bluuebunny/crossref_metadata_2025 huggingface dataset:
Modeling of Saharan dust outbreaks over the Mediterranean by RegCM3: case studies
Authors: Santese M. , Perrone M. R. , Zakey A. S. , De Tomasi F. , Giorgi F.
Published: April 2010

Abstract. The regional climate model RegCM3 coupled with a radiatively active aerosol model with online feedback is used to investigate direct and semi-direct radiative aerosol effects over the Sahara and Europe in a test case of July 2003. The aerosol model includes dust particles in addition to sulfates, hydrophobic and hydrophilic black carbon and organic carbon. The role of the aerosol online feedback on the radiation budget and the direct radiative forcing (short-wave and long-wave) by dust particles are investigated by intercomparing results from three experiments: REF, including all interactive aerosol components, Exp1, not accounting for the aerosol radiative feedback, and Exp2 not accounting for desert dust particles. The comparison of results in the REF experiment with satellite observations, sun/sky radiometer measurements, and lidar profiles at selected Central Mediterranean sites reveals that the spatio-temporal evolution of the aerosol optical depth is reasonably well reproduced by the model during the entire month of July. Results for the dust outbreaks of 17 and 24 July, averaged over the simulation domain, show that the daily-mean SW direct radiative forcing by all particles is −24 Wm−2 and −3.4 Wm−2 on 17 July and −25 Wm−2 and −3.5 Wm−2 on 24 July at the surface and top of the atmosphere, respectively. This is partially offset by the LW direct radiative forcing, which is 7.6 Wm−2 and 1.9 Wm−2 on 17 July and 8.4 Wm−2 and 1.9 Wm−2 on 24 July at the surface and top of the atmosphere, respectively. Hence, the daily-mean SW forcing is offset by the LW forcing of ~30% at the surface and of ~50% at the ToA. It is also shown that atmospheric dynamics and hence dust production and advection processes are dependent on the simulation assumptions and may significantly change within few tens of kilometers. The comparison of REF and Exp1 shows that the aerosol online feedback on the radiation budget decreases the domain-average daily-mean value of the 2 m-temperature, aerosol column burden (CB), and short-wave (SW) atmospheric forcing by −0.52 °C, 14%, and 0.9%, respectively on 17 July and by −0.39 °C, 12% and 12%, respectively on 24 July. The comparison of REF and Exp2 reveals that on 17 July, radiatively-active dust particles decrease the daily-mean 2 m-temperature averaged over the whole simulation domain by 0.4% even if are responsible for 99.8% and 97% of the daily-mean aerosol column burden and SW atmospheric forcing, respectively.
Comment on "Reinterpreting aircraft measurement in anisotropic scaling turbulence" by Lovejoy et al. (2009)
Authors: Lindborg E. , Tung K. K. , Nastrom G. D. , Cho J. Y.  N. , Gage K. S.
Published: April 2010

Abstract. Recently, Lovejoy et al. (2009) argued that the steep ~k−3 atmospheric kinetic energy spectrum at synoptic scales (≥1000 km) observed by aircraft is a spurious artefact of aircraft following isobars instead of isoheights. Without taking into account the earth's rotation they hypothesise that the horizontal atmospheric energy spectrum should scale as k−5/3 at all scales. We point out that the approximate k−3-spectrum at synoptic scales has been observed by a number of non-aircraft means since the 1960s and that general circulation models and other current models have successfully produced this spectrum. We also argue that the vertical movements of the aircraft are far too small to cause any strong effect on the measured spectrum at synoptic scales.
Aerosol distribution around Svalbard during intense easterly winds
Authors: Dörnbrack A. , Stachlewska I. S. , Ritter C. , Neuber R.
Published: April 2010

Abstract. This paper reports on backscatter and depolarization measurements by an airborne lidar in the Arctic during the ASTAR 2004 campaign. A unique weather situation facilitated the observation of the aerosol concentration under strongly forced atmospheric conditions. The vigorous easterly winds distorted the flow past Svalbard in such a way that mesoscale features were visible in the remote-sensing observations: The formation of a well-mixed aerosol layer inside the Adventdalen and the subsequent thinning of the aerosol plume were observed over the Isfjorden. Additionally, mobilization of sea salt aerosols due to a coastal low-level jet at the northern tip of Svalbard resulted in a sloped boundary layer toward north. Mesoscale numerical modelling was applied to identify the sources of the aerosol particles and to explain the observed patterns.
Smoke injection heights from fires in North America: analysis of 5 years of satellite observations
Authors: Val Martin M. , Logan J. A. , Kahn R. A. , Leung F.-Y. , Nelson D. L. , Diner D. J.
Published: April 2010

Abstract. We analyze an extensive record of aerosol smoke plume heights derived from observations over North America for the fire seasons of 2002 and 2004–2007 made by the Multi-angle Imaging SpectroRadiometer (MISR) instrument on board the NASA Earth Observing System Terra satellite. We characterize the magnitude and variability of smoke plume heights for various biomes, and assess the contribution of local atmospheric and fire conditions to this variability. Plume heights are highly variable, ranging from a few hundred meters up to 5000 m above the terrain at the Terra overpass time (11:00–14:00 local time). The largest plumes are found over the boreal region (median values of ~850 m height, 24 km length and 940 m thickness), whereas the smallest plumes are found over cropland and grassland fires in the contiguous US (median values of ~530 m height, 12 km length and 550–640 m thickness). The analysis of plume heights in combination with assimilated meteorological observations from the NASA Goddard Earth Observing System indicates that a significant fraction (4–12%) of plumes from fires are injected above the boundary layer (BL), consistent with earlier results for Alaska and the Yukon Territories during summer 2004. Most of the plumes located above the BL (>83%) are trapped within stable atmospheric layers. We find a correlation between plume height and the MODerate resolution Imaging Spectroradiometer (MODIS) fire radiative power (FRP) thermal anomalies associated with each plume. Smoke plumes located in the free troposphere (FT) exhibit larger FRP values (1620–1640 MW) than those remaining within the BL (174–465 MW). Plumes located in the FT without a stable layer reach higher altitudes and are more spread-out vertically than those associated with distinct stable layers (2490 m height and 2790 m thickness versus 1880 m height and 1800 m thickness). The MISR plume climatology exhibits a well-defined seasonal cycle of plume heights in boreal and temperate biomes, with greater heights during June–July. MODIS FRP measurements indicate that larger summertime heights are the result of higher fire intensity, likely due to more severe fire weather during these months. This work demonstrates the significant effect of fire intensity and atmospheric structure on the ultimate rise of fire emissions, and underlines the importance of considering such physical processes in modeling smoke dispersion.
27-day variation in cloud amount in the Western Pacific warm pool region and relationship to the solar cycle
Authors: Takahashi Y. , Okazaki Y. , Sato M. , Miyahara H. , Sakanoi K. , Hong P. K. , Hoshino N.
Published: April 2010

Abstract. Although linkages between solar activity and the earth's climate have been suggested and the 11-year cycle in solar activity evident in sunspot numbers is the most examined example of periodicity in previous studies, no quantitative evidence indicating a relationship for tropospheric phenomena has been found for a short period. Based on FFT analysis for OLR (Outgoing Longwave Radiation) compared with the F10.7 index, we clearly demonstrate a 27-day variation in the cloud amount in the region of the Western Pacific warm pool, which is only seen in the maximum years of 11-year solar activity. The average spectrum in such years also shows an enhancement in the range of the MJO (Madden-Julian Oscillation) period. Although there exist some explanations for possible mechanisms, the exact cause is unknown. Therefore, the proposed connection between 27-day cloud variation and solar cycle in the WPWP region is still a hypothesis and various kinds of varification based on other meteorological and solar parameters are strongly required.
Emissions and ambient distributions of Biogenic Volatile Organic Compounds (BVOC) in a ponderosa pine ecosystem: interpretation of PTR-MS mass spectra
Authors: Kim S. , Karl T. , Guenther A. , Tyndall G. , Orlando J. , Harley P. , Rasmussen R. , Apel E.
Published: April 2010

Abstract. Two proton-transfer-reaction mass spectrometry systems were deployed at the Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics and Nitrogen-Southern Rocky Mountain 2008 field campaign (BEACHON-SRM08; July to September, 2008) at the Manitou Forest Observatory in a ponderosa pine woodland near Woodland Park, Colorado USA. The two PTR-MS systems simultaneously measured BVOC emissions and ambient distributions of their oxidation products. Here, we present mass spectral analysis in a wide range of masses (m/z 40+ to 210+) to assess our understanding of BVOC emissions and their photochemical processing inside of the forest canopy. The biogenic terpenoids, 2-methyl-3-butene-2-ol (MBO, 50.2%) and several monoterpenes (MT, 33.5%) were identified as the dominant BVOC emissions from a transmission corrected mass spectrum (PTR-MS), averaged over the daytime (11 a.m. to 3 p.m., local time) of three days. To assess contributions of oxidation products of local BVOC, we calculate an oxidation product spectrum with the OH- and ozone-initiated oxidation product distribution mass spectra of two major BVOC emissions at the ecosystem (MBO and β-pinene) that were observed from laboratory oxidation experiments. The majority (~76%) of the total signal in the transmission corrected PTR-MS spectra could be explained by identified compounds. The remainder are attributed to oxidation products of BVOC emitted from nearby ecosystems and transported to the site, and oxidation products of unidentified BVOC emitted from the ponderosa pine ecosystem.
Tracing the fate of atmospheric nitrate deposited onto a forest ecosystem in Eastern Asia using Δ17O
Authors: Tsunogai U. , Komatsu D. D. , Daita S. , Kazemi G. A. , Nakagawa F. , Noguchi I. , Zhang J.
Published: April 2010

Abstract. The stable isotopic compositions of nitrate in precipitation (wet deposition) and groundwater (spring, lake, and stream water) were determined for the island of Rishiri, Japan, so as to use the 17O anomalies (Δ17O) to trace the fate of atmospheric nitrate that had deposited onto the island ecosystem, which is a representative background forest ecosystem for eastern Asia. The deposited nitrate had large 17O anomalies with Δ17O values ranging from +20.8‰ to +34.5‰ (n = 32) with +26.2‰ being the annual average. The maximum Δ17O value of +34.5‰, obtained for precipitation on the 23rd to 24th of February 2007, was an extraordinarily large value among values for all samples of precipitation in Rishiri. Most nitrate in the sample might have been produced via NO3 radical in a highly polluted air mass that had been supplied from megacities on the eastern coast of the Asian continent. On the other hand, nitrate in groundwater had small Δ17O values ranging from +0.9‰ to 3.2‰ (n = 19), which corresponds to an mixing ratio of atmospheric nitrate to total nitrate of (7.4±2.6)%. Comparing the inflow and outflow of atmospheric nitrate in groundwater within the island, we estimated that the direct drainage accounts for (8.8±4.6)% of atmospheric nitrate that has deposited on the island and that the residual portion has undergone biological processing before being exported from the forest ecosystem.
Estimating mercury emission outflow from East Asia using CMAQ-Hg
Authors: Lin C.-J. , Pan L. , Streets D. G. , Shetty S. K. , Jang C. , Feng X. , Chu H.-W. , Ho T. C.
Published: April 2010

Abstract. East Asia contributes to nearly 50% of the global anthropogenic mercury emissions into the atmosphere. Recently, there have been concerns about the long-range transport of mercury from East Asia, which may lead to enhanced dry and wet depositions in other regions. In this study, we performed four monthly simulations (January, April, July and October in 2005) using CMAQ-Hg v4.6 for a number of emission inventory scenarios in an East Asian model domain. Coupled with mass balance analyses, the chemical transport of mercury in East Asia and the resulted mercury emission outflow were investigated. The total annual mercury deposition in the region was estimated to be 821 Mg, with 396 Mg contributed by wet deposition and 425 Mg by dry deposition. Anthropogenic emissions were responsible for most of the estimated deposition (75%). The deposition caused by emissions from natural sources was less important (25%). Regional mercury transport budgets showed strong seasonal variability, with a net removal of RGM (7–15 Mg month−1) and PHg (13–21 Mg month−1) in the domain, and a net export of GEM (60–130 Mg month−1) from the domain. The outflow caused by East Asian emissions (anthropogenic plus natural) was estimated to be in the range of 1369–1671 Mg yr−1, of which 50–60% was caused by emissions from natural sources. The emission outflow represented about 75% of the total mercury emissions in the region, and would contribute to 20–30% of mercury deposition in remote receptors.
Simultaneous factor analysis of organic particle and gas mass spectra: AMS and PTR-MS measurements at an urban site
Authors: Slowik J. G. , Vlasenko A. , McGuire M. , Evans G. J. , Abbatt J. P. D.
Published: April 2010

Abstract. During the winter component of the SPORT (Seasonal Particle Observations in the Region of Toronto) field campaign, particulate non-refractory chemical composition and concentration of selected volatile organic compounds (VOCs) were measured by an Aerodyne time-of-flight aerosol mass spectrometer (AMS) and a proton transfer reaction-mass spectrometer (PTR-MS), respectively. Sampling was performed in downtown Toronto ~15 m from a major road. The mass spectra from the AMS and PTR-MS were combined into a unified dataset, which was analysed using positive matrix factorization (PMF). The two instruments were given balanced weight in the PMF analysis by the application of a scaling factor to the uncertainties of each instrument. A residual based metric, Δesc, was used to evaluate the instrument relative weight within each solution. The PMF analysis yielded a 6-factor solution that included factors characteristic of regional transport, local traffic emissions, charbroiling and oxidative processing. The unified dataset provides information on emission sources (particle and VOC) and atmospheric processing that cannot be obtained from the datasets of the individual instruments: (1) apportionment of oxygenated VOCs to either direct emission sources or secondary reaction products; (2) improved correlation of oxygenated aerosol factors with photochemical age; and (3) increased detail regarding the composition of oxygenated organic aerosol factors. This analysis represents the first application of PMF to a unified AMS/PTR-MS dataset.
Numerical simulations of contrail-to-cirrus transition – Part 1: An extensive parametric study
Authors: Unterstrasser S. , Gierens K.
Published: April 2010

Abstract. Simulations of contrail-to-cirrus transition over up to 6 h were performed using a LES-model. The sensitivity of microphysical, optical and geometric contrail properties to relative humidity RHi, temperature T and vertical wind shear s was investigated in an extensive parametric study. The dominant parameter for contrail evolution is relative humidity. Substantial spreading is only visible for RHi≳120%. Vertical wind shear has a smaller effect on optical properties than human observers might expect from the visual impression. Our model shows that after a few hours the water vapour removed by falling ice crystals from the contrail layer can be several times higher than the ice mass that is actually present in the contrail at any instance.
Numerical simulations of contrail-to-cirrus transition – Part 2: Impact of initial ice crystal number, radiation, stratification, secondary nucleation and layer depth
Authors: Unterstrasser S. , Gierens K.
Published: April 2010

Abstract. Simulations of contrail-to-cirrus transition were performed with an LES model. In Part 1 the impact of relative humidity, temperature and vertical wind shear was explored in a detailed parametric study. Here, we study atmospheric parameters like stratification and depth of the supersaturated layer and processes which may affect the contrail evolution. We consider contrails in various radiation scenarios herein defined by the season, time of day and the presence of lower-level cloudiness which controls the radiance incident on the contrail layer. Under suitable conditions, controlled by the radiation scenario and stratification, radiative heating lifts the contrail-cirrus and prolongs its lifetime. The potential of contrail-driven secondary nucleation is investigated. We consider homogeneous nucleation and heterogeneous nucleation of preactivated soot cores released from sublimated contrail ice crystals. In our model the contrail dynamics triggered by radiative heating does not suffice to force homogeneous freezing of ambient liquid aerosol particles. Furthermore, our model results suggest that heterogeneous nucleation of preactivated soot cores is unimportant. Contrail evolution is not controlled by the depth of the supersaturated layer as long as it exceeds roughly 500 m. Deep fallstreaks however need thicker layers. A variation of the initial ice crystal number is effective during the whole evolution of a contrail. A cut of the soot particle emission by two orders of magnitude can reduce the contrail timescale by one hour and the optical thickness by a factor of 5. Hence future engines with lower soot particle emissions could potentially lead to a reduction of the climate impact of aviation.
Potential climatic impacts and reliability of very large-scale wind farms
Authors: Wang C. , Prinn R. G.
Published: April 2010

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

Abstract. The composition of residual particles from evaporated cirrus ice crystals near the tropical tropopause as well as unfrozen aerosols were measured with a single particle mass spectrometer. Subvisible cirrus residuals were predominantly composed of internal mixtures of neutralized sulfate with organic material and were chemically indistinguishable from unfrozen sulfate-organic aerosols. Ice residuals were also similar in size to unfrozen aerosol. Heterogeneous ice nuclei such as mineral dust were not enhanced in these subvisible cirrus residuals. Biomass burning particles were depleted in the residuals. Cloud probe measurements showing low cirrus ice crystal number concentrations were inconsistent with conventional homogeneous freezing. Recent laboratory studies provide heterogeneous nucleation scenarios that may explain tropopause level subvisible cirrus formation.
Evaluation of aerosol distributions in the GISS-TOMAS global aerosol microphysics model with remote sensing observations
Authors: Lee Y. H. , Adams P. J.
Published: April 2010

Abstract. The Aerosol Optical Depth (AOD) and Angstrom Coefficient (AC) predictions in the GISS-TOMAS model of global aerosol microphysics are evaluated against remote sensing data from MODIS, MISR, and AERONET. The model AOD agrees well (within a factor of two) over polluted continental (or high sulfate), dusty, and moderate sea-salt regions but less well over the equatorial, high sea-salt, and biomass burning regions. Underprediction of sea-salt in the equatorial region is likely due to GCM meteorology (low wind speeds and high precipitation). For the Southern Ocean, overprediction of AOD is very likely due to high sea-salt emissions and perhaps aerosol water uptake in the model. However, uncertainties in cloud screening at high latitudes make it difficult to evaluate the model AOD there with the satellite-based AOD. AOD in biomass burning regions is underpredicted, a tendency found in other global models but more severely here. Using measurements from the LBA-SMOCC 2002 campaign, the surface-level OC concentration in the model are found to be underpredicted severely during the dry season while much less severely for EC concentration, suggesting the low AOD in the model is due to underpredictions in OM mass. The potential for errors in emissions and wet deposition to contribute to this bias is discussed.
Organic nitrogen in PM2.5 aerosol at a forest site in the Southeast US
Authors: Lin M. , Walker J. , Geron C. , Khlystov A.
Published: April 2010

Abstract. There is growing evidence that organo-nitrogen compounds may constitute a significant fraction of the aerosol nitrogen (N) budget. However, very little is known about the abundance and origin of this aerosol fraction. In this study, the concentration of organic nitrogen (ON) and major inorganic ions in PM2.5 aerosol were measured at the Duke Forest Research Facility near Chapel Hill, NC, during January and June of 2007. A novel on-line instrument was used, which is based on the Steam Jet Aerosol Collector (SJAC) coupled to an on-line total carbon/total nitrogen analyzer and two on-line ion chromatographs. The concentration of ON was determined by tracking the difference in concentrations of total nitrogen and of inorganic nitrogen (determined as the sum of N-ammonium and N-nitrate). The time resolution of the instrument was 30 min with a detection limit for major aerosol components of ~0.1 μg m−3. Nitrogen in organic compounds contributed ~33% on average to the total nitrogen concentration in PM2.5, illustrating the importance of this aerosol component. Absolute concentrations of ON, however, were relatively low (<1.0 μg m−3) with an average of 0.16 μg m−3. The absolute and relative contribution of ON to the total aerosol nitrogen budget was practically the same in January and June. In January, the concentration of ON tended to be higher during the night and early morning, while in June it tended to be higher during the late afternoon and evening. Back-trajectories and correlation with wind direction indicate that higher concentrations of ON occur in air masses originating over the continental US, while marine air masses are characterized by lower ON concentrations. The data presented in this study suggests that ON has a variety of sources, which are very difficult to quantify without information on chemical composition of this important aerosol fraction.
Observations of OM/OC and specific attenuation coefficients (SAC) in ambient fine PM at a rural site in central Ontario, Canada
Authors: Chan T. W. , Huang L. , Leaitch W. R. , Sharma S. , Brook J. R. , Slowik J. G. , Abbatt J. P. D. , Brickell P. C. , Liggio J. , Li S.-M. , Moosmüller H.
Published: April 2010

Abstract. Ambient particulate matter (PM) samples were collected on quartz filters at a rural site in central Ontario during an intensive study in 2007. The concentrations of organic carbon (OC), pyrolysis organic carbon (POC), and elemental carbon (EC) were determined by thermal analysis. The concentrations are compared to the organic aerosol mass concentration (OM) measured with an Aerodyne C-ToF Aerosol Mass Spectrometer (AMS) and to the particle absorption coefficient (basp) obtained from a Radiance Research Particle Soot Absorption Photometer (PSAP). The total organic mass to organic carbon ratios (OM/OC) and specific attenuation coefficients (SAC=basp/EC) are derived. Proportionality of the POC mass with the oxygen mass in the aerosols estimated from the AMS offers a potential means to estimate OM/OC from thermal measurements only. The mean SAC for the study is 3.8±0.3 m2 g−1. It is found that the SAC is independent of or decrease with increasing particle mass loading, depending on whether or not the data are separated between aerosols dominated by more recent anthropogenic input and aerosols dominated by longer residence time or biogenic components. There is no evidence to support an enhancement of light absorption by the condensation of secondary material to particles, suggesting that present model simulations built on such an assumption may overestimate atmospheric warming by BC.
Iodine monoxide in the Antarctic snowpack
Authors: Frieß U. , Deutschmann T. , Gilfedder B. S. , Weller R. , Platt U.
Published: April 2010

Abstract. Recent ground-based and space borne observations suggest the presence of significant amounts of iodine monoxide in the boundary layer of Antarctica, which are expected to have an impact on the ozone budget and might contribute to the formation of new airborne particles. So far, the source of these iodine radicals has been unknown. This paper presents long-term measurements of iodine monoxide at the German Antarctic research station Neumayer, which indicate that high IO concentrations in the order of 50 ppb are present in the snow interstitial air. The measurements have been performed using multi-axis differential optical absorption spectroscopy (MAX-DOAS). Using a coupled atmosphere – snowpack radiative transfer model, the comparison of the signals observed from scattered skylight and from light reflected by the snowpack yields several ppb of iodine monoxide in the upper layers of the sunlit snowpack throughout the year. Snow pit samples from Neumayer Station contain up to 700 ng/l of total iodine, representing a sufficient reservoir for these extraordinarily high IO concentrations.
Linking urban aerosol fluxes in street canyons to larger scale emissions
Authors: Tay B. K. , McFiggans G. B. , Jones D. P. , Gallagher M. W. , Martin C. , Watkins P. , Harrison R. M.
Published: April 2010

Abstract. In this study we investigate ultrafine particle (UFP) fluxes using a first order eddy viscosity turbulence closure Computational Fluid Dynamics (CFD) model and determine the different factors that influence emissions of UFP into the urban boundary layer. Both vertical turbulent fluxes as well as the fluxes due to mean circulatory flow are shown to contribute to the overall ventilation characteristics of street canyons. We then derive a simple parameterised numerical prediction model for canyon top UFP venting which is then compared with tower based micrometeorological flux measurements obtained during the REPARTEE & CityFlux field experiments.
Sources of uncertainties in modelling black carbon at the global scale
Authors: Vignati E. , Karl M. , Krol M. , Wilson J. , Stier P. , Cavalli F.
Published: April 2010

Abstract. Our understanding of the global black carbon (BC) cycle is essentially qualitative due to uncertainties in our knowledge of its properties. This work investigates two source of uncertainties in modelling black carbon: those due to the use of different schemes for BC ageing and its removal rate in the global Transport-Chemistry model TM5 and those due to the uncertainties in the definition and quantification of the observations, which propagate through to both the emission inventories, and the measurements used for the model evaluation. The schemes for the atmospheric processing of black carbon that have been tested with the model are (i) a simple approach considering BC as bulk aerosol and a simple treatment of the removal with fixed 70% of in-cloud black carbon concentrations scavenged by clouds and removed when rain is present and (ii) a more complete description of microphysical ageing within an aerosol dynamics model, where removal is coupled to the microphysical properties of the aerosol, which results in a global average of 40% in-cloud black carbon that is scavenged in clouds and subsequently removed by rain, thus resulting in a longer atmospheric lifetime. This difference is reflected in comparisons between both sets of modelled results and the measurements. Close to the sources, both anthropogenic and vegetation fire source regions, the model results do not differ significantly, indicating that the emissions are the prevailing mechanism determining the concentrations and the choice of the aerosol scheme does not influence the levels. In more remote areas such as oceanic and polar regions the differences can be orders of magnitude, due to the differences between the two schemes. The more complete description reproduces the seasonal trend of the black carbon observations in those areas, although not always the magnitude of the signal, while the more simplified approach underestimates black carbon concentrations by orders of magnitude. The sensitivity to wet scavenging has been tested by varying in-cloud and below-cloud removal. BC lifetime increases by 10% when large scale and convective scale precipitation removal efficiency are reduced by 30%, while the variation is very small when below-cloud scavenging is zero. Since the emission inventories are representative of elemental carbon-like substance, the model output should be compared to elemental carbon measurements and if known, the ratio of black carbon to elemental carbon mass should be taken into account when the model is compared with black carbon observations.
Molecular characterization of urban organic aerosol in tropical India: contributions of primary emissions and secondary photooxidation
Authors: Fu P. Q. , Kawamura K. , Pavuluri C. M. , Swaminathan T. , Chen J.
Published: April 2010

Abstract. Organic molecular composition of PM10 samples, collected at Chennai in tropical India, was studied using capillary gas chromatography/mass spectrometry. Fourteen organic compound classes were detected in the aerosols, including aliphatic lipids, sugar compounds, lignin products, terpenoid biomarkers, sterols, aromatic acids, hydroxy-/polyacids, phthalate esters, hopanes, Polycyclic Aromatic Hydrocarbons (PAHs), and photooxidation products from biogenic Volatile Organic Compounds (VOCs). At daytime, phthalate esters were found to be the most abundant compound class; however, at nighttime, fatty acids were the dominant one. Di-(2-ethylhexyl) phthalate, C16 fatty acid, and levoglucosan were identified as the most abundant single compounds. The nighttime maxima of most organics in the aerosols indicate a land/sea breeze effect in tropical India, although some other factors such as local emissions and long-range transport may also influence the composition of organic aerosols. However, biogenic VOC oxidation products (e.g., 2-methyltetrols, pinic acid, 3-hydroxyglutaric acid and β-caryophyllinic acid) showed diurnal patterns with daytime maxima. Interestingly, terephthalic acid was maximized at nighttime, which is different from those of phthalic and isophthalic acids. A positive relation was found between 1,3,5-triphenylbenzene (a tracer for plastic burning) and terephthalic acid, suggesting that the field burning of municipal solid wastes including plastics is a significant source of terephthalic acid. Organic compounds were further categorized into several groups to clarify their sources. Fossil fuel combustion (24–43%) was recognized as the most significant source for the total identified compounds, followed by plastic emission (16–33%), secondary oxidation (8.6–23%), and microbial/marine sources (7.2–17%). In contrast, the contributions of terrestrial plant waxes (5.9–11%) and biomass burning (4.2–6.4%) were relatively small. This study demonstrates that, in addition to fossil fuel combustion and biomass burning, the open-burning of plastics in urban area also contributes to the organic aerosols in South Asia.
Stochastic fields method for sub-grid scale emission heterogeneity in mesoscale atmospheric dispersion models
Authors: Cassiani M. , Vinuesa J. F. , Galmarini S. , Denby B.
Published: April 2010

Abstract. The stochastic fields method for turbulent reacting flows has been applied to the issue of sub-grid scale emission heterogeneity in a mesoscale model. This method is a solution technique for the probability density function (PDF) transport equation and can be seen as a straightforward extension of currently used mesoscale dispersion models. It has been implemented in an existing mesoscale model and the results are compared with Large-Eddy Simulation (LES) data devised to test specifically the effect of sub-grid scale emission heterogeneity on boundary layer concentration fluctuations. The sub-grid scale emission variability is assimilated in the model as a PDF of the emissions. The stochastic fields method shows excellent agreement with the LES data without adjustment of the constants used in the mesoscale model. The stochastic fields method is a stochastic solution of the transport equations for the concentration PDF of dispersing scalars, therefore it possesses the ability to handle chemistry of any complexity without the need to introduce additional closures for the high order statistics of chemical species. This study shows for the first time the feasibility of applying this method to mesoscale chemical transport models.
Particle characterization at the Cape Verde atmospheric observatory during the 2007 RHaMBLe intensive
Authors: Müller K. , Lehmann S. , van Pinxteren D. , Gnauk T. , Niedermeier N. , Wiedensohler A. , Herrmann H.
Published: April 2010

Abstract. The chemical characterization of filter high volume (HV) and Berner impactor (BI) samples PM during RHaMBLe (Reactive Halogens in the Marine Boundary Layer) 2007 shows that the Cape Verde aerosol particles are mainly composed of sea salt, mineral dust and associated water. Minor components are nss-salts, OC and EC. The influence from the African continent on the aerosol constitution was generally small but air masses which came from south-western Europe crossing the Canary Islands transported dust to the sampling site together with other loadings. The mean mass concentration was determined for PM10 to 17 μg/m3 from impactor samples and to 24.2 μg/m3 from HV filter samples. Non sea salt (nss) components of PM were found in the submicron fractions and nitrate in the coarse mode fraction. Bromide was found in all samples with much depleted concentrations in the range 1–8 ng/m3 compared to fresh sea salt aerosol indicating intense atmospheric halogen chemistry. Loss of bromide by ozone reaction during long sampling time is supposed and resulted totally in 82±12% in coarse mode impactor samples and in filter samples in 88±6% bromide deficits. A chloride deficit was determined to 8% and 1% for the coarse mode particles (3.5–10 μm; 1.2–3.5 μm) and to 21% for filter samples. During 14 May with high mineral dust loads also the maximum of OC (1.71μg/m3) and EC (1.25 μg/m3) was measured. The minimum of TC (0.25 μg/m3) was detected during the period 25 to 27 May when pure marine air masses arrived. The concentrations of carbonaceous material decrease with increasing particle size from 60% for the ultra fine particles to 2.5% in coarse mode PM. Total iron (dust vs. non-dust: 0.53 vs. 0.06 μg m3), calcium (0.22 vs. 0.03 μg m3) and potassium (0.33 vs. 0.02 μg m3) were found as good indicators for dust periods because of their heavily increased concentration in the 1.2 to 3.5 μm fraction as compared to their concentration during the non-dust periods. For the organic constituents, oxalate (78–151 ng/m3) and methanesulfonic acid (MSA, 25–100 ng/m3) are the major compounds identified. A good correlation between nss-sulphate and MSA was found for the majority of days indicating active DMS chemistry and low anthropogenic influences.
The organic fraction of bubble-generated, accumulation mode Sea Spray Aerosol (SSA)
Authors: Modini R. L. , Harris B. , Ristovski Z. D.
Published: April 2010

Abstract. Recent studies have detected a dominant accumulation mode (~100 nm) in the Sea Spray Aerosol (SSA) number distribution. There is evidence to suggest that particles in this mode are composed primarily of organics. To investigate this hypothesis we conducted experiments on NaCl, artificial SSA and natural SSA particles with a Volatility-Hygroscopicity-Tandem-Differential-Mobility-Analyser (VH-TDMA). NaCl particles were atomiser generated and a bubble generator was constructed to produce artificial and natural SSA particles. Natural seawater samples for use in the bubble generator were collected from biologically active, terrestrially-affected coastal water in Moreton Bay, Australia. Differences in the VH-TDMA-measured volatility curves of artificial and natural SSA particles were used to investigate and quantify the organic fraction of natural SSA particles. Hygroscopic Growth Factor (HGF) data, also obtained by the VH-TDMA, were used to confirm the conclusions drawn from the volatility data. Both datasets indicated that the organic fraction of our natural SSA particles evaporated in the VH-TDMA over the temperature range 170–200 °C. The organic volume fraction for 71–77 nm natural SSA particles was 8±6%. Organic volume fraction did not vary significantly with varying water residence time (40 s to 24 h) in the bubble generator or SSA particle diameter in the range 38–173 nm. At room temperature we measured shape- and Kelvin-corrected HGF at 90% RH of 2.46±0.02 for NaCl, 2.35±0.02 for artifical SSA and 2.26±0.02 for natural SSA particles. Overall, these results suggest that the natural accumulation mode SSA particles produced in these experiments contained only a minor organic fraction, which had little effect on hygroscopic growth. Our measurement of 8±6% is an order of magnitude below two previous measurements of the organic fraction in SSA particles of comparable sizes. We stress that our results were obtained using coastal seawater and they can't necessarily be applied on a regional or global ocean scale. Nevertheless, considering the order of magnitude discrepancy between this and previous studies, further research with independent measurement techniques and a variety of different seawaters is required to better quantify how much organic material is present in accumulation mode SSA.
Toward real-time measurement of atmospheric mercury concentrations using cavity ring-down spectroscopy
Authors: Faïn X. , Moosmüller H. , Obrist D.
Published: April 2010

Abstract. Cavity ring-down spectroscopy (CRDS) is a direct absorption technique that utilizes path lengths up to multiple kilometers in a compact absorption cell and has a significantly higher sensitivity than conventional absorption spectroscopy. This tool opens new prospects for study of gaseous elemental mercury (Hg0) because of its high temporal resolution and reduced sample volume requirements (<0.5 l of sample air). We developed a new sensor based on CRDS for measurement of (Hg0) mass concentration. Sensor characteristics include sub-ng m−3 detection limit and high temporal resolution using a frequency-doubled, tuneable dye laser emitting pulses at ~253.65 nm with a pulse repetition frequency of 50 Hz. The dye laser incorporates a unique piezo element attached to its tuning grating allowing it to tune the laser on and off the Hg0 absorption line on a pulse-to-pulse basis to facilitate differential absorption measurements. Hg0 absorption measurements with this CRDS laboratory prototype are highly linearly related to Hg0 concentrations determined by a Tekran 2537B analyzer over an Hg0 concentration range from 0.2 ng m−3 to 573 ng m−3, implying excellent linearity of both instruments. The current CRDS instrument has a sensitivity of 0.10 ng Hg0 m−3 at 10-s time resolution. Ambient-air tests showed that background Hg0 levels can be detected at low temporal resolution (i.e., 1 s), but also highlight a need for high-frequency (i.e., pulse-to-pulse) differential on/off-line tuning of the laser wavelength to account for instabilities of the CRDS system and variable background absorption interferences. Future applications may include ambient Hg0 flux measurements with eddy covariance techniques, which require measurements of Hg0 concentrations with sub-ng m−3 sensitivity and sub-second time resolution.
Study of successive contrasting monsoons (2001–2002) in terms of aerosol variability over a tropical station Pune, India
Authors: Bhawar R. L. , Devara P. C. S.
Published: April 2010

Abstract. The present study suggests that aerosols play a major role in cloud formation and affect significantly the precipitation over a regional scale. The study reveals that there is a high variability of aerosol index during a bad monsoon year 2002, indicating an extension of cycle to more than 100 days from a normal 50 day cycle of absorbing and non-absorbing aerosols over a tropical urban station Pune. Pre-monsoon of 2002 shows a high loading of coarse-mode aerosols (absorbing dust aerosols) which indicate vertical and horizontal temperature variations in turn affecting the seasonal rainfall at a regional scale. Cloud formation highly depends on aerosol concentration, but the activation process is not monotonic. The surface meteorological features help to initiate the cloud process. The surface temperatures were high during the pre-monsoon of 2002 leading to increase of aerosol optical depth as compared to 2001. The effect of surface wind speed, though, complicated to understand, results in low values in 2002 with high aerosol optical depth and vice-versa in 2001.
Uncertainties in estimating mercury emissions from coal-fired power plants in China
Authors: Wu Y. , Streets D. G. , Wang S. X. , Hao J. M.
Published: April 2010

Abstract. A detailed multiple-year inventory of mercury emissions from anthropogenic activities in China has been developed. Coal combustion and nonferrous metals production continue to be the two leading mercury sources in China, together contributing ~80% of total mercury emissions. However, many uncertainties still remain in our knowledge of primary anthropogenic releases of mercury to the atmosphere in China. In situations involving large uncertainties, our previous mercury emission inventory that used a deterministic approach could produce results that might not be a true reflection of reality; and in such cases stochastic simulations incorporating uncertainties need to be performed. Within our inventory, a new comprehensive sub-module for estimation of mercury emissions from coal-fired power plants in China is constructed as an uncertainty case study. The new sub-module integrates up-to-date information regarding mercury content in coal by province, coal washing and cleaning, coal consumption by province, mercury removal efficiencies by control technology or technology combinations, etc. Based on these detailed data, probability-based distribution functions are built into the sub-module to address the uncertainties of these key parameters. The sub-module incorporates Monte Carlo simulations to take into account the probability distributions of key input parameters and produce the mercury emission results in the form of a statistical distribution. For example, the best estimate for total mercury emissions from coal-fired power plants in China in 2003 is 90.5 Mg, with the uncertainty range from 57.1 Mg (P10) to 154.6 Mg (P90); and the best estimate for elemental mercury emissions is 43.0 Mg, with the uncertainty range from 25.6 Mg (P10) to 75.7 Mg (P90). The results further indicate that the majority of the uncertainty in mercury emission estimation comes from two factors: mercury content of coal and mercury removal efficiency.
Iodine-mediated coastal particle formation: an overview of the Reactive Halogens in the Marine Boundary Layer (RHaMBLe) Roscoff coastal study
Authors: McFiggans G. , Bale C. S. E. , Ball S. M. , Beames J. M. , Bloss W. J. , Carpenter L. J. , Dorsey J. , Dunk R. , Flynn M. J. , Furneaux K. L. , Gallagher M. W. , Heard D. E. , Hollingsworth A. M. , Hornsby K. , Ingham T. , Jones C. E. , Jones R. L. , Kramer L. J. , Langridge J. M. , Leblanc C. , LeCrane J.-P. , Lee J. D. , Leigh R. J. , Longley I. , Mahajan A. S. , Monks P. S. , Oetjen H. , Orr-Ewing A. J. , Plane J. M. C. , Potin P. , Shillings A. J. L. , Thomas F. , von Glasow R. , Wada R. , Whalley L. K. , Whitehead J. D.
Published: April 2010

Abstract. This paper presents a summary of the measurements made during the heavily-instrumented Reactive Halogens in the Marine Boundary Layer (RHaMBLe) coastal study in Roscoff on the North West coast of France throughout September 2006. It was clearly demonstrated that iodine-mediated coastal particle formation occurs, driven by daytime low tide emission of molecular iodine, I2, by macroalgal species fully or partially exposed by the receding waterline. Ultrafine particle concentrations strongly correlate with the rapidly recycled reactive iodine species, IO, produced at high concentrations following photolysis of I2. The heterogeneous macroalgal I2 sources lead to variable relative concentrations of iodine species observed by path-integrated and in situ measurement techniques. Apparent particle emission fluxes were associated with an enhanced apparent depositional flux of ozone, consistent with both a direct O3 deposition to macroalgae and involvement of O3 in iodine photochemistry and subsequent particle formation below the measurement height. The magnitude of the particle formation events was observed to be greatest at the lowest tides with the highest concentrations of ultrafine particles growing to the largest sizes, probably by the condensation of anthropogenically-formed condensable material. At such sizes the particles should be able to act as cloud condensation nuclei at reasonable atmospheric supersaturations.