M EnglishAbstract:Polar Stratospheric Clouds (PSCs) are critical elements of Arctic and Antarctic ozone depletion. We establish a PSC microphysics model using coupled chemistry, climate, and microphysics models driven by specific dynamics. We explore the microphysical formation and evolution of STS (Supercooled Ternary Solution) and NAT (Nitric Acid Trihydrate). Characteristics of STS particles dominated by thermodynamics compare well with observations. For example, the mass of STS is close to the thermodynamic equilibrium assumption when the particle surface area is >4 µm2/cm3. We derive a new nucleation rate equation for NAT based on observed denitrification in the 2010–2011 Arctic winter. The homogeneous nucleation scheme leads to supermicron NAT particles as observed. We also find that as the number density of NAT particles increases, the denitrification also increases. Simulations of the PSC lidar backscatter, denitrification, and gas phase species are generally within error bars of the observations. However, the simulations are very sensitive to temperature, which limits our ability to fully constrain some parameters (e.g., denitrification, ozone amount) based on observations.
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Polar processing in a split vortex arctic ozone loss in early winter 2012 2013
Atmospheric Chemistry and Physics, 2015Co-Authors: Gloria L Manney, A Lambert, M L Santee, Zachary D Lawrence, N J Livesey, Michael C PittsAbstract:Abstract. A sudden Stratospheric warming (SSW) in early January 2013 caused the Arctic Polar vortex to split and temperatures to rapidly rise above the threshold for chlorine activation. However, ozone in the lower Stratospheric Polar vortex from late December 2012 through early February 2013 reached the lowest values on record for that time of year. Analysis of Aura Microwave Limb Sounder (MLS) trace gas measurements and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) Polar Stratospheric Cloud (PSC) data shows that exceptional chemical ozone loss early in the 2012/13 Arctic winter resulted from a unique combination of meteorological conditions associated with the early-January 2013 SSW: unusually low temperatures in December 2012, offspring vortices within which air remained well isolated for nearly 1 month after the vortex split, and greater-than-usual vortex sunlight exposure throughout December 2012 and January 2013. Conditions in the two offspring vortices differed substantially, with the one overlying Canada having lower temperatures, lower nitric acid (HNO3), lower hydrogen chloride, more sunlight exposure/higher ClO in late January, and a later onset of chlorine deactivation than the one overlying Siberia. MLS HNO3 and CALIPSO data indicate that PSC activity in December 2012 was more extensive and persistent than at that time in any other Arctic winter in the past decade. Chlorine monoxide (ClO, measured by MLS) rose earlier than previously observed and was the largest on record through mid-January 2013. Enhanced vortex ClO persisted until mid-February despite the cessation of PSC activity when the SSW started. Vortex HNO3 remained depressed after PSCs had disappeared; passive transport calculations indicate vortex-averaged denitrification of about 4 parts per billion by volume. The estimated vortex-averaged chemical ozone loss, ~ 0.7–0.8 parts per million by volume near 500 K (~21 km), was the largest December/January loss in the MLS record from 2004/05 to 2014/15.
Yunqian Zhu - One of the best experts on this subject based on the ideXlab platform.
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development of a Polar Stratospheric Cloud model within the community earth system model assessment of 2010 antarctic winter
Journal of Geophysical Research, 2017Co-Authors: Yunqian Zhu, Owen B Toon, A Lambert, Douglas E Kinnison, Charles G Bardeen, M. C. PittsAbstract:To simulate Polar Stratospheric Clouds (PSCs) during the Antarctic winter of 2010, we have developed a PSC model within the Community Earth System Model framework that includes detailed microphysics of sulfuric aerosols and three types of PSCs: supercooled ternary solution (STS), nitric acid trihydrate (NAT) and ice. Our model includes two major NAT formation mechanisms both of which are essential to reproduce the PSC and gas phase chemical features in the 2010 Antarctic winter. Homogeneous nucleation of NAT from STS produces NAT particles with sizes near 8 μm, which are important to properly simulate denitrification and the gas phase HNO3 observed by the Microwave Limb Sounder (MLS). Heterogeneous nucleation of NAT on ice particles or ice particles on NAT and subsequent evaporation of the ice produces NAT particles with sizes from sub-micrometers to a few micrometers. These particles account for the large backscattering ratio from NAT observed by the CALIPSO satellite, especially in the mid-winter season. Adding temperature fluctuations from gravity waves is important to produce larger number density and higher backscattering ratio from ice and NAT particles. However, our model needs a better representation of waves to improve the backscattering ratio and gas phase HNO3 compared with observations. Our model also includes homogeneous nucleation of ice from STS and heterogeneous nucleation of ice on NAT. The model reproduces the gas phase H2O during the winter within the uncertainty of the MLS observations.
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development of a Polar Stratospheric Cloud model within the community earth system model using constraints on type i pscs from the 2010 2011 arctic winter
Journal of Advances in Modeling Earth Systems, 2015Co-Authors: Yunqian Zhu, Owen B Toon, A Lambert, Douglas E Kinnison, Charles G Bardeen, Matthias Brakebusch, Michael J Mills, Jason M EnglishAbstract:Polar Stratospheric Clouds (PSCs) are critical elements of Arctic and Antarctic ozone depletion. We establish a PSC microphysics model using coupled chemistry, climate, and microphysics models driven by specific dynamics. We explore the microphysical formation and evolution of STS (Supercooled Ternary Solution) and NAT (Nitric Acid Trihydrate). Characteristics of STS particles dominated by thermodynamics compare well with observations. For example, the mass of STS is close to the thermodynamic equilibrium assumption when the particle surface area is >4 µm2/cm3. We derive a new nucleation rate equation for NAT based on observed denitrification in the 2010–2011 Arctic winter. The homogeneous nucleation scheme leads to supermicron NAT particles as observed. We also find that as the number density of NAT particles increases, the denitrification also increases. Simulations of the PSC lidar backscatter, denitrification, and gas phase species are generally within error bars of the observations. However, the simulations are very sensitive to temperature, which limits our ability to fully constrain some parameters (e.g., denitrification, ozone amount) based on observations.
