Does Cosmic-Ray-Induced Heterogeneous Chemistry Influence Stratospheric Polar Ozone Loss ?

Cosmic-ray (CR) -induced heterogeneous reactions of halogenated species have been suggested to play the dominant role in causing the Antarctic ozone hole. However, measurements of total ozone in Antarctica do not show a compact and significant correlation with CR activity. Further, a substantial CR-induced heterogeneous loss of chlorofluorocarbons is incompatible with multiyear satellite observations of N2O and CFC-12. Thus, CR-induced heterogeneous reactions cannot be considered as an alternative mechanism causing the Antarctic ozone hole

Technical note: A stratospheric climatology for O3, H2O and CH4 derived from HALOE measurements

International audienceThe Halogen Occultation Experiment (HALOE) on board the Upper Atmosphere research satellite (UARS) has observed mixing ratios of important trace species in the stratosphere over more than a decade since 1991. Here we present a climatology for the stratosphere compiled from the HALOE data for ozone, H₂O and CH₄ for the period from 1991 to 2002. In this approach, the data are averaged over equivalent latitude instead of latitude in order to correctly reproduce the gradients at the transport barriers like the polar vortex edge. The climatology is compiled for 5 degree equivalent latitude bins. The seasonal dependence is taken into account by choosing intervals of one month. The climatology is available as an electronic supplement

Midlatitude ClO during the maximum atmospheric chlorine burden : in situ balloon measurements and model simulations

Chlorine monoxide (ClO) plays a key role in stratospheric ozone loss processes at midlatitudes. We present two balloonborne in situ measurements of ClO conducted in northern hemisphere midlatitudes during the period of the maximum of total inorganic chlorine loading in the atmosphere. Both ClO measurements were conducted on board the TRIPLE balloon payload, launched in November 1996 in Le´on, Spain, and in May 1999 in Aire sur l’Adour, France. For both flights a ClO daylight and night time vertical profile could be derived over an altitude range of approximately 15–31 km. ClO mixing ratios are compared to model simulations performed with the photochemical box model version of the Chemical Lagrangian Model of the Stratosphere (CLaMS). Simulations along 24-h backward trajectories were performed to study the diurnal variation of ClO in the midlatitude lower stratosphere. Model simulations for the flight launched in Aire sur l’Adour 1999 show a good agreement with the ClO measurements. For the flight launched in Le´on 1996, a similar good agreement is found, except at around ~ 650 K potential temperature (~26km altitude). However, a tendency is found that for solar zenith angles greater than 86°–87° the simulated ClO mixing ratios substantially overestimate measured ClO by approximately a factor of 2.5 or more for both flights. Therefore we conclude that no indication can be deduced from the presented ClO measurements that substantial uncertainties exist in midlatitude chlorine chemistry of the stratosphere. An exception is the situation at solar zenith angles greater than 86°–87° where model simulations substantial overestimate ClO observations

The impact of transport across the polar vortex edge on Match ozone loss estimates

The Match method for the quantification of polar chemical ozone loss is investigated mainly with respect to the impact of the transport of air masses across the vortex edge. For the winter 2002/03, we show that significant transport across the vortex edge occurred and was simulated by the Chemical Lagrangian Model of the Stratosphere. In-situ observations of inert tracers and ozone from HAGAR on the Geophysica aircraft and balloon-borne sondes, and remote observations from MIPAS on the ENVISAT satellite were reproduced well by CLaMS. The model even reproduced a small vortex remnant that remained a distinct feature until June 2003 and was also observed in-situ by a balloon-borne whole air sampler. We use this CLaMS simulation to quantify the impact of transport across the vortex edge on ozone loss estimates from the Match method. We show that a time integration of the determined vortex average ozone loss rates, as performed in Match, results in a larger ozone loss than the polar vortex average ozone loss in CLaMS. The determination of the Match ozone loss rates is also influenced by the transport of air across the vortex edge. We use the model to investigate how the sampling of the ozone sondes on which Match is based represents the vortex average ozone loss rate. Both the time integration of ozone loss and the determination of ozone loss rates for Match are evaluated using the winter 2002/2003 CLaMS simulation. These impacts can explain the majority of the differences between CLaMS and Match column ozone loss. While the investigated effects somewhat reduce the apparent discrepancy in January ozone loss rates reported earlier, a distinct discrepancy between simulations and Match remains. However, its contribution to the accumulated ozone loss over the winter is not large

Impact of climate change on non-communicable diseases caused by altered UV radiation

Background: UV radiation can cause serious skin and eye diseases, especially cancers. UV-related skin cancer incidences have been increasing for decades. The determining factor for this development is the individual UV exposure. Climate change-induced changes in atmospheric factors can influence individual UV exposure. Methods: On the basis of a topic-specific literature research, a review paper was prepared and supplemented by as yet unpublished results of the authors’ own studies. The need for scientific research and development is formulated as well as primary prevention recommendations. Results: Climate change alters the factors influencing UV irradiance and annual UV dose in Germany. First evaluations of satellite data for Germany show an increase in mean peak UV irradiance and annual UV dose for the last decade compared to the last three decades. Conclusions: The climate change-related influences on individual UV exposure and the associated individual disease incidence cannot yet be reliably predicted due to considerable uncertainties. However, the current UV-related burden of disease already requires primary preventive measures to prevent UV-related diseases. This is part of a series of articles that constitute the German Status Report on Climate Change and Health 2023

Long-term changes of hydrogen-containing species in the stratosphere

Understanding the 1% per year increase of stratospheric water vapour from 1954 to 2000 is a great challenge in atmospheric science. The increase is predominantly caused by long-term changes in transport of water vapour into the stratosphere and systematic increases of tropospheric methane levels. This paper gives a review on stratospheric water vapour changes for the 1980 and 2000 time period with emphasis on the contribution of methane oxidation. Predictions for 2050 indicate that likely increases of tropospheric methane levels will lead to an increase of upper stratospheric water vapour values of about 0.4 ppmv. A similar value is predicted as an upper limit of effects of a future hydrogen economy. (c) 2006 Elsevier Ltd. All rights reserved

The impact of mixing across the polar vortex edge on Match ozone loss estimates

The Match method for quantification of polar chemical ozone loss is investigated mainly with respect to the impact of mixing across the vortex edge onto this estimate. We show for the winter 2002/03 that significant mixing across the vortex edge occurred and was accurately modeled by the Chemical Lagrangian Model of the Stratosphere. Observations of inert tracers and ozone in-situ from HAGAR on the Geophysica aircraft and sondes and also remote from MIPAS on ENVISAT were reproduced well. The model even reproduced a small vortex remnant that was isolated until June 2003 and was observed in-situ by a balloon-borne whole air sampler. We use this CLaMS simulation to quantify the impact of cross vortex edge mixing on the results of the Match method. It is shown that a time integration of the determined vortex average ozone loss rates as performed in Match results in larger ozone loss than the polar vortex average ozone loss in CLaMS. Also, the determination of the Match ozone loss rates can be influenced by mixing. This is especially important below 430 K, where ozone outside the vortex is lower than inside and the vortex boundary is not a strong transport barrier. This effect and further sampling effects cause an offset between vortex average ozone loss rates derived from Match and deduced from CLaMS with an even sampling for the entire vortex. Both, the time-integration of ozone loss and the determination of ozone loss rates for Match are evaluated using the winter 2002/03 CLaMS simulation. These impacts can explain the differences between CLaMS and Match column ozone loss. While the investigated effects somewhat reduce the apparent discrepancy in January ozone loss rates, a discrepancy between simulations and Match remains. However, its contribution to the accumulated ozone loss over the winter is not large

Simulation of denitrification and ozone loss for the Arctic winter 2002/2003

We present simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS) for the Arctic winter 2002/2003. We integrated a Lagrangian denitrification scheme into the three-dimensional version of CLaMS that calculates the growth and sedimentation of nitric acid trihydrate (NAT) particles along individual particle trajectories. From those, we derive the HNO3 downward flux resulting from different particle nucleation assumptions. The simulation results show a clear vertical redistribution of total inorganic nitrogen (NOy), with a maximum vortex average permanent NOy removal of over 5 ppb in late December between 500 and 550 K and a corresponding increase of NOy of over 2 ppb below about 450 K. The simulated vertical redistribution of NOy is compared with balloon observations by MkIV and in-situ observations from the high altitude aircraft Geophysica. Assuming a globally uniform NAT particle nucleation rate of 3.4·10&#8722;6 cm&#8722;3 h&#8722;1 in the model, the observed denitrification is well reproduced. In the investigated winter 2002/2003, the denitrification has only moderate impact (<=10%) on the simulated vortex average ozone loss of about 1.1 ppm near the 460 K level. At higher altitudes, above 600 K potential temperature, the simulations show significant ozone depletion through NOx-catalytic cycles due to the unusual early exposure of vortex air to sunlight

What causes the irregular cycle of the atmospheric tape recorder signal in HCN?

Variations in the mixing ratio of long-lived trace gases entering the stratosphere in the tropics are carried upward with the rising air with the signal being observable throughout the tropical lower stratosphere. This phenomenon, referred to as "atmospheric tape recorder" has previously been observed for water vapor, CO2, and CO which exhibit an annual cycle. Recently, based on Microwave Limb Sounder (MLS) and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) satellite measurements, the tape recorder signal has been observed for hydrogen cyanide (HCN) but with an approximately two-year period. Here we report on a model simulation of the HCN tape recorder for the time period 2002-2008 using the Chemical Lagrangian Model of the Stratosphere (CLaMS). The model can reproduce the observed pattern of the HCN tape recorder signal if time-resolved emissions from fires in Indonesia are used as lower boundary condition. This finding indicates that inter-annual variations in biomass burning in Indonesia, which are strongly influenced by El Nino events, control the HCN tape recorder signal. A longer time series of tropical HCN data will probably exhibit an irregular cycle rather than a regular biannual cycle. Citation: Pommrich, R., R. Muller, J.-U. Grooss, G. Gunther, P. Konopka, M. Riese, A. Heil, M. Schultz, H.-C. Pumphrey, and K. A. Walker (2010), What causes the irregular cycle of the atmospheric tape recorder signal in HCN?, Geophys. Res. Lett., 37, L16805, doi:10.1029/2010GL044056

Stratospheric ozone chemistry in the Antarctic: what determines the lowest ozone values reached and their recovery?

Balloon-borne observations of ozone from the South Pole Station have been reported to reach ozone mixing ratios below the detection limit of about 10 ppbv at the 70 hPa level by late September. After reaching a minimum, ozone mixing ratios increase to above 1 ppmv on the 70 hPa level by late December. While the basic mechanisms causing the ozone hole have been known for more than 20 yr, the detailed chemical processes determining how low the local concentration can fall, and how it recovers from the minimum have not been explored so far. Both of these aspects are investigated here by analysing results from the Chemical Lagrangian Model of the Stratosphere (CLaMS). As ozone falls below about 0.5 ppmv, a balance is maintained by gas phase production of both HCl and HOCl followed by heterogeneous reaction between these two compounds in these simulations. Thereafter, a very rapid, irreversible chlorine deactivation into HCl can occur, either when ozone drops to values low enough for gas phase HCl production to exceed chlorine activation processes or when temperatures increase above the polar stratospheric cloud (PSC) threshold. As a consequence, the timing and mixing ratio of the minimum ozone depends sensitively on model parameters, including the ozone initialisation. The subsequent ozone increase between October and December is linked mainly to photochemical ozone production, caused by oxygen photolysis and by the oxidation of carbon monoxide and methane