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The comprehensive model system COSMO-ART – Radiative impact of aerosol on the state of the atmosphere on the regional scale

A new fully online coupled model system developed for the evaluation of the interaction of aerosol particles with the atmosphere on the regional scale is described. The model system is based on the operational weather forecast model of the Deutscher Wetterdienst. Physical processes like transport, turbulent diffusion, and dry and wet deposition are treated together with photochemistry and aerosol dynamics using the modal approach. Based on detailed calculations we have developed parameterisations to examine the impact of aerosol particles on photolysis and on radiation. Currently the model allows feedback between natural and anthropogenic aerosol particles and the atmospheric variables that are initialized by the modification of the radiative fluxes. The model system is applied to two summer episodes, each lasting five days, with a model domain covering Western Europe and adjacent regions. The first episode is characterised by almost cloud free conditions and the second one by cloudy conditions. The simulated aerosol concentrations are compared to observations made at 700 stations distributed over Western Europe. For each episode two model runs are performed; one where the feedback between the aerosol particles and the atmosphere is taken into account and a second one where the feedback is neglected. Comparing these two sets of model runs, the radiative feedback on temperature and other variables is evaluated. In the cloud free case a clear correlation between the aerosol optical depth and changes in global radiation and temperature is found. In the case of cloudy conditions the pure radiative effects are superposed by changes in the liquid water content of the clouds due to changes in the thermodynamics of the atmosphere. In this case the correlation between the aerosol optical depth and its effects on temperature is low. However, on average a decrease in the 2 m temperature is still found. For the area of Germany we found on average for both cases a reduction in the global radiation of about 6 W m2, a decrease of the 2 m temperature of 0.1 K, and a reduction in the daily temperature range of −0.13 K.
Photolysis imprint in the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cycling

The nitrogen (δ15N) and triple oxygen (δ17O and δ18O) isotopic composition of nitrate (NO3−) was measured year-round in the atmosphere and snow pits at Dome C, Antarctica (DC, 75.1° S, 123.3° E), and in surface snow on a transect between DC and the coast. Comparison to the isotopic signal in atmospheric NO3− shows that snow NO3− is significantly enriched in δ15N by >200&permil; and depleted in δ18O by <40&permil;. Post-depositional fractionation in Δ17O(NO3−) is small, potentially allowing reconstruction of past shifts in tropospheric oxidation pathways from ice cores. Assuming a Rayleigh-type process we find fractionation constants ε of −60±15&permil;, 8±2&permil; and 1±1&permil;, for δ15N, δ18O and Δ17O, respectively. A photolysis model yields an upper limit for the photolytic fractionation constant 15ε of δ15N, consistent with lab and field measurements, and demonstrates a high sensitivity of 15ε to the incident actinic flux spectrum. The photolytic 15ε is process-specific and therefore applies to any snow covered location. Previously published 15ε values are not representative for conditions at the Earth surface, but apply only to the UV lamp used in the reported experiment (Blunier et al., 2005; Jacobi et al., 2006). Depletion of oxygen stable isotopes is attributed to photolysis followed by isotopic exchange with water and hydroxyl radicals. Conversely, 15N enrichment of the NO3− fraction in the snow implies 15N depletion of emissions. Indeed, δ15N in atmospheric NO3− shows a strong decrease from background levels (4±7&permil;) to −35&permil; in spring followed by recovery during summer, consistent with significant snowpack emissions of reactive nitrogen. Field and lab evidence therefore suggest that photolysis is an important process driving fractionation and associated NO3− loss from snow. The Δ17O signature confirms previous coastal measurements that the peak of atmospheric NO3− in spring is of stratospheric origin. After sunrise photolysis drives then redistribution of NO3− from the snowpack photic zone to the atmosphere and a snow surface skin layer, thereby concentrating NO3− at the surface. Little NO3− appears to be exported off the EAIS plateau, still snow emissions from as far as 600 km inland can contribute to the coastal NO3− budget.
Aerosol indirect effects – general circulation model intercomparison and evaluation with satellite data

Aerosol indirect effects continue to constitute one of the most important uncertainties for anthropogenic climate perturbations. Within the international AEROCOM initiative, the representation of aerosol-cloud-radiation interactions in ten different general circulation models (GCMs) is evaluated using three satellite datasets. The focus is on stratiform liquid water clouds since most GCMs do not include ice nucleation effects, and none of the model explicitly parameterises aerosol effects on convective clouds. We compute statistical relationships between aerosol optical depth (τa) and various cloud and radiation quantities in a manner that is consistent between the models and the satellite data. It is found that the model-simulated influence of aerosols on cloud droplet number concentration (Nd) compares relatively well to the satellite data at least over the ocean. The relationship between τa and liquid water path is simulated much too strongly by the models. This suggests that the implementation of the second aerosol indirect effect mainly in terms of an autoconversion parameterisation has to be revisited in the GCMs. A positive relationship between total cloud fraction (fcld) and τa as found in the satellite data is simulated by the majority of the models, albeit less strongly than that in the satellite data in most of them. In a discussion of the hypotheses proposed in the literature to explain the satellite-derived strong fcld–τa relationship, our results indicate that none can be identified as a unique explanation. Relationships similar to the ones found in satellite data between τa and cloud top temperature or outgoing long-wave radiation (OLR) are simulated by only a few GCMs. The GCMs that simulate a negative OLR–τa relationship show a strong positive correlation between τa and fcld. The short-wave total aerosol radiative forcing as simulated by the GCMs is strongly influenced by the simulated anthropogenic fraction of τa, and parameterisation assumptions such as a lower bound on Nd. Nevertheless, the strengths of the statistical relationships are good predictors for the aerosol forcings in the models. An estimate of the total short-wave aerosol forcing inferred from the combination of these predictors for the modelled forcings with the satellite-derived statistical relationships yields a global annual mean value of −1.5±0.5 Wm−2. In an alternative approach, the radiative flux perturbation due to anthropogenic aerosols can be broken down into a component over the cloud-free portion of the globe (approximately the aerosol direct effect) and a component over the cloudy portion of the globe (approximately the aerosol indirect effect). An estimate obtained by scaling these simulated clear- and cloudy-sky forcings with estimates of anthropogenic τa and satellite-retrieved Nd–τa regression slopes, respectively, yields a global, annual-mean aerosol direct effect estimate of −0.4±0.2 Wm−2 and a cloudy-sky (aerosol indirect effect) estimate of −0.7±0.5 Wm−2, with a total estimate of −1.2±0.4 Wm−2.
Sensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics

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 Cl2O2 photolysis reaction, which arises from uncertainty in laboratory-measured molecular cross sections at atmospherically important wavelengths. This estimated uncertainty in JCl2O2 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.
On the capability of IASI measurements to inform about CO surface emissions

Between July and November 2008, simultaneous observations were conducted by several orbiting instruments that monitor carbon monoxide in the atmosphere, among them the Infrared Atmospheric Sounding Instrument (IASI) and Measurements Of Pollution In The Troposphere (MOPITT). In this paper, the concentration retrievals at about 700 hPa from these two instruments are successively used in a variational Bayesian system to infer the global distribution of CO emissions. Starting from a global emission budget of 479 Tg for the considered period, the posterior estimate of CO emissions using IASI retrievals gives a total of 643 Tg, which is in close agreement with the budget calculated with version 3 of the MOPITT data (649 Tg). The regional totals are also broadly consistent between the two inversions. Even though our theoretical error budget indicates that IASI constrains the emissions slightly less than MOPITT, because of lesser sensitivity in the lower troposphere, these first results indicate that IASI may play a major role in the quantification of the emissions of CO.
Explicit calculation of indirect global warming potentials for halons using atmospheric models

The concept of Global Warming Potentials (GWPs) has been extensively used in policy consideration as a relative index for comparing the climate impact of an emitted greenhouse gas (GHG), relative to carbon dioxide with equal mass emissions. Ozone depletion due to emission of chlorinated or brominated halocarbons leads to cooling of the climate system in the opposite direction to the direct warming contribution by halocarbons as GHGs. This cooling is a key indirect effect of the halocarbons on climatic radiative forcing, which is accounted for by indirect GWPs. With respect to climate, it is critical to understand net influences considering direct warming and indirect cooling effects especially for Halons due to the greater ozone-depleting efficiency of bromine over chlorine. Until now, the indirect GWPs have been calculated using a parameterized approach based on the concept of Equivalent Effective Stratospheric Chlorine (EESC) and the observed ozone depletion over the last few decades. As a step towards obtaining indirect GWPs through a more robust approach, we use atmospheric models to explicitly calculate the indirect GWPs of Halon-1211 and Halon-1301 for a 100-year time horizon. State-of-the-art global chemistry-transport models (CTMs) were used as the computational tools to derive more realistic ozone depletion changes caused by an added pulse emission of the two major Halons at the surface. The radiative forcings on climate from the ozone changes have been calculated for indirect GWPs using an atmospheric radiative transfer model (RTM). The simulated temporal variations of global average total column Halons after a pulse perturbation follow an exponential decay with an e-folding time which is consistent with the expected chemical lifetimes of the Halons. Our calculated indirect GWPs for the two Halons are much smaller than those from past studies but are within a single standard deviation of WMO (2007) values and the direct GWP values derived agree with the published values. Our model-based assessment of the Halon indirect GWPs thus confirms the significant importance of indirect effects on climate.
Closing the dimethyl sulfide budget in the tropical marine boundary layer during the Pacific Atmospheric Sulfur Experiment

Fourteen research flights were conducted with the National Center for Atmospheric Research (NCAR) C-130 near Christmas Island (2° N, 157° W) during the summer of 2007 as part of the Pacific Atmospheric Sulfur Experiment (PASE). In order to tightly constrain the scalar budget of DMS, vertical eddy fluxes were measured at various levels in the marine boundary layer (MBL) from ~30 m to the top of the mixed layer (~500 m) providing improved accuracy of the flux divergence calculation in the DMS budget. The observed mean mole fraction of DMS in the MBL exhibited the well-known diurnal cycle, ranging from 50–95 pptv in the daytime to 90–110 pptv at night. Contributions from horizontal advection are included using a multivariate regression of all DMS flight data within the MBL to estimate the mean gradients and trends. With this technique we can use the residual term in the DMS budget as an estimate of overall photochemical oxidation. Error analysis of the various terms in the DMS budget indicate that chemical losses acting on time scales of up to 110 h can be inferred with this technique. On average, photochemistry accounted for ~7.4 ppt hr −1 loss rate for the seven daytime flights, with an estimated error of 0.6 ppt hr−1. The loss rate due to expected OH oxidation is sufficient to explain the net DMS destruction without invoking the action of additional oxidants (e.g., reactive halogens.) The observed ocean flux of DMS averaged 3.1 (±1.5) μmol m−2 d−1, and generally decreased throughout the sunlit hours. Over the entire mission, the horizontal advection contribution to the overall budget was merely -0.1 ppt hr−1, indicating a mean atmospheric DMS gradient nearly perpendicular to the east-southeasterly trade winds and the chlorophyll gradient in the equatorial upwelling ocean. Nonetheless, horizontal advection was a significant term in the budget of any given flight, ranging from −1.2 to 2.5 ppt hr−1 , indicating a patchy and variable surface seawater DMS distribution, and thus needs to be accounted for in budget studies.
Coastal measurements of short-lived reactive iodocarbons and bromocarbons at Roscoff, Brittany during the RHaMBLe campaign

Atmospheric concentrations of the volatile reactive iodocarbons C2H5I, 1-C3H7I, 2-C3H7I, CH2ICl, CH2IBr, CH2I2 and bromocarbons CH2Br2 and CHBr3 were determined by GC/MS analysis of marine boundary layer air at Roscoff, Brittany on the northwest coast of France during September 2006. Comparison with other coastal studies suggests that emissions of these trace gases are strongly influenced by site topography, seaweed populations and distribution, as well as wind speed and direction and tide height. Concentrations of the very short-lived dihalomethanes CH2IBr and CH2I2 in particular showed evidence of tidal dependence, with higher concentrations observed at low tide during maximum exposure of seaweed beds. We also present a limited number of halocarbon measurements in surface seawater and estimate sea-air fluxes based on these and simultaneous air measurements. CH2Br2 and CHBr3 were strongly correlated both in air and in seawater, with CH2Br2/CHBr3 ratios of 0.19 in air and 0.06 in water. The combined midday I atom flux from the photolabile diahlomethanes CH2I2, CH2IBr and CH2ICl of ~5×103 molecules cm−3 s−1 is several orders of magnitude lower than the estimated I atom flux from I2 based on coinciding measurements at the same site, which indicates that at Roscoff the major I atom precursor was I2 rather than reactive iodocarbons.
UV Raman lidar measurements of relative humidity for the characterization of cirrus cloud microphysical properties

Raman lidar measurements performed in Potenza by the Raman lidar system BASIL in the presence of cirrus clouds are discussed. Measurements were performed on 6 September 2004 in the frame of the Italian phase of the EAQUATE Experiment. The major feature of BASIL is represented by its capability to perform high-resolution and accurate measurements of atmospheric temperature and water vapour, and consequently relative humidity, both in daytime and night-time, based on the application of the rotational and vibrational Raman lidar techniques in the UV. BASIL is also capable to provide measurements of the particle backscatter and extinction coefficient, and consequently lidar ratio (at the time of these measurements, only at one wavelength), which are fundamental to infer geometrical and microphysical properties of clouds. A case study is discussed in order to assess the capability of Raman lidars to measure humidity in presence of cirrus clouds, both below and inside the cloud. While air inside the cloud layers is observed to be always under-saturated with respect to water, both ice super-saturation and under-saturation conditions are found inside these clouds. Upper tropospheric moistening is observed below the lower cloud layer. The synergic use of the data derived from the ground based Raman Lidar and of spectral radiances measured by the NAST-I Airborne Spectrometer allows the determination of the temporal evolution of the atmospheric cooling/heating rates due to the presence of the cirrus cloud. Lidar measurements beneath the cirrus cloud layer have been interpreted using a 1-D cirrus cloud model with explicit microphysics. The 1-D simulations indicate that sedimentation-moistening has contributed significantly to the moist anomaly, but other mechanisms are also contributing. This result supports the hypothesis that the observed mid-tropospheric humidification is a real feature which is strongly influenced by the sublimation of precipitating ice crystals. Results illustrated in this study demonstrate that Raman lidars, like the one used in this study, can resolve the spatial and temporal scales required for the study of cirrus cloud microphysical processes and appear sensitive enough to reveal and quantify upper tropospheric humidification associated with cirrus cloud sublimation.
Application of φ-IASI to IASI: retrieval products evaluation and radiative transfer consistency

Retrieval products for temperature, water vapour and ozone have been obtained from spectral radiances measured by the Infrared Atmospheric Sounding Interferometer flying onboard the first European Meteorological Operational satellite. These products have been used to check the consistency of the forward model and its accuracy and the expected retrieval performance. The study has been carried out using a research-oriented forward-inverse methodology, called φ-IASI, that the authors have specifically developed for the new sounding interferometer. The performance of the forward-inversion strategy has been assessed by comparing the retrieved profiles to profiles of temperature, water vapour and ozone obtained by co-locating in space and time profiles from radiosonde observations and from the European Centre for Medium-Range Weather Forecasts analysis. Spectral residuals have also been computed and analyzed to assess the quality of the forward model. Two versions of the high-resolution transmission molecular absorption database have been used, which mostly differ for ozone absorption line parameters, line and continuum absorption of both CO2 and H2O molecules. Their performance has been assessed by inter-comparing the results, and a consistent improvement in the spectral residual has been found when using the most updated release.