bluuebunny/crossref_metadata_2025 huggingface dataset:
Size distributions, sources and source areas of water-soluble organic carbon in urban background air
Authors: Timonen H. , Saarikoski S. , Tolonen-Kivimäki O. , Aurela M. , Saarnio K. , Petäjä T. , Aalto P. P. , Kulmala M. , Pakkanen T. , Hillamo R.
Published: April 2010

Abstract. This paper represents the results of one year long measurement period of the size distributions of water-soluble organic carbon (WSOC), inorganic ions and gravimetric mass of particulate matter. Measurements were done at an urban background station (SMEAR III) by using a micro-orifice uniform deposit impactor (MOUDI). The site is located in northern European boreal region in Helsinki, Finland. The WSOC size distribution measurements were completed with the chemical analysis of inorganic ions, organic carbon (OC) and monosaccharide anhydrides from the filter samples. During the measurements gravimetric mass in the MOUDI collections varied between 3.4 and 55.0 μg m−3 and the WSOC concentration was between 0.3 and 7.4 μg m−3. On average, water-soluble particulate organic matter (WSPOM, WSOC multiplied by 1.6) comprised 25±7.7% and 7.5±3.4% of aerosol PM1 mass and the PM1−10 mass, respectively. Inorganic ions contributed 33±12% and 28±19% of the analyzed PM1 and PM1−10 aerosol mass. Five different aerosol categories corresponding to different sources or source areas were identified (long-range transport aerosols, biomass burning aerosols from wild land fires and from small-scale wood combustion, aerosols originating from marine areas and from the clean arctic areas). Clear differences in WSOC concentrations and size distributions originating from different sources or source areas were observed, although there are also many other factors which might affect the results. E.g. the local conditions and sources of volatile organic compounds (VOCs) and aerosols as well as various transformation processes are likely to have an impact on the measured aerosol composition. Using the source categories, it was identified that especially the oxidation products of biogenic VOCs in summer had a clear effect on WSOC concentrations.
Technical Note: Continuity of MIPAS-ENVISAT ozone data quality from full- to reduced-spectral-resolution operation mode
Authors: Ceccherini S. , Cortesi U. , Verronen P.T. , Kyrölä E.
Published: April 2010

Abstract. MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) is operating on the ENVIronmental SATellite (ENVISAT) since March 2002. After two years of nearly continuous limb scanning measurements, at the end of March 2004, the instrument was stopped due to problems with the mirror drive of the interferometer. Operations with reduced maximum path difference, corresponding to both a reduced-spectral-resolution and a shorter measurement time, were resumed on January 2005. In order to exploit the reduction in measurement time, the measurement scenario was changed adopting a finer vertical limb scanning. The change of spectral resolution and of measurement scenario entailed an update of the data processing strategy. The aim of this paper is the assessment of the differences in the quality of the MIPAS ozone data acquired before and after the stop of the operations. Two sets of MIPAS ozone profiles acquired in 2003–2004 (full-resolution measurements) and in 2005–2006 (reduced-resolution measurements) are compared with collocated ozone profiles obtained by GOMOS (Global Ozone Monitoring by Occultation of Stars), itself also onboard ENVISAT. The continuity of the GOMOS data quality allows to assess a possible discontinuity of the MIPAS performances. The relative bias and precision of MIPAS ozone profiles with respect to the GOMOS ones have been compared for the measurements acquired before and after the stop of the MIPAS operations. The results of the comparison show that, in general, the quality of the MIPAS ozone profiles retrieved from reduced-resolution measurements is comparable or better than that obtained from the full-resolution dataset. The only significant change in MIPAS performances is observed at pressures around 2 hPa, where the relative bias of the instruments increases by a factor of 2 from the 2003–2004 to 2005–2006 measurements.
SO2 emissions from Popocatépetl volcano: emission rates and plume imaging using optical remote sensing techniques
Authors: Grutter M. , Basaldud R. , Rivera C. , Harig R. , Junkerman W. , Caetano E. , Delgado-Granados H.
Published: April 2010

Abstract. Sulfur dioxide emissions from Popocatépetl volcano in central Mexico were measured during the MILAGRO field campaign in March 2006. A stationary scanning DOAS (Differential Optical Absorption Spectrometer) was used to monitor the SO2 emissions from the volcano and the results were compared with traverses done with a COSPEC from the ground and a DOAS instrument on board an ultra-light aircraft. Daytime evolutions as well as day-to-day variation of the SO2 emissions are reported. A value of 2.45±1.39 Gg/day of SO2 is reported from all the daily averages obtained during the month of March 2006, with large variation in maximum and minimum daily averages of 5.97 and 0.56 Gg/day, respectively. The large short-term fluctuations in the SO2 emissions obtained could be confirmed through 2-D visualizations of the SO2 plume measured with a scanning imaging infrared spectrometer. This instrument, based on the passive detection of thermal radiation from the volcanic gas and analysis with FTIR spectrometry, is used for the first time for plume visualization of a specific volcanic gas. A 48-h forward trajectory analysis indicates that the volcanic plume was predominately directed towards the Puebla/Tlaxcala region (63%), followed by the Mexico City and Cuernavaca/Cuautla regions with 19 and 18% occurrences, respectively. 25% of the modeled trajectories going towards the Puebla region reached altitudes lower than 4000 m a.s.l. and all trajectories remained over this altitude for the other two regions.
Technical Note: New ground-based FTIR measurements at Ile de La Réunion: observations, error analysis, and comparisons with independent data
Authors: Senten C. , De Mazière M. , Dils B. , Hermans C. , Kruglanski M. , Neefs E. , Scolas F. , Vandaele A. C. , Vanhaelewyn G. , Vigouroux C. , Carleer M. , Coheur P. F. , Fally S. , Barret B. , Baray J. L. , Delmas R. , Leveau J. , Metzger J. M. , Mahieu E. , Boone C. , Walker K. A. , Bernath P. F. , Strong K.
Published: April 2010

Abstract. Ground-based high spectral resolution Fourier-transform infrared (FTIR) solar absorption spectroscopy is a powerful remote sensing technique to obtain information on the total column abundances and on the vertical distribution of various constituents in the atmosphere. This work presents results from two short-term FTIR measurement campaigns in 2002 and 2004, held at the (sub)tropical site Ile de La Réunion (21°S, 55°E). These campaigns represent the first FTIR observations carried out at this site. The results include total column amounts from the surface up to 100 km of ozone (O3), methane (CH4), nitrous oxide (N2O), carbon monoxide (CO), ethane (C2H6), hydrogen chloride (HCl), hydrogen fluoride (HF) and nitric acid (HNO3), as well as some vertical profile information for the first four mentioned trace gases. The data are characterised in terms of the vertical information content and associated error budget. In the 2004 time series, the seasonal increase of the CO concentration was observed by the end of October, along with a sudden rise that has been attributed to biomass burning events in southern Africa and Madagascar. This attribution was based on trajectory modeling. In the same period, other biomass burning gases such as C2H6 also show an enhancement in their total column amounts which is highly correlated with the increase of the CO total columns. The observed total column values for CO are consistent with correlative data from MOPITT (Measurements Of Pollution In The Troposphere). Comparisons between our ground-based FTIR observations and space-borne observations from ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) and HALOE (Halogen Occultation Experiment) confirm the feasibility of the FTIR measurements at Ile de La Réunion.
Global temperature estimates in the troposphere and stratosphere: a validation study of COSMIC/FORMOSAT-3 measurements
Authors: Kishore P. , Namboothiri S. P. , Jiang J. H. , Sivakumar V. , Igarashi K.
Published: April 2010

Abstract. This paper mainly focuses on the validation of temperature estimates derived with the newly launched Constellation Observing System for Meteorology Ionosphere and Climate (COSMIC)/Formosa Satellite 3 (FORMOSAT-3) system. The analysis is based on the radio occultation (RO) data sample collected during the first year observation from April 2006 to April 2007. For the validation, we have used the operational stratospheric analyses (models) including the National Centers for Environmental Prediction-Reanalysis (NCEP-Reanalysis), the Japanese 25-year Reanalysis (JRA-25), and the United Kingdom Met Office (MetO) data sets. Comparisons done in different formats reveal excellent agreement between the COSMIC and model outputs. Spatially, the largest deviations are noted in the polar latitudes, and height-wise, the tropical tropopause region noted the maximum differences. However, these differences are only 2–4 K. We found that among the three models the NCEP data sets have the best resemblance with the COSMIC measurements. We also have done comparison of specific humidity and refractivity profiles with other measurements/models. Specific humidity profiles show comparatively large differences at altitudes below 5 km. Refractivity profiles derived by the COSMIC and other datasets show very good agreement.
A multi-model assessment of pollution transport to the Arctic
Authors: Shindell D. T. , Teich H. , Chin M. , Dentener F. , Doherty R. M. , Faluvegi G. , Fiore A. M. , Hess P. , MacKenzie I. A. , Sanderson M. G. , Schultz M. G. , Schulz M. , Stevenson D. S. , Textor C. , Wild O. , Bergmann D. J. , Bian H. , Cuvelier C. , Duncan B. N. , Folberth G. , Horowitz L. W. , Jonson J. , Kaminski J. W. , Marmer E. , Park R. , Pringle K. J. , Schroeder S. , Szopa S. , Takemura T. , Zeng G. , Keating T. J. , Zuber A.
Published: April 2010

Abstract. We examine the response of Arctic gas and aerosol concentrations to perturbations in pollutant emissions from Europe, East and South Asia, and North America using results from a coordinated model intercomparison. These sensitivities to regional emissions (mixing ratio change per unit emission) vary widely across models and species. Intermodel differences are systematic, however, so that the relative importance of different regions is robust. North America contributes the most to Arctic ozone pollution. For aerosols and CO, European emissions dominate at the Arctic surface but Asian emissions become progressively more important with altitude, and are dominant in the upper troposphere. Sensitivities show strong seasonality: surface sensitivities typically maximize during boreal winter for European and during spring for East Asian and North American emissions. Mid-tropospheric sensitivities, however, nearly always maximize during spring or summer for all regions. Deposition of black carbon (BC) onto Greenland is most sensitive to North American emissions. North America and Europe each contribute ~40% of total BC deposition to Greenland, with ~20% from East Asia. Elsewhere in the Arctic, both sensitivity and total BC deposition are dominated by European emissions. Model diversity for aerosols is especially large, resulting primarily from differences in aerosol physics and removal. Comparison of aerosols with observations indicates problems in either the models or interpretation of the measurements. For gas phase pollutants such as CO and O3, which are relatively well-simulated, the processes contributing most to uncertainties depend on the source region. Uncertainties in the Arctic surface CO response to emissions perturbations are dominated by emissions for East Asian sources, while uncertainties in transport, emissions, and oxidation are comparable for European and North American sources. At higher levels, model-to-model variations in transport and oxidation are most important. Differences in photochemistry appear to play the largest role in the intermodel variations in Arctic ozone sensitivity.
Assimilation of stratospheric and mesospheric temperatures from MLS and SABER into a global NWP model
Authors: Hoppel K. W. , Baker N. L. , Coy L. , Eckermann S. D. , McCormack J. P. , Nedoluha G. E. , Siskind D. E.
Published: April 2010

Abstract. The forecast model and three-dimensional variational data assimilation components of the Navy Operational Global Atmospheric Prediction System (NOGAPS) have each been extended into the upper stratosphere and mesosphere to form an Advanced Level Physics High Altitude (ALPHA) version of NOGAPS extending to ~100 km. This NOGAPS-ALPHA NWP prototype is used to assimilate stratospheric and mesospheric temperature data from the Microwave Limb Sounder (MLS) and the Sounding of the Atmosphere using Broadband Radiometry (SABER) instruments. A 60-day analysis period in January and February, 2006, was chosen that includes a well documented stratospheric sudden warming. SABER temperatures indicate that the SSW caused the polar winter stratopause at ~40 km to disappear, then reform at ~80 km altitude and slowly descend during February. The NOGAPS-ALPHA analysis reproduces this observed stratospheric and mesospheric temperature structure, as well as realistic evolution of zonal winds, residual velocities, and Eliassen-Palm fluxes that aid interpretation of the vertically deep circulation and eddy flux anomalies that developed in response to this wave-breaking event. The observation minus forecast (O-F) standard deviations for MLS and SABER are ~2 K in the mid-stratosphere and increase monotonically to about 6 K in the upper mesosphere. Increasing O-F standard deviations in the mesosphere are expected due to increasing instrument error and increasing geophysical variance at small spatial scales in the forecast model. In the mid/high latitude winter regions, 10-day forecast skill is improved throughout the upper stratosphere and mesosphere when the model is initialized using the high-altitude analysis based on assimilation of both SABER and MLS data.
Contribution of very short-lived organic substances to stratospheric chlorine and bromine in the tropics – a case study
Authors: Laube J. C. , Engel A. , Bönisch H. , Möbius T. , Worton D. R. , Sturges W. T. , Grunow K. , Schmidt U.
Published: April 2010

Abstract. The total stratospheric organic chlorine and bromine burden was derived from balloon-borne measurements in the tropics (Teresina, Brazil, 5°04´S, 42°52´W) in 2005. Whole air samples were collected cryogenically at altitudes between 15 and 34 km. For the first time, we report measurements of a set of 28 chlorinated and brominated substances in the tropical upper troposphere and stratosphere including ten substances with an atmospheric lifetime of less than half a year. The substances were quantified using pre-concentration techniques followed by Gas Chromatography with Mass Spectrometric detection. In the tropical tropopause layer at an altitude of 15.2 km we found 1.4% of the chlorine and 8% of the bromine to be present in the form of very short-lived compounds. By combining the data with tropospheric reference data and age of air observations the abundances of inorganic chlorine and bromine (Cly and Bry) were derived. At an altitude of 34 km we calculated 3062 ppt of Cly and 17.5 ppt of Bry from organic source gases. Furthermore we present indications for the presence of additional organic brominated substances in the tropical upper troposphere and stratosphere.
Determination of the evaporation coefficient of D2O
Authors: Drisdell W. S. , Cappa C. D. , Smith J. D. , Saykally R. J. , Cohen R. C.
Published: April 2010

Abstract. The evaporation rate of D2O has been determined by Raman thermometry of a droplet train (12–15 µm diameter) injected into vacuum (~10-5 torr). The cooling rate measured as a function of time in vacuum was fit to a model that accounts for temperature gradients between the surface and the core of the droplets, yielding an evaporation coefficient (γe) of 0.57±0.06. This is nearly identical to that found for H2O (0.62±0.09) using the same experimental method and model, and indicates the existence of a kinetic barrier to evaporation. The application of a recently developed transition-state theory (TST) model suggests that the kinetic barrier is due to librational and hindered translational motions at the liquid surface, and that the lack of an isotope effect is due to competing energetic and entropic factors. The implications of these results for cloud and aerosol particles in the atmosphere are discussed.
Direct SW aerosol radiative forcing over Portugal
Authors: Santos D. , Costa M. J. , Silva A. M.
Published: April 2010

Abstract. The estimation of radiative forcing due to desert dust and forest fires aerosols is a very important issue since these particles are very efficient at scattering and absorbing both short and longwave radiation. In this work, the evaluation of the aerosol radiative forcing at the top of the atmosphere over the south of Portugal is made, particularly in the regions of Évora and of Cabo da Roca. The radiative transfer calculations combine ground-based and satellite measurements, to estimate the top of the atmosphere direct SW aerosol radiative forcing. The method developed to retrieve the surface spectral reflectance is also presented, based on ground-based measurements of the aerosol optical properties combined with the satellite-measured radiances. The aerosol direct radiative effect is shown to be very sensitive to the underlying surface, since different surface spectral reflectance values may originate different forcing values. The results obtained also illustrate the importance of considering the actual aerosol properties, in this case measured by ground-based instrumentation, particularly the aerosol single scattering albedo, because different aerosol single scattering albedo values can flip the sign of the direct SW aerosol radiative forcing. The instantaneous direct SW aerosol radiative forcing values obtained at the top of the atmosphere are, in the majority of the cases, negative, indicating a tendency for cooling the Earth. For Desert Dust aerosols, over Évora land region, the average forcing efficiency is estimated to be −25 W/m2/AOT0.55 whereas for Cabo da Roca area, the average forcing efficiency is −46 W/m2/AOT0.55. In the presence of Forest Fire aerosols, over Cabo da Roca region, the average value of forcing efficiency is −28 W/m2/AOT0.55 and over Évora region an average value of −33 W/m2/AOT0.55 is found.
An investigation into seasonal and regional aerosol characteristics in East Asia using model-predicted and remotely-sensed aerosol properties
Authors: Song C. H. , Park M. E. , Ahn H. J. , Lee K. H. , Lee Y. , Kim J. Y. , Han K. M. , Kim J. , Ghim Y. S. , Kim Y. J.
Published: April 2010

Abstract. In this study, the spatio-temporal and seasonal distributions of EOS/Terra Moderate Resolution Imaging Spectroradiometer (MODIS)-derived aerosol optical depth (AOD) over East Asia were analyzed in conjunction with US EPA Models-3/CMAQ v4.3 modeling. In this study, two MODIS AOD products (τ MODIS:τM-BAER and τNASA) retrieved through a modified Bremen Aerosol Retrieval (M-BAER) algorithm and NASA collection 5 (C005) algorithm were compared with the AOD (τCMAQ) that was calculated from the US EPA Models-3/CMAQ model simulations. In general, the CMAQ-predicted AOD values captured the spatial and temporal variations of the two MODIS AOD products over East Asia reasonable well. Since τMODIS cannot provide information on the aerosol chemical composition in the atmosphere, different aerosol formation characteristics in different regions and different seasons in East Asia cannot be described or identified by τMODIS itself. Therefore, the seasonally and regionally varying aerosol formation and distribution characteristics were investigated by the US EPA Models-3/CMAQ v4.3 model simulations. The contribution of each particulate chemical species to τM-BAER, τNASA, and τCMAQ showed strong spatial, temporal and seasonal variations. For example, during the summer episode, τM-BAER, τNASA, and τCMAQ were mainly raised due to high concentrations of (NH4)2SO4 over Chinese urban and industrial centers and secondary organic aerosols (SOAs) over the southern parts of China, whereas during the winter episode, τM-BAER, τNASA, and τCMAQ were higher due largely to high levels of NH3NO3 formed over the urban and industrial centers, as well as in areas with high NH3 emissions. In addition, the accuracy of τM-BAER and τNASA was evaluated by a comparison with the AOD (τAERONET) from the AERONET sites in East Asia. Both τM-BAER and τNASA showed a strong correlation with τAERONETR around the 1:1 line (R=0.79), indicating promising potential for the application of both the M-BAER and NASA aerosol retrieval algorithms to satellite-based air quality monitoring studies in East Asia.
Observations of mesoscale and boundary-layer circulations affecting dust uplift and transport in the Saharan boundary layer
Authors: Marsham J. H. , Parker D. J. , Grams C. M. , Grey W. M. F. , Johnson B. T.
Published: April 2010

Abstract. Observations of the Saharan boundary layer, made during the GERBILS field campaign, show that mesoscale land surface temperature variations (which were related to albedo variations) induced mesoscale circulations, and that mesoscale and boundary-layer circulations affected dust uplift and transport. These processes are unrepresented in many climate models, but may have significant impacts on the vertical transport and uplift of desert dust. Mesoscale effects in particular tend to be difficult to parameterise. With weak winds along the aircraft track, land surface temperature anomalies with scales of greater than 10 km are shown to significantly affect boundary-layer temperatures and winds. Such anomalies are expected to affect the vertical mixing of the dusty and weakly stratified Saharan Air Layer (SAL). Mesoscale variations in winds are also shown to affect dust loadings in the boundary-layer. In a region of local uplift, with strong along-track winds, boundary-layer rolls are shown to lead to warm moist dusty updraughts in the boundary layer. Large eddy model (LEM) simulations suggest that these rolls increased uplift by approximately 30%. The modelled effects of boundary-layer convection on uplift is shown to be larger when the boundary-layer wind is decreased, and most significant when the mean wind is below the threshold for dust uplift and the boundary-layer convection leads to uplift which would not otherwise occur.
UV variability in Moscow according to long-term UV measurements and reconstruction model
Authors: Chubarova N. Y.
Published: April 2010

Abstract. Long-term measurements of erythemally weighted UV irradiance (Qer) have been analyzed for the 1999–2006 period as well as UV variability according to reconstruction model since 1968. The estimates of different atmospheric parameters effects, including NO2 content, on Qer) have been obtained on seasonal and interannual scales. It has been shown that NO2 content in conditions of large megalopolis provides average Qer decrease of about 1.5–2%. The seasonal variations of the observed UV indices are discussed from the point of view of the impact on health. Using the reconstruction model we showed a distinct growth in Qer since 1980 due to decrease in total ozone (+2.5% per decade), effective cloud amount transmission (+2.1% per decade) and aerosol loading (+1.1% per decade). However, there is no changes in Qer over larger 1968–2006 period due to significant decrease in effective cloud amount transmission (−11% per decade) in 1968–1980.
Direct determination of highly size-resolved turbulent particle fluxes with the disjunct eddy covariance method and a 12 – stage electrical low pressure impactor
Authors: Schmidt A. , Klemm O.
Published: April 2010

Abstract. During summer 2007, turbulent vertical particle fluxes were measured for a period of 98 days near the city centre of Münster in north-west Germany. For this purpose, a valve controlled disjunct eddy covariance system was mounted at 65 m a.g.l. on a military radio tower. The concentration values for 11 size bins with aerodynamic diameters (D50) from 0.03 to 10 μm were measured with an electrical low pressure impactor. After comparison with other fluxes obtained from 10 Hz measurements with the classical eddy covariance method, the loss of information concerning high frequent parts of the flux could be stated as negligible. The results offer an extended insight in the turbulent atmospheric exchange of aerosol particles by highly size-resolved particle fluxes covering 11 size bins and show that the city of Münster acts as a relevant source for aerosol particles. Significant differences occur between the fluxes of the various particle size classes. While the total particle number flux shows a pattern which is strictly correlated to the diurnal course of the turbulence regime and the traffic intensity, the total mass flux exhibits a single minimum in the evening hours when coarse particles start to deposit. As a result, a mean mass deposition of about 10 g m−2 per day was found above the urban test site, covering the aerosol size range from 40 nm to 2.0 μm. By contrast, the half-hourly total number fluxes accumulated over the lower ELPI stages range from –4.29×107 to +1.44×108 particles m−2 s-1 and are clearly dominated by the sub-micron particle fraction of the impactor stages with diameters between 40 nm and 320 nm. The averaged number fluxes of particles with diameters between 2.0 and 6.4 μm show lower turbulent dynamics during daytime and partially remarkably high negative fluxes with mean deposition velocities of 2×10−3 m s−1 that appear temporary during noontime and in the evening hours.
Precipitation of salts in freezing seawater and ozone depletion events: a status report
Authors: Morin S. , Marion G. M. , von Glasow R. , Voisin D. , Bouchez J. , Savarino J.
Published: April 2010

Abstract. In springtime, the polar marine boundary layer exhibits drastic ozone depletion events (ODEs), associated with elevated bromine oxide (BrO) mixing ratios. The current interpretation of this peculiar chemistry requires the existence of acid and bromide-enriched surfaces to heterogeneously promote and sustain ODEs. In a recent study, Sander et al. (2006) have proposed that calcium carbonate (CaCO3) precipitation in any seawater-derived medium could potentially decrease its alkalinity, making it easier for atmospheric acids such as HNO3 and H2SO4 to acidify it. We performed simulations using the state-of-the-art FREZCHEM model, capable of handling concentrated electrolyte solutions, to check the preliminary results of Sander et al. (2006). We show that the alkalinity of brine is indeed reduced to about half and a third of the initial alkalinity of seawater, at 263 K and 253 K, respectively. Such levels of alkalinity depletion have been shown to speed-up the onset of ODEs (Sander et al., 2006; Piot and von Glasow, 2008a), suggesting that carbonate precipitation could well be a key phenomenon linked with ODEs, in polar regions but also in other cold areas, such as altitude salt lakes. In addition, the evolution of the Cl/Br ratio in the brine during freezing was computed using FREZCHEM, taking into account Br substitutions in Cl–containing salts.
Factor analytical modeling of C2–C7 hydrocarbon sources at an urban background site in Zurich (Switzerland): changes between 1993–1994 and 2005–2006
Authors: Lanz V. A. , Buchmann B. , Hueglin C. , Locher R. , Reimann S. , Staehelin J.
Published: April 2010

Abstract. Hourly measurements of 13 volatile hydrocarbons (C2–C7) were performed at an urban background site in Zurich (Switzerland) in the years 1993–1994 and again in 2005–2006. Changes in hydrocarbon profiles and source strengths were recovered by positive matrix factorization (PMF). Eight and six factors could be related to hydrocarbon sources in 1993–1994 and in 2005–2006, respectively. The modeled source profiles were verified by hydrocarbon profiles reported in the literature. The source strengths were validated by independent measurements, such as inorganic trace gases (NOx, CO, SO2), methane (CH4), oxidized hydrocarbons (OVOCs) and meteorological data (temperature, wind speed etc.). Our analysis suggests that the contribution of most hydrocarbon sources (i.e. road traffic, solvents use, and wood burning) decreased by a factor of about two to three between the early 1990s and 2005–2006. On the other hand, hydrocarbon losses from natural gas leakage remained at relatively constant (−20%) concentration levels. The estimated emission trends are in line with the results from different top-down approaches reported for other European cities. Their discrepancies to national emission inventories are discussed.
Mesoscale temperature fluctuations in the Southern Hemisphere stratosphere
Authors: Gary B. L.
Published: April 2010

Abstract. Isentrope surfaces in the Southern Hemisphere stratosphere reveal that air parcels undergo mesoscale temperature fluctuations that depend on latitude and season. The largest temperature fluctuations occur at high latitude winter, whereas the smallest fluctuations occur at high latitude summer. This is the same pattern found for the Northern Hemisphere stratosphere. However, the amplitude of the seasonal dependence in the Southern Hemisphere is only 37% of the Northern Hemisphere's seasonal amplitude.
The effect of temperature and water on secondary organic aerosol formation from ozonolysis of limonene, Δ³-carene and α-pinene
Authors: Jonsson Å. M. , Hallquist M. , Ljungström E.
Published: April 2010

Abstract. The effect of reaction temperature and how water vapour influences the formation of secondary organic aerosol (SOA) in ozonolysis of limonene, Δ3-carene and α-pinene, both regarding number and mass of particles, has been investigated by using a laminar flow reactor G-FROST. Experiments with cyclohexane and 2-butanol (~3.5×1014 molecules cm−3) as OH scavengers were compared to experiments without any scavenger. The reactions were conducted in the temperature range between 298 and 243 K, and at relative humidities between <10 and 80%. Results showed that there is still a scavenger effect on number and mass concentrations at low temperatures between experiments with and without OH scavenger. This shows that the OH chemistry is influencing the SOA formation also at these temperatures. The overall temperature dependence on SOA formation is not as strong as expected from the partitioning theory. In some cases there is even a positive temperature dependence that must be related to changes in the chemical mechanism and/or reduced rates of secondary chemistry at low temperatures. The water effect at low temperature could be explained by physical uptake and cluster stabilisation. At higher temperatures, only a physical explanation is not sufficient and the observations are in line with water changing the chemical mechanism or reaction rates. The data presented adds to the understanding of SOA contribution to atmospheric aerosol composition, new particle formation and atmospheric degradation mechanisms.
Consistent simulation of bromine chemistry from the marine boundary layer to the stratosphere – Part 2: Bromocarbons
Authors: Kerkweg A. , Jöckel P. , Warwick N. , Gebhardt S. , Brenninkmeijer C.A.M. , Lelieveld J.
Published: April 2010

Abstract. In this second part of a series of articles dedicated to a detailed analysis of bromine chemistry in the atmosphere we address one (out of two) dominant natural sources of reactive bromine. The two main source categories are the release of bromine from sea salt and the decomposition of bromocarbons by photolysis and reaction with OH. Here, we focus on C1-bromocarbons. We show that the atmospheric chemistry general circulation model ECHAM5/MESSy realistically simulates their emission, transport and decomposition from the boundary layer up to the mesosphere. We included oceanic emission fluxes of the short-lived bromocarbons CH2Br2, CH2ClBr, CHClBr2, CHCl2Br, CHBr3 and of CH3Br. The vertical profiles and the surface mixing ratios of the bromocarbons are in general agreement with the (few available) observations, especially in view of the limited information available and the consequent coarseness of the emission fields. For CHBr3, CHCl2Br and CHClBr2 photolysis is the most important degradation process in the troposphere. In contrast to this, tropospheric CH2Br2, CH3Br and CH2ClBr are more efficiently decomposed by reaction with OH. In the free troposphere approximately one third of the C1-bromocarbons decomposes by reaction with OH. In the boundary layer the reaction with OH is relatively important, whereas it is negligible in the stratosphere. Our results indicate an approximately 50% longer lifetime of CH3Br (≈1 year) than assumed previously, implying a relatively strong contribution to stratospheric bromine and consequent ozone destruction.
CCN activity and droplet growth kinetics of fresh and aged monoterpene secondary organic aerosol
Authors: Engelhart G. J. , Asa-Awuku A. , Nenes A. , Pandis S. N.
Published: April 2010

Abstract. The ability of secondary organic aerosol (SOA) produced from the ozonolysis of α-pinene and monoterpene mixtures (α-pinene, β-pinene, limonene and 3-carene) to become cloud droplets was investigated. Monoterpene SOA is quite active and would likely be a good source of cloud condensation nuclei (CCN) in the atmosphere. A static CCN counter and a Scanning Mobility CCN Analyser (a Scanning Mobility Particle Sizer coupled with a Continuous Flow counter) were used for the CCN measurements. A decrease in CCN activation diameter for α-pinene SOA of approximately 3 nm h−1 was observed as the aerosol continued to react with oxidants. Hydroxyl radicals further oxidize the SOA particles thereby enhancing the particle CCN activity with time. The initial concentrations of ozone and monoterpene precursor (for concentrations lower than 40 ppb) do not appear to affect the activity of the resulting SOA. Köhler Theory Analysis (KTA) is used to infer the molar mass of the SOA sampled online and offline from atomized filter samples. KTA suggests that the aged aerosol (both from α-pinene and the mixed monoterpene oxidation) is primarily water-soluble (around 70–80%), with an estimated average molar mass of 180±55 g mol−1 (consistent with existing SOA speciation studies). CCN activity measurements of the SOA mixed with (NH4)2SO4 suggest that the organic can depress surface tension by as much as 10 nM m−1 (with respect to pure water). The droplet growth kinetics of SOA samples are similar to (NH4)2SO4, except at low supersaturation, where SOA tends to grow more slowly. The CCN activity of α-pinene and mixed monoterpene SOA can be modelled by a very simple implementation of Köhler theory, assuming complete dissolution of the particles, no dissociation into ions, molecular weight of 180 g mol−1, density of 1.5 g cm−3, and surface tension to within 10–15% of water.
PM10 data assimilation over Europe with the optimal interpolation method
Authors: Tombette M. , Mallet V. , Sportisse B.
Published: April 2010

Abstract. This paper presents experiments of PM10 data assimilation with the optimal interpolation method. The observations are provided by BDQA (Base de Données sur la Qualité de l'Air), whose monitoring network covers France. Two other databases (EMEP and AirBase) are used to evaluate the improvements in the analyzed state over one month (January, 2001) and for several outputs (PM10, PM2.5 and chemical composition). Then, the method is applied in operational conditions. The results show that the assimilation of PM10 observations significantly improves the one-day forecast for total mass (PM10 and PM2.5). The errors on aerosol chemical composition are not reduced and are sometimes amplified by the assimilation procedure, which shows the need for chemical data. As the observations cover a limited part of the domain (France versus Europe) and as the method used for assimilation is sequential, we focus on the horizontal and temporal impacts of assimilation in the last part of this paper. To conclude, we discuss the perspectives, especially the use of a variational method for assimilation or the investigation of the sensitivity to a few choices (e.g., the error statistics, etc.).
SO2 oxidation products other than H2SO4 as a trigger of new particle formation – Part 2: Comparison of ambient and laboratory measurements, and atmospheric implications
Authors: Laaksonen A. , Kulmala M. , Berndt T. , Stratmann F. , Mikkonen S. , Ruuskanen A. , Lehtinen K. E. J. , Dal Maso M. , Aalto P. , Petäjä T. , Riipinen I. , Sihto S.-L. , Janson R. , Arnold F. , Hanke M. , Ücker J. , Umann B. , Sellegri K. , O’Dowd C. D. , Viisanen Y.
Published: April 2010

Abstract. Atmospheric new particle formation is generally thought to occur due to homogeneous or ion-induced nucleation of sulphuric acid. We compare ambient nucleation rates with laboratory data from nucleation experiments involving either sulphuric acid or oxidized SO2. Atmospheric nucleation occurs at H2SO4 concentrations 2–4 orders of magnitude lower than binary or ternary H2SO4 nucleation. In contrast, the atmospheric nucleation rates and H2SO4 concentrations are very well replicated in the SO2 oxidation experiments. We explain these features by the formation of free HSO5 radicals in pace with H2SO4 during the SO2 oxidation. We suggest that at temperatures above ~250 K these radicals produce nuclei of new aerosols much more efficiently than H2SO4. These nuclei are activated to further growth by H2SO4 and possibly other trace species. However, at lower temperatures the atmospheric relative acidity is high enough for the H2SO4–H2O nucleation to dominate.
SO2 oxidation products other than H2SO4 as a trigger of new particle formation – Part 1: Laboratory investigations
Authors: Berndt T. , Stratmann F. , Bräsel S. , Heintzenberg J. , Laaksonen A. , Kulmala M.
Published: April 2010

Abstract. Mechanistic investigations of atmospheric H2SO4 particle formation have been performed in a laboratory study taking either H2SO4 from a liquid reservoir or using the gas-phase reaction of OH radicals with SO2. Applying both approaches for H2SO4 generation simultaneously we found that H2SO4 evaporated from the liquid reservoir acts considerably less effective for the process of particle formation and growth than the products originating from the reaction of OH radicals with SO2. Furthermore, for NOx concentrations >5×1011 molecule cm−3 the formation of new particles from the reaction of OH radicals with SO2 is inhibited. This suggests that substances other than H2SO4 (likely products from sulphur-containing peroxy radicals) trigger lower tropospheric new particle formation and growth. The currently accepted mechanism for SO2 gas-phase oxidation does not consider the formation of such substances making a revision necessary.
Effects of aerosol organics on cloud condensation nucleus (CCN) concentration and first indirect aerosol effect
Authors: Wang J. , Lee Y.-N. , Daum P. H. , Jayne J. , Alexander M. L.
Published: April 2010

Abstract. Aerosol microphysics, chemical composition, and CCN properties were measured on the Department of Energy Gulfstream-1 aircraft during the Marine Stratus/Stratocumulus Experiment (MASE) conducted over the coastal waters between Point Reyes National Seashore and Monterey Bay, California, in July 2005. Aerosols measured during MASE included free tropospheric aerosols, marine boundary layer aerosols, and aerosols with high organic concentration within a thin layer above the cloud. Closure analysis was carried out for all three types of aerosols by comparing the measured CCN concentrations at 0.22% supersaturation to those predicted based on size distribution and chemical composition using Köhler theory. The effect of aerosol organic species on predicted CCN concentration was examined using a single hygroscopicity parameterization. For aerosols with organics volume fraction up to 70%, such as the marine boundary layer and free troposphere aerosols, CCN concentration and the corresponding first indirect aerosol effect are insensitive to the properties of organics, and can be accurately predicted with a constant hygroscopicity for all organic species. This simplification can facilitate the prediction of indirect aerosol effects using physically-based parameterizations in large scale models. However, for the aerosols within the thin layers above clouds, organics contributed up to 90% of the total aerosol volume, and a detailed knowledge of organic hygroscopicity is required to accurately predict CCN concentrations. Derivations of organic properties in future closure studies, when aerosols are dominated by organic species, would help constrain the descriptions of organics and aerosol-cloud parameterizations in large scale models.
Cloud and surface classification using SCIAMACHY polarization measurement devices
Authors: Lotz W. A. , Vountas M. , Dinter T. , Burrows J. P.
Published: April 2010

Abstract. A simple scheme has been developed to discriminate surface, sun glint and cloud properties in satellite based spectrometer data utilizing visible and near infrared information. It has been designed for the use with data measured by SCIAMACHY's (SCanning Imaging Absorption SpectroMeter for Atmospheric CHartographY) Polarization Measurement Devices but the applicability is not strictly limited to this instrument. The scheme is governed by a set of constraints and thresholds developed by using satellite imagery and meteorological data. Classification targets are ice, water and generic clouds, sun glint and surface parameters, such as water, snow/ice, desert and vegetation. The validation is done using MERIS (MEdium Resolution Imaging Spectrometer) and meteorological data from METAR (MÉTéorologique Aviation Régulière – a network for the provision of meteorological data for aviation). Qualitative and quantitative validation using MERIS satellite imagery shows good agreement. The comparison with METAR data exhibits very good agreement.
Measurement of black carbon at Syowa station, Antarctica: seasonal variation, transport processes and pathways
Authors: Hara K. , Osada K. , Yabuki M. , Hayashi M. , Yamanouchi T. , Shiobara M. , Wada M.
Published: April 2010

Abstract. Measurement of black carbon (BC) was carried out at Syowa station Antarctica (69° S, 39° E) from February 2004 until January 2007. The BC concentration at Syowa ranged from below detection to 176 ng m−3 during the measurements. Higher BC concentrations were observed mostly under strong wind (blizzard) conditions due to the approach of a cyclone and blocking event. The BC-rich air masses traveled from the lower troposphere of the Atlantic and Indian Oceans to Syowa (Antarctic coast). During the summer (November–February), the BC concentration showed a diurnal variation together with surface wind speed and increased in the katabatic wind from the Antarctic continent. Considering the low BC source strength in the Antarctic continent, the higher BC concentration in the continental air (katabatic wind) might be caused by long range transport of BC via the free troposphere from mid- and low- latitudes. The seasonal variation of BC at Syowa had a maximum in August, while at the other coastal stations (Halley, Neumayer, and Ferraz) and the continental station (Amundsen-Scott), the maximum occurred in October. This difference may result from different transport pathways and scavenging of BC by precipitation during the transport from the source regions. During the austral summer, long-range transport of BC via the free troposphere is likely to make an important contribution to the ambient BC concentration. The BC transport flux indicated that BC injection into the Antarctic region strongly depended on the frequency of storm (blizzard) conditions. The seasonal variation of BC transport flux increased by 290 mg m−2 month−1 in winter–spring when blizzards frequently occurred, whereas the flux decreased to lower than 50 mg m−2 month−1 in the summer with infrequent blizzards.
MATRIX (Multiconfiguration Aerosol TRacker of mIXing state): an aerosol microphysical module for global atmospheric models
Authors: Bauer S. E. , Wright D. , Koch D. , Lewis E. R. , McGraw R. , Chang L.-S. , Schwartz S. E. , Ruedy R.
Published: April 2010

Abstract. A new aerosol microphysical module MATRIX, the Multiconfiguation Aerosol TRacker of mIXing state, and its application in the Goddard Institute for Space Studies (GISS) climate model (ModelE) is described. This module, which is based on the quadrature method of moments (QMOM), represents nucleation, condensation, coagulation, internal and external mixing, and cloud-drop activation and provides aerosol particle mass and number concentration and particle size information for up to 16 mixed-mode aerosol populations. Internal and external mixing among aerosol components sulfate, nitrate, ammonium, carbonaceous aerosols, dust and sea-salt particles are represented. The solubility of each aerosol mode, which is explicitly calculated based on its soluble and insoluble components, enables calculation of the dependence of cloud drop activation on the microphysical characterization of multiple soluble modes. A detailed model description and results of box-model simulations of various mode configurations are presented. The number concentration of aerosol particles activated to cloud drops depends on the mode configuration. Simulations on the global scale with the GISS climate model are evaluated against aircraft and station measurements of aerosol mass and number concentration and particle size. The model accurately captures the observed size distributions in the aitken and accumulation modes up to particle diameter 1 μm, in which sulfate, nitrate, black and organic carbon are predominantly located; however the model underestimates coarse-mode number concentration and size, especially in the marine environment.
IASI spectral radiance performance validation: case study assessment from the JAIVEx field campaign
Authors: Larar A. M. , Smith W. L. , Zhou D. K. , Liu X. , Revercomb H. , Taylor J. P. , Newman S. M. , Schlüssel P.
Published: April 2010

Abstract. Advanced satellite sensors are tasked with improving global-scale measurements of the Earth's atmosphere, clouds, and surface to enable enhancements in weather prediction, climate monitoring, and environmental change detection. Measurement system validation is crucial to achieving this goal and maximizing research and operational utility of resultant data. Field campaigns employing satellite under-flights with well-calibrated Fourier Transform Spectrometer (FTS) sensors aboard high-altitude aircraft are an essential part of this validation task. The National Polar-orbiting Operational Environmental Satellite System (NPOESS) Airborne Sounder Testbed-Interferometer (NAST-I) has been a fundamental contributor in this area by providing coincident high spectral and spatial resolution observations of infrared spectral radiances along with independently-retrieved geophysical products for comparison with like products from satellite sensors being validated. This manuscript focuses on validating infrared spectral radiance from the Infrared Atmospheric Sounding Interferometer (IASI) through a case study analysis using data obtained during the recent Joint Airborne IASI Validation Experiment (JAIVEx) field campaign. Emphasis is placed upon the benefits achievable from employing airborne interferometers such as the NAST-I since, in addition to IASI radiance calibration performance assessments, cross-validation with other advanced sounders such as the AQUA Atmospheric InfraRed Sounder (AIRS) is enabled.