scholarly journals Lagrangian analysis of microphysical and chemical processes in the Antarctic stratosphere: a case study

2015 ◽  
Vol 15 (12) ◽  
pp. 6651-6665 ◽  
Author(s):  
L. Di Liberto ◽  
R. Lehmann ◽  
I. Tritscher ◽  
F. Fierli ◽  
J. L. Mercer ◽  
...  
Keyword(s):  
Surface Area ◽  
Ozone Depletion ◽  
Heterogeneous Chemistry ◽  
Relative Role ◽  
Lagrangian Analysis ◽  
Particle Sedimentation ◽  
Air Mass ◽  
Ozone Loss ◽  
The Antarctic ◽  
The Impact

Abstract. We investigated chemical and microphysical processes in the late winter in the Antarctic lower stratosphere, after the first chlorine activation and initial ozone depletion. We focused on a time interval when both further chlorine activation and ozone loss, but also chlorine deactivation, occur. We performed a comprehensive Lagrangian analysis to simulate the evolution of an air mass along a 10-day trajectory, coupling a detailed microphysical box model to a chemistry model. Model results have been compared with in situ and remote sensing measurements of particles and ozone at the start and end points of the trajectory, and satellite measurements of key chemical species and clouds along it. Different model runs have been performed to understand the relative role of solid and liquid polar stratospheric cloud (PSC) particles for the heterogeneous chemistry, and for the denitrification caused by particle sedimentation. According to model results, under the conditions investigated, ozone depletion is not affected significantly by the presence of nitric acid trihydrate (NAT) particles, as the observed depletion rate can equally well be reproduced by heterogeneous chemistry on cold liquid aerosol, with a surface area density close to background values. Under the conditions investigated, the impact of denitrification is important for the abundances of chlorine reservoirs after PSC evaporation, thus stressing the need to use appropriate microphysical models in the simulation of chlorine deactivation. We found that the effect of particle sedimentation and denitrification on the amount of ozone depletion is rather small in the case investigated. In the first part of the analyzed period, when a PSC was present in the air mass, sedimentation led to a smaller available particle surface area and less chlorine activation, and thus less ozone depletion. After the PSC evaporation, in the last 3 days of the simulation, denitrification increases ozone loss by hampering chlorine deactivation.

scholarly journals Lagrangian analysis of microphysical and chemical processes in the Antarctic stratosphere: a case study

2014 ◽  
Vol 14 (23) ◽  
pp. 32629-32665
Author(s):  
L. Di Liberto ◽  
R. Lehmann ◽  
I. Tritscher ◽  
F. Fierli ◽  
J. L. Mercer ◽  
...  
Keyword(s):  
Surface Area ◽  
Ozone Depletion ◽  
Time Interval ◽  
Heterogeneous Chemistry ◽  
Relative Role ◽  
Lagrangian Analysis ◽  
Particle Sedimentation ◽  
Ozone Loss ◽  
The Antarctic ◽  
The Impact

Abstract. We investigated chemical and microphysical processes in the late winter in the Antarctic lower stratosphere, after the first chlorine activation and initial ozone depletion. We focused on a time interval when both further chlorine activation and ozone loss, but also chlorine deactivation, occur. We performed a comprehensive Lagrangian analysis to simulate the evolution of an airmass along a ten-day trajectory, coupling a detailed microphysical box model with a chemistry model. Model results have been compared with in-situ and remote sensing measurements of particles and ozone at the start and end points of the trajectory, and satellite measurements of key chemical species and clouds along it. Different model runs have been performed to understand the relative role of solid and liquid Polar Stratospheric Cloud (PSC) particles for the heterogeneous chemistry, and for the denitrification caused by particle sedimentation. According to model results, under the conditions investigated, ozone depletion is not affected significantly by the presence of Nitric Acid Trihydrate (NAT) particles, as the observed depletion rate can equally well be reproduced by heterogeneous chemistry on cold liquid aerosol, with a surface area density close to background values. Under the conditions investigated, the impact of denitrification is important for the abundances of chlorine reservoirs after PSC evaporation, thus stressing the need of using appropriate microphysical models in the simulation of chlorine deactivation. Conversely, we found that the effect of particle sedimentation and denitrification on the amount of ozone depletion is rather small in the case investigated. In the first part of the analysed period, when a PSC was present in the airmass, sedimentation led to smaller available particle surface area and less chlorine activation, and thus less ozone depletion. After the PSC evaporation, in the last three days of the simulation, denitrification increases ozone loss by hampering chlorine deactivation.

scholarly journals Modelling the effect of denitrification on polar ozone depletion for Arctic winter/spring 2004/05

2011 ◽  
Vol 11 (2) ◽  
pp. 3857-3884 ◽  
Author(s):  
W. Feng ◽  
M. P. Chipperfield ◽  
S. Davies ◽  
G. W. Mann ◽  
K. S. Carslaw ◽  
...  
Keyword(s):  
Standard Model ◽  
Ozone Depletion ◽  
Transport Model ◽  
The Arctic ◽  
Chemical Transport Model ◽  
Particle Sedimentation ◽  
Ozone Loss ◽  
The Standard Model ◽  
The Impact ◽  
Polar Ozone

Abstract. A three-dimensional (3-D) chemical transport model (CTM), SLIMCAT, has been used to quantify the effect of denitrification on ozone loss for the Arctic winter/spring 2004/05. The simulated HNO3 is found to be highly sensitive to the polar stratospheric cloud (PSC) scheme used in the model. Here the standard SLIMCAT full chemistry model, which uses a thermodynamic equilibrium PSC scheme, overpredicts the Arctic ozone loss for Arctic winter/spring 2004/05 due to the overestimation of denitrification and stronger chlorine activation than observed. A model run with a detailed microphysical denitrification scheme, DLAPSE (Denitrification by Lagrangian Particle Sedimentation), is less denitrified than the standard model run and better reproduces the observed HNO3 as measured by Airborne SUbmillimeter Radiometer (ASUR) and Aura Microwave Limb Sounder (MLS) instruments. The overestimated denitrification causes a small overestimation of Arctic polar ozone loss (~5–10% at ~17 km) by the standard model. Use of the DLAPSE scheme improves the simulation of Arctic ozone depletion compared with the inferred partial column ozone loss from ozonesondes and satellite data. Overall, denitrification is responsible for a ~30% enhancement in O3 depletion for Arctic winter/spring 2004/05, suggesting that the successful simulation of the impact of denitrification on Arctic ozone depletion also requires the use of a detailed microphysical PSC scheme in the model.

Observational evidence of solar activity interaction with chlorine chemistry curbing Antarctic ozone loss

2021 ◽  
Author(s):  
Annika Seppälä ◽  
Emily Gordon ◽  
Bernd Funke ◽  
Johanna Tamminen ◽  
Kaley Walker
Keyword(s):  
Solar Activity ◽  
Observational Evidence ◽  
High Solar Activity ◽  
Quasi Biennial Oscillation ◽  
Ozone Loss ◽  
Reservoir Species ◽  
Antarctic Ozone ◽  
Catalytic Ozone Destruction ◽  
The Antarctic ◽  
The Impact

<p>We present the impact of the so-called energetic particle precipitation (EPP), part of natural solar forcing on the atmosphere, on polar stratospheric NO<sub>x</sub>, ozone, and chlorine chemistry in the Antarctic springtime, using multi-satellite observations covering the overall period of 2005–2017. We find consistent ozone increases when high solar activity occurs during years with easterly phase of the quasi biennial oscillation. These ozone enhancements are also present in total O<sub>3</sub> column observations. We find consistent decreases in springtime active chlorine following winters of elevated solar activity. Further analysis shows that this is accompanied by increase of chemically inactive chlorine reservoir species, explaining the observed ozone increase. This provides the first observational evidence supporting the previously proposed mechanism relating to EPP modulating chlorine driven ozone loss. Our findings suggest that solar activity via EPP has played an important role in modulating Antarctic ozone depletion in the last 15 years. As chlorine loading in the polar stratosphere continues to decrease in the future, this buffering mechanism will become less effective and catalytic ozone destruction by EPP produced NO<sub>x</sub> will likely become a major contributor to Antarctic ozone loss.</p>

scholarly journals Estimation of Antarctic ozone loss from ground-based total column measurements

2010 ◽  
Vol 10 (14) ◽  
pp. 6569-6581 ◽  
Author(s):  
J. Kuttippurath ◽  
F. Goutail ◽  
J.-P. Pommereau ◽  
F. Lefèvre ◽  
H. K. Roscoe ◽  
...  
Keyword(s):  
Ozone Depletion ◽  
Sensitivity Study ◽  
Satellite Measurements ◽  
Macquarie Island ◽  
Ozone Loss ◽  
Antarctic Ozone ◽  
The Antarctic ◽  
Ozone Column ◽  
Total Column ◽  
Good Agreement

Abstract. The passive tracer method is used to estimate ozone loss from ground-based measurements in the Antarctic. A sensitivity study shows that the ozone depletion can be estimated within an accuracy of ~4%. The method is then applied to the ground-based observations from Arrival Heights, Belgrano, Concordia, Dumont d'Urville, Faraday, Halley, Marambio, Neumayer, Rothera, South Pole, Syowa, and Zhongshan for the diagnosis of ozone loss in the Antarctic. On average, the ten-day boxcar average of the vortex mean ozone column loss deduced from the ground-based stations was about 55±5% in 2005–2009. The ozone loss computed from the ground-based measurements is in very good agreement with those derived from satellite measurements (OMI and SCIAMACHY) and model simulations (REPROBUS and SLIMCAT), where the differences are within ±3–5%. The historical ground-based total ozone observations in October show that the depletion started in the late 1970s, reached a maximum in the early 1990s and stabilised afterwards due to saturation. There is no indication of ozone recovery yet. At southern mid-latitudes, a reduction of 20–50% is observed for a few days in October–November at the newly installed Rio Gallegos station. Similar depletion of ozone is also observed episodically during the vortex overpasses at Kerguelen in October–November and at Macquarie Island in July–August of the recent winters. This illustrates the significance of measurements at the edges of Antarctica.

scholarly journals Polar tropospheric ozone depletion events observed in the International Geophysical Year of 1958

2006 ◽  
Vol 6 (11) ◽  
pp. 3303-3314 ◽  
Author(s):  
H. K. Roscoe ◽  
J. Roscoe
Keyword(s):  
Ozone Depletion ◽  
Surface Ozone ◽  
General Increase ◽  
Ozone Loss ◽  
International Geophysical Year ◽  
Obvious Reason ◽  
Frost Flowers ◽  
The Antarctic ◽  
International Geophysical

Abstract. The Royal Society expedition to Antarctica established a base at Halley Bay, in support of the International Geophysical Year of 1957–1958. Surface ozone was measured during 1958 only, using a prototype Brewer-Mast sonde. The envelope of maximum ozone was an annual cycle from 10 ppbv in January to 22 ppbv in August. These values are 35% less at the start of the year and 15% less at the end than modern values from Neumayer, also a coastal site. This may reflect a general increase in surface ozone since 1958 and differences in summer at the less windy site of Halley, or it may reflect ozone loss on the inlet together with long-term conditioning. There were short periods in September when ozone values decreased rapidly to near-zero, and some in August when ozone values were rapidly halved. Such ozone-loss episodes, catalysed by bromine compounds, became well-known in the Artic in the 1980s, and were observed more recently in the Antarctic. In 1958, very small ozone values were recorded for a week in midwinter during clear weather with light winds. The absence of similar midwinter reductions at Neumayer, or at Halley in the few measurements during 1987, means we must remain suspicious of these small values, but we can find no obvious reason to discount them. The dark reaction of ozone and seawater ice observed in the laboratory may be fast enough to explain them if the salinity and surface area of the ice is sufficiently amplified by frost flowers.

scholarly journals A Match-based approach to the estimation of polar stratospheric ozone loss using Aura Microwave Limb Sounder observations

2015 ◽  
Vol 15 (17) ◽  
pp. 9945-9963 ◽  
Author(s):  
N. J. Livesey ◽  
M. L. Santee ◽  
G. L. Manney
Keyword(s):  
Stratospheric Ozone ◽  
Potential Temperature ◽  
Polar Vortex ◽  
Rate Of Change ◽  
The Arctic ◽  
Air Mass ◽  
Ozone Loss ◽  
Chemical Destruction ◽  
Induced Changes ◽  
The Impact

Abstract. The well-established "Match" approach to quantifying chemical destruction of ozone in the polar lower stratosphere is applied to ozone observations from the Microwave Limb Sounder (MLS) on NASA's Aura spacecraft. Quantification of ozone loss requires distinguishing transport- and chemically induced changes in ozone abundance. This is accomplished in the Match approach by examining cases where trajectories indicate that the same air mass has been observed on multiple occasions. The method was pioneered using ozonesonde observations, for which hundreds of matched ozone observations per winter are typically available. The dense coverage of the MLS measurements, particularly at polar latitudes, allows matches to be made to thousands of observations each day. This study is enabled by recently developed MLS Lagrangian trajectory diagnostic (LTD) support products. Sensitivity studies indicate that the largest influence on the ozone loss estimates are the value of potential vorticity (PV) used to define the edge of the polar vortex (within which matched observations must lie) and the degree to which the PV of an air mass is allowed to vary between matched observations. Applying Match calculations to MLS observations of nitrous oxide, a long-lived tracer whose expected rate of change is negligible on the weekly to monthly timescales considered here, enables quantification of the impact of transport errors on the Match-based ozone loss estimates. Our loss estimates are generally in agreement with previous estimates for selected Arctic winters, though indicating smaller losses than many other studies. Arctic ozone losses are greatest during the 2010/11 winter, as seen in prior studies, with 2.0 ppmv (parts per million by volume) loss estimated at 450 K potential temperature (~ 18 km altitude). As expected, Antarctic winter ozone losses are consistently greater than those for the Arctic, with less interannual variability (e.g., ranging between 2.3 and 3.0 ppmv at 450 K). This study exemplifies the insights into atmospheric processes that can be obtained by applying the Match methodology to a densely sampled observation record such as that from Aura MLS.

scholarly journals Antarctic Ozone Transport and Depletion in Austral Spring 2002

2005 ◽  
Vol 62 (3) ◽  
pp. 838-847 ◽  
Author(s):  
Peter Siegmund ◽  
Henk Eskes ◽  
Peter van Velthoven
Keyword(s):  
Mass Flux ◽  
Ozone Depletion ◽  
Antarctic Region ◽  
Austral Spring ◽  
Ozone Loss ◽  
Ozone Flux ◽  
Depletion Rate ◽  
Eddy Transport ◽  
Ozone Transport ◽  
The Antarctic

Abstract The ozone budget in the Antarctic region during the stratospheric warming in 2002 is studied, using ozone analyses from the Royal Netherlands Meteorological Institute (KNMI) ozone-transport and assimilation model called TM3DAM. The results show a strong poleward ozone mass flux during this event south of 45°S between about 20 and 40 hPa, which is about 5 times as large as the ozone flux in 2001 and 2000, and is dominated by eddy transport. Above 10 hPa, there exists a partially compensating equatorward ozone flux, which is dominated by the mean meridional circulation. During this event, not only the ozone column but also the ozone depletion rate in the Antarctic region, computed as a residual from the total ozone tendency and the ozone mass flux into this region, is large. The September–October integrated ozone depletion in 2002 is similar to that in 2000 and larger than that in 2001. Simulations for September 2002 with and without ozone assimilation and parameterized ozone chemistry indicate that the parameterized ozone chemistry alone is able to produce the evolution of the ozone layer in the Antarctic region in agreement with observations. A comparison of the ozone loss directly computed from the model’s chemistry parameterization with the residual ozone loss in a simulation with parameterized chemistry but without ozone assimilation shows that the numerical error in the residual ozone loss is small.

scholarly journals Contribution of liquid, NAT and ice particles to chlorine activation and ozone depletion during Antarctic winter and spring

2014 ◽  
Vol 14 (10) ◽  
pp. 14833-14854
Author(s):  
O. Kirner ◽  
R. Müller ◽  
R. Ruhnke ◽  
H. Fischer
Keyword(s):  
Ozone Depletion ◽  
Climate Model ◽  
Heterogeneous Reactions ◽  
Heterogeneous Chemistry ◽  
Ice Particles ◽  
Reservoir Species ◽  
Almost All ◽  
Column Ozone ◽  
Open Question ◽  
The Impact

Abstract. Heterogeneous reactions in the Antarctic stratosphere are the cause of chlorine activation and ozone depletion, but the relative roles of different types of PSCs in chlorine activation is an open question. We use multi-year simulations of the chemistry-climate model EMAC to investigate the impact that the various types of PSCs have on Antarctic chlorine activation and ozone loss. One standard and three sensitivity EMAC simulations have been performed. The results of these simulations show that the significance of heterogeneous reactions on NAT and ice particles, in comparison to liquid particles, is subordinate regarding chlorine activation and ozone depletion in Antarctic winter and spring. The heterogeneous chemistry on liquid particles is sufficient to activate at least 90% of the chlorine reservoir species. With the exception of the upper PSC regions between 10 and 30 hPa where temporarily the ice particles have a relevant contribution to the chlorine activation and during the initial PSC occurrence with short NAT contributions the liquid particles alone are sufficient to activate almost all of the available chlorine. In the model simulations heterogeneous chemistry on liquid particles is responsible for more than 90% of the ozone depletion in Antarctic spring. Only up to 5 DU of column ozone in high southern latitudes is depleted by chlorine activation due to additional heterogeneous chemistry on ice particles and less than 0.5 DU due to additional heterogeneous chemistry on NAT particles.

scholarly journals Influence of the Change in Total Ozone Column (TOC) on the Occurrence of Tropospheric Ozone Depletion Events (ODEs) in the Antarctic

2021 ◽  
Author(s):  
Le Cao ◽  
Linjie Fan ◽  
Simeng Li ◽  
Shuangyan Yang
Keyword(s):  
Observational Data ◽  
Ozone Depletion ◽  
Tropospheric Ozone ◽  
Total Ozone ◽  
Numerical Models ◽  
Total Ozone Column ◽  
Speed Up ◽  
The Antarctic ◽  
The Impact ◽  
Ozone Column

Abstract. The occurrence of the tropospheric ozone depletion events (ODEs) in the Antarctic can be influenced by the change in Total Ozone Column (TOC). In this study, we combined the observational data obtained from ground observation stations with two numerical models (TUV and KINAL), to figure out the relationship between the TOC change and the occurrence of ODEs in the Antarctic. A sensitivity analysis was also performed on the change in ozone and major bromine species (BrO, HOBr and HBr) to find out key photolysis reactions determining the impact on the occurrence of tropospheric ODEs brought by the change in TOC. From the analysis of the observational data and the numerical results, we suggested that the occurrence frequency of ODEs in the Antarctic seems negatively correlated with the variation of TOC. Moreover, major ODE accelerating reactions (i.e. photolysis of ozone, H2O2 and HCHO) and decelerating reactions (i.e. photolysis of BrO and HOBr), which heavily control the start of ODEs, were also identified. It was found that when TOC varies, the major ODE accelerating reactions speed up significantly, while major ODE decelerating reactions are only slightly affected, thus leading to the negative dependence of the ODE occurrence on the change in TOC.

scholarly journals Seasonal impact of biogenic very short-lived bromocarbons on lowermost stratospheric ozone between 60° N and 60° S during the 21st century

2020 ◽  
Vol 20 (13) ◽  
pp. 8083-8102
Author(s):  
Javier Alejandro Barrera ◽  
Rafael Pedro Fernandez ◽  
Fernando Iglesias-Suarez ◽  
Carlos Alberto Cuevas ◽  
Jean-Francois Lamarque ◽  
...  
Keyword(s):  
21St Century ◽  
Ozone Depletion ◽  
Hemispheric Asymmetry ◽  
Stratospheric Ozone ◽  
Ozone Loss ◽  
Seasonal Impact ◽  
Low Sensitivity ◽  
The Tropics ◽  
The Impact ◽  
Ozone Column

Abstract. Biogenic very short-lived bromocarbons (VSLBr) currently represent ∼25 % of the total stratospheric bromine loading. Owing to their much shorter lifetime compared to anthropogenic long-lived bromine (e.g. halons) and chlorine (e.g. chlorofluorocarbons), the impact of VSLBr on ozone peaks in the lowermost stratosphere, which is a key climatic and radiative atmospheric region. Here we present a modelling study of the evolution of stratospheric ozone and its chemical loss within the tropics and at mid-latitudes during the 21st century. Two different experiments are explored: considering and neglecting the additional stratospheric injection of 5 ppt biogenic bromine naturally released from the ocean. Our analysis shows that the inclusion of VSLBr results in a realistic stratospheric bromine loading and improves the agreement between the model and satellite observations of the total ozone column (TOC) for the 1980–2015 period at mid-latitudes. We show that the overall ozone response to VSLBr at mid-latitudes follows the stratospheric evolution of long-lived inorganic chlorine and bromine throughout the 21st century. Additional ozone loss due to VSLBr is maximized during the present-day period (1990–2010), with TOC differences of −8 DU (−3 %) and −5.5 DU (−2 %) for the Southern Hemisphere and Northern Hemisphere mid-latitudes (SH-MLs and NH-MLs), respectively. Moreover, the projected TOC differences at the end of the 21st century are ∼50 % lower than the values found for the present-day period. We find that seasonal VSLBr impact on lowermost stratospheric ozone at mid-latitude is influenced by the seasonality of the heterogeneous inorganic-chlorine reactivation processes on ice crystals. Indeed, due to the more efficient reactivation of chlorine reservoirs (mainly ClONO2 and HCl) within the colder SH-ML lowermost stratosphere, the seasonal VSLBr impact shows a small but persistent hemispheric asymmetry through the whole modelled period. Our results indicate that, although the overall VSLBr-driven ozone destruction is greatest during spring, the halogen-mediated (Halogx-Loss) ozone loss cycle in the mid-latitude lowermost stratosphere during winter is comparatively more efficient than the HOx cycle with respect to other seasons. Indeed, when VSLBr are considered, Halogx-Loss dominates wintertime lowermost stratospheric ozone loss at SH-MLs between 1985 and 2020, with a contribution of inter-halogen ClOx–BrOx cycles to Halogx-Loss of ∼50 %. Within the tropics, a small (<-2.5 DU) and relatively constant (∼-1 %) ozone depletion mediated by VSLBr is closely related to their fixed emissions throughout the modelled period. By including the VSLBr sources, the seasonal Halogx-Loss contribution to lowermost stratospheric ozone loss is practically dominated by the BrOx cycle, reflecting the low sensitivity of very short-lived (VSL) bromine to background halogen abundances to drive tropical stratospheric ozone depletion. We conclude that the link between biogenic bromine sources and seasonal changes in heterogeneous chlorine reactivation is a key feature for future projections of mid-latitude lowermost stratospheric ozone during the 21st century.

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