bluuebunny/crossref_metadata_2025 huggingface dataset:
Evaluation of near-tropopause ozone distributions in the Global Modeling Initiative combined stratosphere/troposphere model with ozonesonde data
Authors: Considine D. B. , Logan J. A. , Olsen M. A.
Published: April 2010

Abstract. The NASA Global Modeling Initiative has developed a combined stratosphere/troposphere chemistry and transport model which fully represents the processes governing atmospheric composition near the tropopause. We evaluate model ozone distributions near the tropopause, using two high vertical resolution monthly mean ozone profile climatologies constructed with ozonesonde data, one by averaging on pressure levels and the other relative to the thermal tropopause. Model ozone is high-biased at the SH tropical and NH midlatitude tropopause by ~45% in a 4° latitude × 5° longitude model simulation. Increasing the resolution to 2°×2.5° increases the NH tropopause high bias to ~60%, but decreases the tropical tropopause bias to ~30%, an effect of a better-resolved residual circulation. The tropopause ozone biases appear not to be due to an overly vigorous residual circulation or excessive stratosphere/troposphere exchange, but are more likely due to insufficient vertical resolution or excessive vertical diffusion near the tropopause. In the upper troposphere and lower stratosphere, model/measurement intercomparisons are strongly affected by the averaging technique. NH and tropical mean model lower stratospheric biases are <20%. In the upper troposphere, the 2°×2.5° simulation exhibits mean high biases of ~20% and~35% during April in the tropics and NH midlatitudes, respectively, compared to the pressure-averaged climatology. However, relative-to-tropopause averaging produces upper troposphere high biases of ~30% and 70% in the tropics and NH midlatitudes. This is because relative-to-tropopause averaging better preserves large cross-tropopause O3 gradients, which are seen in the daily sonde data, but not in daily model profiles. The relative annual cycle of ozone near the tropopause is reproduced very well in the model Northern Hemisphere midlatitudes. In the tropics, the model amplitude of the near-tropopause annual cycle is weak. This is likely due to the annual amplitude of mean vertical upwelling near the tropopause, which analysis suggests is ~30% weaker than in the real atmosphere.
Ship emitted NO2 in the Indian Ocean: comparison of model results with satellite data
Authors: Franke K. , Richter A. , Bovensmann H. , Eyring V. , Jöckel P. , Burrows J. P.
Published: April 2010

Abstract. An inventory of NOx emission from international shipping has been evaluated by comparing NO2 tropospheric columns derived from the satellite instruments SCIAMACHY (January 2003 to February 2008), GOME (January 1996 to June 2003), and GOME-2 (March 2007 to February 2008) to NO2 columns calculated with the atmospheric chemistry general circulation model ECHAM5/MESSy1 (January 2000 to October 2005). The data set from SCIAMACHY yields the first monthly analysis of ship induced NO2 enhancements in the Indian Ocean. For both data and model consistently the tropospheric excess method was used to obtain mean NO2 columns over the shipping lane from India to Indonesia, and over two ship free regions, the Bay of Bengal and the central Indian Ocean. In general, the model simulates the differences between the regions affected by ship pollution and ship free regions reasonably well. Minor discrepancies between model results and satellite data were identified during biomass burning seasons in March to May over India and the Indochinese Peninsula and August to October over Indonesia. We conclude that the NOx ship emission inventory used in this study is a good approximation of NOx ship emissions in the Indian Ocean for the years 2002 to 2007. It assumes that around 6 Tg(N) yr−1 are emitted by international shipping globally, resulting in 90 Gg(N) yr−1 in the region of interest when using Automated Mutual Assistance Vessel Rescue System (AMVER) or 72 Gg(N) yr−1 when using the International Comprehensive Ocean-Atmosphere Data Set (ICOADS) as spatial proxy. The results do not support some previously published lower ship emissions estimates of 3–4 Tg(N) yr−1 globally, making this study the first that evaluates atmospheric response to NOx ship emission estimates from space.
Uncertainty in global CCN concentrations from uncertain aerosol nucleation and primary emission rates
Authors: Pierce J. R. , Adams P. J.
Published: April 2010

Abstract. The indirect effect of aerosols on climate is highly uncertain and limits our ability to assess anthropogenic climate change. The foundation of this uncertainty is uncertainty in the number of cloud condensation nuclei (CCN), which itself stems from uncertainty in aerosol nucleation, primary emission and growth rates. In this paper, we use a global general circulation model with aerosol microphysics to assess how the uncertainties in aerosol nucleation, emission and growth rates affect our prediction of CCN(0.2%) concentrations. Using two nucleation rate parameterizations that differ in globally averaged nucleation rate by 106, the tropospheric average CCN(0.2%) concentrations vary by 17% and the boundary layer average vary by 12%. This sensitivity of tropospheric average CCN(0.2%) to the nucleation parameterizations increases to 33% and 20% when the total primary emissions are reduced by a factor of 3 and the SOA condensation rates are increased by a factor of 3.5, respectively. These results show that it is necessary to understand better global nucleation rates when determining CCN concentrations. When primary emissions rates are varied by a factor of 3 while using the slower nucleation rate parameterization, tropospheric average CCN(0.2%) concentrations also vary by 17%, but boundary layer average vary by 40%. Using the faster nucleation rate parameterization, these changes drop to 3% and 22%, respectively. These results show the importance of reducing uncertainties in primary emissions, which appear from these results to be somewhat more important for CCN than the much larger uncertainties in nucleation. These results also show that uncertainties in nucleation and primary emissions are more important when sufficient condensable material is available to grow them to CCN sizes. The percent change in CCN(0.2%) concentration between pre-industrial times and present day does not depend greatly on the nucleation rate parameterization used for our base case scenarios; however, because other factors, such as primary emissions and SOA, are uncertain in both time periods, this may be a coincidence.
Tropospheric NO2 column densities deduced from zenith-sky DOAS measurements in Shanghai, China, and their application to satellite validation
Authors: Chen D. , Zhou B. , Beirle S. , Chen L. M. , Wagner T.
Published: April 2010

Abstract. Zenith-sky scattered sunlight observations using differential optical absorption spectroscopy (DOAS) technique were carried out in Shanghai, China (31.3° N, 121.5° E) since December 2006. At this polluted urban site, the measurement provided NO2 total columns in the daytime. Here, we present a new method to extract time series of tropospheric vertical column densities (VCD) of NO2 from these observations. The derived tropospheric NO2 VCD is an important quantity for the estimation of emissions and for the validation of satellite observations. Our method makes use of assumptions on the relative NO2 height profiles and on the diurnal variation of the stratospheric NO2 VCD. The influence of these parameters on the retrieved tropospheric NO2 VCD is discussed; for a polluted site like Shanghai, the accuracy of our method is estimated to be <20% for solar zenith angle (SZA) lower than 85°. From simultaneously performed long-path DOAS measurement, the NO2 surface concentration at the same site was observed and the corresponding tropospheric NO2 VCD was estimated using the assumed seasonal NO2 profiles in the planetary boundary layer (PBL). By making a comparison between the tropospheric NO2 VCD from zenith-sky and long-path DOAS measurements, it was found that the former provided more realistic information about total tropospheric pollution than the latter, so it's more suitable for satellite data validation than the in situ measurement. A comparison between the tropospheric NO2 VCD from ground-based zenith-sky measurement and SCIAMACHY was also made. Satellite validation for a strongly polluted area is highly needed, but exhibits also a great challenge. Our comparison showed good agreement, considering in particular the different spatial resolutions between the two measurements.
Carbonyl sulfide in air extracted from a South Pole ice core: a 2000 year record
Authors: Aydin M. , Williams M. B. , Tatum C. , Saltzman E. S.
Published: April 2010

Abstract. In this study, we present carbonyl sulfide (COS) measurements from an ice core drilled near South Pole, East Antarctica (SPRESSO). The samples are from 135–291 m, with estimated mean COS ages ranging from 278 to 2155 years before present (defined as 2000 C.E.). When combined with the previous records of COS from Antarctic ice cores and firn air, the current data provide a continuous record of COS extending beyond the last two millennia. The general agreement between ice cores, firn air, and modern air measurements supports the idea that polar ice is a valid archive for paleoatmospheric COS. The average COS mixing ratio of the SPRESSO data set is (331±18) ppt (parts per trillion as mol/mol, ±1σ, n=100), excluding 6 outliers. These data confirm earlier firn air and ice core measurements indicating that the late 20th century COS levels of 500 ppt are greatly increased over preindustrial levels and represent the highest atmospheric levels over the past 2000 years. The data also provide evidence of climate-related variability on centennial time-scales, with relative maxima at the peaks of Medieval Climate Anomaly and Little Ice Age. There is evidence for a long-term increasing trend in COS of 1.8 ppt per 100 years. Further ice core studies will be needed to determine whether this trend reflects secular variability in atmospheric COS, or a slow post-depositional chemical loss of COS in the ice core.
Evaluating the performance of pyrogenic and biogenic emission inventories against one decade of space-based formaldehyde columns
Authors: Stavrakou T. , Müller J.-F. , De Smedt I. , Van Roozendael M. , van der Werf G. R. , Giglio L. , Guenther A.
Published: April 2010

Abstract. A new one-decade dataset of formaldehyde (HCHO) columns retrieved from GOME and SCIAMACHY is compared with HCHO columns simulated by an updated version of the IMAGES global chemical transport model. This model version includes an optimized chemical scheme with respect to HCHO production, where the short-term and final HCHO yields from pyrogenically emitted non-methane volatile organic compounds (NMVOCs) are estimated from the Master Chemical Mechanism (MCM) and an explicit speciation profile of pyrogenic emissions. The model is driven by the Global Fire Emissions Database (GFED) version 1 or 2 for biomass burning, whereas biogenic emissions are provided either by the Global Emissions Inventory Activity (GEIA), or by a newly developed inventory based on the Model of Emissions of Gases and Aerosols from Nature (MEGAN) algorithms driven by meteorological fields from the European Centre for Medium-Range Weather Forecasts (ECMWF). The comparisons focus on tropical ecosystems, North America and China, which experience strong biogenic and biomass burning NMVOC emissions reflected in the enhanced measured HCHO columns. These comparisons aim at testing the ability of the model to reproduce the observed features of the HCHO distribution on the global scale and at providing a first assessment of the performance of the current emission inventories. The high correlation coefficients (r>0.8) between the observed and simulated columns over most regions indicate a very good consistency between the model, the implemented inventories and the HCHO dataset. The use of the MEGAN-ECMWF inventory improves the model/data agreement in almost all regions, but biases persist over parts of Africa and the Northern Australia. Although neither GFED version is consistent with the data over all regions, a better match is achieved over Indonesia and Southern Africa when GFEDv2 is used, but GFEDv1 succeeds better in getting the correct seasonal patterns and intensities of the fire episodes over the Amazon basin, as reflected by the higher correlations calculated in this region.
Temporal trends of anthropogenic SO2 emitted by non-ferrous metal smelters in Peru and Russia estimated from Satellite observations
Authors: Khokhar M. F. , Platt U. , Wagner T.
Published: April 2010

Abstract. We report on satellite observations of atmospheric Sulfur Dioxide (SO2) emitted from metal smelting industries in Peru, South America and Siberia, Russia. Most of the non-ferrous metal ores are sulfidic and during the smelting process the sulfur is emitted as SO2. In addition to Norilsk, Russia, Peruvian copper smelters are among the most polluting point sources in the world. We retrieve SO2 column amounts from spectra of the Global Ozone Monitoring Experiment (GOME) on the Earth Research Satellite 2 (ERS-2) for the years 1996 to 2002 using an algorithm based on differential Optical Absorption Spectroscopy (DOAS). Areas of enhanced SO2 column amounts are clearly identified on a 7-years mean map of GOME observations over the regions with La Oroya and Ilo copper smelters of Peru and Norilsk smelters of Russia. Since the instrument sensitivity is highly dependent on surface albedo, SO2 vertical profile, solar zenith angle (SZA), wavelength, clouds, and aerosol, radiative transfer modelling is used to convert the analysed slant column densities into vertical column densities. In this study, the full spherical Monte-Carlo radiative transport model TRACY-II is used for SO2 AMF calculation. GOME data is analysed in further detail by calculating time series over these regions. For the different locations, the results demonstrate both, increasing and decreasing trends in the SO2 column amounts over the time period of 1996–2002. The decreasing trend for the Ilo copper smelter is in good agreement with implemented measures for emission reductions. However, even for the cases with decreasing trends, these point sources are still a dominant source of anthropogenic SO2 emissions in their region. For the smelters in Peru, the potential influence due to SO2 emission by the nearby volcanoes is investigated and found to be negligible.
Ozone Monitoring Instrument spectral UV irradiance products: comparison with ground based measurements at an urban environment
Authors: Kazadzis S. , Bais A. , Arola A. , Krotkov N. , Kouremeti N. , Meleti C.
Published: April 2010

Abstract. We have compared spectral ultraviolet overpass irradiances from the Ozone Monitoring Instruments (OMI) against ground-based Brewer measurements at Thessaloniki, Greece from September 2004 to December 2007. It is demonstrated that OMI overestimates UV irradiances by 30%, 17% and 13% for 305 nm, 324 nm, and 380 nm respectively and 20% for erythemally weighted irradiance. The bias between OMI and Brewer increases with increasing aerosol absorption optical thickness. We present methodologies that can be applied for correcting this bias based on experimental results derived from the comparison period and also theoretical approaches using radiative transfer model calculations. All correction approaches minimize the bias and the standard deviation of the ratio OMI versus Brewer ratio. According to the results, the best correction approach suggests that the OMI UV product has to be multiplied by a correction factor CA(λ) are in the order of 0.8, 0.88 and 0.9 for 305 nm, 324 nm and 380 nm respectively. Limitations and possibilities for applying such methodologies in a global scale are also discussed.
MAX-DOAS measurements in southern China: 1. automated aerosol profile retrieval using oxygen dimers absorptions
Authors: Li X. , Brauers T. , Shao M. , Garland R. M. , Wagner T. , Deutschmann T. , Wahner A.
Published: April 2010

Abstract. We performed MAX-DOAS measurements during the PRiDe-PRD2006 campaign in the Pearl River Delta region 50 km north of Guangzhou, China, for 4 weeks in June 2006. We used an instrument which simultaneously sampled the wavelength range from 292 nm to 443 nm at 7 different elevation angles between 3° and 90°. Here we show that the O4 (O2 dimer) absorption at 360 nm can be used to retrieve the aerosol extinction and the height of the boundary layer. A comparison with simultaneously recorded, ground based nephelometer data shows an excellent agreement.
Hourly resolved cloud modification factors in the ultraviolet
Authors: Staiger H. , den Outer P. N. , Bais A. F. , Feister U. , Johnsen B. , Vuilleumier L.
Published: April 2010

Abstract. Cloud impacts on the transfer of Ultraviolet (UV) radiation through the atmosphere can be assessed using a cloud modification factor (CMF). The total global solar irradiation has proven to be a solid basis to derive CMF's for the UV radiation (UV_CMF). Total global irradiance is frequently measured and forecasted by numerical weather prediction systems. Its advantage compared to for instance cloud cover is that measured solar global irradiance contains already the effect of multiple reflection between cloud layers, reflection between the sides of the clouds, as well as the distinct difference whether the solar disc is obscured by clouds or not. In the UV range clouds decrease the irradiance to a lesser extent than in the visible and infrared spectral range; Rayleigh scattering in the atmosphere yields a larger fraction of scatter radiation compared to that of light and infrared, hence, obscuring the solar disc will not totally block out the irradiation. Thus the relationship between CMF's for solar radiation and for UV-radiation is not straight forwards, but will depend on e.g. the solar zenith angle (SZA) and wavelength band or action spectrum in the UV considered. Den Outer et al. (2005) provide a UV_CMF algorithm on a daily base accounting for these influences. It requires as input a daily CMF in total global radiation (SOL_CMF) and the SZA at noon. The calculation of SOL-CMF uses the clear sky algorithm of the European Solar Radiation Atlas to account for varying turbidity impacts. The algorithm's capability to derive hourly UV_CMF's based on the SZA at the corresponding hour and its worldwide applicability is validated using hourly resolved observational data retrieved from the databases of the COST-Action 726 on "Long term changes and climatology of UV radiation over Europe" and the USDA UV-B Monitoring and Research Program. The model performance for hourly resolution is shown to be comparable in absolute and relative deviations from a measured mean smoothed dependent on SZA with the well performing daily models of the COST-726 model intercomparison (Koepke et al., 2006).
Spatio-temporal variability and principal components of the particle number size distribution in an urban atmosphere
Authors: Costabile F. , Birmili W. , Klose S. , Tuch T. , Wehner B. , Wiedensohler A. , Franck U. , König K. , Sonntag A.
Published: April 2010

Abstract. Due to the presence of diffusive anthropogenic sources in urban areas, the spatio-temporal variability of fine (diameter <1 μm) and ultrafine (<0.1 μm) aerosol particles has been a challenging issue in particle exposure assessment as well as atmospheric research in general. We examined number size distributions of atmospheric aerosol particles (size range 3–800 nm) that were measured simultaneously at a maximum of eight observation sites in and around a city in Central Europe (Leipzig, Germany). Two main experiments were conducted with different time span and number of observation sites (2 years at 3 sites; 1 month at 8 sites). A general observation was that the particle number size distribution varied in time and space in a complex fashion as a result of interaction between local and far-range sources, and the meteorological conditions. To identify statistically independent factors in the urban aerosol, different runs of principal component analysis were conducted encompassing aerosol, gas phase, and meteorological parameters from the multiple sites. Several of the resulting principal components, outstanding with respect to their temporal persistence and spatial coverage, could be associated with aerosol particle modes: a first accumulation mode ("droplet mode", 300–800 nm), considered to be the result of liquid phase processes and far-range transport; a second accumulation mode (centered around diameters 90–250 nm), considered to result from primary emissions as well as aging through condensation and coagulation; an Aitken mode (30–200 nm) linked to urban traffic emissions in addition to an urban and a rural Aitken mode; a nucleation mode (5–20 nm) linked to urban traffic emissions; nucleation modes (3–20 nm) linked to photochemically induced particle formation; an aged nucleation mode (10–50 nm). A number of additional components were identified to represent only local sources at a single site each, or infrequent phenomena. In summary, the analysis of size distributions of high time and size resolution yielded a surprising wealth of statistical aerosol components occurring in the urban atmosphere over one single city. Meanwhile, satisfactory physical explanations could be found for the components with the greatest temporal persistence and spatial coverage. Therefore a paradigm on the behaviour of sub-μm urban aerosol particles is proposed, with recommendations how to efficiently monitor individual sub-fractions across an entire city.
Homogeneous vs. heterogeneous nucleation in water-dicarboxylic acid systems
Authors: Hienola A. I. , Vehkamäki H. , Riipinen I. , Kulmala M.
Published: April 2010

Abstract. Binary heterogeneous nucleation of water-succinic/glutaric/malonic/adipic acid on nanometer-sized particles is investigated within the frame of classical heterogeneous nucleation theory. Homogeneous nucleation is also included for comparison. It is found that the nucleation probabilities depend on the contact angle and on the size of the seed particles. New thermodynamical properties, such as saturation vapor pressure, density and surface tension for all the dicarboxylic acid aqueous solutions are included in the calculations. While the new surface tension and density formulations do not bring any significant difference in the computed nucleation rate for homogeneous nucleation for succinic and glutaric acids, the use of the newly derived equations for the vapor pressure decrease the acid concentrations in gas phase with 3 orders of magnitude. According to our calculations, the binary heterogeneous nucleation of succinic acid-water and glutaric acid-water – although it requires a 3–4 orders of magnitude lower vapor concentrations than the homogeneous nucleation – cannot take place in atmospheric conditions. On the other hand binary homogeneous nucleation of adipic acid-water systems might be possible in conditions occuring in upper boundary layer. However, a more detailed characterization of the interaction between the surface and the molecules of the nucleating vapor should be considered in the future.
Relating observations of contrail persistence to numerical weather analysis output
Authors: Duda D. P. , Palikonda R. , Minnis P.
Published: April 2010

Abstract. The potential for using high-resolution meteorological data from two operational numerical weather analyses (NWA) to diagnose and predict persistent contrail formation is evaluated using two independent contrail observation databases. Contrail occurrence statistics derived from surface and satellite observations between April 2004 and June 2005 are matched to the humidity, vertical velocity, wind shear and atmospheric stability derived from analyses from the Rapid Update Cycle (RUC) and the Advanced Regional Prediction System (ARPS) models. The relationships between contrail occurrence and the NWA-derived statistics are analyzed to determine under which atmospheric conditions persistent contrail formation is favored within NWAs. Humidity is the most important factor determining whether contrails are short-lived or persistent, and persistent contrails are more likely to appear when vertical velocities are positive, and more likely to spread when the atmosphere is less stable. Although artificial upper limits on upper tropospheric humidity within the NWAs prevent a direct quantitative agreement of model data with contrail formation theory, logistic regression or similar statistical methods may improve the prediction of contrail occurrence.
Contribution of atmospheric processes affecting the dynamics of air pollution in south-western Europe during a typical summertime photochemical episode
Authors: Gonçalves M. , Jiménez-Guerrero P. , Baldasano J. M.
Published: April 2010

Abstract. The southern Mediterranean region frequently experiences critical levels of photochemical pollutants during summertime. In order to account for the contribution of different atmospheric processes during this type of episodes, the WRF-ARW/HERMES/CMAQ modelling system was applied with high resolution (1 km2, 33 sigma vertical layers, 1 h) to assess the different dynamics in a coastal environment and an inland-continental zone: the North-eastern and Central Iberian Peninsula (NEIP and CIP, respectively). The former is characterized by a very complex terrain, while the latter behaves as a flat area, which clearly affects the pattern of local flows. A representative type of photochemical pollution episode (occurring over 78% of summer days) which occurred during 17–18 June 2004 is selected as the study period. The CMAQ Integrated Process Rate provides the hourly contributions of atmospheric processes to net O3, NOx and NMVOCs concentrations. The O3 photochemical formation occurs mainly in downwind areas from the main NOx emission sources during midday. At surface level it accounts for 50 to 75 μg m−3 h−1. The urban areas and main roads, as main sources of NOx emissions, act as O3 sinks, quenching up to −200 μg m−3 per hour during the traffic circulation peaks. The O3 concentration gradient generated, larger during daytime, increases the contribution of diffusion processes to ground-level O3 (up to 200 μg m−3 h−1 fluxes, mainly from upper vertical layers). The maximum positive contributions of gas-phase chemistry to O3 occur in the coastal domain at high levels, while in the continental domain they take place in the whole atmospheric column under the PBL. The transport of ozone precursors by advective flows sets the location of the maximum O3 surface concentrations. The O3 chemical formation involves the oxidation of less NMVOCs in the NEIP than in the CIP domains, due to differences in chemical sensitivity between these areas. The dry deposition is an important sink in the lowest layer of the model, together with vertical diffusion flows. Finally, the contributions from cloud processes, wet deposition and heterogeneous chemistry are negligible during the whole episode, characterized by a high solar radiation and neither precipitation nor cloudiness. This process analysis provides new quantitative information about the origin of the peaks of O3 and its precursors, aiding the design of abatement strategies in south-western Europe.
Evidence of mineral dust altering cloud microphysics and precipitation
Authors: Min Q.-L. , Li R. , Lin B. , Joseph E. , Wang S. , Hu Y. , Morris V. , Chang F.
Published: April 2010

Abstract. Multi-platform and multi-sensor observations are employed to investigate the impact of mineral dust on cloud microphysical and precipitation processes in mesoscale convective systems. It is clearly evident that for a given convection strength,small hydrometeors were more prevalent in the stratiform rain regions with dust than in those regions that were dust free. Evidence of abundant cloud ice particles in the dust sector, particularly at altitudes where heterogeneous nucleation process of mineral dust prevails, further supports the observed changes of precipitation. The consequences of the microphysical effects of the dust aerosols were to shift the precipitation size spectrum from heavy precipitation to light precipitation and ultimately suppressing precipitation.
Coastal and open ocean aerosol characteristics: investigating the representativeness of coastal aerosol sampling over the North-East Atlantic Ocean
Authors: Rinaldi M. , Facchini M. C. , Decesari S. , Carbone C. , Finessi E. , Mircea M. , Fuzzi S. , Ceburnis D. , Ehn M. , Kulmala M. , de Leeuw G. , O'Dowd C. D.
Published: April 2010

Abstract. In order to achieve a better understanding of the modifications of the physical and chemical properties of marine aerosol particles during transport from offshore to the coast, size distribution and chemical composition were measured concurrently in clean air masses over the open North Atlantic Ocean and at an Irish coastal site. Open ocean sampling was performed on board the oceanographic vessel Celtic Explorer sailing 100–300 km off the Irish west coast, while coastal measurements were performed at the Mace Head GAW station. The experiment took place between 11 June and 6 July 2006, during the period of phytoplankton bloom. The number size distribution and size-resolved chemical composition of coastal and open ocean samples were very similar, indicating homogeneous physical and chemical aerosol properties over a wide region in the marine boundary layer. The results also show that submicron chemical and physical aerosol properties measured at the coastal Mace Head Atmospheric Research Station were not unduly influenced by coastal artefacts and are thus representative of open water properties. Greater differences between the coastal site and the open ocean were observed for the aerosol supermicron sea spray components; this could be due to a variety of reasons, ranging from higher local wind speeds at the coastal site over the comparison period, to differences in sampling heights and increased local surf-zone production. Evidence of ageing processes was observed: at the costal site the ratio between non-sea-salt sulphate and methanesulphonic acid was higher, and the aerosol water soluble organic compounds were more oxidized than in the open ocean.
The influence of European pollution on ozone in the Near East and northern Africa
Authors: Duncan B. N. , West J. J. , Yoshida Y. , Fiore A. M. , Ziemke J. R.
Published: April 2010

Abstract. We present a modeling study of the long-range transport of pollution from Europe, showing that European emissions regularly elevate surface ozone by as much as 20 ppbv in summer in northern Africa and the Near East. European emissions cause 50–150 additional violations per year (i.e., above those that would occur without European pollution) of the European health standard for ozone (8-h average >120 μg/m3 or ~60 ppbv) in northern Africa and the Near East. We estimate that 19 000 additional mortalities occur annually in these regions from exposure to European ozone pollution and 50 000 additional deaths globally; the majority of the additional deaths occurs outside of Europe. Much of the pollution from Europe is exported southward at low altitudes in summer to the Mediterranean Sea, northern Africa and the Near East, regions with favorable photochemical environments for ozone production. Our results suggest that assessments of the human health benefits of reducing ozone precursor emissions in Europe should include effects outside of Europe, and that comprehensive planning to improve air quality in northern Africa and the Near East likely needs to address European emissions. We also show that the tropospheric ozone column data product derived from the OMI and MLS instruments is currently of limited value for air quality applications as the portion of the column above the boundary layer and below the tropopause is large and variable, effectively obscuring the boundary layer signal.
The governing processes and timescales of stratosphere-to-troposphere transport and its contribution to ozone in the Arctic troposphere
Authors: Liang Q. , Douglass A. R. , Duncan B. N. , Stolarski R. S. , Witte J. C.
Published: April 2010

Abstract. We used the seasonality of a combination of atmospheric trace gases and idealized tracers to examine stratosphere-to-troposphere transport and its influence on tropospheric composition in the Arctic. Maximum stratosphere-to-troposphere transport of CFCs and O3 occurs in April as driven by the Brewer-Dobson circulation. Stratosphere-troposphere exchange (STE) occurs predominantly between 40° N to 80° N with stratospheric influx in the mid-latitudes (30–70° N) accounting for 67–81% of the air of stratospheric origin in the Northern Hemisphere extratropical troposphere. Transport from the lower stratosphere to the lower troposphere (LT) takes three months on average, one month to cross the tropopause, the second month to travel from the upper troposphere (UT) to the middle troposphere (MT), and the third month to reach the LT. During downward transport, the seasonality of a trace gas can be greatly impacted by wet removal and chemistry. A comparison of idealized tracers with varying lifetimes suggests that when initialized with the same concentrations and seasonal cycles at the tropopause, trace gases that have shorter lifetimes display lower concentrations, smaller amplitudes, and earlier seasonal maxima during transport to the LT. STE contributes to O3 in the Arctic troposphere directly from the transport of O3 and indirectly from the transport of NOy. Direct transport of O3 from the stratosphere accounts for 78% of O3 in the Arctic UT with maximum contributions occurring from March to May. The stratospheric contribution decreases significantly in the MT/LT (20–25% of total O3) and shows a very weak March–April maximum. Our NOx budget analysis in the Arctic UT shows that during spring and summer, the stratospheric injection of NOy-rich air increases NOx concentrations above the 20 pptv threshold level, thereby shifting the Arctic UT from a regime of net photochemical ozone loss to one of net production with rates as high as +16 ppbv/month.
Properties of atmospheric humic-like substances – water system
Authors: Salma I. , Ocskay R. , Láng G.
Published: April 2010

Abstract. Urban-type PM2.5-fraction aerosol samples were collected and samples of pure atmospheric humic-like substances (HULIS) were isolated from them. Atmospheric concentrations of organic carbon (OC), water soluble organic carbon (WSOC) and HULIS were determined, and UV/Vis spectroscopic properties, solubility and conductivity of HULIS in aqueous samples were investigated. Mean atmospheric concentrations of OC and WSOC were 8.5 and 4.6 μg m−3, respectively. Hydrophilic WSOC accounted for 39% of WSOC, carbon in HULIS made up 47% of WSOC, and 14% of WSOC was retained on the separation column by irreversible adsorption. Average molecular mass and aromatic carbon abundance of HULIS were both estimated from molar absorptivity to be 556 Da and 12%, respectively. Both results are substantially smaller than for standard reference fulvic acids, which imply different mechanisms for the formation processes of atmospheric HULIS and aquatic or terrestrial humic matter. HULIS were found to be water soluble as ionic unimers with a saturation concentration of 2–3 g l−1. Their solubility increased again with total HULIS concentration being above approximately 4 g l−1, which was most likely explained by the formation of HULIS aggregates. Solubility increased linearly from approximately 5 up to 20 g l−1 of dissolved HULIS concentration. The ionic dissolution was confirmed by electrochemical conductivity in the investigated concentration interval. Limiting molar conductivity was extrapolated and this was utilized to determine the apparent dissociation degree of HULIS for different concentrations. The dissociation degree was further applied to derive the concentration dependence of the van't Hoff factor of HULIS. The van't Hoff factor decreased monotonically with HULIS concentration; the decrease was substantial for dilute solutions and the relationship became weak for rather concentrated solutions.
Calibrated sky imager for aerosol optical properties determination
Authors: Cazorla A. , Shields J. E. , Karr M. E. , Burden A. , Olmo F. J. , Alados-Arboledas L.
Published: April 2010

Abstract. The calibrated ground-based sky imager developed in the Marine Physical Laboratory, the Whole Sky Imager (WSI), has been tested to determine optical properties of the atmospheric aerosol. Different neural network-based models calculate the aerosol optical depth (AOD) for three wavelengths using the radiance extracted from the principal plane of sky images from the WSI as input parameters. The models use data from a CIMEL CE318 photometer for training and validation and the wavelengths used correspond to the closest wavelengths in both instruments. The spectral dependency of the AOD, characterized by the Ångström exponent α in the interval 440–870, is also derived using the standard AERONET procedure and also with a neural network-based model using the values obtained with a CIMEL CE318. The deviations between the WSI derived AOD and the AOD retrieved by AERONET are within the nominal uncertainty assigned to the AERONET AOD calculation (±0.01), in 80% of the cases. The explanation of data variance by the model is over 92% in all cases. In the case of α, the deviation is within the uncertainty assigned to the AERONET α (±0.1) in 50% for the standard method and 84% for the neural network-based model. The explanation of data variance by the model is 63% for the standard method and 77% for the neural network-based model.
An evaluation of the simulation of the edge of the Antarctic vortex by chemistry-climate models
Authors: Struthers H. , Bodeker G. E. , Austin J. , Bekki S. , Cionni I. , Dameris M. , Giorgetta M. A. , Grewe V. , Lefèvre F. , Lott F. , Manzini E. , Peter T. , Rozanov E. , Schraner M.
Published: April 2010

Abstract. The dynamical barrier to meridional mixing at the edge of the Antarctic spring stratospheric vortex is examined. Diagnostics are presented which demonstrate the link between the shape of the meridional mixing barrier at the edge of the vortex and the meridional gradients in total column ozone across the vortex edge. Results derived from reanalysis and measurement data sets are compared with equivalent diagnostics from five coupled chemistry-climate models to test how well the models capture the interaction between the dynamical structure of the stratospheric vortex and the chemical processes occurring within the vortex. Results show that the accuracy of the simulation of the dynamical vortex edge varies widely amongst the models studied here. This affects the ability of the models to simulate the large observed meridional gradients in total column ozone. Three of the models in this study simulated the inner edge of the vortex to be more than 7° closer to the pole than observed. This is expected to have important implications for how well these models simulate the extent of severe springtime ozone loss that occurs within the Antarctic vortex.
Sulfuric acid and OH concentrations in a boreal forest site
Authors: Petäjä T. , Mauldin, III R. L. , Kosciuch E. , McGrath J. , Nieminen T. , Boy M. , Adamov A. , Kotiaho T. , Kulmala M.
Published: April 2010

Abstract. As demonstrated in a number of investigations, gaseous sulfuric acid plays a central role in atmospheric aerosol formation. Using chemical ionization mass spectrometer the gas-phase sulfuric acid and OH concentration were measured in Hyytiälä, SMEAR II station, Southern Finland during 24 March to 28 June 2007. Clear diurnal cycles were observed as well as differences between new particle formation event days and non-event days. The typical daily maximum concentrations of gas phase sulfuric acid varied from 3·105 to 2·106 molec cm−3 between non-event and event days. Noon-time OH concentrations varied from 3–6·105 molec cm−3 and not a clear difference between event and non-events was detected. Since it is still challenging to measure sulfuric acid, and due to its significant role in atmospheric particle formation, three different proxies and one chemical box model calculation were compared to the measured data. The proxies for the sulfuric acid concentration worked reasonably, and with caution, could be applied to other environments.
Mechanisms controlling surface ozone over East Asia: a multiscale study coupling regional and global chemical transport models
Authors: Lin M. , Holloway T. , Oki T. , Streets D. G. , Richter A.
Published: April 2010

Abstract. Mechanisms controlling surface ozone (O3) over East Asia are examined using the regional Community Multiscale Air Quality (CMAQ) model at two horizontal scales: 81 km and 27 km. Through sensitivity studies and comparison with recently available satellite data and surface measurements in China and Japan, we find that the O3 budget over East Asia shows complex interactions among photochemical production, regional transport, meteorological conditions, burning of agricultural residues, and global inflows. For example, wintertime surface O3 over northern domain is sensitive to boundary conditions derived from the MOZART (Model for Ozone and Related Tracers) global model, whereas summertime O3 budget is controlled by the competitive processes between photochemical production and monsoonal intrusion of low-O3 marine air masses from tropical Pacific. We find that simulated surface O3 for 2001 does not exhibit the same sharp drop in July and August concentrations that is observed at two mountaintop sites (Tai and Hua) for 2004 and Beijing for 1995–2005. CMAQ sensitivity tests with two widely used photochemical schemes demonstrate that over the industrial areas in East Asia north of 30° N, SAPRC99 produces higher values of mean summertime O3 than CBIV, amounting to a difference of 10 ppb. In addition, analysis of NCEP winds and geopotential heights suggests that southwesterly monsoonal intrusion in central east China is weakened in August 2001 as compared with the climatologically mean for 1980–2005. Further examination of the O3 diurnal cycle at nine Japanese sites shows that boundary layer evolution has an important effect on the vertical mixing of ground-level O3, and error in near surface meteorology might contribute to overprediction of nighttime O3 in urban and rural areas. In conclusion, the uncertainties in simulating cloud activities and convection mixing, Asian monsoon circulation, photochemical production, and nighttime cooling explain why CMAQ with 81 km horizontal scale overpredicts the observed surface O3 in July and August over central east China and central Japan by 5–15 ppb (CBIV) and 15–25 ppb (SAPRC99). The results suggest clear benefits in evaluating atmospheric chemistry over Asia with high resolution regional model.
What would have happened to the ozone layer if chlorofluorocarbons (CFCs) had not been regulated?
Authors: Newman P. A. , Oman L. D. , Douglass A. R. , Fleming E. L. , Frith S. M. , Hurwitz M. M. , Kawa S. R. , Jackman C. H. , Krotkov N. A. , Nash E. R. , Nielsen J. E. , Pawson S. , Stolarski R. S. , Velders G. J. M.
Published: April 2010

Abstract. Ozone depletion by chlorofluorocarbons (CFCs) was first proposed by Molina and Rowland in their 1974 Nature paper. Since that time, the scientific connection between ozone losses and CFCs and other ozone depleting substances (ODSs) has been firmly established with laboratory measurements, atmospheric observations, and modeling research. This science research led to the implementation of international agreements that largely stopped the production of ODSs. In this study we use a fully-coupled radiation-chemical-dynamical model to simulate a future world where ODSs were never regulated and ODS production grew at an annual rate of 3%. In this "world avoided" simulation, 17% of the globally-average column ozone is destroyed by 2020, and 67% is destroyed by 2065 in comparison to 1980. Large ozone depletions in the polar region become year-round rather than just seasonal as is currently observed in the Antarctic ozone hole. Very large temperature decreases are observed in response to circulation changes and decreased shortwave radiation absorption by ozone. Ozone levels in the tropical lower stratosphere remain constant until about 2053 and then collapse to near zero by 2058 as a result of heterogeneous chemical processes (as currently observed in the Antarctic ozone hole). The tropical cooling that triggers the ozone collapse is caused by an increase of the tropical upwelling. In response to ozone changes, ultraviolet radiation increases, more than doubling the erythemal radiation in the northern summer midlatitudes by 2060.
Analysis of atmospheric neutral and charged molecular clusters in boreal forest using pulse-height CPC
Authors: Lehtipalo K. , Sipilä M. , Riipinen I. , Nieminen T. , Kulmala M.
Published: April 2010

Abstract. We measured the size distribution of atmospheric neutral and charged clusters and particles down to mobility diameter around 1.5 nm by applying pulse-height CPC technique at SMEAR II station in Hyytiälä, southern Finland during spring 2007 and May 2008. The concentration of molecular clusters smaller than 3 nm seems to be highly variable in boreal forest environment. The concentration varied typically between 500–50 000 cm−3, the medians being 8060 cm−3 in year 2007 and 3380 cm−3 in 2008. By comparing to concentrations measured with ion spectrometers, we conclude that ion clusters and neutral clusters produced by ion-ion recombination are usually not sufficient to explain all of the observed clusters; the median fraction of recombination products from all neutral clusters was 4.9%. Before and during most new particle formation events the cluster formation rate rose only slightly, or remained close to stable. Nocturnal formation of clusters was also frequently observed.
Evaluation of the atmospheric transport in a GCM using radon measurements: sensitivity to cumulus convection parameterization
Authors: Zhang K. , Wan H. , Zhang M. , Wang B.
Published: April 2010

Abstract. The radioactive species radon (222Rn) has long been used as a test tracer for the numerical simulation of large scale transport processes. In this study, radon transport experiments are carried out using an atmospheric GCM with a finite-difference dynamical core, the van Leer type FFSL advection algorithm and two state-of-the-art cumulus convection parameterization schemes. Measurements of surface concentration and vertical distribution of radon collected from literature are used as references in model evaluation. The simulated radon concentrations using both convection schemes turn out to be consistent with earlier studies with many other models. Comparison with measurements indicates that at the locations where significant seasonal variations are observed in reality, the model can reproduce both the monthly mean surface radon concentration and the annual cycle quite well. At those sites where the seasonal variation is not large, the model is able to give a correct magnitude of the annual mean. In East Asia, where radon simulations are rarely reported in literature, detailed analysis shows that our results compare reasonably well with the observations. The most evident changes caused by the use of a different convection scheme are found in the vertical distribution of the tracer. The scheme associated with a weaker upward transport gives higher radon concentration up to about 6 km above the surface, and lower values in higher altitudes. In the lower part of the atmosphere results from this scheme does not agree as well with the measurements as the other scheme. Differences from 6 km to the model top are even larger, although we are not yet able to tell which simulation is better due to the lack of observations at such high altitudes.