bluuebunny/crossref_metadata_2025 huggingface dataset:
Interannual variability and long term changes in planetary wave activity in the middle atmosphere observed by lidar
Authors: Hauchecorne A. , Keckhut P. , Chanin M. L.
Published: April 2010

Abstract. The upwelling planetary wave activity (PW) from the troposphere controls the intensity of the equator to pole transport of stratospheric ozone by the Brewer-Dobson circulation and thereby modulates the total ozone content at mid- and high-latitudes. Rayleigh lidar temperature data obtained from 1981 to 2001 at mid-latitude were used to study the interannual variability of PW activity in winter (October to April). The spectrum of stratospheric temperature fluctuations exhibits 2 peaks corresponding to 2 dominant modes of free travelling Rossby waves known as 16 day- and 12 day-waves. The 12 day-wave activity is shown to be anticorrelated with the equatorial QBO wind at 40 hPa. During the period 1981–2000 the global PW activity shows a negative trend for months October to January and a positive trend in March and April.
Observations and analysis of polar stratospheric clouds detected by POAM III and SAGE III during the SOLVE II/VINTERSOL campaign in the 2002/2003 Northern Hemisphere winter
Authors: Alfred J. , Fromm M. , Bevilacqua R. , Nedoluha G. , Strawa A. , Poole L. , Wickert J.
Published: April 2010

Abstract. The Polar Ozone and Aerosol Measurement and Stratospheric Aerosol and Gas Experiment instruments both observed high numbers of polar stratospheric clouds (PSCs) in the polar region during the second SAGE Ozone Loss and Validation Experiment (SOLVE II) and Validation of INTERnational Satellites and Study of Ozone Loss (VINTERSOL) campaign, conducted during the 2002/2003 Northern Hemisphere winter. Between 15 November 2002 (14 November 2002) and 18 March 2003 (21 March 2003) SAGE (POAM) observed 122 (151) aerosol extinction profiles containing PSCs. PSCs were observed on an almost daily basis, from early December through 15 January, in both instruments. No PSCs were observed from either instrument until 4 February, and sparingly in three periods in mid-and-late February and mid-March. In early December, PSCs were observed in the potential temperature range from roughly 375 K to 750 K. Throughout December the top of this range decreases to near 600 K. In February and March, PSC observations were primarily constrained to potential temperatures below 500 K. The PSC observation frequency as a function of ambient temperature relative to the NAT saturation point was used to infer irreversible denitrification. By late December 38% denitrification was inferred at both the 400–475 K and 475–550 K potential temperature ranges. By early January extensive levels of denitrification near 80% were inferred at both potential temperature ranges, and the air remained denitrified at least through early March.
Near-UV photolysis cross sections of CH3OOH and HOCH2OOH determined via action spectroscopy
Authors: Roehl C. M. , Marka Z. , Fry J. L. , Wennberg P. O.
Published: April 2010

Abstract. Knowledge of molecular photolysis cross sections is important for determining atmospheric lifetimes and fates of many species. A method and laser apparatus for measurement of these cross sections in the near-ultraviolet (UV) region is described. The technique is based on action spectroscopy, where the yield of a photodissociation product (in this case OH) is measured as a function of excitation energy. For compounds yielding OH, this method can be used to measure near-UV photodissociation cross section as low as 10−23 cm2 molecule−1. The method is applied to determine the photodissociation cross sections for methyl hydroperoxide (CH3OOH; MHP) and hydroxymethyl hydroperoxide (HOCH2OOH; HMHP) in the 305–365 nm wavelength range. The measured cross sections are in good agreement with previous measurements of absorption cross sections.
The tropospheric processing of acidic gases and hydrogen sulphide in volcanic gas plumes as inferred from field and model investigations
Authors: Aiuppa A. , Franco A. , von Glasow R. , Allen A. G. , D’Alessandro W. , Mather T. A. , Pyle D. M. , Valenza M.
Published: April 2010

Abstract. Improving the constraints on the atmospheric fate and depletion rates of acidic compounds persistently emitted by non-erupting (quiescent) volcanoes is important for quantitatively predicting the environmental impact of volcanic gas plumes. Here, we present new experimental data coupled with modelling studies to investigate the chemical processing of acidic volcanogenic species during tropospheric dispersion. Diffusive tube samplers were deployed at Mount Etna, a very active open-conduit basaltic volcano in eastern Sicily, and Vulcano Island, a closed-conduit quiescent volcano in the Aeolian Islands (northern Sicily). Sulphur dioxide (SO2), hydrogen sulphide (H2S), hydrogen chloride (HCl) and hydrogen fluoride (HF) concentrations in the volcanic plumes (typically several minutes to a few hours old) were repeatedly determined at distances from the summit vents ranging from 0.1 to ~10 km, and under different environmental conditions. At both volcanoes, acidic gas concentrations were found to decrease exponentially with distance from the summit vents (e.g., SO2 decreases from ~10 000 μg/m3 at 0.1 km from Etna's vents down to ~7 μg/m3 at ~10 km distance), reflecting the atmospheric dilution of the plume within the acid gas-free background troposphere. Conversely, SO2/HCl, SO2/HF, and SO2/H2S ratios in the plume showed no systematic changes with plume aging, and fit source compositions within analytical error. Assuming that SO2 losses by reaction are small during short-range atmospheric transport within quiescent (ash-free) volcanic plumes, our observations suggest that, for these short transport distances, atmospheric reactions for H2S and halogens are also negligible. The one-dimensional model MISTRA was used to simulate quantitatively the evolution of halogen and sulphur compounds in the plume of Mt. Etna. Model predictions support the hypothesis of minor HCl chemical processing during plume transport, at least in cloud-free conditions. Larger variations in the modelled SO2/HCl ratios were predicted under cloudy conditions, due to heterogeneous chlorine cycling in the aerosol phase. The modelled evolution of the SO2/H2S ratios is found to be substantially dependent on whether or not the interactions of H2S with halogens are included in the model. In the former case, H2S is assumed to be oxidized in the atmosphere mainly by OH, which results in minor chemical loss for H2S during plume aging and produces a fair match between modelled and measured SO2/H2S ratios. In the latter case, fast oxidation of H2S by Cl leads to H2S chemical lifetimes in the early plume of a few seconds, and thus SO2 to H2S ratios that increase sharply during plume transport. This disagreement between modelled and observed plume compositions suggests that more in-detail kinetic investigations are required for a proper evaluation of H2S chemical processing in volcanic plumes.
Technical Note: A new SIze REsolved Aerosol Model (SIREAM)
Authors: Debry E. , Fahey K. , Sartelet K. , Sportisse B. , Tombette M.
Published: April 2010

Abstract. We briefly present in this short paper a new SIze REsolved Aerosol Model (SIREAM) which simulates the evolution of atmospheric aerosol by solving the General Dynamic Equation (GDE). SIREAM segregates the aerosol size distribution into sections and solves the GDE by splitting coagulation and condensation/evaporation. A moving sectional approach is used to describe the size distribution change due to condensation/evaporation and a hybrid method has been developed to lower the computational burden. SIREAM uses the same physical parameterizations as those used in the Modal Aerosol Model, MAM sartelet05development. It is hosted in the modeling system POLYPHEMUS (Mallet et al., 2006) but can be linked to any other three-dimensional Chemistry-Transport Model.
Scavenging of black carbon in mixed phase clouds at the high alpine site Jungfraujoch
Authors: Cozic J. , Verheggen B. , Mertes S. , Connolly P. , Bower K. , Petzold A. , Baltensperger U. , Weingartner E.
Published: April 2010

Abstract. The scavenging of black carbon (BC) in liquid and mixed phase clouds was investigated during intensive experiments in winter 2004, summer 2004 and winter 2005 at the high alpine research station Jungfraujoch (3580 m a.s.l., Switzerland). Aerosol residuals were sampled behind two well characterized inlets; a total inlet which collected cloud particles (drops and ice particles) as well as interstitial aerosol particles; an interstitial inlet which collected only interstitial (unactivated) aerosol particles. BC concentrations were measured behind each of these inlets along with the submicrometer aerosol number size distribution, from which a volume concentration was derived. These measurements were complemented by in-situ measurements of cloud microphysical parameters. BC was found to be scavenged into the cloud phase to the same extent as the bulk aerosol, which suggests that BC was covered with soluble material through aging processes, rendering it more hygroscopic. The scavenged fraction of BC (FScav,BC), defined as the fraction of BC that is incorporated into cloud droplets and ice crystals, decreases with increasing cloud ice mass fraction (IMF) from FScav,BC=60% in liquid phase clouds to FScav,BC~10% in mixed-phase clouds with IMF>0.2. This is explained by the evaporation of liquid droplets in the presence of ice crystals (Wegener-Bergeron-Findeisen process), releasing BC containing cloud condensation nuclei back into the interstitial phase. In liquid clouds, the scavenged BC fraction is found to decrease with decreasing cloud liquid water content. The scavenged BC fraction is also found to decrease with increasing BC mass concentration since there is an increased competition for the available water vapour.
McSCIA: application of the Equivalence Theorem in a Monte Carlo radiative transfer model for spherical shell atmospheres
Authors: Spada F. , Krol M. C. , Stammes P.
Published: April 2010

Abstract. A new multiple-scattering Monte Carlo 3-D radiative transfer model named McSCIA (Monte Carlo for SCIAmachy) is presented. The backward technique is used to efficiently simulate narrow field of view instruments. The McSCIA algorithm has been formulated as a function of the Earth's radius, and can thus perform simulations for both plane-parallel and spherical atmospheres. The latter geometry is essential for the interpretation of limb satellite measurements, as performed by SCIAMACHY on board of ESA's Envisat. The model can simulate UV-vis-NIR radiation. First the ray-tracing algorithm is presented in detail, and then successfully validated against literature references, both in plane-parallel and in spherical geometry. A simple 1-D model is used to explain two different ways of treating absorption. One method uses the single scattering albedo while the other uses the equivalence theorem. The equivalence theorem is based on a separation of absorption and scattering. It is shown that both methods give, in a statistical way, identical results for a wide variety of scenarios. Both absorption methods are included in McSCIA, and it is shown that also for a 3-D case both formulations give identical results. McSCIA limb profiles for atmospheres with and without absorption compare well with the one of the state of the art Monte Carlo radiative transfer model MCC++. A simplification of the photon statistics may lead to very fast calculations of absorption features in the atmosphere. However, these simplifications potentially introduce biases in the results. McSCIA does not use simplifications and is therefore a relatively slow implementation of the equivalence theorem. For the first time, however, the validity of the equivalence theorem is demonstrated in a spherical 3-D radiative transfer model.
Surface tensions of multi-component mixed inorganic/organic aqueous systems of atmospheric significance: measurements, model predictions and importance for cloud activation predictions
Authors: Topping D. O. , McFiggans G. B. , Kiss G. , Varga Z. , Facchini M. C. , Decesari S. , Mircea M.
Published: April 2010

Abstract. In order to predict the physical properties of aerosol particles, it is necessary to adequately capture the behaviour of the ubiquitous complex organic components. One of the key properties which may affect this behaviour is the contribution of the organic components to the surface tension of aqueous particles in the moist atmosphere. Whilst the qualitative effect of organic compounds on solution surface tensions has been widely reported, our quantitative understanding on mixed organic and mixed inorganic/organic systems is limited.  Furthermore, it is unclear whether models that exist in the literature can reproduce the surface tension variability for binary and higher order multi-component organic and mixed inorganic/organic systems of atmospheric significance. The current study aims to resolve both issues to some extent. Surface tensions of single and multiple solute aqueous solutions were measured and compared with predictions from a number of model treatments. On comparison with binary organic systems, two predictive models found in the literature provided a range of values resulting from sensitivity to calculations of pure component surface tensions.  Results indicate that a fitted model can capture the variability of the measured data very well, producing the lowest average percentage deviation for all compounds studied.  The performance of the other models varies with compound and choice of model parameters. The behaviour of ternary mixed inorganic/organic systems was unreliably captured by using a predictive scheme and this was composition dependent. For more "realistic" higher order systems, entirely predictive schemes performed poorly. It was found that use of the binary data in a relatively simple mixing rule, or modification of an existing thermodynamic model with parameters derived from binary data, was able to accurately capture the surface tension variation with concentration. Thus, it would appear that in order to model multi-component surface tensions involving compounds used in this study one requires the use of appropriate binary data. The effect of deviations between predicted and measured surface tensions on predicted cloud activation properties was quantified, by incorporating the surface tension models into an existing thermodynamic framework. Critical saturation ratios as a function of dry size for all of the multi-component systems were computed and it was found that deviations between predictions increased with decreasing particle dry size.  As expected, use of the surface tension of pure water, rather than calculate the influence of the solutes explicitly, led to a consistently higher value of the critical saturation ratio indicating that neglect of the compositional effects will lead to significant differences in predicted activation behaviour even at large particle dry sizes.
Contribution of mixing to the upward transport across the TTL
Authors: Konopka P. , Günther G. , Müller R. , dos Santos F. H. S. , Schiller C. , Ravegnani F. , Ulanovsky A. , Schlager H. , Volk C. M. , Viciani S. , Pan L. , McKenna D.-S. , Riese M.
Published: April 2010

Abstract. During the second part of the TROCCINOX campaign that took place in Brazil in early 2005, chemical species were measured on-board of the high altitude research aircraft Geophysica (ozone, water vapor, NO, NOy, CH4 and CO) in the altitude range up to 20 km (or up to 450 K potential temperature), i.e. spanning the TTL region roughly extending between 350 and 420 K. Analysis of transport across TTL is performed using a new version of the Chemical Lagrangian Model of the Stratosphere (CLaMS). In this new version, the stratospheric model has been extended to the earth surface. Above the tropopause, the isentropic and cross-isentropic advection in CLaMS is driven by ECMWF winds and heating/cooling rates derived from a radiation calculation. Below the tropopause the model smoothly transforms from the isentropic to hybrid-pressure coordinate and, in this way, takes into account the effect of large-scale convective transport as implemented in the ECMWF vertical wind. As with other CLaMS simulations, the irreversible transport, i.e. mixing, is controlled by the local horizontal strain and vertical shear rates. Stratospheric and tropospheric signatures in the TTL can be seen both in the observation and in the model. The composition of air above ≈350 K is mainly controlled by mixing on a time scale of weeks or even months. Based on CLaMS transport studies where mixing can be completely switched off, we deduce that vertical mixing, mainly driven by the vertical shear in the outflow regions of the large-scale convection and in the vicinity of the subtropical jets, is necessary to understand the upward transport of the tropospheric air from the main convective outflow around 350 K up to the tropical tropopause around 380 K. This mechanism is most effective if the outflow of the mesoscale convective systems interacts with the subtropical jets.
Chemical characterization of the inorganic fraction of aerosols and mechanisms of the neutralization of atmospheric acidity in Athens, Greece
Authors: Karageorgos E. T. , Rapsomanikis S. , Wåhlin P.
Published: April 2010

Abstract. Mass concentration levels and the inorganic chemical composition of PM10 (two fractions; PM10−2.5 and PM2.5) were determined during August 2003 and March 2004, in the centre of Athens, Greece. August 2003 monthly mean PM10 mass concentration, at 5 m above ground, was 56 μg/m3 and the EU imposed daily limit of 50 μg/m3 was exceeded on 16 occasions. The corresponding monthly mean for March 2004 was 92 μg/m3 and the aforementioned daily limit was exceeded on 23 occasions. The PM10 (PM10−2.5+PM2.5) mass concentrations at 1.5 m above ground were found to be approximately 20% higher compared to the respective PM10 measured at 5 m. Consequently, for a realistic estimation of the exposure of citizens to particulate matter, PM10 sampling at a height of 1.5–3 m above ground, in the "breathing zone" is necessary. Such data are presented for the first time for the centre of Athens. In both campaigns, calcium was found to be the predominant component of the coarse fraction while crust-related aluminosilicates and iron were found to be the other major components of the same fraction. The above elements constitute the most important components of the fine fraction, together with the predominant sulphur. Toxic metals were found to be below the air quality limits and in lower concentrations compared to older studies, with the exception of Cu and V for which some increase was observed. Pb, in particular, appeared mostly in the fine fraction and in very low concentrations compared to studies dating more than a decade back. The major ions of the coarse fraction have been found to be Ca2+, NO3− and Cl−, while SO4−2, Ca2+ and NH4+ were the major ionic components of the fine fraction. The low molar ratio of NH4+/SO4−2 indicated an ammonium-poor ambient air, where atmospheric ammonia is not sufficient to neutralize all acidity and the formation of NH4NO3 does not occur to a significant extend. Calcium predominated the coarse fraction and its good correlations with NO3− and SO4−2 indicated its role as an important neutralizing agent of atmospheric acidity in this particle size range. In the fine fraction, both Ca2+ and NH4+ participate in the neutralizing processes with NH4+ being the major neutralizing agent of SO4−2. Chloride depletion from NaCl or MgCl2 was not found to occur to a significant extend. Total analyzed inorganic mass (elemental+ionic) was found to be ranging between approximately 25–33% of the total coarse particle mass and 35–42% of the total fine particle mass.
Global 2-D intercomparison of sectional and modal aerosol modules
Authors: Weisenstein D. K. , Penner J. E. , Herzog M. , Liu X.
Published: April 2010

Abstract. We present an intercomparison of two aerosol modules, one sectional, one modal, in a global 2-D model in order to differentiate their behavior for tropospheric and stratospheric applications. We model only binary sulfuric acid-water aerosols in this study. Two versions of the sectional model and three versions of the modal model are used to test the sensitivity of background aerosol mass and size distribution to the number of bins or modes and to the prescribed width of the largest mode. We find modest sensitivity to the number of bins (40 vs 150) used in the sectional model. Aerosol mass is found to be reduced in a modal model if care is not taken in selecting the width of the largest lognormal mode, reflecting differences in sedimentation in the middle stratosphere. The size distributions calculated by the sectional model can be better matched by a modal model with four modes rather than three modes in most but not all situations. A simulation of aerosol decay following the 1991 eruption of Mt. Pinatubo shows that the representation of the size distribution can have a signficant impact on model-calculated aerosol decay rates in the stratosphere. Between 1991 and 1995, aerosol mass and surface area density calculated by two versions of the modal model adequately match results from the sectional model. Calculated effective radius for the same time period shows more intermodel variability.
The Assimilation of Envisat data (ASSET) project
Authors: Lahoz W. A. , Geer A. J. , Bekki S. , Bormann N. , Ceccherini S. , Elbern H. , Errera Q. , Eskes H. J. , Fonteyn D. , Jackson D. R. , Khattatov B. , Massart S. , Peuch V.-H. , Rharmili S. , Ridolfi M. , Segers A. , Talagrand O. , Thornton H. E. , Vik A. F. , von Clarmann T.
Published: April 2010

Abstract. This paper discusses the highlights of the EU-funded "Assimilation of Envisat data" (ASSET) project, which has involved assimilation of Envisat atmospheric constituent and temperature data into systems based on Numerical Weather Prediction (NWP) models and chemical transport models (CTMs). Envisat was launched in 2002 and is one of the largest Earth Observation (EO) satellites ever built. It carries several sophisticated EO instruments providing insights into chemistry and dynamics of the atmosphere. The overarching theme of the ASSET project has been to bring together experts from all aspects of the data assimilation problem. This has allowed ASSET to address several themes comprehensively: enhancement of NWP analyses by assimilation of research satellite data; studies of the distribution of stratospheric chemical species by assimilation of research satellite data into CTM systems; objective assessment of the quality of ozone analyses; studies of the spatial and temporal evolution of tropospheric pollutants; enhanced retrievals of Envisat data; and data archival and dissemination. Among the results from the ASSET project, many of which are firsts in their field, we can mention: a positive impact on NWP analyses from assimilation of height-resolved stratospheric humidity and temperature data, and assimilation of limb radiances; the extraction of temperature information from the assimilation of chemical species into CTMs; a first intercomparison between ozone assimilation systems; the extraction of information on tropospheric pollution from assimilation of Envisat data; and the large potential of the Envisat MIPAS dataset. This paper discusses these, often novel, developments and results. Finally, achievements of, and recommendations from, the ASSET project are presented.
Latitudinal aerosol size distribution variation in the Eastern Atlantic Ocean measured aboard the FS-Polarstern
Authors: Williams P. I. , McFiggans G. , Gallagher M. W.
Published: April 2010

Abstract. Aerosol size distribution measurements from 0.03 μm to 25 μm diameter were taken at ambient humidity aboard the German research vessel, FS-Polarstern, during a transect from Bremerhaven in northern Germany, to Cape Town in South Africa across latitudes 53°32' N to 33°55' S, denoted cruise number ANT XXI/1. The data were segregated according to air mass history, wind speed and latitude. Under clean marine conditions, the averaged size distributions were generally in good agreement with those reported previously for diameters less than 0.5 μm and can be approximated by two log-normal modes, with significant variation in the mean modal diameters. Two short periods of tri-modal behaviour were observed. Above 0.5 μm, there is indication of a limit to the mechanical generation of marine aerosol over the range of wind speeds observed. A new technique to determine the errors associated with aerosol size distribution measurements using Poisson statistics has been applied to the dataset, providing a tool to determine the necessary sample or averaging times for correct interpretation of such data. Finally, the data were also used to investigate the loss rate of condensing gases with potentially important consequences for heterogeneous marine photochemical cycles.
Observations of total peroxy nitrates and aldehydes: measurement interpretation and inference of OH radical concentrations
Authors: Cleary P. A. , Wooldridge P. J. , Millet D. B. , Cohen R. C. , McKay M. , Goldstein A. H.
Published: April 2010

Abstract. We describe measurements of total peroxy nitrates (ΣPNs), NO2, O3 and several aldehydes at Granite Bay, California, during the Chemistry and Transport of the Sacramento Urban Plume (CATSUP) campaign, from 19 July–16 September 2001. We observed a strong photochemically driven variation of ΣPNs during the day with the median of 1.2 ppb at noon. Acetaldehyde, pentanal, hexanal and methacrolein had median abundances in the daytime of 1.2 ppb, 0.093 ppb, 0.14 ppb, and 0.27 ppb, respectively. We compare a steady state and a time dependent calculations of the dependence of ΣPNs on aldehydes, OH, NO and NO2 showing that the steady state calculations of are be accurate to ±30% between 10:00 a.m. and 06:00. We use the steady state calculation to investigate the composition of ΣPNs and the concentration of OH at Granite Bay. We find that PN molecules that have never been observed before make up an unreasonably large fraction of the ΣPNs unless we assume that there exists a PAN source that is much larger than the acetaldehyde source. We calculate that OH at the site varied between 1 and 6×106 molecules cm−3 at noon during the 8 weeks of the experiment.
Temperature climatology and trend estimates in the UTLS region as observed over a southern subtropical site, Durban, South Africa
Authors: Bencherif H. , Diab R. D. , Portafaix T. , Morel B. , Keckhut P. , Moorgawa A.
Published: April 2010

Abstract. Temperature trends in the UTLS region are under-reported, particularly in the Southern Hemisphere, and yet temperature is one of the most important indicators of changes in dynamical and radiative processes in the atmosphere. Here radiosonde data from Durban, South Africa (30.0° S, 30.9° E) over the period 1980 to 2001 (22 years) between 250 and 20 hPa are used to derive a mean temperature climatology and to determine trends. The seasonal cycle at the 250-hPa level is anti-correlated with the seasonal cycles at the 150-hPa and 100-hPa heights. The 100-hPa level (local tropopause) exhibits a minimum temperature in late summer and a maximum in winter, and closely corresponds to previous results for tropical regions. Based on a Fourier analysis, both the annual cycle (AO) and the semi-annual cycle (SAO) are dominant, although the former is about 4 times stronger. The AO is strongest at the 100-hPa height. A trend analysis reveals a cooling trend at almost all heights in the UTLS region, with a maximum cooling rate of 1.09±0.27 K per decade, at 70-hPa. Cooling rates are in good agreement with other studies and are slightly higher in summer than in winter.
Behaviour of tracer diffusion in simple atmospheric boundary layer models
Authors: Anderson P. S.
Published: April 2010

Abstract. 1-D profiles and time series from an idealised atmospheric boundary layer model are presented, which show agreement with measurements of polar photogenic NO and NO2. Diffusion models are increasingly being used as the framework for studying tropospheric air chemistry dynamics. Models based on standard boundary layer diffusivity profiles have an intrinsic behaviour that is not necessarily intuitive, due to the variation of turbulent diffusivity with height. The relatively simple model provides both a programming and a conceptual tool in the analysis of observed trace gas evolution. A time scale inherent in the model can be tuned by fitting model time series to observations. This scale is then applicable to the more physically simple but chemically complex zeroth order or box models of chemical interactions.
Temporal and spectral variation of desert dust and biomass burning aerosol scenes from 1995–2000 using GOME
Authors: de Graaf M. , Stammes P. , Aben I.
Published: April 2010

Abstract. Global Ozone Monitoring Experiment (GOME) Absorbing Aerosol Index (AAI) and AAI-related residue data were used to investigate areas with UV-absorbing aerosols. Time series of regionally averaged residues show the seasonal variation and trends of aerosols and clouds in climatologically important parts of the globe. GOME spectra were used to study scenes containing specific types of aerosols. AAI data are specifically sensitive to biomass burning aerosols (BBA) and desert dust aerosols (DDA). Areas where these aerosols are regularly found were analysed to find spectral fingerprints in the ultraviolet (UV), visible and near-infrared (near-IR), to establish an aerosol type classification of BBA and DDA. Spectral residues are different for BBA and DDA, but over deserts the surface albedo is dominant beyond the UV and spectral residues cannot be used over land. Over oceans, about half of the BBA scenes show a very high reflectance that is never observed for DDA scenes. However, in the case of low reflectance scenes BBA and DDA cannot be distinguished. This is in part due to the microphysical and optical properties of biomass burning aerosols, which are highly variable in time, making it difficult to specify them spectrally as one type. Because of their high hygroscopicity BBA are often found in the presence of clouds, which disturb the spectrum of the scenes. Desert dust aerosols are much less hygroscopic and behave spectrally more uniformly.
Regional pollution potentials of megacities and other major population centers
Authors: Lawrence M. G. , Butler T. M. , Steinkamp J. , Gurjar B. R. , Lelieveld J.
Published: April 2010

Abstract. Megacities and other major population centers represent important, concentrated sources of anthropogenic pollutants to the atmosphere, with consequences for both local air quality and for regional and global atmospheric chemistry. The tradeoff between the regional buildup of pollutants near their sources versus long-range export depends on meteorological characteristics which vary as a function of geographical location and season. Both horizontal and vertical transport contribute to pollutant export, and the overall degree of export is strongly governed by the chemical lifetimes of pollutants. We provide a first quantification of this tradeoff and the main factors influencing it in terms of "regional pollution potentials", metrics based on simulations of artificial, representative tracers using the 3-D global model MATCH (Model of Atmospheric Transport and Chemistry). The tracers have three different lifetimes (1, 10, and 100 days) and are emitted from 36 continental point sources representing the 30 current largest cities around the world plus 6 additional major population centers. Several key features of the export characteristics emerge: 1) long-range near-surface pollutant export is generally strongest in the middle and high latitudes, especially for source locations in Eurasia; 2) on the other hand, pollutant export to the upper troposphere is greatest in the tropics, due to transport by deep convection; 3) not only are there order of magnitude interregional differences, such as between low and high latitudes, but also often substantial intraregional differences, for instance between the sources in western India and Pakistan versus eastern India and Bangladesh; 4) contrary to what one might initially expect, efficient long-range export does not necessarily correspond with a more significant dilution of pollutants near their source, rather the amount of low-level, long-range export (e.g., below 1 km and beyond 1000 km) is well-correlated with exceedences of surface density thresholds on regional scales near the source (e.g., within ~1000 km), implying that pollutant buildup to high densities in the surface layer of the region surrounding the source location is more strongly influenced by vertical than horizontal transport.
Aerosol single-scattering albedo and asymmetry parameter from MFRSR observations during the ARM Aerosol IOP 2003
Authors: Kassianov E. I. , Ackerman T. P. , Barnard J. C. , Flynn C. J.
Published: April 2010

Abstract. Multi-filter Rotating Shadowband Radiometers (MFRSRs) provide routine measurements of the aerosol optical depth (τ) at six wavelengths (0.415, 0.5, 0.615, 0.673, 0.870 and 0.94 μm). The single-scattering albedo (ϖ0) is typically estimated from the MFRSR measurements by assuming the asymmetry parameter (g). In most instances, however, it is not easy to set an appropriate value of g due to its strong temporal and spatial variability. Here, we introduce and validate an updated version of our retrieval technique that allows one to estimate simultaneously ϖ0 and g for different types of aerosol. We use the aerosol and radiative properties obtained during the Atmospheric Radiation Measurement (ARM) Aerosol Intensive Operational Period (IOP) to validate our retrieval in two ways. First, the MFRSR-retrieved optical properties are compared with those obtained from independent surface, Aerosol Robotic Network (AERONET) and aircraft measurements. The MFRSR-retrieved optical properties are in reasonable agreement with these independent measurements. Second, we perform radiative closure experiments using the MFRSR-retrieved optical properties. The calculated broadband values of the direct and diffuse fluxes are comparable (~5 W/m2) to those obtained from measurements.
Modelling of nitrate particles: importance of sea salt
Authors: Myhre G. , Grini A.
Published: April 2010

Abstract. A thermo dynamical model for treatment of gas/aerosol partitioning of semi volatile inorganic aerosols has been implemented in a global chemistry and aerosol transport model (Oslo CTM2). The sulphur cycle and sea salt particles have been implemented earlier in the Oslo CTM2 and the focus of this study is on whether nitrate particles are formed as fine mode ammonium nitrate or react on existing sea salt particles. The model results show that ammonium nitrate particles play a non-negligible role in the total aerosol composition in certain industrialized regions and therefore have a significant local radiative forcing. On a global scale the aerosol optical depth of ammonium nitrate is relatively small due to limited availability of ammonia and reaction with sea salt particles. Inclusion of sea salt in the calculations reduces the aerosol optical depth and burden of ammonium nitrate particles by 25% on a global scale but with large regional variations.
Some ice nucleation characteristics of Asian and Saharan desert dust
Authors: Field P. R. , Möhler O. , Connolly P. , Krämer M. , Cotton R. , Heymsfield A. J. , Saathoff H. , Schnaiter M.
Published: April 2010

Abstract. The large (7 m×4 m cylinder) AIDA (Aerosol Interactions and Dynamics in the Atmosphere) cloud chamber facility at Forschungszentrum, Karlsruhe, Germany was used to test the ice nucleating ability of two desert dust samples from the Sahara and Asia. At temperatures warmer than −40°C droplets were formed before ice crystals formed, there was no deposition nucleation observed. At temperatures colder than −40°C both dust samples exhibited dual nucleation events that were observed during the same expansion experiment. The primary nucleation event occurred at ice saturation ratios of 1.1 to 1.3 and is likely to be a deposition nucleation mode. The secondary nucleation event occurred at ice saturation ratios between 1.35 and 1.5. It is unclear whether this ice nucleation event is via a further deposition mode or a condensation mode. The activated fractions of desert dust ranged from ~5–10% at −20°C to 20–40% at temperatures colder than −40°C. There was no obvious difference between the nucleation behaviour of the two dust samples.
Efficiency of the deposition mode ice nucleation on mineral dust particles
Authors: Möhler O. , Field P. R. , Connolly P. , Benz S. , Saathoff H. , Schnaiter M. , Wagner R. , Cotton R. , Krämer M. , Mangold A. , Heymsfield A. J.
Published: April 2010

Abstract. The deposition mode ice nucleation efficiency of various dust aerosols was investigated at cirrus cloud temperatures between 196 K and 223 K using the aerosol chamber facility AIDA (Aerosol Interaction and Dynamics in the Atmosphere). Arizona test dust (ATD) as a reference material and two dust samples from the Takla Makan desert in Asia (AD1) and Sahara (SD2) were used for the experiments at simulated cloud conditions. The dust particle sizes were almost lognormally distributed with mode diameters between 0.3 µm and 0.5 µm and geometric standard deviations between 1.6 and 1.9. Deposition ice nucleation was most efficient on ATD particles with ice-active particle fractions of about 0.6 and 0.8 at an ice saturation ratio Si<1.15 and temperatures of 223 K and 209 K, respectively. No significant change of the ice nucleation efficiency was found in up to three subsequent cycles of ice activation and evaporation with the same ATD aerosol. The desert dust samples SD2 and AD1 showed a significantly lower fraction of active deposition nuclei, about 0.25 at 223 K and Si<1.35. For all samples the ice activated aerosol fraction could be approximated by an exponential equation as function of Si. This formulation of ice activation spectra may be used to calculate the formation rate of ice crystals in models, if the number concentration of dust particles is known. More experimental work is needed to quantify the variability of the ice activation spectra as function of the temperature and dust particle properties.
Atmospheric carbonyl sulfide (OCS) variation from 1992–2004 by ground-based solar FTIR spectrometry
Authors: Deutscher N. M. , Jones N. B. , Griffith D. W. T. , Wood S. W. , Murcray F. J.
Published: April 2010

Abstract. Analysis of ground-based high-resolution solar FTIR absorption spectra from four sites was performed to determine trends and variability in OCS columns over the period 1992–2004. The sites were Wollongong, Australia (34.45° S, 150.88° E), Lauder, New Zealand (45.0° S, 169.7° E), Arrival Heights, Antarctica (77.8° S, 166.6° E) and Mauna Loa, Hawaii (19.5° N, 155.6° W). Small but significant long-term trends of −0.18±0.02% yr-1 above Hawaii, −0.30±0.12% yr-1 above Wollongong and −0.29±0.14% yr-1 above Lauder, were seen. No significant trend was seen above Arrival Heights. A large peak-to-peak seasonal difference observed in 1996–1997 above Wollongong and reported earlier was confirmed, but not repeated in later years. This seasonal feature correlated with particularly high water vapour columns present during late summer and early autumn, and suggests a link to warm oceanic airmasses. Seasonal variation of approximately 6% per year is observed in the total column in other years for all four locations.
Development and testing of a desert dust module in a regional climate model
Authors: Zakey A. S. , Solmon F. , Giorgi F.
Published: April 2010

Abstract. We develop a desert dust module and implement it within a regional climate model (RegCM). The dust module includes emission, transport, gravitational settling, wet and dry removal and calculations of dust optical properties. The coupled RegCM-dust model is applied to the simulation of two dust episodes over the Sahara region (a northeastern Africa dust outbreak, and a west Africa-Atlantic dust outbreak observed during the SHADE "Saharan Dust Experiment") as well as a three month simulation over an extended domain covering the Africa-Europe sector. Comparison with satellite and insitu (for SHADE) measurements shows that the model captures the main spatial (both horizontal and vertical) and temporal features of the dust distribution. The main model deficiency occurred in the SHADE case, when the model failed to accurately simulate the development of a mesoscale low associated with an easterly wave that contributed to the generation of the dust outbreak. The model appears suitable to conduct long term simulations of the effects of Saharan dust on African and European climate.
Imaging gravity waves in lower stratospheric AMSU-A radiances, Part 1: simple forward model
Authors: Eckermann S. D. , Wu D. L.
Published: April 2010

Abstract. Using a simplified model of in-orbit radiance acquisition by the Advanced Microwave Sounding Unit (AMSU-A), we derive three-dimensional temperature weighting functions for Channel 9 measurements (peaking at ~60–90 hPa) at all 30 cross-track beam positions and use them to investigate the sensitivity of these radiances to gravity waves. The vertical widths of the weighting functions limit detection to waves with vertical wavelengths of ≳10 km, with slightly better vertical wavelength sensitivity at the outermost scan angles due to the limb effect. Fourier Transforms of two-dimensional cross-track weighting functions reveal optimal sensitivity to cross-track wavelengths at the near-nadir scan angles, where horizontal measurement footprints are smallest. This sensitivity is greater for the AMSU-A on the Aqua satellite than for the identical instruments on the NOAA meteorological satellites, due to a lower orbit altitude and thus smaller horizontal footprints from antenna spreading. Small cross-track asymmetries in the radiance response to gravity waves are found that peak at the mid-range scan angles, with more symmetric responses at near-nadir and far off-nadir scan angles. Three-dimensional simulations show gravity wave oscillations imaged in horizontal AMSU-A radiance maps swept out by the scan pattern and satellite motion. A distorting curvature is added to imaged wave phase lines due to vertical variations in weighting function peaks with cross-track scan angle. This wave distortion is analogous to the well-known ''limb darkening'' and ''limb brightening'' of microwave radiances acquired from purely vertical background temperature profiles by cross-track scanners. Waves propagating along track are more visible in these images at the outermost scan angles than those propagating cross track, due to oversampling and narrower widths of the horizontal measurement footprints in the along track direction. Based on nominal noise floors and representative lower stratospheric wave temperature amplitudes, our modeling indicates that Channel 9 AMSU-A radiances can resolve and horizontally image gravity waves with horizontal wavelengths of ≳150 km and vertical wavelengths of ≳10 km.
Technical note: Evaluation of standard ultraviolet absorption ozone monitors in a polluted urban environment
Authors: Dunlea E. J. , Herndon S. C. , Nelson D. D. , Volkamer R. M. , Lamb B. K. , Allwine E. J. , Grutter M. , Ramos Villegas C. R. , Marquez C. , Blanco S. , Cardenas B. , Kolb C. E. , Molina L. T. , Molina M. J.
Published: April 2010

Abstract. The performance of the EPA Federal Equivalent Method (FEM) technique for monitoring ambient concentrations of O3 via ultraviolet absorption (UV) has been evaluated using data from the Mexico City Metropolitan Area (MCMA-2003) field campaign. Comparisons of UV O3 monitors with open path Differential Optical Absorption Spectroscopy (DOAS) and open path Fourier Transform Infrared (FTIR) spectroscopy instruments in two locations revealed average discrepancies in the measured concentrations of +13% to −10%. Excellent agreement of two separate open path DOAS measurements at one location indicated that spatial and temporal inhomogeneities were not substantially influencing comparisons of the point sampling and open path instruments. The poor agreement between the UV O3 monitors and the open path instruments was attributed to incorrect calibration factors for the UV monitors, although interferences could not be completely ruled out. Applying a linear correction to these calibration factors results in excellent agreement of the UV O3 monitors with the co-located open path measurements; regression slopes were 0.94 to 1.04 and associated R2 values were >0.89. A third UV O3 monitor suffered from large spurious interferences, which were attributed to extinction of UV radiation within the monitor by fine particles (<0.2 μm) due to a particulate filter with too large a pore size. The overall performance of this particular monitor was poor owing to a combination of interferences from a contaminated particle filter and/or ozone scrubber. Suggestions for improved operation practices of these UV O3 monitors and recommendations for future testing are made.
Measuring atmospheric CO2 from space using Full Spectral Initiation (FSI) WFM-DOAS
Authors: Barkley M. P. , Frieß U. , Monks P. S.
Published: April 2010

Abstract. Satellite measurements of atmospheric CO2 concentrations are a rapidly evolving area of scientific research which can help reduce the uncertainties in the global carbon cycle fluxes and provide insight into surface sources and sinks. One of the emerging CO2 measurement techniques is a relatively new retrieval algorithm called Weighting Function Modified Differential Optical Absorption Spectroscopy (WFM-DOAS) that has been developed by Buchwitz et al. (2000). This algorithm is designed to measure the total columns of CO2 (and other greenhouse gases) through the application to spectral measurements in the near infrared (NIR), made by the SCIAMACHY instrument on-board ENVISAT. The algorithm itself is based on fitting the logarithm of a model reference spectrum and its derivatives to the logarithm of the ratio of a measured nadir radiance and solar irradiance spectrum. In this work, a detailed error assessment of this technique has been conducted and it has been found necessary to include suitable a priori information within the retrieval in order to minimize the errors on the retrieved CO2 columns. Hence, a new CO2 retrieval algorithm called Full Spectral Initiation (FSI) WFM-DOAS has been developed which generates a reference spectrum for each individual SCIAMACHY observation using the known properties of the atmosphere and surface at the time of the measurement. Initial retrievals over Siberia during the summer of 2003 show that the measured CO2 columns are not biased from the input a priori data and that whilst the monthly averaged CO2 distributions contain a high degree of variability, they also contain significant spatial features.
Optical properties and mineralogical composition of different Saharan mineral dust samples: a laboratory study
Authors: Linke C. , Möhler O. , Veres A. , Mohácsi Á. , Bozóki Z. , Szabó G. , Schnaiter M.
Published: April 2010

Abstract. In aerosol chamber experiments optical properties of airborne mineral dust samples of defined size distribution were measured. Extinction coefficients (bext) and mass specific extinction cross sections (σext) were determined for Saharan dust samples from different locations. The results for σext were not very sensitive to the type of dust and varied at λ=550 nm between 3.3±0.4 m2 g−1 and 3.7±0.4 m2 g−1. The absorption coefficients (babs) and mass specific absorption cross sections (σabs) were determined with a novel multi-wavelength photo-acoustic absorption spectrometer (PAS). Between λ=266 nm and λ=1064 nm the derived single scattering albedos (SSA) ranged from 0.63±0.04 to 0.99±0.01. Additionally the chemical and mineralogical composition of the dust samples was analysed with special regard to the iron oxide phases hematite and goethite. At λ=266 nm the mineral dust sample without any detectable iron oxides showed a significantly higher SSA compared to the sample with a hematite content of 0.6 wt-%.