bluuebunny/crossref_metadata_2025 huggingface dataset:
The contribution of anthropogenic bromine emissions to past stratospheric ozone trends: a modelling study
Authors: Sinnhuber B.-M. , Sheode N. , Sinnhuber M. , Chipperfield M. P. , Feng W.
Published: April 2010

Abstract. Bromine compounds play an important role in the depletion of stratospheric ozone. We have calculated the changes in stratospheric ozone in response to changes in the halogen loading over the past decades, using a two-dimensional (latitude/height) model constrained by source gas mixing ratios at the surface. Model calculations of the decrease of total column ozone since 1980 agree reasonably well with observed ozone trends, in particular when the contribution from very short-lived bromine compounds is included. Model calculations with bromine source gas mixing ratios fixed at 1959 levels, corresponding approximately to a situation with no anthropogenic bromine emissions, show an ozone column reduction between 1980 and 2005 at Northern Hemisphere mid-latitudes of only ≈55% compared to a model run including all halogen source gases. In this sense anthropogenic bromine emissions are responsible for ≈45% of the model estimated column ozone loss at Northern Hemisphere mid-latitudes. However, since a large fraction of the bromine induced ozone loss is due to the combined BrO/ClO catalytic cycle, the effect of bromine would have been smaller in the absence of anthropogenic chlorine emissions. The chemical efficiency of bromine relative to chlorine for global total ozone depletion from our model calculations, expressed by the so called α-factor, is 64 on an annual average. This value is much higher than previously published results. Updates in reaction rate constants can explain only part of the differences in α. The inclusion of bromine from very short-lived source gases has only a minor effect on the global mean α-factor.
Technical Note: Feasibility of CO2 profile retrieval from limb viewing solar occultation made by the ACE-FTS instrument
Authors: Foucher P. Y. , Chédin A. , Dufour G. , Capelle V. , Boone C. D. , Bernath P.
Published: April 2010

Abstract. Major limitations of our present knowledge of the global distribution of CO2 in the atmosphere are the uncertainty in atmospheric transport mixing and the sparseness of in situ concentration measurements. Limb viewing space-borne sounders, observing the atmosphere along tangential optical paths, offer a vertical resolution of a few kilometers for profiles, which is much better than currently flying or planned nadir sounding instruments can achieve. In this paper, we analyse the feasibility of obtaining CO2 vertical profiles in the 5–25 km altitude range from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS, launched in August 2003), high spectral resolution solar occultation measurements. Two main difficulties must be overcome: (i) the accurate determination of the instrument pointing parameters (tangent heights) and pressure/temperature profiles independently from an a priori CO2 profile, and (ii) the potential impact of uncertainties in the temperature knowledge on the retrieved CO2 profile. The first difficulty has been solved using the N2 collision-induced continuum absorption near 4 μm to determine tangent heights, pressure and temperature from the ACE-FTS spectra. The second difficulty has been solved by a careful selection of CO2 spectral micro-windows. Retrievals using synthetic spectra made under realistic simulation conditions show a vertical resolution close to 2.5 km and accuracy of the order of 2 ppm after averaging over 25 profiles. These results open the way to promising studies of transport mechanisms and carbon fluxes from the ACE-FTS measurements. First CO2 vertical profiles retrieved from real ACE-FTS occultations shown in this paper confirm the robustness of the method and applicability to real measurements.
Assessment of the MODIS Collections C005 and C004 aerosol optical depth products over the Mediterranean basin
Authors: Papadimas C. D. , Hatzianastassiou N. , Mihalopoulos N. , Kanakidou M. , Katsoulis B. D. , Vardavas I.
Published: April 2010

Abstract. The second generation Collection 005 (C005) MODIS operational algorithm for retrieval of aerosol properties was evaluated and validated for the greater Mediterranean basin (29.5° N–46.5° N and 10.5° W–38.5° E), a region with an atmosphere under siege by air pollution and diminishing water resources that are exacerbated by high aerosol loads and climatic change. The present study aims to quantify the differences between the C005 and the previous (C004) MODIS collections, and re-assess the results of previous studies that have been performed for the region using MODIS C004 aerosol optical depth (AOD) products. Daily data of AOD from EOS-Terra covering the 6-year period 2000–2006 were taken from both C005 and C004 Level-3 datasets, and were inter-compared and validated against ground-based measurements from 29 AERONET stations. The C005 data were found to significantly better agree with the AERONET data than those of C004. The correlation coefficient between MODIS and AERONET was found to increase from 0.66 to 0.76 and the slope of linear regression MODIS/AERONET from 0.79 to 0.85. The MODIS C005 data still overestimate/underestimate the AERONET AOD values smaller/larger than 0.25, but to a much smaller extent than C004 data. The better agreement of C005 with AERONET data arises from the generally lower C005 values, with regional mean AOD values equal to 0.27 and 0.22 for C004 and C005, respectively. This decrease, however, is not uniform over the region and involves a significant decrease over land and a small increase over the ocean for AOD values greater than 0.1 (opposite changes were found under aerosol-clean conditions). Both data sets indicate a decrease in the regional mean AOD over the period 2000–2006, equal to 20% based on C005 and 17% based on C004 datasets, though the intra-annual and inter-annual variation did not change significantly, thus indicating a systematic correction to C004 values.
Size-resolved aerosol chemistry on Whistler Mountain, Canada with a high-resolution aerosol mass spectrometer during INTEX-B
Authors: Sun Y. , Zhang Q. , Macdonald A. M. , Hayden K. , Li S. M. , Liggio J. , Liu P. S. K. , Anlauf K. G. , Leaitch W. R. , Steffen A. , Cubison M. , Worsnop D. R. , van Donkelaar A. , Martin R. V.
Published: April 2010

Abstract. An Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed at the peak of Whistler Mountain (2182 m above sea level), British Columbia, from 19 April to 16 May 2006, as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign. The mass concentrations and size distributions of non-refractory submicron particle (NR-PM1) species (i.e., sulfate, nitrate, ammonium, chloride, and organics) were measured in situ at 10-min time resolution. The HR-ToF-AMS results agreed well with collocated measurements. The average concentration of non-refractory submicron particulate matter (NR-PM1; 1.9 μg m−3) is similar to those observed at other remote, high elevation sites in North America. Episodes of enhanced aerosol loadings were observed, due to influences of regional and trans-Pacific transport of air pollution. Organics and sulfate were the dominant species, on average accounting for 55% and 30%, respectively, of the NR-PM1 mass. The average size distributions of sulfate and ammonium both showed an accumulation mode peaking at ~500 nm in vacuum aerodynamic diameter (Dva) while those of organic aerosol (OA) and nitrate peaked at ~300 nm. The size differences suggested that sulfate and OA were mostly present in external mixtures from different source origins. We also quantitatively determined the elemental composition of OA using the high resolution mass spectra. Overall, OA at Whistler Peak was highly oxygenated, with an average organic-mass-to-organic-carbon ratio (OM/OC) of 2.28±0.23 and an atomic ratio of oxygen-to-carbon (O/C) of 0.83±0.17. The nominal formula for OA was C1H1.66N0.03O0.83 for the entire study. Two significant trans-Pacific dust events originated from Asia were observed at Whistler Peak during this study. While both events were characterized with significant enhancements of coarse mode particles and mineral contents, the composition and characteristics of NR-PM1 were significantly different between them. One trans-Pacific event occurred on 15 May 2006, during which ammonium sulfate contributed >90% of the total NR-PM1 mass. This event was followed by a high OA episode likely associated with regional emissions. In total, three enhanced regional OA events, each of which lasted 2–3 days, were observed during this study. In contrast to the two dust events, the regional OA events were generally characterized with higher OA/sulfate ratio, less oxidized OA, and lower OM/OC ratio.
Variable CCN formation potential of regional sulfur emissions
Authors: Manktelow P. T. , Carslaw K. S. , Mann G. W. , Spracklen D. V.
Published: April 2010

Abstract. Aerosols are short lived so their geographical distribution and impact on climate depends on where they are emitted. Previous model studies have shown that the mass of sulfate aerosol produced per unit sulfur emission (the sulfate burden potential) and the associated direct radiative forcing vary regionally because of differences in meteorology and photochemistry. Using a global model of aerosol microphysics, we show that the total number of aerosol particles produced per unit sulfur emission (the aerosol number potential) has a different regional variation to that of sulfate mass. The aerosol number potential of N. American and Asian emissions is calculated to be a factor of 3 to 4 times greater than that of European emissions, even though Europe has a higher sulfate burden potential. Pollution from N. America and Asia tends to reach higher altitudes than European pollution so forms more new particles through nucleation. Regional differences in particle production and growth mean that sulfur emissions from N. America and E. Asia produce 50 nm diameter cloud condensation nuclei up to 70% more efficiently than Europe. For 80 nm diameter CCN, N. America and Europe produce CCN 2.5 times more efficiently than E. Asia. The impact of regional sulfur emissions on particle concentrations is also much more widely spread than the impact on sulfate mass, due to efficient particle production in the free troposphere during long range transport. These results imply that regional sulfur emissions will have different climate forcing potentials through changes in cloud drop number.
A multimethodological approach to study the spatial distribution of air pollution in an Alpine valley during wintertime
Authors: Schnitzhofer R. , Norman M. , Wisthaler A. , Vergeiner J. , Harnisch F. , Gohm A. , Obleitner F. , Fix A. , Neininger B. , Hansel A.
Published: April 2010

Abstract. In order to investigate the spatial distribution of air pollutants in the Inn valley (Tyrol, Austria) during wintertime, a joint field campaign of the three research projects ALPNAP (Monitoring and Minimisation of Traffic-Induced Noise and Air Pollution Along Major Alpine Transport Routes), INNAP (Boundary Layer Structure in the Inn Valley during high Air Pollution) and INNOX (NOx-structure in the Inn Valley during High Air Pollution) was carried out in January/February 2006. In addition to continuous ground based measurements, vertical profiles of various air pollutants and meteorological parameters were obtained on six selected days. For in-situ investigations, a tethered balloon was used to analyse the lowest atmospheric layers, 0–500 m above the valley bottom (a.v.b.), and a research aircraft sampled at 150–2200 m a.v.b. An aircraft equipped with an aerosol backscatter lidar performed nadir measurements at 3000 m a.v.b. Combined results from a typical day show a strongly polluted layer up to about 125 m a.v.b. in the morning. Around midday concentrations on the valley floor decrease indicating some vertical air exchange despite thermally stable conditions. Strong vertical and horizontal gradients with enhanced pollution levels along the sunny side of the valley up to 1300 m a.v.b. were observed in the afternoon. This vertical mixing due to thermally or dynamically driven slope winds reduces the concentration of air pollutants at the bottom of the valley and causes the formation of elevated pollution layers.
Process-based modelling of biogenic monoterpene emissions combining production and release from storage
Authors: Schurgers G. , Arneth A. , Holzinger R. , Goldstein A. H.
Published: April 2010

Abstract. Monoterpenes, primarily emitted by terrestrial vegetation, can influence atmospheric ozone chemistry, and can form precursors for secondary organic aerosol. The short-term emissions of monoterpenes have been well studied and understood, but their long-term variability, which is particularly important for atmospheric chemistry, has not. This understanding is crucial for the understanding of future changes. In this study, two algorithms of terrestrial biogenic monoterpene emissions, the first one based on the short-term volatilization of monoterpenes, as commonly used for temperature-dependent emissions, and the second one based on long-term production of monoterpenes (linked to photosynthesis) combined with emissions from storage, were compared and evaluated with measurements from a Ponderosa pine plantation (Blodgett Forest, California). The measurements were used to parameterize the long-term storage of monoterpenes, which takes place in specific storage organs and which determines the temporal distribution of the emissions over the year. The difference in assumptions between the first (emission-based) method and the second (production-based) method, which causes a difference in upscaling from instantaneous to daily emissions, requires roughly a doubling of emission capacities to bridge the gap to production capacities. The sensitivities to changes in temperature and light were tested for the new methods, the temperature sensitivity was slightly higher than that of the short-term temperature dependent algorithm. Applied on a global scale, the first algorithm resulted in annual total emissions of 29.6 Tg C a−1, the second algorithm resulted in 31.8 Tg C a−1 when applying the correction factor 2 between emission capacities and production capacities. However, the exact magnitude of such a correction is spatially varying and hard to determine as a global average.
Statistical analysis of anthropogenic non-methane VOC variability at a European background location (Jungfraujoch, Switzerland)
Authors: Lanz V. A. , Henne S. , Staehelin J. , Hueglin C. , Vollmer M. K. , Steinbacher M. , Buchmann B. , Reimann S.
Published: April 2010

Abstract. In-situ measurements of 7 volatile hydrocarbons, CxHy, and 3 chlorinated organic compounds, CxHyClz, were performed at Jungfraujoch (Switzerland) during eight years (2000–2007). The analysis of 4-h resolved non-methane volatile organic compounds (NMVOCs) was achieved by using gas-chromatography coupled with mass spectrometry (GC-MS). Variabilities in the NMVOC time series dataset were modeled by factor analysis (positive matrix factorization, PMF). Four factors defined the solution space and could be related to NMVOC sources and atmospheric processes. In order to facilitate factor interpretations the retrieved contributions were compared with independent measurements, such as trace gases (NOx, CO, and CH4) and back trajectories. The most dominant factor (accounting on average for ~42% of the total mixing ratio of the considered NMVOCs) was found to be most active in winter, co-varying with CO and CH4 and could be related to aged combustive emissions as well as natural gas distribution. The other three factors represent both industrial and evaporative sources. Trajectory statistics suggest that the most influential anthropogenic NMVOC sources for Jungfraujoch are located in Eastern Europe, but the Po Valley has been identified as a potential source region for specific industrial sources as well. Aging of the arriving NMVOCs, the derived factors as well as limitations of the methods are discussed. This is the first report of a PMF application on NMVOC data from a background mountain site.
Ice supersaturations and cirrus cloud crystal numbers
Authors: Krämer M. , Schiller C. , Afchine A. , Bauer R. , Gensch I. , Mangold A. , Schlicht S. , Spelten N. , Sitnikov N. , Borrmann S. , de Reus M. , Spichtinger P.
Published: April 2010

Abstract. Upper tropospheric observations outside and inside of cirrus clouds indicate water vapour mixing ratios sometimes exceeding water saturation. Relative humidities over ice (RHice) of up to and more than 200% have been reported from aircraft and balloon measurements in recent years. From these observations a lively discussion continues on whether there is a lack of understanding of ice cloud microphysics or whether the water measurements are tainted with large uncertainties or flaws. Here, RHice in clear air and in ice clouds is investigated. Strict quality-checked aircraft in situ observations of RHice were performed during 28 flights in tropical, mid-latitude and Arctic field experiments in the temperature range 183–240 K. In our field measurements, no supersaturations above water saturation are found. Nevertheless, super- or subsaturations inside of cirrus are frequently observed at low temperatures (<205 K) in our field data set. To explain persistent RHice deviating from saturation, we analysed the number densities of ice crystals recorded during 20 flights. From the combined analysis – using conventional microphysics – of supersaturations and ice crystal numbers, we show that the high, persistent supersaturations observed inside of cirrus can possibly be explained by unexpected, frequent very low ice crystal numbers that could scarcely be caused by homogeneous ice nucleation. Heterogeneous ice formation or the suppression of freezing might better explain the observed ice crystal numbers. Thus, our lack of understanding of the high supersaturations, with implications for the microphysical and radiative properties of cirrus, the vertical redistribution of water and climate, is traced back to the understanding of the freezing process at low temperatures.
Peroxy radical observations over West Africa during AMMA 2006: photochemical activity in the outflow of convective systems
Authors: Andrés-Hernández M. D. , Kartal D. , Reichert L. , Burrows J. P. , Meyer Arnek J. , Lichtenstern M. , Stock P. , Schlager H.
Published: April 2010

Abstract. Peroxy radical measurements made on board the DLR-Falcon research aircraft over West Africa within the African Monsoon Multidisciplinary Analysis (AMMA) campaign during the 2006 wet monsoon are presented in this study. The analysis of data focuses on the photochemical activity of air masses sampled during episodes of intense convection and biomass burning. Generally, the total sum of peroxy radical mixing ratios, measured in the outflow of convective clouds, are quite variable but occasionally are coupled with the NO variations indicating the coexistence or simultaneous emission of NOx, with a potential radical precursor (i.e. formaldehyde, acetone or peroxides), which has likely been transported to higher atmospheric altitudes. Based on the measurements, significant O3 production rates around 1 ppb/h in the MCS outflow are estimated by using a box model with simplified chemistry. Peroxy radicals having mixing ratios around 20–25 pptv and with peak values of up to 60–70 pptv are measured within biomass burning plumes, detected at the coast in Ghana. Calculations of back-trajectory densities confirm the origin of these air masses being a biomass burning region at southern latitudes and close to the Gulf of Guinea, according to satellite pictures. Measured peroxy radical concentrations agree reasonably with modelled estimations taking into account simple local chemistry. Moreover, the vertical profiles taken at the aircraft base in Ouagadougou, Burkina Faso, indicate the common feature of having maximum concentrations between 2 and 4 km, in agreement with other literature values obtained under similar conditions.
Primary and secondary contributions to aerosol light scattering and absorption in Mexico City during the MILAGRO 2006 campaign
Authors: Paredes-Miranda G. , Arnott W. P. , Jimenez J. L. , Aiken A. C. , Gaffney J. S. , Marley N. A.
Published: April 2010

Abstract. A photoacoustic spectrometer, a nephelometer, an aethalometer, and an aerosol mass spectrometer were used to measure at ground level real-time aerosol light absorption, scattering, and chemistry at an urban site located in North East Mexico City (Instituto Mexicano del Petroleo, Mexican Petroleum Institute, denoted by IMP), as part of the Megacity Impact on Regional and Global Environments field experiment, MILAGRO, in March 2006. Photoacoustic and reciprocal nephelometer measurements at 532 nm accomplished with a single instrument compare favorably with conventional measurements made with an aethalometer and a TSI nephelometer. The diurnally averaged single scattering albedo at 532 nm was found to vary from 0.60 to 0.85 with the peak value at midday and the minimum value at 07:00 a.m. local time, indicating that the Mexico City plume is likely to have a net warming effect on local climate. The peak value is associated with strong photochemical generation of secondary aerosol. It is estimated that the photochemical production of secondary aerosol (inorganic and organic) is approximately 75% of the aerosol mass concentration and light scattering in association with the peak single scattering albedo. A strong correlation of aerosol scattering at 532 nm and total aerosol mass concentration was found, and an average mass scattering efficiency factor of 3.8 m2/g was determined. Comparisons of photoacoustic and aethalometer light absorption with oxygenated organic aerosol concentration (OOA) indicate a very small systematic bias of the filter based measurement associated with OOA and the peak aerosol single scattering albedo.
Impact of climate change on photochemical air pollution in Southern California
Authors: Millstein D. E. , Harley R. A.
Published: April 2010

Abstract. The effects of future climate and emissions-related perturbations on ozone air quality in Southern California are considered, with an assumed increase to 2× pre-industrial levels for global background levels of carbon dioxide. Effects of emission and climate-related forcings on air quality are superimposed on a summer 2005 high-ozone time period. Perturbations considered here include (a) effect of increased temperature on atmospheric reaction rates, (b) effect of increased temperature on biogenic emissions, (c) effect of increased water vapor concentrations, (d) effect of increased pollutant levels at the inflow (western) boundary, and (e) effect of population growth and technology change on emissions within Southern California. Various combinations of the above perturbations are also considered. The climate-related perturbations (a–c) led to combined peak 1-h ozone increases of up to 11 ppb. The effect on ozone was greatly reduced when the temperature increase was applied mostly during nighttime hours rather than uniformly throughout the day. Increased pollutant levels at the inflow boundary also led to ozone increases up to 5 ppb. These climate and inflow-related changes offset some of the anticipated benefits of emission controls within the air basin.
Comparisons of WRF/Chem simulations in Mexico City with ground-based RAMA measurements during the 2006-MILAGRO
Authors: Zhang Y. , Dubey M. K. , Olsen S. C. , Zheng J. , Zhang R.
Published: April 2010

Abstract. Simulations using the fully coupled WRF/Chem (Weather Research and Forecasting – Chemistry) model at 3-km resolution in Mexico City have been performed to examine the temperature, relative humidity, wind, and gaseous criteria pollutants (CO, O3, NO, NO2, and NOy) during the MCMA-2006/MILAGRO field campaign. Comparison of the model simulations with measurements from the ground-based air quality monitoring network (RAMA) is presented. The model resolves reasonably well the observed surface temperature, relative humidity and wind speed; however, large discrepancies are identified between the simulated and the observed surface wind direction for wind speeds below 2 m s−1. The simulated chemical species concentrations (CO, O3, NO, NO2, and NOy) compare favorably with the observations. Simulated O3 concentrations agree especially well with the observations. The simulated 10 VOC species compare generally favorably with the observations at the T0 supersite although lower correlation coefficients and larger biases exist for propene, acetone and propanal, isoprene, and c10-aromatics when compared to the other VOC species. The model performs much better during daytime than nighttime for both chemical species and meteorological variables, although the model tends to underestimate daytime temperature and relative humidity. Simulations using combinations of the available PBL schemes and land surface models (LSMs) do not show a preferred combination in reproducing the observations. The simulated meteorological fields under the O3-South, O3-North and EI Norte weather episodes exhibit similar correlation coefficients and biases for the same variable. However, the model performs well for the O3-South episode but inferiorly for the El Norte events in resolving the observed chemical species.
SCIAMACHY CO over land and oceans: 2003–2007 interannual variability
Authors: Gloudemans A. M. S. , de Laat A. T. J. , Schrijver H. , Aben I. , Meirink J. F. , van der Werf G. R.
Published: April 2010

Abstract. We present a new method to obtain accurate SCIAMACHY CO columns over clouded ocean scenes. Based on an improved version of the Iterative Maximum Likelihood Method (IMLM) retrieval algorithm, we now have retrieved five years of data over both land and clouded ocean scenes between 2003 and 2007. The ocean-cloud method uses the CH4 columns retrieved simultaneously with the CO columns to determine the cloud top height. The CH4 cloud top height is in good agreement with the FRESCO+ cloud top height determined from UV-VIS oxygen-A band measurements, providing confidence that the CH4 cloud top height is a good diagnostic of the cloud top height over (partially) clouded ocean scenes. The CO measurements over clouded ocean scenes have been compared with collocated modeled CO columns over the same clouds and agree well. Using clouded ocean scenes quadruples the number of useful CO measurements compared to land-only measurements. The five-year CO data set over land and clouded ocean scenes presented here is based on an improved version of the IMLM algorithm which includes a more accurate determination of the random instrument-noise error for CO. This leads to a smaller spread in the differences between single CO measurements and the corresponding model values. The new version, IMLM version 7.4, also uses updated spectroscopic parameters for H2O and CH4 but this has only a minor impact on the retrieved CO columns. The five-year data set shows significant interannual variability over land and over clouded ocean scenes. Three examples are highlighted: the Asian outflow of pollution over the northern Pacific, the biomass-burning outflow over the Indian Ocean originating from Indonesia, and biomass burning in Brazil. In general there is good agreement between observed and modeled seasonal cycles and interannual variability.
Secondary organic aerosol from biogenic VOCs over West Africa during AMMA
Authors: Capes G. , Murphy J. G. , Reeves C. E. , McQuaid J. B. , Hamilton J. F. , Hopkins J. R. , Crosier J. , Williams P. I. , Coe H.
Published: April 2010

Abstract. This paper presents measurements of organic aerosols above subtropical West Africa during the wet season using data from the UK Facility for Airborne Atmospheric Measurements (FAAM) aircraft. Measurements of biogenic volatile organic compounds (BVOC) at low altitudes over these subtropical forests were made during the African Monsoon Multidisciplinary Analysis (AMMA) field experiment during July and August 2006 mainly above Benin, Nigeria and Niger. Data from an Aerodyne Quadrupole Aerosol Mass Spectrometer show a median organic aerosol loading of 1.07 μg m−3 over tropical West Africa, which represents the first regionally averaged assessment of organic aerosol mass (OM) in this region during the wet season. This is broadly in agreement with global model predictions based on partitioning schemes, although there are large uncertainties associated with such estimates. In contrast our own calculations based on aerosol yields from isoprene and monoterpenes during chamber studies under represent the OM measured in this region on a comparable scale to the under representations of OM by predictive models in the mid latitudes. As global models rely on similar yield calculations in their global estimates, as our calculations this points to further systematic differences between global model estimates and measurements of SOA, most likely caused by use of incorrect BVOC emission rates. The under predictions of OM by our calculations and those in the mid latitudes employ yields extrapolated from chamber data obtained at higher mass concentrations – more recent yield data for α-pinene obtained at ambient concentrations in a flow through chamber (Shilling et al., 2008) show considerably better agreement with our data.
Validation of urban NO2 concentrations and their diurnal and seasonal variations observed from the SCIAMACHY and OMI sensors using in situ surface measurements in Israeli cities
Authors: Boersma K. F. , Jacob D. J. , Trainic M. , Rudich Y. , DeSmedt I. , Dirksen R. , Eskes H. J.
Published: April 2010

Abstract. We compare a full-year (2006) record of surface air NO2 concentrations measured in Israeli cities to coinciding retrievals of tropospheric NO2 columns from satellite sensors (SCIAMACHY aboard ENVISAT and OMI aboard Aura). This provides a large statistical data set for validation of NO2 satellite measurements in urban air, where validation is difficult yet crucial for using these measurements to infer NOx emissions by inverse modeling. Assuming that NO2 is well-mixed throughout the boundary layer (BL), and using observed average seasonal boundary layer heights, near-surface NO2 concentrations are converted into BL NO2 columns. The agreement between OMI and (13:45) BL NO2 columns (slope=0.93, n=542), and the comparable results at 10:00 h for SCIAMACHY, allow a validation of the seasonal, weekly, and diurnal cycles in satellite-derived NO2. OMI and BL NO2 columns show consistent seasonal cycles (winter NO2 1.6–2.7× higher than summer). BL and coinciding OMI columns both show a strong weekly cycle with 45–50% smaller NO2 columns on Saturday relative to the weekday mean, reflecting the reduced weekend activity, and validating the weekly cycle observed from space. The diurnal difference between SCIAMACHY (10:00) and OMI (13:45) NO2 is maximum in summer when SCIAMACHY is up to 40% higher than OMI, and minimum in winter when OMI slightly exceeds SCIAMACHY. A similar seasonal variation in the diurnal difference is found in the source region of Cairo. The surface measurements in Israel cities confirm this seasonal variation in the diurnal cycle. Using simulations from a global 3-D chemical transport model (GEOS-Chem), we show that this seasonal cycle can be explained by a much stronger photochemical loss of NO2 in summer than in winter.
Size resolved dust emission fluxes measured in Niger during 3 dust storms of the AMMA experiment
Authors: Sow M. , Alfaro S. C. , Rajot J. L. , Marticorena B.
Published: April 2010

Abstract. During the 2006 and 2007 special observing periods of the African Monsoon Multidisciplinary Analysis campaign an original experimental system has been implemented in Banizoumbou (Niger) for measuring the size-resolved dust emission flux in natural conditions and documenting the possible influence of wind speed on its size distribution. The instrumental set-up, associated methodology, and the quality tests applied to the data set are described before the results acquired during 2 events of the Monsoon type and 1 of the convective type are analyzed in detail. In good agreement with the theory of sandblasting, it is found in all cases that saltation must take place for a vertical emission flux to be detected. During a particular erosion event, the magnitude of the vertical flux is controlled by the surface roughness, which conditions the saltation threshold, and by the wind friction velocity. The dust flux released by the high energy convective event is also found to be much richer in very fine (<2 µm) particles than those of the relatively moderate Monsoon event, which shows that aerodynamic conditions definitely influence the initial size distribution of the erosion flux as previously suggested by wind tunnel experiments. However, the size distribution of the dust released by a given event is fairly constant and insensitive to even relatively important variations of u*. This is interpreted as a possible result of the rather long duration (15 min) over which wind fluctuations must be averaged for computing u*, which could make it an inadequate parameter for representing the very short response-time physical processes that are at the origin of fine dust emission at the measurement sites.
Global upper-tropospheric formaldehyde: seasonal cycles observed by the ACE-FTS satellite instrument
Authors: Dufour G. , Szopa S. , Barkley M. P. , Boone C. D. , Perrin A. , Palmer P. I. , Bernath P. F.
Published: April 2010

Abstract. Seasonally-resolved upper tropospheric profiles of formaldehyde (HCHO) observed by the ACE Fourier transform spectrometer (ACE-FTS) on a near-global scale are presented for the time period from March 2004 to November 2006. Large upper tropospheric HCHO mixing ratios (>150 pptv) are observed during the growing season of the terrestrial biosphere in the Northern Hemisphere and during the biomass burning season in the Southern Hemisphere. The total errors estimated for the retrieved mixing ratios range from 30 to 40% in the upper troposphere and increase in the lower stratosphere. The sampled HCHO concentrations are in satisfactory agreement with previous aircraft and satellite observations with a negative bias (<25%) within observation errors. An overview of the seasonal cycle of the upper tropospheric HCHO is given for different latitudes, with a particular focus on mid-to-high latitudes that are well sampled by the observations. A maximum is observed during summer, i.e. during the growing season, in the northern mid- and high latitudes. The influence of biomass burning is visible in HCHO upper tropospheric concentrations during the September-to-October period in the southern tropics and subtropics. Comparisons with two state-of-the-art models (GEOS-Chem and LMDz-INCA) show that the models capture well the seasonal variations observed in the Northern Hemisphere (correlation >0.9). Both models underestimate the summer maximum over Europe and Russia and differences in the emissions used for North America result in a good reproduction of the summer maximum by GEOS-Chem but in an underestimate by LMDz-INCA. Globally, GEOS-Chem reproduces well the observations on average over one year but has some difficulties in reproducing the spatial variability of the observations. LMDz-INCA shows significant bias in the Southern Hemisphere, perhaps related to an underestimation of methane, but better reproduces the temporal and spatial variations. The differences between the models underline the large uncertainties that remain in the emissions of HCHO precursors.
Towards closing the gap between hygroscopic growth and activation for secondary organic aerosol – Part 2: Theoretical approaches
Authors: Petters M. D. , Wex H. , Carrico C. M. , Hallbauer E. , Massling A. , McMeeking G. R. , Poulain L. , Wu Z. , Kreidenweis S. M. , Stratmann F.
Published: April 2010

Abstract. We examine the hygroscopic properties of secondary organic aerosol particles generated through the reaction of α-pinene and ozone using a continuous flow reaction chamber. The water activity versus composition relationship is calculated from measurements of growth factors at relative humidities up to 99.6% and from measurements of cloud condensation nuclei activity. The observed relationships are complex, suggesting highly non-ideal behavior for aerosol water contents at relative humidities less than 98%. We present two models that may explain the observed water activity-composition relationship equally well. The first model assumes that the aerosol is a pseudo binary mixture of infinitely water soluble compounds and sparingly soluble compounds that gradually enter the solution as dilution increases. The second model is used to compute the Gibbs free energy of the aerosol-water mixture and shows that the aerosol behaves similarly to what can be expected for single compounds that contain a certain fraction of oxygenated and non-polar functional groups.
Oceanic influence on atmospheric mercury at coastal and inland sites: a springtime noreaster in New England
Authors: Sigler J. M. , Mao H. , Sive B. C. , Talbot R.
Published: April 2010

Abstract. Continuous measurements of elemental (Hg0) and reactive mercury were conducted at two sites in New Hampshire during a powerful April 2007 noreaster. During the most intense period of the storm, enhancements of ~30–50 ppqv in Hg0 were observed at a coastal and a high elevation inland site. This enhancement occurred simultaneously with elevated mixing ratios of three marine tracers, CH3I, CH2Br2 and CHBr3. These observations suggest a marine source of Hg0, possibly outgassing from the ocean surface during strong turbulence. The Hg0 enhancement observed 100 km inland suggests that the impact of coastal storms on terrestrial Hg cycling may not be limited to near-shore environments. Combining Hg0 and marine tracer measurements during the storm with estimates of oceanic tracer fluxes during previous strong storms yields an order-of-magnitude estimate of the oceanic source of Hg0 during the storm (~7 ppqv h−1) which can account for the observed enhancement at the field sites.
How important is the vertical structure for the representation of aerosol impacts on the diurnal cycle of marine stratocumulus?
Authors: Sandu I. , Brenguier J.-L. , Thouron O. , Stevens B.
Published: April 2010

Abstract. Large-Eddy Simulations (LES) are performed to examine the impact of hygroscopic aerosols on the diurnal cycle of marine stratocumulus clouds, under varying meteorological forcing conditions. When the cloud condensation nuclei concentration increase is sufficient to inhibit drizzle formation in the cloud layer, the precipitating and the non-precipitating cloud layers exhibit contrasting evolutions, with noticeable differences in liquid water path. Aerosol-induced modifications of the droplet sedimentation and drizzle precipitation result in noticeable changes of the entrainment velocity at cloud top, but also in significant changes of the vertical stratification in the boundary layer. This set of simulations is then used to evaluate whether a model which does not explicitly represent the effects of the interactions occurring within the boundary layer on its vertical stratification (i.e. such as a mixed-layer model) is capable of reproducing at least the sign, if not the amplitude, of these aerosol impacts on the liquid water path. It is shown that the evolution of the vertical structure is key to the responses we simulate, and must be considered in bulk models that wish to predict the impact of aerosol perturbations on the radiative properties of stratocumulus-topped boundary layers.
Surface ozone at the Caucasian site Kislovodsk High Mountain Station and the Swiss Alpine site Jungfraujoch: data analysis and trends (1990–2006)
Authors: Tarasova O. A. , Senik I. A. , Sosonkin M. G. , Cui J. , Staehelin J. , Prévôt A. S. H.
Published: April 2010

Abstract. Long-term ozone measurements of two background mountain sites, namely the Kislovodsk High Mountain Station in Caucasus, Russia (KHMS, 43.70° N, 42.70° E, 2070 m a.s.l.) and the Jungfraujoch in Switzerland (JFJ, 46.55° N, 7.98° E, 3580 m a.s.l.) are compared. Despite of more than 1.5 km altitude difference ozone mixing ratios are comparable at JFJ an KHMS in the beginning of measurements (1990–1993) while the annually averaged levels at JFJ are around 15 ppb higher than the ones at KHMS for the most recent years (1997–2006). The seasonal cycle of the surface ozone mixing ratios is characterized by a double spring-summer maximum at both sites with a spring one being more pronounced for the air masses with the longest contact with the upper free troposphere and stratosphere. Ozone mixing ratio increased at JFJ but decreased at KHMS for the period 1990–2006. Trends are more pronounced for the 1990s (+0.73±0.20 ppb/year at JFJ and −0.91±0.17 ppb/year at KHMS for the period 1991–2001) in comparison with the later years (+0.04±0.21 ppb/year at JFJ and −0.37±0.14 ppb/year at KHMS for the period 1997–2006). Trends show a distinct seasonality, which is different for the different periods. To investigate possible reasons for this remarkable trends difference 3-D trajectories using LAGRANTO trajectory model are used. Effects of horizontal and vertical transport on ozone trends are considered. No substantial systematic changes in the transport patterns were detected which could lead to strong changes in the trend magnitude between 1991–2001 and 1997–2006. The geographical position of the sites relative to the main topographic features and emission sources as well as distance from the coast are interpreted to be among the main reasons for the opposite surface ozone trends. During the 90s the JFJ trend reflects increase of the ozone in the upper free troposphere/lower stratosphere, while KHMS is not sensitive to this change or even showing the opposite tendency. The analysis provided evidence for a stronger influence of processes in the lower troposphere, in particular the dramatic emission decrease in the earlier 1990s in former USSR and emissions regulations in Western Europe on the surface ozone trend at KHMS.
Effects of the 2006 El Niño on tropospheric ozone and carbon monoxide: implications for dynamics and biomass burning
Authors: Chandra S. , Ziemke J. R. , Duncan B. N. , Diehl T. L. , Livesey N. J. , Froidevaux L.
Published: April 2010

Abstract. We have studied the effects of the 2006 El Niño on tropospheric O3 and CO at tropical and sub-tropical latitudes measured from the OMI and MLS instruments on the Aura satellite. The 2006 El Niño-induced drought caused forest fires (largely set to clear land) to burn out of control during October and November in the Indonesian region. The effects of these fires are clearly seen in the enhancement of CO concentration measured from the MLS instrument. We have used a global model of atmospheric chemistry and transport (GMI CTM) to quantify the relative importance of biomass burning and large scale transport in producing observed changes in tropospheric O3 and CO. The model results show that during October and November biomass burning and meteorological changes contributed almost equally to the observed increase in tropospheric O3 in the Indonesian region. The biomass component was 4–6 DU but it was limited to the Indonesian region where the fires were most intense. The dynamical component was 4–8 DU but it covered a much larger area in the Indian Ocean extending from South East Asia in the north to western Australia in the south. By December 2006, the effect of biomass burning was reduced to zero and the observed changes in tropospheric O3 were mostly due to dynamical effects. The model results show an increase of 2–3% in the global burden of tropospheric ozone. In comparison, the global burden of CO increased by 8–12%.
Aerosol composition of the tropical upper troposphere
Authors: Froyd K. D. , Murphy D. M. , Sanford T. J. , Thomson D. S. , Wilson J. C. , Pfister L. , Lait L.
Published: April 2010

Abstract. Aerosol composition was measured by the NOAA single-particle mass spectrometer (PALMS) aboard the NASA WB-57 high altitude aircraft platform during two Aura Validation Experiment (AVE) campaigns based in Costa Rica in 2004 and 2006. These studies yielded the most complete set of aerosol composition measurements to date throughout the tropical tropopause layer (TTL) and tropical lower stratosphere. We describe the aerosol properties of the tropical atmosphere and use composition tracers to examine particle sources, the role of recent convection, and cirrus-forming potential in the TTL. Tropical dynamics and regional air sources played principal roles in dictating tropospheric aerosol properties. There was a sharp change in aerosol chemical composition at about 12 km altitude coincident with a change in convective influence. Below this level, maritime convection lofted condensable material that generated acidic, sulfate-rich aerosol. These particles contained significant amounts of methanesulfonic acid (MSA) and showed evidence of cloud processes. In contrast, continental convection injected particles and precursors directly into the TTL, yielding a population of neutralized, organic-rich aerosol. The organics were often highly oxidized and particles with oxidized organics also contained nitrate. Above the tropopause, chemical composition gradually changed toward sulfuric acid particles but neutralized particles were still abundant 2 km above the tropopause. Deep continental convection, though sporadic and geographically localized, may strongly influence TTL aerosol properties on a global scale. The abundance of organic-rich aerosol may inhibit ice nucleation and formation of tropopause level cirrus.