Chemical ozone loss in the arctic polar stratosphere derived from satellite observations

In dieser Arbeit wurde der chemische Ozonverlust in der arktischen Stratosphäre über elf Jahre hinweg, zwischen 1991 und 2002, mit Hilfe der so genannten "Ozon-Tracer Korrelationstechnik" (TRAC), untersucht. Bei dieser Methode werden Korrelationen zwischen Ozon und langlebigen Spurenstoffen im Verlauf des Winters im Polarwirbels beobachtet und so der jährliche akkumulierte Ozonverlust berechnet. Die Ergebnisse dieser Arbeit basieren im wesentlichen auf Messdaten der Satelliteninstrumente: HALOE (Halogen Occultation Experiment) auf UARS (Upper Atmosphere Research Satellite) und ILAS (Improved Limb Atmospheric Spectrometer) Instrument auf ADEOS (Advanced Earth Observing Satellite). Das HALOE Instrument misst seit Oktober 1991 kontinuierlich alle zwei bis drei Monate für einige Tage in höheren nördlichen Breiten. ILAS lieferte ausschließlich für den Winter 1996-97 Messungen, die über sieben Monate hinweg in hohen Breiten aufgenommen wurden. Aufgrund der eingeführten Erweiterungen und Verbesserungen der Methode in dieser Arbeit, konnte die Methode anhand einer detaillierten Studie für den Winter 1996-97 validiert werden. Die ILAS Messreihe wurde dazu verwendet, erstmals die Untersuchung der zeitlichen Entwicklung von Ozon-Tracer Korrelationen kontinuierlich für die gesamte Lebensdauer des Polarwirbels durchzuführen. Dabei wurden auch Korrelationen während der Bildung des Wirbels untersucht und im Besonderen mögliche Mischungsvorgänge zwischen Wirbelluft und Luftmassen außerhalb des Wirbels. Ausserdem wurde ein Vergleich der Ergebnisse von ILAS und HALOE Messdaten durchgeführt und Unterschiede in den Ergebnissen tiefgreifend analysiert. Basierend auf HALOE Messungen konnte die erweiterte TRAC Methode über elf Jahren hinweg angewendet werden. Damit war erstmals eine konsistente Analyse von Ozonverlust und Chloraktivierung über diesen Zeitraum möglich. Die Erweiterungen führten zu einer Verringerung und genauen Quantifizierung von Unsicherheiten der Ergebnisse. Ein deutlicher Zusammenhang zwischen meteorologischen Bedingungen, Chloraktivierung und dem chemischen Ozonverlust wurde deutlich. Weiterhin zeigte sich eine Abhängigkeit zwischen den meteorologischen Bedingungen und der Homogenität des Ozonverlustes innerhalb eines Winters, sowie der mögliche Einfluss von horizontaler Mischung auf Luftmassen in einem schwach ausgeprägten Polarwirbel. In dieser Arbeit wurde eine positive Korrelation zwischen den über die gesamte Lebensdauer des Wirbels auftretenden möglichen PSC-Flächen und den akkumulierten Ozonverlusten für die elf untersuchten Jahre deutlich. Es konnte darüber hinaus gezeigt werden, dass der Ozonverlust von deutlich mehr Einflüssen als nur von der Fläche möglichen PSC Auftretens bestimmt wird, sondern zum Beispiel von der Stärke der Sonneneinstrahlung abhängt. Außerdem lassen sich Auswirkungen von Vulkanausbrüchen, wie zum Beispiel im Jahr 1991 der des Mount Pinatubo, identifizieren

Impact of biogenic very short-lived bromine on the Antarctic ozone hole during the 21st century

Active bromine released from the photochemical decomposition of biogenic very short-lived bromocarbons (VSL_Br ) enhances stratospheric ozone depletion. Based on a dual set of 1960-2100 coupled chemistry-climate simulations (i.e. with and without VSL Br ), we show that the maximum Antarctic ozone hole depletion increases by up to 14% when natural VSLBr are considered, in better agreement with ozone observations. The impact of the additional 5 pptv VSL Br on Antarctic ozone is most evident in the periphery of the ozone hole, producing an expansion of the ozone hole area of ~5 million km 2 , which is equivalent in magnitude to the recently estimated Antarctic ozone healing due to the implementation of the Montreal Protocol. We find that the inclusion of VSL Br in CAM-Chem does not introduce a significant delay of the modelled ozone return date to 1980 October levels, but instead affect the depth and duration of the simulated ozone hole. Our analysis further shows that total bromine-catalysed ozone destruction in the lower stratosphere surpasses that of chlorine by year 2070, and indicates that natural VSL Br chemistry would dominate Antarctic ozone seasonality before the end of the 21 st century. This work suggests a large influence of biogenic bromine on the future Antarctic ozone layer.Fil: Fernandez, Rafael Pedro. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; España. Universidad Tecnologica Nacional. Facultad Regional Mendoza. Secretaría de Ciencia, Tecnología y Postgrado; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; ArgentinaFil: Kinnison, Douglas E.. National Center For Atmospheric Research. Amospheric Chemistry División; Estados UnidosFil: Lamarque, Jean Francois. National Center For Atmospheric Research. Amospheric Chemistry División; Estados UnidosFil: Tilmes, Simone. National Center For Atmospheric Research. Amospheric Chemistry División; Estados UnidosFil: Saiz-lopez, Alfonso. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; Españ

Upper tropospheric ice sensitivity to sulfate geoengineering

Abstract. Aside from the direct surface cooling that sulfate geoengineering (SG) would produce, investigations of the possible side effects of this method are still ongoing, such as the exploration of the effect that SG may have on upper tropospheric cirrus cloudiness. The goal of the present study is to better understand the SG thermodynamical effects on the freezing mechanisms leading to ice particle formation. This is undertaken by comparing SG model simulations against a Representative Concentration Pathway 4.5 (RCP4.5) reference case. In the first case, the aerosol-driven surface cooling is included and coupled to the stratospheric warming resulting from the aerosol absorption of terrestrial and solar near-infrared radiation. In a second SG perturbed case, the surface temperatures are kept unchanged with respect to the reference RCP4.5 case. When combined, surface cooling and lower stratospheric warming tend to stabilize the atmosphere, which decreases the turbulence and updraft velocities (−10 % in our modeling study). The net effect is an induced cirrus thinning, which may then produce a significant indirect negative radiative forcing (RF). This RF would go in the same direction as the direct effect of solar radiation scattering by aerosols, and would consequently influence the amount of sulfur needed to counteract the positive RF due to greenhouse gases. In our study, given an 8 Tg-SO2 yr−1 equatorial injection into the lower stratosphere, an all-sky net tropopause RF of −1.46 W m−2 is calculated, of which −0.3 W m−2 (20 %) is from the indirect effect on cirrus thinning (6 % reduction in ice optical depth). When surface cooling is ignored, the ice optical depth reduction is lowered to 3 %, with an all-sky net tropopause RF of −1.4 W m−2, of which −0.14 W m−2 (10 %) is from cirrus thinning. Relative to the clear-sky net tropopause RF due to SG aerosols (−2.1 W m−2), the cumulative effect of the background clouds and cirrus thinning accounts for +0.6 W m−2, due to the partial compensation of large positive shortwave (+1.6 W m−2) and negative longwave adjustments (−1.0 W m−2). When surface cooling is ignored, the net cloud adjustment becomes +0.8 W m−2, with the shortwave contribution (+1.5 W m−2) almost twice as much as that of the longwave (−0.7 W m−2). This highlights the importance of including all of the dynamical feedbacks of SG aerosols

Improvement of the Prediction of Surface Ozone Concentration Over Conterminous U.S. by a Computationally Efficient Second-Order Rosenbrock Solver in CAM4-Chem

The global chemistry-climate model (CAM4-Chem) overestimates the surface ozone concentration over the conterminous U.S. (CONUS). Reasons for this positive bias include emission, meteorology, chemical mechanism, and solver. In this study, we explore the last possibility by examining the sensitivity to the numerical methods for solving the chemistry equations. A second-order Rosenbrock (ROS-2) solver is implemented in CAM4-Chem to examine its influence on the surface ozone concentration and the computational performance of the chemistry program. Results show that under the same time step size (1800 s), statistically significant reduction of positive bias is achieved by the ROS-2 solver. The improvement is as large as 5.2 ppb in Eastern U.S. during summer season. The ROS-2 solver is shown to reduce the positive bias in Europe and Asia as well, indicating the lower surface ozone concentration over the CONUS predicted by the ROS-2 solver is not a trade-off consequence with increasing the ozone concentration at other global regions. In addition, by refining the time step size to 180 s, the first-order implicit solver does not provide statistically significant improvement of surface ozone concentration. It reveals that the better prediction from the ROS-2 solver is not only due to its accuracy but also due to its suitability for stiff chemistry equations. As an added benefit, the computation cost of the ROS-2 solver is almost half of first-order implicit solver. The improved computational efficiency of the ROS-2 solver is due to the reuse of the Jacobian matrix and lower upper (LU) factorization during its multistage calculation

Impact of Stratospheric Geoengineering on Sea Surface Temperature in the Northern Gulf of Guinea

Among techniques proposed to limit global warming, there is Stratospheric Aerosol Geoengineering (SAG) which is aiming to increase Earth-atmosphere albedo by injecting sulfur dioxide into the stratosphere in order to reduce the solar radiation that reaches the earth. This study aims to assess the potential impact of SAG on Sea Surface Temperature (SST) in the Northern Gulf of Guinea and its causes using GLENS (Geoengineering Large Ensemble) simulations performed under a high anthropogenic emission scenario (RCP8.5). Here, we focus on two dynamically different regions: Sassandra Upwelling in Côte d’Ivoire (SUC, located east of Cape Palmas) and Takoradi Upwelling in Ghana (TUG, located east of Cape Three Points). Results show that in the SUC region, under climate change, there is an increase in SST (referred to as the current climate) all year long (by 1.52 °C on average) mainly due to an increase in net heat flux (lead by the decrease in longwave radiation) and also in weak vertical mixing (caused by strong stratification which dominates the vertical shear). Under SAG, SST decreases all the seasonal cycle with its maximum in December (−0.4 °C) due to a reduction in the net heat flux (caused by a diminution of solar radiation) and an increase in vertical advection (due to an increase in vertical temperature gradient and vertical velocity). In the TUG region, under climate change, SST warming is a little more intense than in the SUC region and SST changes are driven by an increase in the net heat flux and strong stratification. The cooling of the SST in TUG is similar to the SUC region, but contrary to this region, the cooling under SAG is not only explained by a decrease in the net heat flux but also by the remote forcing of wind changes at the western equatorial Atlantic

Chemical ozone loss in the Arctic winter 1991–1992

Chemical ozone loss in winter 1991–1992 is recalculated based on observations of the HALOE satellite instrument, Version 19, ER-2 aircraft measurements and balloon data. HALOE satellite observations are shown to be reliable in the lower stratosphere below 400 K, at altitudes where the measurements are most likely disturbed by the enhanced sulfate aerosol loading, as a result of the Mt.~Pinatubo eruption in June 1991. Significant chemical ozone loss (13–17 DU) is observed below 380 K from Kiruna balloon observations and HALOE satellite data between December 1991 and March 1992. For the two winters after the Mt. Pinatubo eruption, HALOE satellite observations show a stronger extent of chemical ozone loss towards lower altitudes compared to other Arctic winters between 1991 and 2003. In spite of already occurring deactivation of chlorine in March 1992, MIPAS-B and LPMA balloon observations indicate that chlorine was still activated at lower altitudes, consistent with observed chemical ozone loss occurring between February and March and April. Large chemical ozone loss of more than 70 DU in the Arctic winter 1991–1992 as calculated in earlier studies is corroborated here

Stratospheric Ozone Response in Experiments G3 and G4 of the Geoengineering Model Intercomparison Project (GeoMIP)

Geoengineering with stratospheric sulfate aerosols has been proposed as a means of temporarily cooling the planet, alleviating some of the side effects of anthropogenic CO2 emissions. However, one of the known side effects of stratospheric injections of sulfate aerosols is a decrease in stratospheric ozone. Here we show results from two general circulation models and two coupled chemistry climate models that have simulated stratospheric sulfate aerosol geoengineering as part of the Geoengineering Model Intercomparison Project (GeoMIP). Changes in photolysis rates and upwelling of ozone-poor air in the tropics reduce stratospheric ozone, suppression of the NOx cycle increases stratospheric ozone, and an increase in available surfaces for heterogeneous chemistry modulates reductions in ozone. On average, the models show a factor 20-40 increase of the sulfate aerosol surface area density (SAD) at 50 hPa in the tropics with respect to unperturbed background conditions and a factor 3-10 increase at mid-high latitudes. The net effect for a tropical injection rate of 5 Tg SO2 per year is a decrease in globally averaged ozone by 1.1-2.1 DU in the years 2040-2050 for three models which include heterogeneous chemistry on the sulfate aerosol surfaces. GISS-E2-R, a fully coupled general circulation model, performed simulations with no heterogeneous chemistry and a smaller aerosol size; it showed a decrease in ozone by 9.7 DU. After the year 2050, suppression of the NOx cycle becomes more important than destruction of ozone by ClOx, causing an increase in total stratospheric ozone. Contribution of ozone changes in this experiment to radiative forcing is 0.23 W m-2 in GISS-E2-R and less than 0.1 W m-2 in the other three models. Polar ozone depletion, due to enhanced formation of both sulfate aerosol SAD and polar stratospheric clouds, results in an average 5 percent increase in calculated surface UV-B