bluuebunny/crossref_metadata_2025 huggingface dataset:
Characterization of the South Atlantic marine boundary layer aerosol using an Aerodyne Aerosol Mass Spectrometer
Authors: Zorn S. R. , Drewnick F. , Schott M. , Hoffmann T. , Borrmann S.
Published: April 2010

Abstract. Measurements of the submicron fraction of the atmospheric aerosol in the marine boundary layer were performed from January to March 2007 (Southern Hemisphere summer) onboard the French research vessel Marion Dufresne in the Southern Atlantic and Indian Ocean (20° S–60° S, 70° W–60° E). For chemical composition measurements an Aerodyne High-Resolution-Time-of-Flight AMS was used to measure mass concentrations and species-resolved size distributions of non-refractory aerosol components in the submicron range. Within the "standard" AMS compounds (ammonium, chloride, nitrate, sulfate, organics) "sulfate" is the dominating species in the marine boundary layer reaching concentrations between 50 ng m−3 and 3 μg m−3. Furthermore, what is seen as "sulfate" by the AMS seems to be mostly sulfuric acid. Another sulfur containing species that can ubiquitously be found in marine environments is methanesulfonic acid (MSA). Since MSA has not been directly measured before with an AMS, and is not part of the standard AMS analysis, laboratory experiments needed to be performed in order to be able to identify it within the AMS raw data and to extract mass concentrations for MSA from the field measurements. To identify characteristic air masses and their source regions backwards trajectories were used and averaged concentrations for AMS standard compounds were calculated for each air mass type. Sulfate mass size distributions were measured for these periods showing a distinct difference between oceanic air masses and those from African outflow. While the peak size in the mass distribution was roughly 250 nm in marine air masses it was shifted to 470 nm in African outflow air. Correlations between the mass concentrations of sulfate, organics and MSA were calculated which show a narrow correlation for MSA with sulfate/sulfuric acid coming from the ocean but not with continental sulfate.
Measurements of HNO3 and N2O5 using Ion drift – Chemical Ionization Mass Spectrometry during the MCMA – 2006 Campaign
Authors: Zheng J. , Zhang R. , Fortner E. C. , Molina L. , Aiken A. C. , Jimenez J. L. , Gäggeler K. , Dommen J. , Dusanter S. , Stevens P. S . , Tie X.
Published: April 2010

Abstract. An ion drift – chemical ionization mass spectrometry (ID-CIMS) was deployed in Mexico City between 5 and 31 March to measure HNO3 and N2O5 during the 2006 Mexico City Metropolitan Area (MCMA) field campaign. The observation site, T0, was located at the Instituto Mexicano del Petróleo at the center of the Mexico City Basin with major emissions of pollutants from both domestic and industrial sources. Diurnally, HNO3 was less than 200 parts per trillion (ppt) during the night and in the early morning, increased steadily from around 09:00 a.m. central standard time (CST), reached a peak value of 0.5 to 3 parts per billion (ppb) in the early afternoon, and declined sharply to less than half of the peak value near 05:00 p.m. CST. An inter-comparison between the ID-CIMS and an ion chromatograph/mass spectrometer (ICMS) showed a good correlation in the HNO3 measurements (R2=0.75). The HNO3 mixing ratio was found to anti-correlate with aerosol nitrate, suggesting that the gaseous HNO3 concentration was controlled by the gas-particle partitioning process. During most times of the MCMA 2006 field campaign, N2O5 was found to be under the detection limit (about 20 ppt for a 10 s integration time) of the ID-CIMS, because of high NO mixing ratio (>100 ppb) during the night. With one exception on 26 March 2006, about 40 ppt N2O5 was observed during the late afternoon and early evening hours under a cloudy condition, before NO built up at the surface site. The results revealed that during the 2006 MCMA field campaign HNO3 was primarily produced by the reaction of OH with NO2 and regulated by gas/particle partitioning, and HNO3 production from N2O5 hydrolysis during the nighttime was small because of high NO and low O3 concentrations near the surface.
Seasonal and inter-annual variations in Troposphere-to-Stratosphere Transport from the Tropical Tropopause Layer
Authors: Levine J. G. , Braesicke P. , Harris N. R. P. , Pyle J. A.
Published: April 2010

Abstract. In an earlier study of troposphere-to-stratosphere transport (TST) via the tropical tropopause layer (TTL), we found that the vast majority of air parcels undergoing TST from the base of the TTL enter the extratropical lowermost stratosphere quasi-horizontally and show little or no regional preference with regards to origin in the TTL or entry into the stratosphere. We have since repeated the trajectory calculations - originally limited to a single northern hemisphere winter period - in a variety of months and years to assess how robust our earlier findings are to change of timing. To first order, we find that the main conclusions hold, irrespective of the season, year and phase of the El Niño Southern Oscillation (ENSO). We also explore: the distribution of TST between the northern and southern hemispheres; the sensitivity of modelled TST to the definition of the tropopause; and the routes by which air parcels undergo transport exclusively to the stratospheric overworld. Subject to a dynamical definition of the tropopause, we identify a strong bias towards TST in the southern hemisphere, particularly during the northern hemisphere summer. The main difference on switching to the World Meteorological Organization's thermal tropopause definition is that much less TST is modelled in the subtropics and, relative to the dynamical definition, we calculate significantly less transport into the extratropical lowermost stratosphere (ELS) – an important region with regards to ozone chemistry. In contrast to the rather homogeneous nature of TST into the ELS, we find that transport to the overworld takes place from relatively well-defined regions of the TTL, predominantly above the West Pacific and Indonesia, except for an El Niño period in which most transport takes place from regions above the East Pacific and South America.
Quality assessment of O3 profiles measured by a state-of-the-art ground-based FTIR observing system
Authors: Schneider M. , Hase F. , Blumenstock T. , Redondas A. , Cuevas E.
Published: April 2010

Abstract. Ground-based FTIR measurements are an important component of the global atmospheric monitoring system. Their essential role in validating satellite measurements requires a precise documentation of their quality. Here we present an extensive quality documentation of ground-based FTIR O3 profiles. This is done in form of theoretical and empirical error estimations. The latter is achieved by intercomparison to ECC-sonde O3 profiles. The FTIR O3 amounts are obtained by applying the currently most advanced instrumentation and retrieval strategies. It consequently presents the current potential of this remote sensing technique.
Chemistry of the antarctic boundary layer and the interface with snow: an overview of the CHABLIS campaign
Authors: Jones A. E. , Wolff E. W. , Salmon R. A. , Bauguitte S. J.-B. , Roscoe H. K. , Anderson P. S. , Ames D. , Clemitshaw K. C. , Fleming Z. L. , Bloss W. J. , Heard D. E. , Lee J. D. , Read K. A. , Hamer P. , Shallcross D. E. , Jackson A. , Walker S. , Lewis A. C. , Mills G. P. , Plane J. M. C. , Saiz-Lopez A. , Sturges W. T. , Worton D. R.
Published: April 2010

Abstract. CHABLIS (Chemistry of the Antarctic Boundary Layer and the Interface with Snow) was a collaborative UK research project aimed at probing the detailed chemistry of the Antarctic boundary layer and the exchange of trace gases at the snow surface. The centre-piece to CHABLIS was the measurement campaign, conducted at the British Antarctic Survey station, Halley, in coastal Antarctica, from January 2004 through to February 2005. The campaign measurements covered an extremely wide range of species allowing investigations to be carried out within the broad context of boundary layer chemistry. Here we present an overview of the CHABLIS campaign. We provide details of the measurement location and introduce the Clean Air Sector Laboratory (CASLab) where the majority of the instruments were housed. We describe the meteorological conditions experienced during the campaign and present supporting chemical data, both of which provide a context within which to view the campaign results. Finally we provide a brief summary of highlights from the measurement campaign. Unexpectedly high halogen concentrations profoundly affect the chemistry of many species at Halley throughout the sunlit months, with a secondary role played by emissions from the snowpack. This overarching role for halogens in coastal Antarctic boundary layer chemistry was completely unanticipated, and the results have led to a step-change in our thinking and understanding.
Weekly patterns of aerosol in the United States
Authors: Murphy D. M. , Capps S. L. , Daniel J. S. , Frost G. J. , White W. H.
Published: April 2010

Abstract. Data from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network of aerosol samplers and NOAA monitoring sites are examined for weekly cycles. Fine particle elemental carbon, crustal elements, and coarse particle mass had pronounced (up to 20%) weekly cycles with minima on Sunday or Monday. Fine particle organic carbon and mass had smaller amplitude cycles, also with Sunday or Monday minima. There was no statistically significant weekly cycle in fine particle sulfate despite a 10 to 15% weekly cycle in power plant SO2 emissions. Although results for nitrate must be treated with caution, it showed a pronounced weekly cycle with an amplitude similar to elemental carbon. The only species found with a weekend maximum was Pb, probably from general aviation on weekends. Aerosol optical properties at NOAA monitoring sites were consistent with the IMPROVE chemical data, with significant weekly cycles in aerosol light absorption but not light scattering. These results support a large role of diesel emissions in elemental carbon aerosol over the entire United States and suggest that a large fraction of the airborne soil dust is anthropogenic. They also suggest that studies of weekly cycles in temperature, cloudiness, or precipitation should look for causes more in light-absorbing particles and dust rather than sulfate or total aerosol. There are also implications for personal exposure and epidemiological studies of aerosol health effects.
Oxidative capacity of the Mexico City atmosphere – Part 2: A ROx radical cycling perspective
Authors: Sheehy P. M. , Volkamer R. , Molina L. T. , Molina M. J.
Published: April 2010

Abstract. A box model using measurements from the Mexico City Metropolitan Area study in the spring of 2003 (MCMA-2003) is presented to study ROx (ROx=OH+HO2+RO2+RO) radical cycling in the troposphere. Model simulations were performed with the Master Chemical Mechanism (MCMv3.1) constrained with 10 min averaged measurements of major radical sources (i.e., HCHO, HONO, O3, CHOCHO, etc.), radical sink precursors (i.e., NO, NO2, SO2, CO, and 102 volatile organic compounds VOC), meteorological parameters (temperature, pressure, water vapor concentration, dilution), and photolysis frequencies. Modeled HOx concentrations compare favorably with measured concentrations for most of the day; however, the model under-predicts the concentrations of radicals in the early morning. This "missing reactivity" is highest during peak photochemical activity, and is least visible in a direct comparison of HOx radical concentrations. The true uncertainty due to "missing reactivity" is apparent in parameters like chain length, and ozone production (P(O3)). For example, the integral amount of ozone produced could be under-predicted by a factor of two. Our analysis highlights that apart from uncertainties in emissions, and meteorology, there is an additional major chemical uncertainty in current models.
Observations of convective clouds generated by solar heating of dark smoke plumes
Authors: Klüser L. , Rosenfeld D. , Macke A. , Holzer-Popp T.
Published: April 2010

Abstract. The SEVIRI instrument on the Meteosat Second Generation satellite with both fine spatial and temporal resolution allows to detect and follow the dynamics of fast developing meteorological events like spreading smoke plumes and the lifecycles of convective clouds. Smoke plumes have the ability to change the atmospheric heat content due to absorption and reduced reflection of solar radiation. By these means they can alter the temperature profile of the atmosphere and trigger convective clouds. A heavy smoke plume emerging from burning Lebanese oil tanks and spreading over adjacent deserts on 17 July 2006 has been observed as an example of such an effect. This study suggests a physical explanation of the observed convection along the edge of the smoke plume, namely the strong thermal contrast resulting from solar heating of the smoke layer.
The influence of chemical composition and mixing state of Los Angeles urban aerosol on CCN number and cloud properties
Authors: Cubison M. J. , Ervens B. , Feingold G. , Docherty K. S. , Ulbrich I. M. , Shields L. , Prather K. , Hering S. , Jimenez J. L.
Published: April 2010

Abstract. The relationship between cloud condensation nuclei (CCN) number and the physical and chemical properties of the atmospheric aerosol distribution is explored for a polluted urban data set from the Study of Organic Aerosols at Riverside I (SOAR-1) campaign conducted at Riverside, California, USA during summer 2005. The mixing state and, to a lesser degree, the average chemical composition are shown to be important parameters in determining the activation properties of those particles around the critical activation diameters for atmospherically-realistic supersaturation values. Closure between predictions and measurements of CCN number at several supersaturations is attempted by modeling a number of aerosol chemical composition and mixing state schemes of increasing complexity. It is shown that a realistic treatment of the state of mixing of the urban aerosol distribution is critical in order to eliminate model bias. Fresh emissions such as elemental carbon and small organic particles must be treated as non-activating and explicitly accounted for in the model scheme. The relative number concentration of these particles compared to inorganics and oxygenated organic compounds of limited hygroscopicity plays an important role in determining the CCN number. Furthermore, expanding the different composition/mixing state schemes to predictions of cloud droplet number concentration in a cloud parcel model highlights the dependence of cloud optical properties on the state of mixing and hygroscopic properties of the different aerosol modes, but shows that the relative differences between the different schemes are reduced compared to those from the CCN model.
Contribution of residential wood combustion to hourly winter aerosol in Northern Sweden determined by positive matrix factorization
Authors: Krecl P. , Hedberg Larsson E. , Ström J. , Johansson C.
Published: April 2010

Abstract. The combined effect of residential wood combustion (RWC) emissions with stable atmospheric conditions, which is a frequent occurrence in Northern Sweden during wintertime, can deteriorate the air quality even in small towns. To estimate the contribution of RWC to the total atmospheric aerosol loading, the positive matrix factorization (PMF) method was applied to hourly mean particle number size distributions measured in a residential area in Lycksele during winter 2005/2006. The sources were identified based on the particle number size distribution profiles of the PMF factors, the diurnal contributions patterns estimated by PMF for both weekends and weekdays, and correlation of the modeled particle number concentration per factor with measured aerosol mass concentrations (PM10, PM1, and light-absorbing carbon MLAC). Through these analyses, the factors were identified as local traffic (factor 1), local RWC (factor 2), and local RWC plus long-range transport (LRT) of aerosols (factor 3). In some occasions, it was difficult to detach the contributions of local RWC from background concentrations since their particle number size distributions partially overlapped and the model was not able to separate these two sources. As a consequence, we report the contribution of RWC as a range of values, being the minimum determined by factor 2 and the possible maximum as the contributions of both factors 2 and 3. A multiple linear regression (MLR) of observed PM10, PM1, total particle number, and MLAC concentrations is carried out to determine the source contribution to these aerosol variables. The results reveal RWC is an important source of atmospheric particles in the size range 25–606 nm (44–57%), PM10 (36–82%), PM1 (31–83%), and MLAC (40–76%) mass concentrations in the winter season. The contribution from RWC is especially large on weekends between 18:00 LT and midnight whereas local traffic emissions show similar contributions every day.
Parameterization of sea-salt optical properties and physics of the associated radiative forcing
Authors: Li J. , Ma X. , von Salzen K. , Dobbie S.
Published: April 2010

Abstract. The optical properties of sea-salt aerosol have been parameterized at solar and longwave wavelengths. The optical properties were parameterized in a simple functional form in terms of the ambient relative humidity based on Mie optical property calculations. The proposed parameterization is tested relative to Mie calculations and is found to be accurate to within a few percent. In the parameterization, the effects of the size distribution on the optical properties are accounted for in terms of effective radius of the sea-salt size distribution. This parameterization differs from previous works by being formulated directly with the wet sea-salt size distribution (and compared to AERONET results) and, to our knowledge, this is the first published sea-salt parameterization to provide a parameterization for both solar and longwave wavelengths. We have used this parameterization in a set of idealized 1-D radiative transfer calculations to investigate the sensitivity of various attributes of sea-salt forcing, such as dependence with sea-salt column loading, effective variance, solar angle, and surface albedo. From these sensitivity tests, it is found that sea-salt forcings for both solar and longwave spectra are linearly related to the sea-salt loading for realistic values of loadings. The radiative forcing results illustrate that the shortwave forcing is an order of magnitude greater than the longwave forcing results and opposite in sign, for various loadings. Studies of the sensitivity of forcing results to variations in effective variance show there to be minimal variation; therefore, only one value of effective variance is used in the parameterization. The dependence of sea-salt forcing with solar angle illustrates an interesting result that sea-salt can generate a positive top-of-the-atmosphere result (i.ewarming) when the solar zenith angle is relatively small 30° Finally, it is found that the surface albedo significantly affects the solar radiative forcing, with the forcing diminishing to zero as the surface albedo tends to unity. We anticipate this new sea-salt optical property parameterization will be useful for GCM models due to its simplicity, computational efficiency, and that its sensitivities have been explored and summarized in this work.
A single parameter representation of hygroscopic growth and cloud condensation nucleus activity – Part 2: Including solubility
Authors: Petters M. D. , Kreidenweis S. M.
Published: April 2010

Abstract. The ability of a particle to serve as a cloud condensation nucleus in the atmosphere is determined by its size, hygroscopicity and its solubility in water. Usually size and hygroscopicity alone are sufficient to predict CCN activity. Single parameter representations for hygroscopicity have been shown to model successfully complex, multicomponent particles types. Under the assumption of either complete solubility, or complete insolubility of a component, it is not necessary to explicitly include that components solubility into the single parameter framework. This is not the case if sparingly soluble particles are present. In this work we explicitly account for solubility by modifying the single parameter equations. We demonstrate that sensitivity to the actual value of solubility emerges only in the narrow regime of 1×10−1–5×10−3, where the solubility values are expressed as volume of solute per unit volume of water present in a saturated solution. Since only a few pure compounds fall inside this sparingly soluble envelope and those only make up a small fraction of the total organic fraction most organic species in the atmospheric aerosol can be adequately modeled assuming they are either infinitely soluble in water or completely insoluble .
Airborne dust distributions over the Tibetan Plateau and surrounding areas derived from the first year of CALIPSO lidar observations
Authors:   Zhaoyan Liu,   Dong Liu,   Jianping Huang, Vaughan M. ,   Itsushi Uno,   Nobuo Sugimoto,   Chieko Kittaka, Trepte C. ,   Zhien Wang, Hostetler C. , Winker D.
Published: April 2010

Abstract. Airborne dust is a major environmental hazard in Asia. Using an analysis of the first full year of CALIPSO lidar measurements, this paper derives unprecedented, altitude-resolved seasonal distributions of desert dust transported over the Tibetan Plateau (TP) and the surrounding areas. The CALIPSO lidar observations include numerous large dust plumes over the northern slope and eastern part of the TP, with the largest number of dust events occurring in the spring of 2007, and some layers being lofted to altitudes of 10 km and higher. Generation of the Tibetan airborne dusts appears to be largely associated with source regions to the north and on the eastern part of the plateau. Examination of the CALIPSO time history reveals an "airborne dust corridor" due to the eastward transport of dusts originating primarily in these source areas. This corridor extends from west to east and shows a seasonality largely modulated by the TP through its dynamical and thermal forcing on the atmospheric flows. On the southern side, desert dust particles originate predominately in North India and Pakistan. The dust transport occurs primarily in dry seasons around the TP western and southern slopes and dust particles become mixed with local polluted aerosols. No significant amount of dust appears to be transported over the Himalayas. Extensive forward trajectory simulations are also conducted to confirm the dust transport pattern from the nearby sources observed by the CALIPSO lidar.
Multiphase modeling of nitrate photochemistry in the quasi-liquid layer (QLL): implications for NOx release from the Arctic and coastal Antarctic snowpack
Authors: Boxe C. S. , Saiz-Lopez A.
Published: April 2010

Abstract. We utilize a multiphase model, CON-AIR (Condense Phase to Air Transfer Model), to show that the photochemistry of nitrate (NO3−) in and on ice and snow surfaces, specifically the quasi-liquid layer (QLL), can account for NOx volume fluxes, concentrations, and [NO]/[NO2](γ=[NO]/[NO2]) measured just above the Arctic and coastal Antarctic snowpack. Maximum gas phase NOx volume fluxes, concentrations and γ simulated for spring and summer range from 5.0×104 to 6.4×105 molecules cm−3 s−1, 5.7×108 to 4.8×109 molecules cm−3, and ~0.8 to 2.2, respectively, which are comparable to gas phase NOx volume fluxes, concentrations and γ measured in the field. The model incorporates the appropriate actinic solar spectrum, thereby properly weighting the different rates of photolysis of NO3− and NO2−. This is important since the immediate precursor for NO, for example, NO2−, absorbs at wavelengths longer than nitrate itself. Finally, one-dimensional model simulations indicate that both gas phase boundary layer NO and NO2 exhibit a negative concentration gradient as a function of height although [NO]/[NO2] are approximately constant. This gradient is primarily attributed to gas phase reactions of NOx with halogens oxides (i.e., as BrO and IO), HOx, and hydrocarbons, such as CH3O2.
Modelling of cirrus clouds – Part 1: Model description and validation
Authors: Spichtinger P. , Gierens K. M.
Published: April 2010

Abstract. A double–moment bulk microphysics scheme for modelling cirrus clouds including explicit impact of aerosols on different types of nucleation mechanism is described. Process rates are formulated in terms of generalised moments of the underlying a priori size distributions in order to allow simple switching between various distribution types. The scheme has been implemented into a simple box model and into the anelastic non-hydrostatic model EULAG. The new microphysics is validated against simulations with detailed microphysics for idealised process studies and for a well documented case of arctic cirrostratus. Additionally, the formation of ice crystals with realistic background aerosol concentration is modelled and the effect of ambient pressure on homogeneous nucleation is investigated in the box model. The arctic cirrostratus case study is also supplemented with sensitivity studies including different vertical velocities, temperature fluctuations and wind shear. The model stands all tests and is thus suitable for cloud–resolving simulations of cirrus clouds. Last but not least, some new results are shown, corroborating the importance of sedimentation and dynamics inside cirrus clouds for forming the structure of the cirrus.
A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients
Authors: Zuend A. , Marcolli C. , Luo B. P. , Peter Th.
Published: April 2010

Abstract. Tropospheric aerosols contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. Interactions between these substances in liquid mixtures lead to discrepancies from ideal thermodynamic behaviour. By means of activity coefficients, non-ideal behaviour can be taken into account. We present here a thermodynamic model named AIOMFAC (Aerosol Inorganic–Organic Mixtures Functional groups Activity Coefficients) that is able to calculate activity coefficients covering inorganic, organic, and organic–inorganic interactions in aqueous solutions over a wide concentration range. This model is based on the activity coefficient model LIFAC by Yan et al. (1999) that we modified and reparametrised to better describe atmospherically relevant conditions and mixture compositions. Focusing on atmospheric applications we considered H+, Li+, Na+, K+, NH4+, Mg2+, Ca2+, Cl−, Br−, NO3−, HSO4−, and SO42− as cations and anions and a wide range of alcohols/polyols composed of the functional groups CHn and OH as organic compounds. With AIOMFAC, the activities of the components within an aqueous electrolyte solution are well represented up to high ionic strength. Most notably, a semi-empirical middle-range parametrisation of direct organic–inorganic interactions in alcohol + water + salt solutions strongly improves the agreement between experimental and modelled activity coefficients. At room temperature, this novel thermodynamic model offers the possibility to compute equilibrium relative humidities, gas/particle partitioning and liquid–liquid phase separations with high accuracy. In further studies, other organic functional groups will be introduced. The model framework is not restricted to specific ions or organic compounds and is therefore also applicable for other research topics.
Basic characteristics of atmospheric particles, trace gases and meteorology in a relatively clean Southern African Savannah environment
Authors: Laakso L. , Laakso H. , Aalto P. P. , Keronen P. , Petäjä T. , Nieminen T. , Pohja T. , Siivola E. , Kulmala M. , Kgabi N. , Molefe M. , Mabaso D. , Phalatse D. , Pienaar K. , Kerminen V.-M.
Published: April 2010

Abstract. We have analyzed one year (July 2006–July 2007) of measurement data from a relatively clean background site located in dry savannah in South Africa. The annual-median trace gas concentrations were equal to 0.7 ppb for SO2, 1.4 ppb for NOx, 36 ppb for O3 and 105 ppb for CO. The corresponding PM1, PM2.5 and PM10 concentrations were 9.0, 10.5 and 18.8 μg m−3, and the annual median total particle number concentration in the size range 10–840 nm was 2340 cm−3. Gases and particles had a clear seasonal and diurnal variation, which was associated with field fires and biological activity together with local meteorology. Atmospheric new-particle formation was observed to take place in more than 90% of the analyzed days. The days with no new particle formation were cloudy or rainy days. The formation rate of 10 nm particles varied in the range of 0.1–28 cm−3 s−1 (median 1.9 cm−3 s−1) and nucleation mode particle growth rates were in the range 3–21 nm h−1 (median 8.5 nm h−1). Due to high formation and growth rates, observed new particle formation gives a significant contribute to the number of cloud condensation nuclei budget, having a potential to affect the regional climate forcing patterns.
Evaluation of a new lightning-produced NOx parameterization for cloud resolving models and its associated uncertainties
Authors: Barthe C. , Barth M. C.
Published: April 2010

Abstract. A new parameterization of the lightning-produced NOx has been developed for cloud-resolving models. This parameterization is based on three unique characteristics. First, the cells that can produce lightning are identified using a vertical velocity threshold. Second, the flash rate in each cell is estimated from the non-precipitation and precipitation ice mass flux product. Third, the source location is filamentary instead of volumetric as in previous parameterizations. This parameterization has been tested on the 10 July 1996 Stratospheric-Tropospheric Experiment: Radiation, Aerosols and Ozone (STERAO) storm. Comparisons of the simulated flash rate and NO mixing ratio with observations at different locations and stages of the storm show a good agreement. An individual flash produces on average 121±41 moles of NO (7.3±2.5×1025 molecules NO) for the simulated high cloud base, high shear storm. Sensitivity tests have been performed to study the impact of the flash rate, the cloud-to-ground flash ratio, the flash length, the spatial distribution of the NO molecules, and the production rate per flash on the NO concentration and distribution. Results show a strong impact from the flash rate, the spatial placement of the lightning-NOx source and the number of moles produced per flash.
Ship plume dispersion rates in convective boundary layers for chemistry models
Authors: Chosson F. , Paoli R. , Cuenot B.
Published: April 2010

Abstract. Detailed ship plume simulations in various convective boundary layer situations have been performed using a Lagrangian Dispersion Model driven by a Large Eddy Simulation Model. The simulations focus on early stage (1–2 h) of plume dispersion regime and take into account the effects of plume rise on dispersion. Results are presented in an attempt to provide to chemical modellers community a realistic description of the impact of characteristic dispersion on exhaust ship plume chemistry. Plume dispersion simulations are used to derive analytical dilution rate functions. Even though results exhibit striking effects of plume rise parameter on dispersion patterns, it is shown that initial buoyancy fluxes at ship stack have minor effect on plume dilution rate. After initial high dispersion regimes a simple characteristic dilution time scale can be used to parameterize the subgrid plume dilution effects in large scale chemistry models. The results show that this parameter is directly related to the typical turn-over time scale of the convective boundary layer.
Laboratory studies of H2SO4/H2O binary homogeneous nucleation from the SO2+OH reaction: evaluation of the experimental setup and preliminary results
Authors: Young L.-H. , Benson D. R. , Kameel F. R. , Lee S.-H.
Published: April 2010

Abstract. We have developed a new laboratory nucleation setup to study binary homogeneous nucleation (BHN) of sulphuric acid and water (H2SO4/H2O). Here we provide a detailed evaluation of this new experimental setup and also discuss our preliminary results by comparing with other laboratory studies. H2SO4 is produced from the SO2+OH →HSO3 reaction and OH radicals are produced from water vapor UV absorption. The residual H2SO4 concentrations ([H2SO4]) are measured at the end of the fast flow nucleation reactor with a chemical ionization mass spectrometer. The measured BHN rates (J) ranged from 0.02 and 550 cm−3 s−1 at the residual [H2SO4] from 108 to 1010 cm−3, a temperature of 288 K and relative humidity (RH) from 6 to 23%; J increased with increasing [H2SO4] and RH. J also showed a power dependence on [H2SO4] with the exponential power of 3 to 8. These results are consistent with other laboratory studies under similar [H2SO4] and RH, but different from atmospheric field observations which showed that particle number concentrations are often linearly dependent on [H2SO4]. Both particle sizes and number concentrations increased with increasing [H2SO4], RH, and nucleation time, consistent with the predictions from nucleation theories. Particle growth rates were estimated between 28 to 127 nm h−1, much higher than those seen from atmospheric field observations, because of the higher [H2SO4] used in our study. While these experimental results demonstrate a validation of our laboratory setup, there are also technical difficulties associated with nucleation studies, including wall loss and H2SO4 measurements.
A computationally-efficient secondary organic aerosol module for three-dimensional air quality models
Authors: Liu P. , Zhang Y.
Published: April 2010

Abstract. Accurately simulating secondary organic aerosols (SOA) in three-dimensional (3-D) air quality models is challenging due to the complexity of the physics and chemistry involved and the high computational demand required. A computationally-efficient yet accurate SOA module is necessary in 3-D applications for long-term simulations and real-time air quality forecasting. A coupled gas and aerosol box model (i.e., 0-D CMAQ-MADRID 2) is used to optimize relevant processes in order to develop such a SOA module. Solving the partitioning equations for condensable volatile organic compounds (VOCs) and calculating their activity coefficients in the multicomponent mixtures are identified to be the most computationally-expensive processes. The two processes can be speeded up by relaxing the error tolerance levels and reducing the maximum number of iterations of the numerical solver for the partitioning equations for organic species; turning on organic-inorganic interactions only when the water content associated with organic compounds is significant; and parameterizing the calculation of activity coefficients for organic mixtures in the hydrophilic module. The optimal speed-up method can reduce the total CPU cost by up to a factor of 29.7 with ±15% deviation from benchmark results. These speedup methods are applicable to other SOA modules that are based on partitioning theories.
Direct detection of OH formation in the reactions of HO2 with CH3 C(O)O2 and other substituted peroxy radicals
Authors: Dillon T. J. , Crowley J. N.
Published: April 2010

Abstract. This work details the first direct observation of OH as a product from (R1): HO2+CH3C(O)O2→(products), which has generally been considered an atmospheric radical termination process. The technique of pulsed laser photolysis radical generation, coupled to calibrated laser induced fluorescence detection was used to measure an OH product yield for (R1) of (α1=0.5±0.2). This study of (R1) included the measurement of a rate coefficient k1(298 K)=1.4±0.5)×10-11cm3 molecule−1 s−1, substantially reducing the uncertainties in modelling this important atmospheric reaction. OH was also detected as a product from the reactions of HO2 with three other carbonyl-containing peroxy radicals, albeit at smaller yield, e.g. (R2): HO2+CH3C(O)CH2O2→(products), α2≈0.15. By contrast, OH was not observed (α<0.06) as a major product from reactions where carbonyl functionality was absent, e.g. HO2+HOCH2CH2O2 (R8), and HO2+CH3CH(OH)CH2O2 (R9).
Ternary solution of sodium chloride, succinic acid and water – surface tension and its influence on cloud droplet activation
Authors: Vanhanen J. , Hyvärinen A.-P. , Anttila T. , Viisanen Y. , Lihavainen H.
Published: April 2010

Abstract. Surface tension of ternary solution of sodium chloride, succinic acid and water was measured as a function of both composition and temperature by using the capillary rise technique. Both sodium chloride and succinic acid are found in atmospheric aerosols, the former being main constituent of marine aerosol. Succinic acid was found to decrease the surface tension of water already at very low concentrations. Sodium chloride increased the surface tension linearly as a function of the concentration. Surface tensions of both binary solutions agreed well with the previous measurements. Succinic acid was found to lower the surface tension even if sodium chloride is present, indicating that succinic acid as a surface active compound tends to concentrate to the surface. An equation based on thermodynamical relations was fitted to the data. As a result, a surface tension parameterization of ternary solution was obtained over the whole concentration range. The parameterization can safely be used at temperatures from 10 to 30°C. These kinds of parameterizations are important for example in atmospheric nucleation models. To investigate the influence of surface tension on cloud droplet activation, the surface tension parameterization was included in an adiabatic air parcel model. Usually in cloud models the surface tension of pure water is used. Simulations were done for characteristic marine aerosol size distributions consisting of the considered ternary mixture. We found that by using the surface tension of pure water, the amount of activated particles is underestimated up to 8% if particles contain succinic acid and overestimated it up to 8% if particles contain only sodium chloride. The surface tension effect was found to increase with increasing updraft velocity.
Mode resolved density of atmospheric aerosol particles
Authors: Kannosto J. , Lemmetty M. , Virtanen A. , Mäkelä J. M. , Keskinen J. , Junninen H. , Hussein T. , Aalto P. , Kulmala M.
Published: April 2010

Abstract. In this study, we investigate the mode resolved density of ultrafine atmospheric particles measured in boreal forest environment. The method used here enables us to find the distinct density information for each mode in atmospheric fine particle population: the density values for nucleation, Aitken, and accumulation mode particles are presented. The experimental data was gained during 2 May 2005–19 May 2005 at the boreal forest measurement station "SMEAR II" in Hyytiälä, southern Finland. The density values for accumulation mode varied from 1.1 to 2 g/cm3 (average 1.5 g/cm3) and for Aitken mode from 0.4 to 2 g/cm3 (average 0.97 g/cm3. As an overall trend during the two weeks campaign, the density value of Aitken mode was seen to gradually increase. With the present method, the time dependent behaviour of the particle density can be investigated in time scale of 10 min. This allows us the follow the density evolution of the nucleation mode particles during the particle growth process following the nucleation burst. The density of nucleation mode particles decreased during the growth process. The density values for 15 nm particles were 1.2–1.5 g/cm3 and for grown 30 nm particles 0.5–1 g/cm3. These values are consistent with the present knowledge that the condensing species are semi volatile organics, emitted from the Boreal forest.
The role of atmospheric ions in aerosol nucleation – a review
Authors: Enghoff M. B. , Svensmark H.
Published: April 2010

Abstract. Atmospheric aerosols affect climate and yet the reason for many observed events of new aerosol formation is not understood. One of the theories put forward to explain these events is that the presence of ions can enhance the formation of aerosols. The theory is called Ion Induced Nucleation and in this paper the state of observations, theory and experiments within the field will be reviewed. While evidence for Ion Induced Nucleation is accumulating the exact mechanism is still not known and more research is required to understand and quantify the effect.
Technical Note: A new global database of trace gases and aerosols from multiple sources of high vertical resolution measurements
Authors: Hassler B. , Bodeker G. E. , Dameris M.
Published: April 2010

Abstract. A new database of trace gases and aerosols with global coverage, derived from high vertical resolution profile measurements, has been assembled as a collection of binary data files; hereafter referred to as the "Binary DataBase of Profiles" (BDBP). Version 1.0 of the BDBP, described here, includes measurements from different satellite- (HALOE, POAM II and III, SAGE I and II) and ground-based measurement systems (ozonesondes). In addition to the primary product of ozone, secondary measurements of other trace gases, aerosol extinction, and temperature are included. All data are subjected to very strict quality control and for every measurement a percentage error on the measurement is included. To facilitate analyses, each measurement is added to 3 different instances (3 different grids) of the database where measurements are indexed by: (1) geographic latitude, longitude, altitude (in 1 km steps) and time, (2) geographic latitude, longitude, pressure (at levels ~1 km apart) and time, (3) equivalent latitude, potential temperature (8 levels from 300 K to 650 K) and time. In contrast to existing zonal mean databases, by including a wider range of measurement sources (both satellite and ozonesondes), the BDBP is sufficiently dense to permit calculation of changes in ozone by latitude, longitude and altitude. In addition, by including other trace gases such as water vapour, this database can be used for comprehensive radiative transfer calculations. By providing the original measurements rather than derived monthly means, the BDBP is applicable to a wider range of applications than databases containing only monthly mean data. Monthly mean zonal mean ozone concentrations calculated from the BDBP are compared with the database of Randel and Wu, which has been used in many earlier analyses. As opposed to that database which is generated from regression model fits, the BDBP uses the original (quality controlled) measurements with no smoothing applied in any way and as a result displays higher natural variability.
Elemental content of PM2.5 aerosol particles collected in Göteborg during the Göte-2005 campaign in February 2005
Authors: Boman J. , Gatari M. J. , Janhäll S. , Shannigrahi A. S. , Wagner A.
Published: April 2010

Abstract. Göte–2005 was a measurement campaign in the city of Göteborg with the aim of studying the influence of the winter thermal inversions on urban air pollution. Elemental speciation of PM2.5 aerosol particles, collected on Teflon filters at three urban sites and one rural site in the Göteborg region, was a major part of the study. Trace element analysis was done by Energy Dispersive X-Ray Fluorescence (EDXRF) spectrometry and the concentrations of S, Cl, K, Ca, Ti, V, Mn, Fe, Ni, Cu, Zn, Br and Pb were determined. The elemental content of the particles in combination with information of local wind speed and direction and also backward trajectories were used to estimate the source areas of the pollutants. We can conclude that S, V, Ni, Br, and Pb have their main sources outside the Göteborg area, since we cannot see elevated concentrations of these elements during an inversion episode. Sea traffic and harbour activities were also identified, primarily by the S and V content of the particles. This study proves that the elemental analysis by EDXRF presents valuable information for tracing the origin of air masses arriving at a measurement site.
Measurement-based modeling of bromine chemistry at the Dead Sea boundary layer – Part 2: The influence of NO2 on bromine chemistry at mid-latitude areas
Authors: Tas E. , Peleg M. , Pedersen D. U. , Matveev V. , Biazar A. P. , Luria M.
Published: April 2010

Abstract. Understanding the interaction between anthropogenic air pollution and Reactive Halogen Species (RHS) activity has had only limited support of direct field measurements, due to the fact that past field measurements of RHS have been mainly performed in Polar Regions. The present paper investigates the interaction between NO2 and Reactive Bromine Species (RBS) activity by model simulations based on extensive field measurements performed in the Dead Sea area, as described in a companion paper (Tas et al., 2006). The Dead Sea is an excellent natural laboratory for this investigation since elevated concentrations of BrO (up to more than 150 pptv) are frequently observed, while the average levels of NO2 are around several ppb. The results of the present study show that under the chemical mechanisms that occur at the Dead Sea, higher levels of NO2 lead to higher daily average concentrations of BrOX, as a result of an increase in the rate of the heterogeneous decomposition of BrONO2 that in turn causes an increase in the rate of the "Bromine Explosion" mechanism. The present study has shown that the influence of NO2 on BrOX production clearly reflects an enhancement of RBS activity caused by anthropogenic activity. However, above a certain threshold level of NO2 (daily average mixing ratios of 0.2 ppbv during RBS activity), the daily average concentrations of BrOX decrease for a further increase in the NO2 concentrations.
Utilising shade to optimize UV exposure for vitamin D
Authors: Turnbull D. J. , Parisi A. V.
Published: April 2010

Abstract. Numerous studies have stated that humans need to utilise full sun radiation, at certain times of the day, to assist the body in synthesising the required levels of vitamin D3. The time needed to be spent in the full sun depends on a number of factors, for example, age, skin type, latitude, solar zenith angle. Current Australian guidelines suggest exposure to approximately 1/6 to 1/3 of a minimum erythemal dose (MED), depending on age, would be appropriate to provide adequate vitamin D3 levels. The aim of the study was to determine the exposure times to diffuse solar UV to receive exposures of 1/6 and 1/3 MED for a changing solar zenith angle in order to assess the possible role that diffuse UV (scattered radiation) may play in vitamin D3 effective UV exposures (UVD3). Diffuse and global erythemal UV measurements were conducted at five minute intervals over a twelve month period for a solar zenith angle range of 4° to 80° at a latitude of 27.6° S. For diffuse UV exposures of 1/6 and 1/3 MED, solar zenith angles smaller than 60° and 50° respectively can be utilised for exposure times of less than 10 min. Spectral measurements showed that, for a solar zenith angle of 40°, the UVA (315–400 nm) in the diffuse component of the solar UV is reduced by approximately 62% compared to the UVA in the global UV, whereas UVD3 wavelengths are only reduced by approximately 43%. At certain latitudes, diffuse UV under shade may play an important role in providing the human body with adequate levels of UVD3 (290–330 nm) radiation without experiencing the high levels of damaging UVA observed in full sun.