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- ItemRetrievals of chlorine chemistry kinetic parameters from Antarctic ClO microwave radiometer measurements(München : European Geopyhsical Union, 2011) Kremser, S.; Schofield, R.; Bodeker, G.E.; Connor, B.J.; Rex, M.; Barret, J.; Mooney, T.; Salawitch, R.J.; Canty, T.; Frieler, K.; Chipperfield, M.P.; Langematz, U.; Feng, W.Key kinetic parameters governing the partitioning of chlorine species in the Antarctic polar stratosphere were retrieved from 28 days of chlorine monoxide (ClO) microwave radiometer measurements made during the late winter/early spring of 2005 at Scott Base (77.85° S, 166.75° E). During day-time the loss of the ClO dimer chlorine peroxide (ClOOCl) occurs mainly by photolysis. Some time after sunrise, a photochemical equilibrium is established and the ClO/ClOOCl partitioning is determined by the ratio of the photolysis frequency, J, and the dimer formation rate, kf. The values of J and kf from laboratory studies remain uncertain to a considerable extent, and as a complement to these ongoing studies, the goal of this work is to provide a constraint on that uncertainty based on observations of ClO profiles in the Antarctic. First an optimal estimation technique was used to derive J/kf ratios for a range of Keq values. The optimal estimation forward model was a photochemical box model that takes J, kf, and Keq as inputs, together with a priori profiles of activated chlorine (ClOx = ClO+2×ClOOCl), profiles of ozone, temperature, and pressure. JPL06 kinetics are used as a priori in the optimal estimation and for all other chemistry in the forward model. Using the more recent JPL09 kinetics results in insignificant differences in the retrieved value of J/kf. A complementary approach was used to derive the optimal kinetic parameters; the full parameter space of J, kf, Keq and ClOx was sampled to find the minimum in differences between measured and modelled ClO profiles. Furthermore, values of Keq up to 2.0 times larger than recommended by JPL06 were explored to test the sensitivity of the J/kf ratio to changes in Keq. The results show that the retrieved J/kf ratios bracket the range of 1.23 to 1.97 times the J/kf value recommended by JPL06 over the range of Keq values considered. The retrieved J/kf ratios lie in the lower half of the large uncertainty range of J/kf recommended by JPL06 and towards the upper portion of the smaller uncertainty range recommended by JPL09.
- ItemSensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics(Göttingen : Copernicus GmbH, 2009) Kawa, S.R.; Stolarski, R.S.; Newman, P.A.; Douglass, A.R.; Rex, M.; Hofmann, D.J.; Santee, M.L.; Frieler, K.The impact and significance of uncertainties in model calculations of stratospheric ozone loss resulting from known uncertainty in chemical kinetics parameters is evaluated in trajectory chemistry simulations for the Antarctic and Arctic polar vortices. The uncertainty in modeled ozone loss is derived from Monte Carlo scenario simulations varying the kinetic (reaction and photolysis rate) parameters within their estimated uncertainty bounds. Simulations of a typical winter/spring Antarctic vortex scenario and Match scenarios in the Arctic produce large uncertainty in ozone loss rates and integrated seasonal loss. The simulations clearly indicate that the dominant source of model uncertainty in polar ozone loss is uncertainty in the Cl2O 2 photolysis reaction, which arises from uncertainty in laboratory-measured molecular cross sections at atmospherically important wavelengths. This estimated uncertainty in JCl 2O2 from laboratory measurements seriously hinders our ability to model polar ozone loss within useful quantitative error limits. Atmospheric observations, however, suggest that the Cl2O2 photolysis uncertainty may be less than that derived from the lab data. Comparisons to Match, South Pole ozonesonde, and Aura Microwave Limb Sounder (MLS) data all show that the nominal recommended rate simulations agree with data within uncertainties when the Cl2O2 photolysis error is reduced by a factor of two, in line with previous in situ ClOx measurements. Comparisons to simulations using recent cross sections from Pope et al. (2007) are outside the constrained error bounds in each case. Other reactions producing significant sensitivity in polar ozone loss include BrO + ClO and its branching ratios. These uncertainties challenge our confidence in modeling polar ozone depletion and projecting future changes in response to changing halogen emissions and climate. Further laboratory, theoretical, and possibly atmospheric studies are needed.
- ItemLong-term wintertime trend of zonally asymmetric ozone in boreal extratropics during 1979-2016(Basel : MDPI AG, 2018) Schneidereit, A.; Peters, D.H.W.Strong zonally asymmetric ozone (ZAO) changes are observed in the boreal extratropics for winter. During the TOMS (Total Ozone Mapping Spectrometer) period (1979-1992) the decrease of zonally asymmetric total ozone (ZATO) was twice as large as the observed zonal mean total ozone trend over Europe in January mainly caused by ultra-long wave transport. Recent studies have demonstrated that the ozone evolution reveals three different quasi-bidecadal trend stages: (i) Decline, (ii) leveling, and (ii) healing. This study focuses on the ZAO structure in boreal extratropics and on ozone transport changes by ultra-long waves during winter months. ERA-Interim data together with a linearized transport model are used. During the healing stage ZATO increases significantly over the North Atlantic/European region for January. The ZATO increase (healing stage) and ZATO decrease (decline stage) are caused by different monthly mean ozone transport characteristics of ultra-long planetary waves over the North Atlantic/European region. Furthermore, the vertical advection (ageostrophic transport) of ozone versus its horizontal component dominates in the lower and middle stratosphere during the healing stage. It is hypothesized that these ageostrophic wind changes are mainly caused by a wave train directed northeastwards which seems to be directly linked to the Arctic warming. © 2018 by the authors.
- ItemNOy production, ozone loss and changes in net radiative heating due to energetic particle precipitation in 2002–2010(Katlenburg-Lindau : EGU, 2018-1-29) Sinnhuber, Miriam; Berger, Uwe; Funke, Bernd; Nieder, Holger; Reddmann, Thomas; Stiller, Gabriele; Versick, Stefan; von Clarmann, Thomas; Wissing, Jan MaikWe analyze the impact of energetic particle precipitation on the stratospheric nitrogen budget, ozone abundances and net radiative heating using results from three global chemistry-climate models considering solar protons and geomagnetic forcing due to auroral or radiation belt electrons. Two of the models cover the atmosphere up to the lower thermosphere, the source region of auroral NO production. Geomagnetic forcing in these models is included by prescribed ionization rates. One model reaches up to about 80 km, and geomagnetic forcing is included by applying an upper boundary condition of auroral NO mixing ratios parameterized as a function of geomagnetic activity. Despite the differences in the implementation of the particle effect, the resulting modeled NOy in the upper mesosphere agrees well between all three models, demonstrating that geomagnetic forcing is represented in a consistent way either by prescribing ionization rates or by prescribing NOy at the model top. Compared with observations of stratospheric and mesospheric NOy from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument for the years 2002–2010, the model simulations reproduce the spatial pattern and temporal evolution well. However, after strong sudden stratospheric warmings, particle-induced NOy is underestimated by both high-top models, and after the solar proton event in October 2003, NOy is overestimated by all three models. Model results indicate that the large solar proton event in October 2003 contributed about 1–2 Gmol (109 mol) NOy per hemisphere to the stratospheric NOy budget, while downwelling of auroral NOx from the upper mesosphere and lower thermosphere contributes up to 4 Gmol NOy. Accumulation over time leads to a constant particle-induced background of about 0.5–1 Gmol per hemisphere during solar minimum, and up to 2 Gmol per hemisphere during solar maximum. Related negative anomalies of ozone are predicted by the models in nearly every polar winter, ranging from 10–50 % during solar maximum to 2–10 % during solar minimum. Ozone loss continues throughout polar summer after strong solar proton events in the Southern Hemisphere and after large sudden stratospheric warmings in the Northern Hemisphere. During mid-winter, the ozone loss causes a reduction of the infrared radiative cooling, i.e., a positive change of the net radiative heating (effective warming), in agreement with analyses of geomagnetic forcing in stratospheric temperatures which show a warming in the late winter upper stratosphere. In late winter and spring, the sign of the net radiative heating change turns to negative (effective cooling). This spring-time cooling lasts well into summer and continues until the following autumn after large solar proton events in the Southern Hemisphere, and after sudden stratospheric warmings in the Northern Hemisphere.
- ItemZonal asymmetries in middle atmospheric ozone and water vapour derived from Odin satellite data 2001-2010(Göttingen : Copernicus, 2011) Gabriel, A.; Körnich, H.; Lossow, S.; Peters, D.H.W.; Urban, J.; Murtagh, D.Stationary wave patterns in middle atmospheric ozone (O3) and water vapour (H2O) are an important factor in the atmospheric circulation, but there is a strong gap in diagnosing and understanding their configuration and origin. Based on Odin satellite data from 2001 to 2010 we investigate the stationary wave patterns in O3 and H2O as indicated by the seasonal long-term means of the zonally asymmetric components O3* Combining double low line O3-[O3] and H2O* Combining double low line H2O-[H2O] ([O3], [H2O]: zonal means). At mid-and polar latitudes we find a pronounced wave one pattern in both constituents. In the Northern Hemisphere, the wave patterns increase during autumn, maintain their strength during winter and decay during spring, with maximum amplitudes of about 10-20 % of the zonal mean values. During winter, the wave one in O3* shows a maximum over the North Pacific/Aleutians and a minimum over the North Atlantic/Northern Europe and a double-peak structure with enhanced amplitude in the lower and in the upper stratosphere. The wave one in H2O* extends from the lower stratosphere to the upper mesosphere with a westward shift in phase with increasing height including a jump in phase at upper stratosphere altitudes. In the Southern Hemisphere, similar wave patterns occur mainly during southern spring. By comparing the observed wave patterns in O 3* and H2O3* with a linear solution of a steady-state transport equation for a zonally asymmetric tracer component we find that these wave patterns are primarily due to zonally asymmetric transport by geostrophically balanced winds, which are derived from observed temperature profiles. In addition temperature-dependent photochemistry contributes substantially to the spatial structure of the wave pattern in O 3* . Further influences, e.g., zonal asymmetries in eddy mixing processes, are discussed.
- ItemGlobal annual methane emission rate derived from its current atmospheric mixing ratio and estimated lifetime(Göttingen : Copernicus, 2014) Sonnemann, G.R.; Grygalashvyly, M.We use the estimated lifetime of methane (CH4), the current methane concentration, and its annual growth rate to calculate the global methane emission rate. The upper and lower limits of the annual global methane emission rate, depending on loss of CH4 into the stratosphere and methane consuming bacteria, amounts to 648.0 Mt a-1 and 608.0 Mt a-1. These values are in reasonable agreement with satellite and with much more accurate in situ measurements of methane. We estimate a mean tropospheric and mass-weighted temperature related to the reaction rate and employ a mean OH-concentration to calculate a mean methane lifetime. The estimated atmospheric lifetime of methane amounts to 8.28 years and 8.84 years, respectively. In order to improve the analysis a realistic 3D-calculations should be performed.
- ItemUpper stratospheric ozone decrease events due to a positive feedback between ozone and the ozone dissociation rate(Göttingen : Copernicus, 2009) Sonnemann, G.R.; Hartogh, P.Ozone measurements taken with a ground based microwave instrument at Lindau (51.66° N, 10.13° E) over some years showed strong ozone decrease events within the stratopause region, particularly during the winter half-year. These events are characterized by a marked drop of the ozone mixing ratio from two to three ppmv to less than half a ppmv in extreme cases. Simultaneous water vapor measurements at the same place, also carried out by a microwave instrument, showed a strong increase of its mixing ratio and the temperature was also enhanced during these episodes. The theoretical analysis brought evidence that these events result from a positive feedback in the complex radiatively-chemical system between the ozone column density and the ozone dissociation rate.