bluuebunny/crossref_metadata_2025 huggingface dataset:
Coastal measurements of short-lived reactive iodocarbons and bromocarbons at Roscoff, Brittany during the RHaMBLe campaign
Authors: Jones C. E. , Hornsby K. E. , Dunk R. M. , Leigh R. J. , Carpenter L. J.
Published: April 2010

Abstract. Atmospheric concentrations of the volatile reactive iodocarbons C2H5I, 1-C3H7I, 2-C3H7I, CH2ICl, CH2IBr, CH2I2 and bromocarbons CH2Br2 and CHBr3 were determined by GC/MS analysis of marine boundary layer air at Roscoff, Brittany on the northwest coast of France during September 2006. Comparison with other coastal studies suggests that emissions of these trace gases are strongly influenced by site topography, seaweed populations and distribution, as well as tide height. Concentrations of the very short-lived dihalomethanes CH2IBr and CH2I2 in particular showed evidence of tidal dependence, with higher concentrations observed at low tide during maximum exposure of seaweed beds. We also present a limited number of halocarbon concentrations in surface seawater and estimate sea-air fluxes based on simultaneous water and air measurements of these gases. CH2Br2 and CHBr3 were strongly correlated both in air and in seawater, with CH2Br2/CHBr3 ratios of 0.19 in air and 0.06 in water. The combined midday I atom flux from the photolabile diahlomethanes CH2I2, CH2IBr and CH2ICl of ~5×103 molecules cm−3 s−1 is several orders of magnitude lower than the estimated I atom flux from I2 based on coinciding measurements at the same site, which indicates that at Roscoff the major I atom precursor was I2 rather than reactive iodocarbons.
A two-step scheme for high-resolution regional atmospheric trace gas inversions based on independent models
Authors: Rödenbeck C. , Gerbig C. , Trusilova K. , Heimann M.
Published: April 2010

Abstract. Mixing ratio measurements of atmospheric tracers like CO2 can be used to estimate regional surface-air tracer fluxes using inverse methods, involving a numerical transport model. Currently available transport models are either global but rather coarse, or more accurate but only over a limited spatial and temporal domain. To obtain higher-resolution flux estimates within a region of interest, existing studies use zoomed or coupled models. The two-step scheme developed here uses global and regional models sequentially in separate inversion steps, coupled only via the data vector. This provides a nested atmospheric inversion scheme without the necessity of a direct coupled model implementation. For example, the scheme allows an easy nesting of Lagrangian models with their potential of very high resolution into global inversions.
Fluxes and concentrations of volatile organic compounds above central London, UK
Authors: Langford B. , Nemitz E. , House E. , Phillips G. J. , Famulari D. , Davison B. , Hopkins J. R. , Lewis A. C. , Hewitt C. N.
Published: April 2010

Abstract. Concentrations and fluxes of eight volatile organic compounds (VOCs) were measured during October 2006 from a high telecom tower above central London, as part of the CityFlux contribution to the REPARTEE I campaign. A continuous flow disjunct eddy covariance technique with analysis by proton transfer reaction mass spectrometry was used. Daily averaged VOC mixing ratios were within the range 1–19 ppb for the oxygenated compounds (methanol, acetaldehyde and acetone) and 0.2–1.3 ppb for the aromatics (benzene, toluene and ethylbenzene). Typical VOC fluxes were in the range 0.1–1.0 mg m−2 h−1. There was a non-linear relationship between VOC fluxes and traffic density for most of the measured compounds. Traffic activity was estimated to account for approximately 70% of the aromatic compound fluxes, whereas non-traffic related sources were found to be more important for methanol and isoprene fluxes. The measured fluxes were comparable to the estimates of the UK national atmospheric emission inventory for the aromatic VOCs and CO. In contrast, fluxes of the oxygenated compounds were about three times larger than inventory estimates. For isoprene and acetonitrile this difference was many times larger. At temperatures over 25°C it is estimated that more than half the isoprene observed in central London is of biogenic origin.
Cross-hemispheric transport of central African biomass burning pollutants: implications for downwind ozone production
Authors: Real E. , Orlandi E. , Law K. S. , Fierli F. , Josset D. , Cairo F. , Schlager H. , Borrmann S. , Kunkel D. , Volk M. , McQuaid J. B. , Stewart D. J. , Lee J. , Lewis A. , Hopkins J. R. , Ravegnani F. , Ulanovski A. , Liousse C.
Published: April 2010

Abstract. Pollutant plumes with enhanced levels of trace gases and aerosols were observed over the southern coast of West Africa during August 2006 as part of the AMMA wet season field campaign. Plumes were observed both in the mid and upper troposphere. In this study we examined both the origin of these pollutant plumes and their potential to produce O3 downwind over the Atlantic Ocean. Runs using the BOLAM mesoscale model including biomass burning CO tracers were used to confirm an origin from central African fires. The plumes in the mid troposphere had significantly higher pollutant concentrations due to the fact that transport occurred from a region nearer or even over the fire region. In contrast, plumes transported into the upper troposphere over West Africa had been transported to the north-east of the fire region before being uplifted. Modelled tracer results showed that pollutants resided for between 9 and 12 days over Central Africa before being transported for 4 days, in the case of the mid-troposphere plume and 2 days in the case of the upper tropospheric plume to the measurement location over the southern part of West Africa. Around 35% of the biomass burning tracer was transported into the upper troposphere compared to that remaining in the mid troposphere. Runs using a photochemical trajectory model, CiTTyCAT, were used to estimate the net photochemical O3 production potential of these plumes. The mid tropospheric plume was still very photochemically active (up to 7 ppbv/day) especially during the first few days of transport westward over the Atlantic Ocean. The upper tropospheric plume was also still photochemically active, although at a slower rate (1–2 ppbv/day). Trajectories show this plume being recirculated around an upper tropospheric anticyclone back towards the African continent (around 20° S). The potential of theses plumes to produce O3 supports the hypothesis that biomass burning pollutants are contributing to the observed O3 maxima over the southern Atlantic at this time of year.
Comment on "Classification of aerosol properties derived from AERONET direct sun data" by G. P. Gobbi et al. (2007)
Authors: O'Neill N. T.
Published: April 2010

Abstract. It is pointed out that the graphical, aerosol classification method of Gobbi et al. (2007) can be interpreted as a manifestation of fundamental analytical relations whose existance depends on the simple assumption that the optical effects of aerosols are essentially bimodal in nature. The families of contour lines in their "Ada" curvature space are essentially empirical and discretized illustrations of analytical parabolic forms in (α, α') space (the space formed by the continuously differentiable Angstrom exponent and its spectral derivative).
Parametric representation of the cloud droplet spectra for LES warm bulk microphysical schemes
Authors: Geoffroy O. , Brenguier J.-L. , Burnet F.
Published: April 2010

Abstract. Parametric functions are currently used to represent droplet spectra in clouds and to develop bulk parameterizations of the microphysical processes and of their interactions with radiation. The most frequently used parametric functions are the Lognormal and the Generalized Gamma which have three and four independent parameters, respectively. In a bulk parameterization, two parameters are constrained by the total droplet number concentration and the liquid water content. In the Generalized Gamma function, one parameter is specified a priori, and the fourth one, like the third parameter of the Lognormal function, shall be tuned, for the parametric function to statistically best fit observed droplet spectra. These parametric functions are evaluated here using droplet spectra collected in non-or slightly precipitating stratocumulus and shallow cumulus. Optimum values of the tuning parameters are derived by minimizing either the absolute or the relative error for successively the first, second, fifth, and sixth moments of the droplet size distribution. A trade-off value is also proposed that minimizes both absolute and relative errors for the four moments concomitantly. Finally, a parameterization is proposed in which the tuning parameter depends on the liquid water content. This approach significantly improves the fit for the smallest and largest values of the moments.
Secondary organic aerosol production from modern diesel engine emissions
Authors: Samy S. , Zielinska B.
Published: April 2010

Abstract. Secondary organic aerosol (SOA) production was observed at significant levels in a series of modern diesel exhaust (DE) aging experiments conducted at the European Outdoor Photoreactor/Simulation Chamber (EUPHORE). The greatest production occurred in DE with toluene addition experiments (>40%), followed by DE with HCHO (for OH radical generation) experiments. A small amount of SOA (3%) was observed for DE in dark with N2O5 (for NO3 radical production) experiments. The analysis for a limited number (54) of polar organic compounds (POC) was conducted to assess the composition of modern DE and the formation of photochemical transformation products. Distinct POC formation in light versus dark experiments suggests the role of OH initiated reactions in these chamber atmospheres. A trend of increasing concentrations of dicarboxylic acids in light versus dark experiments was observed when evaluated on a compound group basis. The four toluene addition experiments in this study were performed at different [tol]o/[NOx]o ratios and displayed an average SOA% yield (in relation to toluene) of 5.3±1.6%, which is compared to past chamber studies that evaluated the impact of [tol]o/[NOx]o on SOA production in more simplified mixtures.
Fluorescent biological aerosol particle concentrations and size distributions measured with an ultraviolet aerodynamic particle sizer (UV-APS) in Central Europe
Authors: Huffman J. A. , Treutlein B. , Pöschl U.
Published: April 2010

Abstract. Primary biological aerosol particles (PBAPs), including bacteria, spores and pollen, are essential for the spread of organisms and disease in the biosphere, and numerous studies have suggested that they may be important for atmospheric processes, including the formation of clouds and precipitation. The atmospheric abundance and size distribution of PBAPs, however, are largely unknown. At a semi-urban site in Mainz, Germany, we used an ultraviolet aerodynamic particle sizer (UV-APS) to measure fluorescent biological aerosol particles (FBAPs), which can be regarded as viable bioaerosol particles representing a lower limit for the actual abundance of PBAPs. Fluorescence of non-biological aerosol components are likely to influence the measurement results obtained for fine particles (<1 μm), but not for coarse particles (1–20 μm). Averaged over the four-month measurement period (August–December 2006), the mean number concentration of coarse FBAPs was ~3×10−2 cm−3, corresponding to ~4% of total coarse particle number. The mean mass concentration of FBAPs was ~1 μg m−3, corresponding to ~20% of total coarse particle mass. The FBAP number size distributions exhibited alternating patterns with peaks at various diameters. A pronounced peak at ~3 μm was essentially always observed and can be described by the following campaign-average lognormal fit parameters: geometric mean diameter 3.2 μm, geometric standard deviation 1.3, number concentration 1.6×10−2 cm−3. This peak is likely due to fungal spores or agglomerated bacteria, and it exhibited a pronounced diel cycle with maximum intensity during early/mid-morning. FBAP peaks around ~1.5 μm, ~5 μm, and ~13 μm were also observed, but less pronounced and less frequent. These may be explained by single bacterial cells, larger fungal spores, and pollen grains, respectively. The observed number concentrations and characteristic sizes of FBAPs are consistent with microscopic, biological and chemical analyses of PBAPs in aerosol filter samples. To our knowledge, however, this study reporting: continuous online measurements of bioaerosol particles over several months, a range of characteristic size distribution patterns, and a persistent bioaerosol peak at ~3 μm. The measurement results confirm that PBAPs account for a substantial proportion of coarse aerosol particle number and mass in continental boundary layer air. Moreover, they suggest that the number concentration of viable bioparticles is dominated by fungal spores or agglomerated bacteria with aerodynamic diameters around 3 μm rather than single bacterial cells with diameters around 1 μm.
The role of sulphates and organic vapours in new particle formation in a eucalypt forest
Authors: Ristovski Z. D. , Suni T. , Kulmala M. , Boy M. , Meyer N. K. , Duplissy J. , Turnipseed A. , Morawska L. , Baltensperger U.
Published: April 2010

Abstract. The influence of biogenic particle formation on climate is a well recognized phenomenon. To understand the mechanisms underlying the biogenic particle formation, determining the chemical composition of the new particles and therefore the species that drive the particle production is of utmost importance. Due to the very small amount of mass involved, indirect approaches are frequently used to infer the composition. We present here the results of such an indirect approach by simultaneously measuring volatile and hygroscopic properties of newly formed particles in a forest environment. We that the particles are composed of both sulphates and organics, with the amount of sulphate component strongly depending on the available gas-phase sulphuric acid, and the organic components being photo-oxidation products of most likely a monoterpene. Our findings confirm a two-step process through nucleation and cluster formation followed by simultaneous growth by condensation of sulphates and organics that take the particles to climatically relevant sizes.
Transpacific pollution transport during INTEX-B: spring 2006 in context to previous years
Authors: Pfister G. G. , Emmons L. K. , Edwards D. P. , Arellano A. , Sachse G. , Campos T.
Published: April 2010

Abstract. We analyze the transport of pollution across the Pacific during the NASA INTEX-B (Intercontinental Chemical Transport Experiment Part B) campaign in spring 2006 and examine how this year compares to the time period for 2000 through 2006. In addition to aircraft measurements of carbon monoxide (CO) collected during INTEX-B, we include in this study multi-year satellite retrievals of CO from the Measurements of Pollution in the Troposphere (MOPITT) instrument and simulations from the chemistry transport model MOZART-4. Model tracers are used to examine the contributions of different source regions and source types to pollution levels over the Pacific. Additional modeling studies are performed to separate the impacts of inter-annual variability in meteorology and dynamics from changes in source strength. Interannual variability in the tropospheric CO burden over the Pacific and the US as estimated from the MOPITT data range up to 7% and a somewhat smaller estimate (5%) is derived from the model. When keeping the emissions in the model constant between years, the year-to-year changes are reduced to (2%), but show that in addition to changes in emissions, variable meteorological conditions also impact transpacific pollution transport. We estimate that about 1/3 of the variability in the tropospheric CO loading over the contiguous US is explained by changes in emissions and about 2/3 by changes in meteorology and transport. Biomass burning sources are found to be a larger driver for inter-annual variability in the CO loading compared to fossil and biofuel sources or photochemical CO production even though their absolute contributions are smaller. Source contribution analysis shows that the aircraft sampling during INTEX-B was fairly representative of the larger scale region, but with a slight bias towards higher influence from Asian contributions.
On the quality of the Nimbus 7 LIMS Version 6 water vapor profiles and distributions
Authors: Remsberg E. E. , Natarajan M. , Lingenfelser G. S. , Thompson R. E. , Marshall B. T. , Gordley L. L.
Published: April 2010

Abstract. This report describes the quality of the Nimbus 7 Limb Infrared Monitor of the Stratosphere (LIMS) water vapor (H2O) profiles of 1978/1979 that were processed with a Version 6 (V6) algorithm and archived in 2002. The V6 profiles incorporate a better knowledge of the instrument attitude for the LIMS measurements along its orbits, leading to improvements for its temperature profiles and for the registration of its water vapor radiances with pressure. As a result, the LIMS V6 zonal-mean distributions of H2O exhibit better hemispheric symmetry than was the case from the original Version 5 (V5) dataset that was archived in 1982. Estimates of the precision and accuracy of the V6 H2O profiles are developed and provided. Individual profiles have a precision of order 5% and an estimated accuracy of about 19% at 3 hPa, 14% at 10 hPa, and 26% at 50 hPa. Profile segments within about 2 km of the tropopause are often affected by emissions from clouds that appear in the finite field-of-view of the detector for the LIMS H2O channel. Zonally-averaged distributions of the LIMS V6 H2O are compared with those from the more recent Microwave Limb Sounder (MLS) satellite experiment for November, February, and May of 2004/2005. The patterns and values of their respective distributions are similar in many respects. Effects of a strengthened Brewer-Dobson circulation are indicated in the MLS distributions of the recent decade versus those of LIMS from 1978/1979. A tropical tape recorder signal is present in the 7-month time series of LIMS V6 H2O with lowest values in February 1979, and the estimated, annually-averaged "entry-level" H2O is 3.5 to 3.8 ppmv. It is judged that this historic LIMS water vapor dataset is of good quality for studies of the near global-scale chemistry and transport for pressure levels from 3 hPa to about 70 to 100 hPa.
Influence of aerosols on the formation and development of radiation fog
Authors: Rangognio J. , Tulet P. , Bergot T. , Gomes L. , Thouron O. , Leriche M.
Published: April 2010

Abstract. This paper assesses the impact of aerosol properties on the formation and the development of radiation fog. Simulations were performed using the Meso-NH meteorological model including the ORILAM aerosol scheme coupled with a two-moment microphysical cloud scheme (number concentration of cloud droplets and cloud water content). The activation scheme used was taken from the work of Abdul-Razzak and Ghan (2004). "Off-line" sensitivity analysis of CCN (Cloud Condensation Nuclei) activation was performed on number, median diameter and chemical compounds of aerosols. During this "off-line" study, the interactions with the other physical processes (e.g. radiative) were not taken into account since the cooling rate was imposed. Different regimes of CCN activation and a critical value of aerosol number concentration were found. This critical aerosol number corresponds to the maximum of activated cloud droplets for a given cooling rate and given aerosol chemical properties. As long as the aerosol number concentration is below this critical value, the cloud droplet number increases when the aerosol number increases. But when the aerosol number concentration exceeds this critical value, the cloud droplet number decreases when aerosol number increases. A sensitivity study on aerosol chemical composition showed that the CCN activation was limited in the case of hydrophilic aerosol composed of material with a solubility in the 10% range. An event observed during the ParisFOG field experiment was simulated. This case took place in the polluted sub-urban area of Paris (France) characterized by particle concentrations of 17 000 aerosols per cm3. 1D simulations successfully reproduced the observed temporal evolution of the fog layer. Beyond the initial fog formation at the surface, cloud droplet formation occurred at the top of the fog layer where the cooling rate was maximum, reaching more than −10 K h−1. These simulations confirm that the aerosol particle number concentration is a key parameter for the accurate prediction of the microphysical properties of a fog layer and also influences the vertical development of fog. The important of the interaction between microphysical and radiative processes is illustrated, showing how the life cycle of a fog layer is determined by the CCN number concentration and chemical properties.
Linking aerosol fluxes in street canyons to urban city-scale emissions
Authors: Tay B. K. , McFiggans G. B. , Jones D. P. , Gallagher M. W. , Martin C. , Watkins P. , Harrison R. M.
Published: April 2010

Abstract. In this study we investigate ultrafine particle (UFP) fluxes using a first order eddy viscosity turbulence closure Computational Fluid Dynamics (CFD) model and determine the different factors that influence emissions of UFP into the urban boundary layer. Both vertical turbulent fluxes as well as the fluxes due to mean flow are shown to contribute to the overall ventilation characteristics of street canyons. We then derive a simple parameterised numerical prediction model for canyon top UFP venting which is then compared with tower based micrometeorological flux measurements obtained during the REPARTEE and CityFlux field experiments.
Sensitivity analyses of OH missing sinks over Tokyo metropolitan area in the summer of 2007
Authors: Chatani S. , Shimo N. , Matsunaga S. , Kajii Y. , Kato S. , Nakashima Y. , Miyazaki K. , Ishii K. , Ueno H.
Published: April 2010

Abstract. OH reactivity is one of key indicators which reflect impacts of photochemical reactions in the atmosphere. An observation campaign has been conducted in the summer of 2007 at the heart of Tokyo metropolitan area to measure OH reactivity. The total OH reactivity measured directly by the laser-induced pump and probe technique was higher than the sum of the OH reactivity calculated from concentrations and reaction rate coefficients of individual species measured in this campaign. And then, three-dimensional air quality simulation has been conducted to evaluate the simulation performance on the total OH reactivity including "missing sinks", which correspond to the difference between the measured and calculated total OH reactivity. The simulated OH reactivity is significantly underestimated because the OH reactivity of volatile organic compounds (VOCs) and missing sinks are underestimated. When scaling factors are applied to input emissions and boundary concentrations, a good agreement is observed between the simulated and measured concentrations of VOCs. However, the simulated OH reactivity of missing sinks is still underestimated. Therefore, impacts of unidentified missing sinks are investigated through sensitivity analyses. In the cases that unknown secondary products are assumed to account for unidentified missing sinks, they tend to suppress formation of secondary aerosol components and enhance formation of ozone. In the cases that unidentified primary emitted species are assumed to account for unidentified missing sinks, a variety of impacts may be observed, which could serve as precursors of secondary organic aerosols (SOA) and significantly increase SOA formation. Missing sinks are considered to play an important role in the atmosphere over Tokyo metropolitan area.
Numerical simulation of tropospheric injection of biomass burning products by pyro-thermal plumes
Authors: Rio C. , Hourdin F. , Chédin A.
Published: April 2010

Abstract. The thermal plume model, a mass-flux scheme originally developed to represent the vertical transport by convective structures within the boundary layer, is adapted to the representation of plumes generated by fires, with the aim of estimating the height at which fire emissions are actually injected in the atmosphere. The parameterization, which takes into account fire characteristics, the induced excess of near surface temperature and mixing with environmental air, is first evaluated on two well-documented fires. Simulations over Southern Africa performed with the general circulation model LMDZ over one month show that the CO2 can be injected far above the boundary layer height, leading to a daily excess of CO2 in the mid-troposphere of an order of 2 ppmv. These results agree with satellite retrievals of a diurnal cycle of CO2 in the free troposphere over regions affected by biomass burning in the Tropics.
Uncertainties in wind speed dependent CO2 transfer velocities due to airflow distortion at anemometer sites on ships
Authors: Griessbaum F. , Moat B. I. , Narita Y. , Yelland M. J. , Klemm O. , Uematsu M.
Published: April 2010

Abstract. Data from research vessels and merchant ships are used to estimate ocean CO2 uptake via parameterizations of the gas transfer velocity (k) and measurements of the difference between the concentration of CO2 in the ocean (pCO2sw) and atmosphere (pCO2atm) and of wind speed. Gas transfer velocities estimated using wind speed dependent parameterisations may be in error due to air flow distortion by the ship's hull and superstructure introducing biases into the measured wind speed. The effect of airflow distortion on estimates of the transfer velocity was examined by modelling the airflow around the three-dimensional geometries of the research vessels Hakuho Maru and Mirai, using the Large Eddy Simulation code GERRIS. For airflows within ±45° of the bow the maximum bias was +16%. For wind speed of 10 m s−1 to 15 m s−1, a +16% bias in wind speed would cause an overestimate in the calculated value of k of 30% to 50%, depending on which k parameterisation is used. This is due to the propagation of errors when using quadratic or cubic parameterizations. Recommendations for suitable anemometer locations on research vessels are given. The errors in transfer velocity may be much larger for typical merchant ships, as the anemometers are generally not as well-exposed as those on research vessels. Flow distortion may also introduce biases in the wind speed dependent k parameterizations themselves, since these are obtained by relating measurements of the CO2 flux to measurements of the wind speed and the CO2 concentration difference. To investigate this, flow distortion effects were estimated for three different platforms from which wind speed dependent parameterizations are published. The estimates ranged from –4% to +14% and showed that flow distortion may have a significant impact on wind speed dependent parameterizations. However, the wind biases are not large enough to explain the differences at high wind speeds in parameterizations which are based on eddy covariance and deliberate tracer methods.
Measurements of coarse mode and primary biological aerosol transmission through a tropical forest canopy using a dual-channel fluorescence aerosol spectrometer
Authors: Gabey A. M. , Gallagher M. W. , Whitehead J. , Dorsey J.
Published: April 2010

Abstract. Aerosol in the size range 0.8–20 μm was characterized according to optical equivalent diameter, DP, morphology and the presence of biological material, the latter determined by recording fluorescence excited by ultraviolet light pulses at two different wavelengths. Single-particle measurements were performed within and subsequently above a tropical rainforest in Borneo, Malaysia, in June and July 2008. In both locations the aerosol number size distribution exhibited a primary biological aerosol (PBA) mode sized 2 μm2 μm and possessed a wider morphological range than non-PBA. It also accounted for around 80% of the total number in the understory and 40% of the total number above canopy. Canopy transmission efficiencies for the total aerosol number and PBA are calculated to be 0.48±0.19 and 0.31±0.15 respectively, with the former appearing to peak during the daytime because of a lack of PBA emission below the canopy.
An emission inventory of sulfur from anthropogenic sources in Antarctica
Authors: Shirsat S. V. , Graf H. F.
Published: April 2010

Abstract. This paper presents first results of a comprehensive emission inventory of chemical species from anthropogenic activities (power generation, vehicles, ships and aircraft) in Antarctica, covering the 2004–2005 period. The inventory is based on estimated emission rates of fuel consumption provided by some of the Antarctic research stations. Since the emission sources have different modes of operation and use a variety of fuel, the emission flux rate of chemical species is calculated by multiplying the fuel consumption value with the density of fuel and appropriate emission factors. A separate inventory is prepared for each anthropogenic emission source in Antarctica. Depending on the type of operation, emission rates of SO2, and BC (Black Carbon, from shipping only) have been calculated using the above technique. However, only results of SO2 emissions from each source are presented here. Emission inventory maps of SO2 depicting the track/path taken by each mobile source are shown. The total annual SO2 is 158 Mg from power generation and vehicle operations, 3873 Mg from ships and 56 Mg from aircraft for 2004–2005 and these values undergo strong seasonality following the human activity in Antarctica. Though these figures are small when compared to the emissions at most other regions of the world, they are an indication that human presence in Antarctica leads to at least local pollution. The sources are mainly line and point sources and thus the local pollution potentially is relatively strong.
Potential climatic impacts and reliability of very large-scale wind farms
Authors: Wang C. , Prinn R. G.
Published: April 2010

Abstract. Meeting future world energy needs while addressing climate change requires large-scale deployment of low or zero greenhouse gas (GHG) emission technologies such as wind energy. The widespread availability of wind power has fueled legitimate interest in this renewable energy source as one of the needed technologies. For very large-scale utilization of this resource, there are however potential environmental impacts, and also problems arising from its inherent intermittency, in addition to the present need to lower unit costs. To explore some of these issues, we use a three-dimensional climate model to simulate the potential climate effects associated with installation of wind-powered generators over vast areas of land or coastal ocean. Using wind turbines to meet 10% or more of global energy demand in 2100, could cause surface warming exceeding 1°C over land installations. In contrast, surface cooling exceeding 1°C is computed over ocean installations, but the validity of simulating the impacts of wind turbines by simply increasing the ocean surface drag needs further study. Significant warming or cooling remote from both the land and ocean installations, and alterations of the global distributions of rainfall and clouds also occur. These results are influenced by the competing effects of increases in roughness and decreases in wind speed on near-surface turbulent heat fluxes, the differing nature of land and ocean surface friction, and the dimensions of the installations parallel and perpendicular to the prevailing winds. These results are also dependent on the accuracy of the model used, and the realism of the methods applied to simulate wind turbines. Additional theory and new field observations will be required for their ultimate validation. Intermittency of wind power on daily, monthly and longer time scales as computed in these simulations and inferred from meteorological observations, poses a demand for one or more options to ensure reliability, including backup generation capacity, very long distance power transmission lines, and onsite energy storage, each with specific economic and/or technological challenges.
Simulating atmospheric composition over a South-East Asian tropical rainforest: Performance of a chemistry box model
Authors: Pugh T. A. M. , MacKenzie A. R. , Hewitt C. N. , Langford B. , Edwards P. M. , Furneaux K. L. , Heard D. E. , Hopkins J. R. , Jones C. E. , Karunaharan A. , Lee J. , Mills G. , Misztal P. , Moller S. , Monks P. S. , Whalley L. K.
Published: April 2010

Abstract. Atmospheric composition and chemistry above tropical rainforests is currently not well established, particularly for south-east Asia. In order to examine our understanding of chemical processes in this region, the performance of a box model of atmospheric boundary layer chemistry is tested against measurements made at the top of the rainforest canopy near Danum Valley, Malaysian Borneo. Multi-variate optimisation against ambient concentration measurements was used to estimate average canopy-scale emissions for isoprene, total monoterpenes and nitric oxide. The excellent agreement between estimated values and measured fluxes of isoprene and total monoterpenes provides confidence in the overall modelling strategy, and suggests that this method may be applied where measured fluxes are not available. The largest contributors to the optimisation cost function at the point of best-fit are OH (41%), NO (18%) and total monoterpenes (16%). Several factors affect the modelled VOC chemistry. In particular concentrations of methacrolein (MACR) and methyl-vinyl ketone (MVK) are substantially overestimated, and the hydroxyl radical [OH] concentration is substantially underestimated; as has been seen before in tropical rainforest studies. It is shown that inclusion of dry deposition of MACR and MVK and wet deposition of species with high Henry's Law values substantially improves the fit of these oxidised species, whilst also substantially decreasing the OH sink. Increasing [OH] production arbitrarily, through a simple OH recycling mechanism, adversely affects the model fit for volatile organic compounds (VOCs). Given the constraints on isoprene flux provided by measurements, a substantial decrease in the rate of reaction of VOCs with OH is the only remaining option to explain the measurement/model discrepancy for OH. A reduction in the isoprene + OH rate constant of 50–70% is able to produce both isoprene and OH concentrations within error of those measured. Whilst we cannot rule out an important role for missing chemistry, particularly in areas of higher isoprene flux, this study demonstrates that the inadequacies apparent in box and global model studies of tropical VOC chemistry may be more strongly influenced by representation of detailed physical and micrometeorological effects than errors in the chemical scheme.
High-accuracy measurements of snow Bidirectional Reflectance Distribution Function at visible and NIR wavelengths – comparison with modelling results
Authors: Dumont M. , Brissaud O. , Picard G. , Schmitt B. , Gallet J.-C. , Arnaud Y.
Published: April 2010

Abstract. High-accuracy measurements of snow Bidirectional Reflectance Distribution Function (BRDF) were performed for four natural snow samples with a spectrogonio-radiometer in the 500–2600 nm wavelength range. These measurements are one of the first set of direct snow BRDF values over a wide range of lighting and viewing geometry. They were compared to BRDF calculated with two optical models. Variations of the snow anisotropy factor with lighting geometry, wavelength and snow physical properties were investigated. Results show that at wavelengths with small penetration depth, scattering mainly occurs in the very top layers and the anisotropy factor is controlled by the phase function. In this condition, forward scattering peak or double scattering peak is observed. In constrast at shorter wavelengths, the penetration of the radiation is much deeper and the number of scattering events increases. The anisotropy factor is thus nearly constant and decreases at grazing observation angles.
Particle number, particle mass and NOx emission factors at a highway and an urban street in Copenhagen
Authors: Wang F. , Ketzel M. , Ellermann T. , Wåhlin P. , Jensen S. S. , Fang D. , Massling A.
Published: April 2010

Abstract. This paper presents measurements of traffic-generated gas and particle pollution at two sites, one near a major highway and one near a busy urban street in Copenhagen, Denmark. Both sites were equipped for a 4-week period with a set of two measurement stations, one close to the kerbside and one background station. Measurements were carried out from March to April 2008, investigating NOx concentrations, submicrometer particle number size distribution (size range 10–700 nm), particle mass (PM2.5, PM10), and meteorological parameters. In this study we further estimate the emission factors for NOx, particle number and particle mass using measured traffic volume and dilution rate calculated by the Operational Street Pollution Model (WinOSPM). The mean concentrations of most of the measured pollutants are similar for the highway and the urban kerbside stations due to similar traffic density. The average concentrations of NOx are 142 μg m
Comparison of aromatic hydrocarbon measurements made by PTR-MS, DOAS and GC-FID in Mexico City during the MCMA 2003 field experiment
Authors: Jobson B. T. , Volkamer R. , Velasco E. , Allwine G. , Westberg H. , Lamb B. , Alexander M. L. , Berkowitz C. M. , Molina L. T.
Published: April 2010

Abstract. A comparison of aromatic hydrocarbon measurements is reported for the CENICA supersite in the district of Iztapalapa during the Mexico City Metropolitan Area field experiment in April 2003 (MCMA 2003). Data from three different measurement methods were compared, a proton transfer reaction mass spectrometer (PTR-MS), long path measurements using a UV differential optical absorption spectrometer (DOAS), and gas chromatography-flame ionization analysis (GC-FID) of canister samples. Lab tests established that the PTR-MS and DOAS calibrations were consistent for a suite of aromatic compounds including benzene, toluene, p-xylene, ethylbenzene, 1,2,4-trimethylbenzene, phenol, and styrene. The point sampling measurements by the PTR-MS and GC-FID showed good correlations (r=0.6), and were in reasonable agreement for toluene, C2-alkylbenzenes, and C3-alkylbenzenes. The PTR-MS benzene data were consistently high, indicating potential interference from fragmenting alkyl aromatics for the 145 Td drift field intensity used in the experiment. Correlations between the open-path data measured at 16-m height over a 860 m path length (retroreflector in 430 m distance), and the point measurements collected at 37-m sampling height were best for benzene (r=0.61), and reasonably good for toluene, C2-alkylbenzenes, naphthalene, styrene, cresols and phenol (r>0.5). While the DOAS data agreed within 20% with both point measurements for benzene, concentrations measured by DOAS were on average a factor of 1.7 times greater than the PTRMS data for toluene, C2-alkylbenzenes, naphthalene, and styrene. The level of agreement for the toluene data was a function of wind direction, establishing that spatial gradients – horizontal, vertical, or both – in VOC mixing ratios were significant, and up to a factor of 2 despite the fact that all measurements were conducted above roof level. Our analysis highlights a potential problem in defining a VOC sampling strategy that is meaningful for comparison with photochemical transport models: meaningful measurements require a spatial fetch that is comparable to the grid cell size of models, which is typically few 10 km2. Long-path DOAS measurements inherently average over a larger spatial scale than point measurements. The spatial representativeness can be further increased if observations are conducted outside the surface roughness sublayer, which might require measurements at altitudes as high as few 10 m above roof level.
Acetaldehyde in the Alaskan subarctic snow pack
Authors: Domine F. , Houdier S. , Taillandier A.-S. , Simpson W. R.
Published: April 2010

Abstract. Acetaldehyde is a reactive intermediate in hydrocarbon oxidation. It is both emitted and taken up by snowpacks and photochemical and physical processes are probably involved. Understanding the reactivity of acetaldehyde in snow and its processes of physical and chemical exchanges requires the knowledge of its incorporation mechanism in snow crystals. We have performed a season-long study of the evolution of acetaldehyde concentrations in the subarctic snowpack near Fairbanks (65° N), central Alaska, which is subjected to a vigorous metamorphism due to persistent elevated temperature gradients in the snowpack, between 20 and 200°C m−1. The snowpack therefore almost entirely transforms into depth hoar. We have also analyzed acetaldehyde in a manipulated snowpack where temperature gradients were suppressed. Snow crystals there transformed much more slowly and their original shapes remained recognizable for months. The specific surface area of snow layers in both types of snowpacks was also measured. We deduce that acetaldehyde is not adsorbed onto the surface of snow crystals and that most of the acetaldehyde is probably not dissolved in the ice lattice of the snow crystals. We propose that most of the acetaldehyde measured is either trapped or dissolved within organic aerosol particles trapped in snow, or that acetaldehyde is formed by the hydrolysis of organic precursors contained in organic aerosols trapped in the snow, when the snow is melted for analysis. These precursors are probably aldehyde polymers formed within the aerosol particles by acid catalysis, but might also be biological molecules. In a laboratory experiment, acetaldehyde-di-n-hexyl acetal, representing a potential acetaldehyde precursor, was subjected to our analytical procedure and reacted to form acetaldehyde. This confirms our suggestion that acetaldehyde in snow could be produced during the melting of snow for analysis.
An overview of the SCOUT-AMMA stratospheric aircraft, balloons and sondes campaign in West Africa, August 2006: rationale, roadmap and highlights
Authors: Cairo F. , Pommereau J. P. , Law K. S. , Schlager H. , Garnier A. , Fierli F. , Ern M. , Streibel M. , Arabas S. , Borrmann S. , Berthelier J. J. , Blom C. , Christensen T. , D'Amato F. , Di Donfrancesco G. , Deshler T. , Diedhiou A. , Durry G. , Engelsen O. , Goutail F. , Harris N. R. P. , Kerstel E. R. T. , Khaykin S. , Konopka P. , Kylling A. , Larsen N. , Lebel T. , Liu X. , MacKenzie A. R. , Nielsen J. , Oulanowski A. , Parker D. J. , Pelon J. , Polcher J. , Pyle J. A. , Ravegnani F. , Rivière E. D. , Robinson A. D. , Röckmann T. , Schiller C. , Simões F. , Stefanutti L. , Stroh F. , Some L. , Siegmund P. , Sitnikov N. , Vernier J. P. , Volk C. M. , Voigt C. , von Hobe M. , Viciani S. , Yushkov V.
Published: April 2010

Abstract. A multi-platform field measurement campaign involving aircraft and balloons took place over West Africa between 26 July and 25 August 2006, in the frame of the concomitant AMMA Special Observing Period and SCOUT-O3 African tropical activities. Specifically aiming at sampling the upper troposphere and lower stratosphere, the high-altitude research aircraft M55 Geophysica was deployed in Ouagadougou (12.3° N, 1.7° W), Burkina Faso, in conjunction with the German D-20 Falcon, while a series of stratospheric balloon and sonde flights were conducted from Niamey (13.5° N, 2.0° E), Niger. The stratospheric aircraft and balloon flights intended to gather experimental evidence for a better understanding of large scale transport, assessing the effect of lightning on NOx production, and studying the impact of intense mesoscale convective systems on water, aerosol, dust and chemical species in the upper troposphere and lower stratosphere. The M55 Geophysica carried out five local and four transfer flights between southern Europe and the Sahel and back, while eight stratospheric balloons and twenty-nine sondes were flown from Niamey. These experiments allowed a characterization of the tropopause and lower stratosphere of the region. We provide here an overview of the campaign activities together with a description of the general meteorological situation during the flights and a summary of the observations accomplished.
Molecular distributions of dicarboxylic acids, ketocarboxylic acids and α-dicarbonyls in biomass burning aerosols: implications for photochemical production and degradation in smoke layers
Authors: Kundu S. , Kawamura K. , Andreae T. W. , Hoffer A. , Andreae M. O.
Published: April 2010

Abstract. Aerosols in the size class <2.5 μm (6 daytime and 9 nighttime samples) were collected at a pasture site in Rondônia, Brazil, during the intensive biomass burning period of 16–26 September 2002 as part of the Large-Scale Biosphere-Atmosphere Experiment in Amazonia – Smoke, Aerosols, Clouds, Rainfall and Climate (LBA-SMOCC). Homologous series of dicarboxylic acids (C2–C11) and related compounds (ketocarboxylic acids and dicarbonyls) were identified using gas chromatography and GC/mass spectrometry (GC/MS). Among the species detected, oxalic acid was found to be the most abundant, followed by succinic, malonic and glyoxylic acids. Average concentrations of total dicarboxylic acids, ketocarboxylic acids and α-dicarbonyls in the aerosol samples were 2180, 167 and 56 ng m−3, respectively. These are 2–8, 3–11 and 2–16 times higher, respectively, than those reported in urban aerosols, such as in 14 Chinese megacities. Higher ratios of dicarboxylic acids and related compounds to biomass burning tracers (levoglucosan and K+) were found in the daytime than in the nighttime, suggesting an importance of photochemical production. On the other hand, higher ratios of oxalic acid to other dicarboxylic acids and related compounds normalized to biomass burning tracers (levoglucosan and K+) in the daytime provide evidence for the possible degradation of dicarboxylic acids (≥C3) in this smoke-polluted environment. Assuming that these and related compounds are photochemically oxidized to oxalic acid in the daytime and given their linear relationship, they could account for, on average, 77% of the formation of oxalic acid. The remaining portion of oxalic acid may have been directly emitted from biomass burning as suggested by a good correlation with the biomass burning tracers (K+, CO and ECa) and organic carbon (OC). However, photochemical production from other precursors could not be excluded.
Chirality and origin of atmospheric humic-like substances
Authors: Salma I. , Mészáros T. , Maenhaut W. , Vass E. , Majer Zs.
Published: April 2010

Abstract. Aerosol water extracts and atmospheric humic-like substances (HULIS) obtained from PM2.5-fraction aerosol samples collected in a rural/continental background environment and in an urban environment in spring and summer, and at a tropical site that was heavily impacted by biomass burning were studied. Mean organic matter-to-organic carbon mass conversion factor and standard deviation of 2.04±0.06 were derived for HULIS from biomass burning. Mean atmospheric concentrations of HULIS for the rural and urban environments, and for the biomass burning during daylight periods and nights were 1.65, 2.2, 43, and 60 μg m