bluuebunny/crossref_metadata_2025 huggingface dataset:
In-situ comparison of the NOy instruments flown in MOZAIC and SPURT
Authors: Pätz H.-W. , Volz-Thomas A. , Hegglin M. I. , Brunner D. , Fischer H. , Schmidt U.
Published: April 2010

Abstract. Two aircraft instruments for the measurement of total odd nitrogen (NOy) were compared side by side aboard a Learjet A35 in April 2003 during a campaign of the AFO2000 project SPURT (Spurengastransport in der Tropopausenregion). The instruments albeit employing the same measurement principle (gold converter and chemiluminescence) had different inlet configurations. The ECO-Physics instrument operated by ETH-Zürich in SPURT had the gold converter mounted outside the aircraft, whereas the instrument operated by FZ-Jülich in the European project MOZAIC III (Measurements of ozone, water vapour, carbon monoxide and nitrogen oxides aboard Airbus A340 in-service aircraft) employed a Rosemount probe with 80 cm of FEP-tubing connecting the inlet to the gold converter. The NOy concentrations during the flight ranged between 0.3 and 3 ppb. The two data sets were compared in a blind fashion and each team followed its normal operating procedures. On average, the measurements agreed within 6%, i.e. within the combined uncertainty of the two instruments. This puts an upper limit on potential losses of HNO3 in the Rosemount inlet of the MOZAIC instrument. Larger transient deviations were observed during periods after calibrations and when the aircraft entered the stratosphere. The time lag of the MOZAIC instrument observed in these instances is in accordance with the time constant of the MOZAIC inlet line determined in the laboratory for HNO3.
A chemical probe technique for the determination of reactive halogen species in aqueous solution: Part 1 – bromide solutions
Authors: Matthew B. M. , Anastasio C.
Published: April 2010

Abstract. Reactive halogen species (X*=X●, ●X2−, X2 and HOX, where X=Br, Cl, or I) in seawater, sea-salt particles, and snowpacks play important roles in the chemistry of the marine boundary layer. Despite this, relatively little is known about the steady-state concentrations or kinetics of reactive halogens in these environmental samples. In part this is because there are few instruments or techniques that can be used to characterize aqueous reactive halogens. To better understand this chemistry, we have developed a chemical probe technique that can detect and quantify aqueous reactive bromine and chlorine species (Br*(aq) and Cl*(aq)). This technique is based on the reactions of short-lived X*(aq) species with allyl alcohol (CH2=CHCH2OH) to form stable 3-halo-1,2-propanediols that are analyzed by gas chromatography. Using this technique in conjunction with competition kinetics allows determination of the steady state concentrations of the aqueous reactive halogens and, in some cases, the rates of formation and lifetimes of X* in aqueous solutions. We report here the results of the method development for aqueous solutions containing only bromide (Br−).
Behavior of CCN to CN fraction during aging and mixing processes of atmospheric particles
Authors: Rojas S. , Gomes L. , Villani P.
Published: April 2010

Abstract. During Spring 2003, field experiments were conducted at the summit of Puy de Dôme (1465 m a.s.l.), in Central France, mainly in the free troposphere and during cloudy conditions. During this experiment, cloud condensation nuclei (CCN) concentrations were measured with a thermal gradient CCN counter at applied supersaturations that ranged between 0.2 and 2%. Aerosol size distributions were obtained with a TSI scanning mobility particle sizer (SMPS) consisting of a DMA and a CPC, and aerosol number (CN) concentrations were derived by integrating the SMPS size spectra between 0.015 and 0.3 µm. The isentropic back trajectories were computed for the altitude of the observation site using the Hybrid Single Particle Lagrangian Integrated Trajectory (HY-SPLIT) code from NOAA. For each air mass type, the aerosol bulk chemical composition used was that previously determined from cascade impactor samples by Sellegri et al. (2003). The methodological approach of this study was, firstly, to determine the relationships between CN and CCN concentrations for various air mass types arriving on the observation site. According to their origin, air masses arriving on the observation site are classified into 4 types: continental, clean marine, modified marine and polar. The CN concentrations appear to clearly depend on the type of air mass with the highest concentrations for the continental event and the lowest ones for the marine events. Moreover, a typical range can be attributed for the CCN/CN ratio to each air mass type. Then, the objective was to observe the hygroscopic behavior of aerosol particles upon heating of the sample in a thermo-desorber. Since the heated sample can be considered as representative of the original state of the aerosol, it appears that the evolution of CN to CCN is much more affected when the air mass is modified by aging and mixing processes with the contact of various atmospheric species all along the transport pathway. This result shows indirectly but clearly the presence of an active chemical layer containing more hygroscopic properties on the aerosol particle surface that can favour the particle growth. However, the role played by organic species is not clear and more work is needed to know if organic compounds may act to increase the CCN concentration.
Air-to-sea flux of soluble iron: is it driven more by HNO3 or SO2? – an examination in the light of dust aging
Authors: Yang H. , Gao Y.
Published: April 2010

Abstract. Aeolian dust provides the major micronutrient of soluble Fe to organisms in certain regions of the global ocean. In this study, we conduct numerical experiments using the MOZART-2 atmospheric chemistry transport model to simulate the global distribution of soluble Fe flux and Fe solubility. One of the mechanisms behind the hypothesis of acid mobilization of Fe in the atmosphere is that the coating of acidic gases changes dust from hydrophobic to hydrophilic, a prerequisite of Fe mobilization. We therefore include HNO3, SO2 and sulfate (SO42−) as dust transformation agents in the model. General agreement in Fe solubility within a factor of 2 is achieved between model and observations. The total flux of soluble Fe to the world ocean is estimated to be 731–924×109 g yr−1, and the average Fe solubility is 6.4–8.0%. Wet deposition contributes over 80% to total soluble Fe flux to most of the world oceans. Special attention is paid to the relative role of HNO3 versus SO2 and sulfate. We demonstrate that coating by HNO3 produces over 36% of soluble Fe fluxes compared to that by SO2 and sulfate combined in every major oceanic basin. Given present trends in the emissions of NOx and SO2, the relative contribution of HNO3 to Fe mobilization may get even larger in the future.
Multiwavelength and polarization lidar measurements of Asian dust layers over Tsukuba, Japan: a case study
Authors: Sakai T. , Nagai T. , Kobayashi T. , Yamazaki A. , Uchiyama A. , Mano Y.
Published: April 2010

Abstract. Elastic and polarization lidar was used to measure the vertical profiles of aerosol backscattering coefficients at wavelengths of 355, 532, 735, and 1064 nm, and the depolarization ratio at 532 nm in order to study the aerosol properties in the free troposphere over Tsukuba, Japan, in 2006. An elevated dust layer was observed at altitudes between 3 and 8.5 km on 1 April during the Asian dust period. The wavelength exponents of the aerosol backscattering coefficient (k) were –0.1 to 0.5, and the depolarization ratio (δp) was 25% for the dust layer, suggesting the predominance of supermicrometer-sized (coarse mode) nonspherical particles. An aerosol layer observed at altitudes between 1.5 and 5 km on 19 October during the less-dust period exhibited the values of k=1.0 to 1.6 and δp=1 to 13%, suggesting the predominance of submicrometer-sized (fine mode) particles. In those layers, the values of k and δp varied with height; they were also negatively correlated, suggesting that the proportion of the coarse nonspherical particles to total particles varied. The particle size distributions estimated from the observed values and the theoretical computation revealed number mode radii of 0.3 &mum; for the coarse mode and 0.1 &mum; for the fine mode, assuming bimodal distribution. These results were consistent with those obtained from the sky-radiometer measurements, although they revealed another mode in the larger radius. The column volume concentration derived from the lidar was 48% lower than that derived from the sky-radiometer on 1 April and 16% lower on 19 October. The optical thickness derived from the lidar was 12% lower than that obtained from the sky-radiometer on 1 April and 29% higher on 19 October. Further case study is necessary to validate the method for estimating aerosol properties based on the lidar measurement.
Evidence of tropospheric layering: interleaved stratospheric and planetary boundary layer intrusions
Authors: Brioude J. , Cammas J.-P. , Zbinden R. M. , Thouret V.
Published: April 2010

Abstract. We present a case study of interleaving in the free troposphere of 4 layers of non-tropospheric origin, with emphasis on their residence time in the troposphere. Two layers are stratospheric intrusions at 4.7 and 2.2 km altitude with residence times of about 2 and 6.5 days, respectively. The two other layers at 7 and 3 km altitude were extracted from the maritime planetary boundary layer by warm conveyor belts associated with two extratropical lows and have residence times of about 2 and 5.75 days, respectively. The event took place over Frankfurt (Germany) in February 2002 and was observed by a commercial airliner from the MOZAIC programme with measurements of ozone, carbon monoxide and water vapour. Origins and residence times in the troposphere of these layers are documented with a trajectory and particle dispersion model. The combination of forward and backward simulations of the Lagrangian model allows the period of time during which the residence time can be assessed to be longer, as shown by the capture of the stratospheric-origin signature of the lowest tropopause fold just about to be completely mixed above the planetary boundary layer. This case study is of interest for atmospheric chemistry because it emphasizes the importance of coherent airstreams that produce laminae in the free troposphere and that contribute to the average tropospheric ozone. The interleaving of these 4 layers also provides the conditions for a valuable case study for the validation of global chemistry transport models used to perform tropospheric ozone budgets.
Observing cirrus halos to constrain in-situ measurements of ice crystal size
Authors: Garrett T. J. , Kimball M. B. , Mace G. G. , Baumgardner D. G.
Published: April 2010

Abstract. In this study, characteristic optical sizes of ice crystals in synoptic cirrus are determined using airborne measurements of ice crystal size distributions, optical extinction and water content. The measurements are compared with coincident visual observations of ice cloud optical phenomena, in particular the 22° and 46° halos. In general, the scattering profiles derived from the in-situ cloud probe measurements are consistent with the observed halo characteristics. It is argued that this implies that the measured ice crystals were small, probably with characteristic optical radii between 10 and 20 μm. There is a current contention that in-situ measurements of high concentrations of small ice crystals reflect artifacts from the shattering of large ice crystals on instrument inlets. Significant shattering cannot be entirely excluded using this approximate technique, but it is not indicated. On the basis of the in-situ measurements, a parameterization is provided that relates the optical effective radius of ice crystals to the temperature in mid-latitude synoptic cirrus.
Properties of polar stratospheric clouds obtained by combined ACE-FTS and ACE-Imager extinction measurements
Authors: Zasetsky A. Y. , Gilbert K. , Galkina I. , McLeod S. , Sloan J. J.
Published: April 2010

Abstract. We report the compositions and size distributions of aerosol particles in typical polar stratospheric clouds (PSCs) observed between 24 January and 28 February 2005 in the Arctic stratosphere. The results are obtained by combining the extinction measurements made by the Atmospheric Chemistry Experiment (ACE) Fourier-Transform Spectrometer and the visible/near IR imagers on the SCISAT satellite. The extended wavenumber range provided by this combination (750 to 20 000 cm−1) enables the retrieval of aerosol particle sizes between 0.05 and 10 μm as well as providing extensive information about the compositions. Our results indicate that liquid ternary solutions with a high (>30 wt%) content of HNO3 were the most probable component of the clouds at the (60–70° N) latitudes accessible by ACE. The mean size of these ternary aerosol particles is in the range of 0.3 to 0.8 μm. Less abundant, although still frequent, were clouds composed of NAT particles having radii in the range of 1 μm and clouds of ice particles having mean radii in the 4–5 μm range. In some cases, these last two types were found in the same observation.
Primary marine aerosol emissions: size resolved eddy covariance measurements with estimates of the sea salt and organic carbon fractions
Authors: Nilsson E. D. , Mårtensson E. M. , Van Ekeren J. S. , de Leeuw G. , Moerman M. , O'Dowd C.
Published: April 2010

Abstract. Primary marine aerosol fluxes were measured using eddy covariance (EC), a condensation particle counter (CPC) and an optical particle counter (OPC) with a heated inlet. The later was used to discriminate between sea salt and total aerosol. Measurements were made from the 25 m tower at the research station Mace Head at the Irish west coast, May to September 2002. The aerosol fluxes were dominated by upward fluxes, sea spray from bubble bursting at the ocean surface. The sea salt aerosol number emissions increased two orders of magnitude with declining diameter from 1 to 0.1 μm where it peaked at values of 105 to 107 particles m−2s−1. The sea salt emissions increased at all sizes in the wind range 4 to 22 ms−1, in consistency with a power function of the wind speed. The sea salt emission data were compared to three recent sub micrometer sea salt source parameterisations. The best agreement was with Mårtensson et al. (2003), which appear to apply from 0.1 to 1.1 μm diameters in temperate water (12°C) as well as tropical water (25°C). The total aerosol emissions were independent of the wind speed below 10 ms−1, but increased with the wind above 10 ms−1. The aerosol volume emissions were larger for the total aerosol than for the sea salt at all wind speeds, while the sea salt number emissions approached the total number emissions at 15 ms−1. It is speculated that this is caused by organic carbon in the surface water that is depleted at high wind speeds. The data are consistent with an internal aerosol mixture of sea salt, organic carbon and water. Using the aerosol model by Ellison et al. (1999) (a mono-layer of organic carbon surrounding a water-sea-salt brine) we show that the total and sea salt aerosol emissions are consistent. This predict that the organic carbon fraction increase with decreasing diameter from a few % at 1 μm over 50% at about 0.5 μm to about 90% at 0.1 μm, in consistency with simultaneous chemical data by Cavalli et al. (2004). The combined models of Mårtensson et al. (2003) and Ellison et al. (1999) reproduce the observed total aerosol emissions and offer an approach to model the organic sea spray fraction.
Non-methane hydrocarbons source apportionment at different sites in Mexico City during 2002–2003
Authors: Vega E. , Sanchez G. , Molina L.
Published: April 2010

Abstract. The atmospheric concentrations of a variety of non-methane hydrocarbons (NMHC) collected at different sites, representing urban and rural environments within Mexico City Metropolitan Area (MCMA) during 1997, 2002 and 2003 field campaigns, were compared and used as an input for the Chemical Mass Balance (CMB) receptor model to determine the source contribution of NMHC to the atmosphere. A common feature at all the locations was the dominance of alkenes (59%), aromatics (16%) and olefins (9%) in the average NMHC burden. At the urban sites the interquartile range of NMHC concentrations showed stabilization over this period with a slight increase in the concentrations of propane and butanes in the southwest site of the MCMA in 2003 due to the increased use of liquefied petroleum gas (LPG). The receptor model CMB version 8.0 was used to apportion the NMHC sources at six locations within the MCMA, representing the heavily industrialized, commercial, residential and rural areas. For the 2003 field campaign, the contribution of vehicular emissions dominated the NMHC concentrations (19.7%±7.1% for gasoline vehicles and 35.4%±17.5% for diesel vehicles) followed by the emissions of marketing and handling of LPG (29.9%±8.0%). The NMHC concentrations showed a weekly cycle with the highest levels towards the end of the week and lowest at weekend and beginning of the week, suggesting that both emissions and accumulations process play a key role in building up NMHC levels. The toluene to benzene ratio was used to determine photochemical ageing of the air samples during the 2003 field campaign. The database was divided into periods with similar wind circulation pattern; the results suggest that ageing process within the MCMA is generally suppressed by the amount of fresh emissions.
Impact of upper-level jet-generated inertia-gravity waves on surface wind and precipitation
Authors: Zülicke C. , Peters D. H. W.
Published: April 2010

Abstract. A meteorological case study for the impact of inertia-gravity waves on surface meteorology is presented. The large-scale environment from 17 to 19 December 1999 was dominated by a poleward breaking Rossby wave transporting subtropical air over the North Atlantic Ocean upward and north-eastward. The synoptic situation was characterized with an upper tropospheric jet streak passing Northern Europe. The unbalanced jet spontaneously radiated inertia-gravity waves from its exit region. Near-inertial waves appeared with a horizontal wavelength of about 200 km and an apparent period of about 12 h. These waves transported energy downwards and interacted with large-scale convection. This configuration is simulated with the nonhydrostatic Fifth-Generation Mesoscale Model. Together with simplified runs without orography and moisture it is demonstrated that the imbalance of the jet (detected with the cross-stream ageostrophic wind) and the deep convection (quantified with the latent heat release) are forcing inertia-gravity waves. This interaction is especially pronounced when the upper tropospheric jet is located above a cold front at the surface and supports deep frontal convection. Weak indication was found for triggering post-frontal convection by inertia-gravity waves. The realism of model simulations was studied in an extended validation study for the Baltic Sea region. It included observations from radar (DWDPI, BALTRAD), satellite (GFZGPS), weather stations (DWDMI) and assimilated products (ELDAS, MESAN). The detected spatio-temporal patterns show wind pulsations and precipitation events at scales corresponding to those of inertia-gravity waves. In particular, the robust features of strong wind and enhanced precipitation near the front appeared with nearly the same amplitudes as in the model. In some datasets we found indication for periodic variations in the post-frontal region. These findings demonstrate the impact of upper tropospheric jet-generated inertia-gravity waves on the dynamics of the boundary layer. It also gives confidence to models, observations and assimilation products for covering such processes. In an application for the Gotland Basin in the Baltic Sea, the implications of such mesoscale events on air-sea interaction and energy and water budgets are discussed.
The effect of harmonized emissions on aerosol properties in global models – an AeroCom experiment
Authors: Textor C. , Schulz M. , Guibert S. , Kinne S. , Balkanski Y. , Bauer S. , Berntsen T. , Berglen T. , Boucher O. , Chin M. , Dentener F. , Diehl T. , Feichter J. , Fillmore D. , Ginoux P. , Gong S. , Grini A. , Hendricks J. , Horowitz L. , Huang P. , Isaksen I. S. A. , Iversen T. , Kloster S. , Koch D. , Kirkevåg A. , Kristjansson J. E. , Krol M. , Lauer A. , Lamarque J. F. , Liu X. , Montanaro V. , Myhre G. , Penner J. E. , Pitari G. , Reddy S. , Seland Ø. , Stier P. , Takemura T. , Tie X.
Published: April 2010

Abstract. The effects of unified aerosol sources on global aerosol fields simulated by different models are examined in this paper. We compare results from two AeroCom experiments, one with different (ExpA) and one with unified emissions, injection heights, and particle sizes at the source (ExpB). Surprisingly, harmonization of aerosol sources has only a small impact on the simulated diversity for aerosol burden, and consequently optical properties, as the results are largely controlled by model-specific transport, removal, chemistry (leading to the formation of secondary aerosols) and parameterizations of aerosol microphysics (e.g. the split between deposition pathways) and to a lesser extent on the spatial and temporal distributions of the (precursor) emissions. The burdens of black carbon and especially sea salt become more coherent in ExpB only, because the large ExpA diversity for these two species was caused by few outliers. The experiment also indicated that despite prescribing emission fluxes and size distributions, ambiguities in the implementation in individual models can lead to substantial differences. These results indicate the need for a better understanding of aerosol life cycles at process level (including spatial dispersal and interaction with meteorological parameters) in order to obtain more reliable results from global aerosol simulations. This is particularly important as such model results are used to assess the consequences of specific air pollution abatement strategies.
Cloud droplet activation: solubility revisited
Authors: Padró L. T. , Nenes A.
Published: April 2010

Abstract. Soluble compounds present in atmospheric aerosol facilitate their transformation into cloud droplets by depressing the equilibrium vapor pressure required for activation. Their impact depends on the amount of dissolved substance in the aerosol aqueous phase, which in turn is controlled by its solubility. This study explores the impact of particle curvature on solubility, expressed in terms of a Kelvin enhancement. The augmented solubility, termed "Curvature Enhanced Solubility" (CES), is then introduced into Köhler theory for assessment of its impact on CCN activity for several organic compounds with a wide range of aqueous solubility. The interfacial energy between solute and aqueous phase required for quantification of CES is determined from existing correlations based on bulk solubility, and concurrent measurements of contact angle and surface tension. A number of important findings arise from this study: i) CES can substantially increase solubility and impact CCN activity but only if the aerosol is initially wet, ii) CES can stabilize highly supersaturated solutions, and provide a mechanism for retention of an aerosol aqueous phase even at very low relative humidity (RH), and, iii) trace amounts of surfactant impurities can magnify the impact of CES.
Extended observations of volcanic SO2 and sulfate aerosol in the stratosphere
Authors: Carn S. A. , Krotkov N. A. , Yang K. , Hoff R. M. , Prata A. J. , Krueger A. J. , Loughlin S. C. , Levelt P. F.
Published: April 2010

Abstract. Sulfate aerosol produced after injection of sulfur dioxide (SO2) into the stratosphere by volcanic eruptions can trigger climate change. We present new satellite data from the Ozone Monitoring Instrument (OMI) and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) missions that reveal the composition, structure and longevity of a stratospheric SO2 cloud and derived sulfate layer following a modest eruption (0.2 Tg total SO2) of Soufriere Hills volcano, Montserrat on 20 May 2006. The SO2 cloud alone was tracked for over 3 weeks and a distance of over 20 000 km; unprecedented for an eruption of this size. Derived sulfate aerosol at an altitude of ~20 km had circled the globe by 22 June and remained visible in CALIPSO data until at least 6 July. These synergistic NASA A-Train observations permit a new appreciation of the potential effects of frequent, small-to-moderate volcanic eruptions on stratospheric composition and climate.
Inferring thermodynamic properties from CCN activation experiments: a) single-component and binary aerosols
Authors: Padró L. T. , Asa-Awuku A. , Morrison R. , Nenes A.
Published: April 2010

Abstract. This study presents a new method, Köhler Theory Analysis (KTA), to infer the molar volume and solubility of organic aerosol constituents. The method is based on measurements of surface tension, chemical composition, and CCN activity coupled with Köhler theory. KTA is evaluated by inferring the molar volume of six known organics (four dicarboxylic acids, one amino acid, and one sugar) in pure form and in mixtures with ammonium sulfate ((NH4)2SO4). Inferred molar volumes are to within 18% of their expected value for organic fractions between 90 and 100%. This suggests that KTA is a powerful and ideal method for determining the CCN characteristic of ambient water soluble organic carbon (WSOC) and provide physically-based constraints for aerosol-cloud interaction parameterizations.
Understanding the formation of biogenic secondary organic aerosol from α-pinene in smog chamber studies: role of organic peroxy radicals
Authors: Bonn B. , Korhonen H. , Petäjä T. , Boy M. , Kulmala M.
Published: April 2010

Abstract. This study focusses on the description of the nucleation process observed during the ozone reaction of the biogenic monoterpene α-pinene in smog chambers. Therefore, a detailed aerosol dynamics model (UHMA) was extended by a tropospheric chemistry module and a detailed description of the first steps of organic nucleation. We assume secondary ozonides to act as nucleation initiating molecules, which are subsequently activated by reactions with organic peroxy radicals (RO2). With this set-up the observed particle size distributions of an exemplary experiment in Valencia was reproduced, when only the long-lived organic compounds like carboxylic acids and carbonyl compounds are detected by the available aerosol size distribution instruments. Our results indicate that fragile or reactive species might get destroyed because of weak bond breakage during the size classification. This assumption would imply a serious detection problem in nucleation studies to be solved.
On the contribution of Aitken mode particles to cloud droplet populations at continental background areas – a parametric sensitivity study
Authors: Anttila T. , Kerminen V.-M.
Published: April 2010

Abstract. Aitken mode particles are potentially an important source of cloud droplets in continental background areas. In order to find out which physico-chemical properties of Aitken mode particles are most important regarding their cloud-nucleating ability, we applied a global sensitivity method to an adiabatic air parcel model simulating the number of cloud droplets formed on Aitken mode particles, CD2. The technique propagates uncertainties in the parameters describing the properties of Aitken mode to CD2. The results show that if the Aitken mode particles do not contain molecules that are able to reduce the particle surface tension more than 30% and/or decrease the mass accommodation coefficient of water, α, below 10−2, the chemical composition and modal properties may have roughly an equal importance at low updraft velocities characterized by maximum supersaturations <0.1%. For larger updraft velocities, however, the particle size distribution is clearly more important than the chemical composition. In general, CD2 exhibits largest sensitivity to the particle number concentration, followed by the particle size. Also the shape of the particle mode, characterized by the geometric standard deviation (GSD), can be as important as the mode mean size at low updraft velocities. Finally, the performed sensitivity analysis revealed also that the chemistry may dominate the total sensitivity of CD2 to the considered parameters if: 1) the value of α varies at least one order of magnitude more than what is expected for pure water surfaces (10−2–1), or 2) the particle surface tension varies more than roughly 30% under conditions close to reaching supersaturation.
Improved total atmospheric water vapour amount determination from near-infrared filter measurements with sun photometers
Authors: Mavromatakis F. , Gueymard C. A. , Franghiadakis Y.
Published: April 2010

Abstract. In this work we explore the effect of the contribution of the solar spectrum to the recorded signal in wavelengths outside the typical 940-nm filter's bandwidth. We use gaussian-shaped filters as well as actual filter transmission curves to study the implications imposed by the non-zero out-of-band contribution to the coefficients used to derive precipitable water from the measured water vapour band transmittance. The moderate-resolution SMARTS radiative transfer code is used to predict the incident spectrum outside the filter bandpass for different atmospheres, solar geometries and aerosol optical depths. The high-resolution LBLRTM radiative transfer code is used to calculate the water vapour transmittance in the 940 nm band. The absolute level of the out-of-band transmittance has been chosen to range from 10−6 to 10−4, and typical response curves of commercially available silicon photodiodes are included into the calculations. It is shown that if the out-of-band transmittance effect is neglected, as is generally the case, then the derived columnar water vapour is systematically underestimated by a few percents. The actual error depends on the specific out-of-band transmittance, optical air mass of observation and water vapour amount. We apply published parameterized transmittance functions to determine the filter coefficients. We also introduce an improved, three-parameter, fitting function that can describe the theoretical data accurately, with significantly less residual effects than with the existing functions. Further investigations will use experimental data from field campaigns to validate these findings.
Aerosol climatology: on the discrimination of aerosol types over four AERONET sites
Authors: Kaskaoutis D. G. , Kambezidis H. D. , Hatzianastassiou N. , Kosmopoulos P. G. , Badarinath K. V. S.
Published: April 2010

Abstract. Aerosols have a significant regional and global effect on climate, which is about equal in magnitude but opposite in sign to that of greenhouse gases. Nevertheless, the aerosol climatic effect changes strongly with space and time because of the large variability of aerosol physical and optical properties, which is due to the variety of their sources, which are natural, and anthropogenic, and their dependence on the prevailing meteorological and atmospheric conditions. Characterization of aerosol properties is of major importance for the assessment of their role for climate. In the present study, 3-year AErosol RObotic NETwork (AERONET) data from ground-based sunphotometer measurements are used to establish climatologies of aerosol optical depth (AOD) and Ångström exponent α in several key locations of the world, characteristic of different atmospheric environments. Using daily mean values of AOD at 500 nm (AOD500) and Ångström exponent at the pair of wavelengths 440 and 870 nm (α 440–870), a discrimination of the different aerosol types occurring in each location is achieved. For this discrimination, appropriate thresholds for AOD500 and α 440–870 are applied. The discrimination of aerosol types in each location is made on an annual and seasonal basis. It is shown that a single aerosol type in a given location can exist only under specific conditions (e.g. intense forest fires or dust outbreaks), while the presence of well-mixed aerosols is the accustomed situation. Background clean aerosol conditions (AOD500<0.06) are mostly found over remote oceanic surfaces occurring on average in ~56.7% of total cases, while this situation is quite rare over land (occurrence of 3.8–13.7%). Our analysis indicates that these percentages change significantly from season to season. The spectral dependence of AOD exhibits large differences between the examined locations, while it exhibits a strong annual cycle.
Observation of Polar Stratospheric Clouds down to the Mediterranean coast
Authors: Keckhut P. , David Ch. , Marchand M. , Bekki S. , Jumelet J. , Hauchecorne A.
Published: April 2010

Abstract. A Polar Stratospheric Cloud (PSC) was detected for the first time in January 2006 over Southern Europe after 25 years of systematic lidar observations. This cloud was observed while the polar vortex was highly distorted during the initial phase of a major stratospheric warming. Very cold stratospheric temperatures (<190 K) centred over the Northern-Western Europe were reported, extending down to the South of France where lidar observations were performed. CTM (Chemical Transport Model) investigations show that this event led to a significant direct ozone destruction (35 ppb/day), within and outside the vortex as chlorine activated air masses were moved to sunlight regions allowing ozone destruction. If such exceptional events of mid-latitudes PSCs were to become frequent in the future, they should not compromise the ozone recovery because their effect appears to be limited temporally and spatially. More importantly, these events might tend to be associated with the initial phase of a stratospheric warming that results into a weakening and warming of the polar vortex and hence into a reduced probability occurrence of PSC temperatures during the rest of the winter.
Heterogeneous uptake of the C1 to C4 organic acids on a swelling clay mineral
Authors: Hatch C. D. , Gough R. V. , Tolbert M. A.
Published: April 2010

Abstract. Mineral aerosol is of interest due to its physiochemical impacts on the Earth's atmosphere. However, adsorbed organics could influence the chemical and physical properties of atmospheric mineral particles and alter their impact on the biosphere and climate. In this work, the heterogeneous uptake of a series of small organic acids on the swelling clay, Na-montmorillonite, was studied at 212 K as a function of relative humidity (RH), organic acid pressure and clay mass. A high vacuum chamber equipped with a quadrupole mass spectrometer and a transmission Fourier transform infrared spectrometer was used to detect the gas and condensed phases, respectively. Sub-monolayer coverage of organic acid on montmorillonite was observed under dry conditions and relevant organic acid pressures. However, the organic acid content increased significantly with increasing humidity. Additionally, while the initial uptake efficiency was found to be independent of organic acid pressure, it increased linearly with increasing clay mass. Thus, the small masses studied allow access to the entire surface area of the clay sample with minimal effects due to surface saturation. Results from this study show that the initial uptake efficiency for n-butyric acid on the clay increases by an order of magnitude as the RH is raised from 0% to 45% RH at 212 K while the uptake of formic, acetic and propionic acids increase only slightly at higher humidities. Additionally, the presence of organic acids was found to slightly enhance the water content of the clay above 45% RH. Our results indicate that heterogeneous uptake of organic acids on swelling clay minerals provides an important heterogeneous sink for these species and may modify the cloud forming potential of the clay particles.
Mesospheric turbulence during PMWE-conducive conditions
Authors: Hall C. M. , Manson A. H. , Meek C. E. , Nozawa S.
Published: April 2010

Abstract. Strong radar returns at VHF known as Polar Mesospheric Winter Echoes (PMWE) seem to occur during periods of intense ionisation of the mesosphere. Apart from a mechanism to produce such ionisation, viz. solar proton precipitation, other prerequisites have been proposed, such as neutral air turbulence. Here, we employ a medium frequency radar to examine whether the atmospheric state is conducive to the appearance of PMWE; echo power signatures (isolated lower mesospheric echoes – "ILME") are indicators of the necessary ionisation at sufficient depth in the middle atmosphere, and also echo fading times give information on turbulence. We fail to find evidence for causal relationship between ILME and turbulence but suggest that on occasion turbulence may be enhanced related to proton precipitation. The results presented provide a basis for investigating whether turbulence is a prerequisite for PMWE.
Chemical composition of atmospheric aerosols between Moscow and Vladivostok
Authors: Kuokka S. , Teinilä K. , Saarnio K. , Aurela M. , Sillanpää M. , Hillamo R. , Kerminen V.-M. , Vartiainen E. , Kulmala M. , Skorokhod A. I. , Elansky N. F. , Belikov I. B.
Published: April 2010

Abstract. The TROICA-9 expedition (Trans-Siberian Observations Into the Chemistry of the Atmosphere) was carried out at the Trans-Siberian railway between Moscow and Vladivostok in October 2005. Measurements of aerosol physical and chemical properties were made from an observatory carriage connected to a passenger train. Black carbon (BC) concentrations in fine particles (PM2.5, aerodynamic diameter <2.5 μm) were measured with an aethalometer using a five-minute time resolution. Concentrations of inorganic ions and some organic compounds (Cl−, NO3−, SO42−, Na+, NH4+, K+, Ca2+, Mg2+, oxalate and methane sulphonate) were measured continuously by using an on-line system with a 15-min time resolution. In addition, particle volume size distributions were determined for particles in the diameter range 3–850 nm using a 10-min. time resolution. The continuous measurements were completed with 24-h. PM2.5 filter samples which were stored in a refrigerator and later analyzed in chemical laboratory. The analyses included mass concentrations of PM2.5, ions, monosaccharide anhydrides (levoglucosan, galactosan and mannosan) and trace elements (Al, As, Cd, Co, Cr, Cu, Fe, Mn, Ni, Pb, Sb, V and Zn). The mass concentrations of PM2.5 varied in the range of 4.3–34.8 μg m−3 with an average of 21.6 μg m−3. Fine particle mass consisted mainly of BC (average 27.6%), SO42− (13.0%), NH4+ (4.1%), and NO3− (1.4%). One of the major constituents was obviously also organic carbon which was not determined. The contribution of BC was high compared with other studies made in Europe and Asia. High concentrations of ions, BC and particle volume were observed between Moscow and roughly 4000 km east of it, as well as close to Vladivostok, primarily due to local anthropogenic sources. In the natural background area between 4000 and 7200 km distance from Moscow, observed concentrations were low, even though there were local particle sources, such as forest fires, that increased occasionally concentrations. The measurements indicated that during forest fire episodes, most of the aerosol mass consisted of organic particulate matter. Concentrations of biomass burning tracers levoglucosan, oxalate and potassium were elevated close to the forest fire areas observed by the MODIS satellite. The polluted air masses from Asia seem to have significant influences on the concentration levels of fine particles over south-eastern Russia.
Contributions of anthropogenic and natural sources of sulfur to SO2, H2SO4(g) and nanoparticle formation
Authors: Lucas D. D. , Akimoto H.
Published: April 2010

Abstract. Atmospheric nanoparticles (NPs) are important intermediates in the transition from gas-phase molecules to new aerosols that can activate into cloud droplets. Through increases in the emissions of sulfur-containing gases, human activities have likely increased the number of NPs produced in the atmosphere. To have significant impacts, however, sulfur pollution must be transported away from the surface, where NP formation is inefficient, to higher altitudes. To characterize this anthropogenic influence, tagged tracers are implemented in a global atmospheric transport model. The tagged tracers are used to track the contributions of sulfur from five sources (anthropogenic, oceanic, volcanic, aircraft, and stratospheric) to the gas-phase burdens of SO2 and H2SO4(g), and the rates of forming atmospheric NPs. Because NPs may be produced by a variety of mechanisms, three different aerosol nucleation schemes (binary, ternary and ion-induced) are used in the model calculations. Of the SO2 in the global troposphere, the tagged tracers indicate that about 69% originates from anthropogenic surface emissions, 20% from the oceans and 10% from de-gassing volcanoes. The same sources contribute about 56%, 24% and 19%, respectively, to the global tropospheric H2SO4(g) burden. The anthropogenic contribution for H2SO4(g) is reduced because anthropogenic SO2 produces H2SO4(g) less efficiently than oceanic and volcanic sulfur. Regardless of the underlying nucleation assumptions, the simulations show a pronounced influence of anthropogenic sulfur on atmospheric NP formation, particularly in the Northern Hemisphere. Utilizing the tagged H2SO4(g) contributions, anthropogenic sulfur is estimated to account for roughly 69% of the NP formation in the Northern Hemisphere, 31% in the Southern Hemisphere and 56% across the global troposphere. In the key region of the upper troposphere, anthropogenic and oceanic sulfur both make sizeable contributions to NP formation (54% and 37%, respectively). The tagged tracer contributions suggest that human activities have probably more than doubled the NP production rate in the atmosphere from preindustrial to modern times.
Contribution of carbonaceous aerosol to cloud condensation nuclei: processes and uncertainties evaluated with a global aerosol microphysics model
Authors: Pierce J. R. , Chen K. , Adams P. J.
Published: April 2010

Abstract. This paper explores the impacts of carbonaceous aerosol on cloud condensation nuclei (CCN) concentrations in a global climate model with size-resolved aerosol microphysics. Organic matter (OM) and elemental carbon (EC) from two emissions inventories were incorporated into a preexisting model with sulfate and sea-salt aerosol. The addition of carbonaceous aerosol increased CCN(0.2%) concentrations by 65–90% in the globally averaged surface layer depending on the carbonaceous emissions inventory used. Sensitivity studies were performed to determine the relative importance of the organic "solute effect", in which CCN concentrations increase because of the added soluble carbonaceous material, versus the "seeding effect", in which CCN concentrations increase because of increased particle number concentrations. In a sensitivity study where carbonaceous aerosol was assumed to be completely insoluble, concentrations of CCN(0.2%) still increased by 40–50% globally over the no carbonaceous simulation because primary carbonaceous emissions were able to become CCN via condensation of sulfuric acid. This shows that approximately half of the contribution of carbonaceous particles to CCN comes from the "seeding effect" and half from the "solute effect". The solute effect tends to dominate more in areas where there is less inorganic aerosol than organic aerosol and the seeding effect tends to dominate in areas where is more inorganic aerosol than organic aerosol. It was found that an accurate simulation of the number size distribution is necessary to predict the CCN concentration but assuming an average chemical composition will generally give a CCN concentration within a factor of 2. If a "typical" size distribution is assumed for each species when calculating CCN, such as is done in bulk aerosol models, the mean error relative to a simulation with size resolved microphysics is on the order of 35%. Predicted values of carbonaceous aerosol mass and aerosol number were compared to observations and the model showed average errors of a factor of 3 for carbonaceous mass and a factor of 4 for total aerosol number. These errors may be reduced by improving the emission size distributions of both primary sulfate and primary carbonaceous aerosol.
Transport and modeling of stratospheric inorganic chlorine
Authors: Waugh D. W. , Strahan S. E. , Newman P. A.
Published: April 2010

Abstract. Correctly modeling stratospheric inorganic chlorine (Cly) is crucial for modeling the past and future evolution of stratospheric ozone. However, comparisons of the chemistry climate models used in the latest international assessment of stratospheric ozone depletion have shown large differences in the modeled Cly, with these differences explaining differences in the simulated evolution of ozone over the next century. Here in, we examine the role of transport in determining the simulated Cly using three simulations from the same off-line chemical transport model that have the same lower tropospheric boundary conditions and the same chemical solver, but differing resolution and/or meteorological fields. These simulations show that transport plays a key role in determining the Cly distribution, and that Cly depends on both the time scales and pathways of transport. The time air spends in the stratosphere (e.g., the mean age) is an important transport factor determining stratospheric Cly, but the relationship between mean age and Cly is not simple. Lower stratospheric Cly depends on the fraction of air that has been in the upper stratosphere, and transport differences between models having the same mean age can result in differences in the fraction of organic chlorine converted into Cly. Differences in transport pathways result in differences in vertical profiles of CFCs, and comparisons of observed and modeled CFC profiles provides a stringent test of transport pathways in models.