bluuebunny/crossref_metadata_2025 huggingface dataset:
Mixing ratios and eddy covariance flux measurements of volatile organic compounds from an urban canopy (Manchester, UK)
Authors: Langford B. , Davison B. , Nemitz E. , Hewitt C. N.
Published: April 2010

Abstract. Mixing ratios and fluxes of six selected volatile organic compounds (VOCs) were measured above the city of Manchester (UK) during the summer of 2006. A proton transfer reaction-mass spectrometer was used for the measurement of mixing ratios, and fluxes were calculated from these using both the disjunct and the virtual disjunct eddy covariance techniques. The two flux systems, which operated in alternate half hours, showed good agreement, with R2 values ranging between 0.74 and 0.9 for the individual analytes. On average, fluxes measured in the disjunct mode were approximately 20% lower than those measured in the virtual mode. This difference is due to both the dampening of the VOC signal by the disjunct flux sampler and carry over from one sample to the next. Correcting for these effects reduced the difference to less than 7%. Observed fluxes are thought to be largely controlled by anthropogenic sources, with vehicle emissions the major contributor. However, both evaporative and biogenic emissions may account for some of the VOCs present. Concentrations and fluxes of the oxygenated compounds were highest on average, ranging between 0.15 to 1 mg m−2 h−1; the fluxes of aromatic compounds were lower, between 0.12 to 0.28 mg m−2 h−1. The observed fluxes were up-scaled to give city wide emission estimates for each compound and the results compared to estimates made by the National Atmospheric Emission Inventory (NAEI) for the same flux footprint. Fluxes of toluene and benzene compared most closely differing by approximately 50%, while in contrast the oxygenated fluxes were found to be between 3.6–6.3 times larger than the annual average predicted by the NAEI.
Modelling trends in OH radical concentrations using generalized additive models
Authors: Jackson L. S. , Carslaw N. , Carslaw D. C. , Emmerson K. M.
Published: April 2010

Abstract. During the TORCH campaign a zero dimensional box model based on the Master Chemical Mechanism was used to model concentrations of OH radicals. The model provided a close overall fit to measured concentrations but with some significant deviations. In this research, an approach was established for applying Generalized Additive Models (GAM) to atmospheric concentration data. Two GAM models were fitted to OH radical concentrations using TORCH data, the first using measured OH data and the second using MCM model results. GAM models with five smooth functions provided a close fit to the data with 78% of the deviance explained for measured OH and 83% for modelled OH. The GAM model for measured OH produced substantially better predictions of OH concentrations than the original MCM model results. The diurnal profile of OH concentration was reproduced and the predicted mean diurnal OH concentration was only 0.2% less than the measured concentration compared to 16.3% over-estimation by the MCM model. Photolysis reactions were identified as most important in explaining concentrations of OH. The GAM models combined both primary and secondary pollutants and also anthropogenic and biogenic species to explain changes in OH concentrations. Differences identified in the dependencies of modelled and measured OH concentrations, particularly for aromatic and biogenic species, may help to understand why the MCM model predictions sometimes disagree with measurements of atmospheric species.
Methyl chavicol: characterization of its biogenic emission rate, abundance, and oxidation products in the atmosphere
Authors: Bouvier-Brown N. C. , Goldstein A. H. , Worton D. R. , Matross D. M. , Gilman J. B. , Kuster W. C. , Welsh-Bon D. , Warneke C. , de Gouw J. A. , Cahill T. M. , Holzinger R.
Published: April 2010

Abstract. We report measurements of ambient atmospheric mixing ratios for methyl chavicol and determine its biogenic emission rate. Methyl chavicol, a biogenic oxygenated aromatic compound, is abundant within and above Blodgett Forest, a ponderosa pine forest in the Sierra Nevada Mountains of California. Methyl chavicol was detected simultaneously by three in-situ instruments – a gas chromatograph with mass spectrometer detector (GC-MS), a proton transfer reaction mass spectrometer (PTR-MS), and a thermal desorption aerosol GC-MS (TAG) – and found to be abundant within and above Blodgett Forest. Methyl chavicol atmospheric mixing ratios are strongly correlated with 2-methyl-3-buten-2-ol (MBO), a light- and temperature-dependent biogenic emission from the ponderosa pine trees at Blodgett Forest. Scaling from this correlation, methyl chavicol emissions account for 4–68% of the carbon mass emitted as MBO in the daytime, depending on the season. From this relationship, we estimate a daytime basal emission rate of 0.72–10.2 μgCg−1 h−1, depending on needle age and seasonality. We also present the first observations of its oxidation products (4-methoxybenzaldehyde and 4-methyoxy benzene acetaldehyde) in the ambient atmosphere. Methyl chavicol is a major essential oil component of many plant species. This work suggests that methyl chavicol plays a significant role in the atmospheric chemistry of Blodgett Forest, and potentially other sites, and should be included explicitly in both biogenic volatile organic carbon emission and atmospheric chemistry models.
In situ measurements of speciated atmospheric mercury and the identification of source regions in the Mexico City Metropolitan Area
Authors: Rutter A. P. , Snyder D. C. , Stone E. A. , Schauer J. J. , Gonzalez-Abraham R. , Molina L. T. , Márquez C. , Cárdenas B. , de Foy B.
Published: April 2010

Abstract. In order to expand the currently limited understanding of atmospheric mercury source-receptor relationships in the Mexico City Metropolitan Area, real time measurements of atmospheric mercury were made at a downtown urban site, and a rural site on the outskirts of Mexico City, during March 2006. Numerous short-lived increases in particulate mercury (PHg) and reactive gaseous mercury (RGM) concentrations were observed at the urban site during the 17 day study, and less frequent increases in gaseous elemental mercury (GEM) concentrations were measured at both the urban and rural sites. The episodic increases observed were attributed to plume impacts from industrial point source emissions in and around Mexico City. Average concentrations and standard deviations measured during the study were as follows: i) urban site; PHg=187±300 pg m−3, RGM=62±64 pg m−3, GEM=7.2±4.8 ng m−3, and; ii) rural site; GEM=5.0±2.8 ng m−3. Several source regions of atmospheric mercury to the urban and rural sites were determined using Concentration Field Analysis, in which atmospheric mercury measurements were combined with back trajectory data to determine source regions. Only some source regions correlated to mercury emission sources listed in the Federal Pollutant Release and Transfer Register, leaving the rest unaccounted for. Contributions of anthropogenic mercury point sources in and around Mexico City to concentration averages measured at the urban site during the study were estimated to be: 93±3% of reactive mercury (PHg and RGM), and; 81±0.4% of GEM. Point source contributions to GEM measured at the rural site were 72±1%. GEM and reactive mercury (PHg+RGM) were not found to correlate with biomass burning at either of the measurement sites.
Spatial heterogeneity of satellite derived land surface parameters and energy flux densities for LITFASS-area
Authors: Tittebrand A. , Berger F. H.
Published: April 2010

Abstract. Based on satellite data in different temporal and spatial resolution, the current use of frequency distribution functions (PDF) for surface parameters and energy fluxes is one of the most promising ways to describe subgrid heterogeneity of a landscape. Objective of this study is to find typical distribution patterns of parameters (albedo, NDVI) for the determination of the actual latent heat flux (L.E) determined from highly resolved satellite data within pixel on coarser scale. Landsat ETM+, Terra MODIS and NOAA-AVHRR surface temperature and spectral reflectance were used to infer further surface parameters and radiant- and energy flux densities for LITFASS-area, a 20×20 km2 heterogeneous area in Eastern Germany, mainly characterised by the land use types forest, crop, grass and water. Based on the Penman-Monteith-approach L.E, as key quantity of the hydrological cycle, is determined for each sensor in the accordant spatial resolution with an improved parametrisation. However, using three sensors, significant discrepancies between the inferred parameters can cause flux distinctions resultant from differences of the sensor filter response functions or atmospheric correction methods. The approximation of MODIS- and AVHRR- derived surface parameters to the reference parameters of ETM (via regression lines and histogram stretching, respectively), further the use of accurate land use classifications (CORINE and a new Landsat-classification), and a consistent parametrisation for the three sensors were realized to obtain a uniform base for investigations of the spatial variability. The analyses for 4 scenes in 2002 and 2003 showed that for forest clear distribution-patterns for NDVI and albedo are found. Grass and crop distributions show higher variability and differ significantly to each other in NDVI but only marginal in albedo. Regarding NDVI-distribution functions NDVI was found to be the key variable for L.E-determination.
What would have happened to the ozone layer if chlorofluorocarbons (CFCs) had not been regulated?
Authors: Newman P. A. , Oman L. D. , Douglass A. R. , Fleming E. L. , Frith S. M. , Hurwitz M. M. , Kawa S. R. , Jackman C. H. , Krotkov N. A. , Nash E. R. , Nielsen J. E. , Pawson S. , Stolarski R. S. , Velders G. J. M.
Published: April 2010

Abstract. Ozone depletion by chlorofluorocarbons (CFCs) was first proposed by Molina and Rowland in their 1974 Nature paper. Since that time, the scientific connection between ozone losses and CFCs and other ozone depleting substances (ODSs) has been firmly established with laboratory measurements, atmospheric observations, and modeling studies. This science research led to the implementation of international agreements that largely stopped the production of ODSs. In this study we use a fully-coupled radiation-chemical-dynamical model to simulate a future world where ODSs were never regulated and ODS production grew at an annual rate of 3%. In this "world avoided" simulation, 17% of the globally-averaged column ozone is destroyed by 2020, and 67% is destroyed by 2065 in comparison to 1980. Large ozone depletions in the polar region become year-round rather than just seasonal as is currently observed in the Antarctic ozone hole. Very large temperature decreases are observed in response to circulation changes and decreased shortwave radiation absorption by ozone. Ozone levels in the tropical lower stratosphere remain constant until about 2053 and then collapse to near zero by 2058 as a result of heterogeneous chemical processes (as currently observed in the Antarctic ozone hole). The tropical cooling that triggers the ozone collapse is caused by an increase of the tropical upwelling. In response to ozone changes, ultraviolet radiation increases, more than doubling the erythemal radiation in the northern summer midlatitudes by 2060.
Stratospheric ozone in the post-CFC era
Authors: Li F. , Stolarski R. S. , Newman P. A.
Published: April 2010

Abstract. Vertical and latitudinal changes in the stratospheric ozone in the post-chlorofluorocarbon (CFC) era are investigated using simulations of the recent past and the 21st century with a coupled chemistry-climate model. Model results reveal that, in the 2060s when the stratospheric halogen loading is projected to return to its 1980 values, the extratropical column ozone is significantly higher than that in 1975–1984, but the tropical column ozone does not recover to 1980 values. Upper and lower stratospheric ozone changes in the post-CFC era have very different patterns. Above 15 hPa ozone increases almost latitudinally uniformly by 6 Dobson Unit (DU), whereas below 15 hPa ozone decreases in the tropics by 8 DU and increases in the extratropics by up to 16 DU. The upper stratospheric ozone increase is a photochemical response to greenhouse gas induced strong cooling, and the lower stratospheric ozone changes are consistent with enhanced mean advective transport due to a stronger Brewer-Dobson circulation. The model results suggest that the strengthening of the Brewer-Dobson circulation plays a crucial role in ozone recovery and ozone distributions in the post-CFC era.
Laboratory measurements of the optical properties of sea salt aerosol
Authors: Irshad R. , Grainger R. G. , Peters D. M. , McPheat R. A. , Smith K. M. , Thomas G.
Published: April 2010

Abstract. The extinction spectra of laboratory generated sea salt aerosols have been measured from 1 μm to 20 μm using a Bruker 66v/S FTIR spectrometer. Concomitant measurements include temperature, pressure, relative humidity and the aerosol size distribution. The refractive indices of the sea salt aerosol have been determined using a simple harmonic oscillator band model (Thomas et al., 2004) for aerosol with relative humidities at eight different values between 0.4% to 86%. The resulting refractive index spectra show significant discrepancies when compared to existing sea salt refractive indices calculated using volume mixing rules (Shettle and Fenn, 1979). Specifically, an additional band is found in the refractive indices of dry sea salt aerosol and the new data shows increased values of refractive index at almost all wavelengths. This implies that the volume mixing rules, currently used to calculate the refractive indices of wet sea salt aerosols, are inadequate. Furthermore, the existing data for the real and imaginary parts of the refractive indices of dry sea salt aerosol are found not to display the Kramers-Kronig relationship. This implies that the original data used for the volume mixing calculations is also inaccurate.
Laboratory investigation of photochemical oxidation of organic aerosol from wood fires 2: analysis of aerosol mass spectrometer data
Authors: Grieshop A. P. , Donahue N. M. , Robinson A. L.
Published: April 2010

Abstract. Experiments were conducted to investigate the effects of photo-oxidation on organic aerosol (OA) in dilute wood smoke by exposing emissions from soft- and hard-wood fires to UV light in a smog chamber. This paper focuses on changes in OA composition measured using a unit-mass-resolution quadrupole Aerosol Mass Spectrometer (AMS). The results highlight how photochemical processing can lead to considerable evolution of the mass, volatility and level of oxygenation of biomass-burning OA. Photochemical oxidation produced substantial new OA, more than doubling the OA mass after a few hours of aging under typical summertime conditions. Aging also decreased the volatility of the OA and made it progressively more oxygenated. The results also illustrate strengths of, and challenges with, using AMS data for source apportionment analysis. For example, the mass spectra of fresh and aged BBOA are distinct from fresh motor-vehicle emissions. The mass spectra of the secondary OA produced from aging wood smoke are very similar to those of the oxygenated OA (OOA) that dominates ambient AMS datasets, further reinforcing the connection between OOA and OA formed from photo-chemistry. In addition, aged wood smoke spectra are similar to those from OA created by photo-oxidizing dilute diesel exhaust. This demonstrates that the OOA observed in the atmosphere can be produced by photochemical aging of dilute emissions from different types of combustion systems operating on fuels with modern or fossil carbon. Since OOA is frequently the dominant component of ambient OA, the similarity of spectra of aged emissions from different sources represents an important challenge for AMS-based source apportionment studies.
Light-absorbing secondary organic material formed by glyoxal in aqueous aerosol mimics
Authors: Shapiro E. L. , Szprengiel J. , Sareen N. , Jen C. N. , Giordano M. R. , McNeill V. F.
Published: April 2010

Abstract. Light-absorbing and high-molecular-weight secondary organic products were observed to result from the reaction of glyoxal in mildly acidic (pH=4) aqueous inorganic salt solutions mimicking aqueous tropospheric aerosol particles. High-molecular-weight (500–600 amu) products were observed when ammonium sulfate ((NH4)2SO4) or sodium chloride (NaCl) was present in the aqueous phase. The products formed in (NH4)2SO4 or ammonium nitrate (NH4NO3) solutions absorb light at UV and visible wavelengths. Substantial absorption at 300–400 nm develops within two hours, and absorption between 400–600 nm develops within days. Pendant drop tensiometry measurements show that the products are not surface-active. The experimental results along with ab initio predictions of the UV/Vis absorption of potential products suggest a mechanism involving the participation of the ammonium ion. If similar products are formed in atmospheric aerosol particles, they could change the optical properties of the seed aerosol over its lifetime.
Quantitative assessment of organosulfates in size-segregated rural fine aerosol
Authors: Lukács H. , Gelencsér A. , Hoffer A. , Kiss G. , Horváth K. , Hartyáni Z.
Published: April 2010

Abstract. Organosulfates have recently come into the focus of organic aerosol research as potentially important components of water-soluble secondary organic aerosol (SOA) which now dominate tropospheric fine aerosol. Their presence has been confirmed by the identification of sulfate esters of abundant biogenic carbonyl compounds in both smog chamber and continental aerosol. However, none of the studies have been able to determine the mass contribution of organosulfates to SOA. In this paper, as possibly the very first attempt to quantify organosulfates in ambient aerosol, we inferred the mass concentrations of organosulfates by concurrently determining mass concentrations of total sulfur, sulfate and methanesulfonate in rural fine aerosol using two highly sensitive analytical techniques. Although uncertainties were relatively large, we found that mass concentrations of organosulfates in water-soluble fine aerosol ranged from 0.02 μgS m−3 to 0.09 μgS m−3 yielding a mass contribution of 6–12% to bulk sulfur concentrations (or 6–14% to sulfate concentrations). The inferred size distribution of organosulfates suggested that they possibly form in heterogeneous reactions from semi-volatile carbonyl compounds with subsequent or concurrent condensation of gaseous sulfuric acid producing a refractory organic film on particle surfaces.
Modelling of cirrus clouds – Part 2: Competition of different nucleation mechanisms
Authors: Spichtinger P. , Gierens K. M.
Published: April 2010

Abstract. We study the competition of two different freezing mechanisms (homogeneous and heterogeneous freezing) in the same environment for cold cirrus clouds. To this goal we use the recently developed and validated ice microphysics scheme (Spichtinger and Gierens, 2009a) which distinguishes between ice classes according to their formation process. We investigate cases with purely homogeneous ice formation and compare them with cases where background ice nuclei in varying concentration heterogeneously form ice prior to homogeneous nucleation. We perform additionally a couple of sensitivity studies regarding threshold humidity for heterogeneous freezing, uplift speed, and ambient temperature, and we study the influence of random motions induced by temperature fluctuations in the clouds. We find three types of cloud evolution, homogeneously dominated, heterogeneously dominated, and a mixed type where neither nucleation process dominates. The latter case is prone to long–lasting in–cloud ice supersaturation of the order 30% and more.
Dispersion of traffic-related exhaust particles near the Berlin urban motorway – estimation of fleet emission factors
Authors: Birmili W. , Alaviippola B. , Hinneburg D. , Knoth O. , Tuch T. , Borken-Kleefeld J. , Schacht A.
Published: April 2010

Abstract. Atmospheric particle number size distributions of airborne particles (diameter range 10–500 nm) were collected over ten weeks at three sites in the vicinity of the A100 urban motorway in Berlin, Germany. The A100 carries about 180 000 vehicles on a weekday. The roadside particle distributions showed a number maximum between 20 and 60 nm clearly related to the motorway emissions. The average total number concentration at roadside was 28 000 cm−3 with a total range of 1200–168 000 cm−3. At distances of 80 and 400 m from the motorway the concentrations decreased to mean levels of 11 000 and 9000 cm−3, respectively. An obstacle-resolving dispersion model was applied to simulate the 3-D flow field and traffic tracer transport in the urban environment around the motorway. By inverse modelling, vehicle emission factors were derived that are representative of a fleet with a relative share of 6% lorry-like vehicles, and driving at a speed of 80 km h−1. Three different calculation approaches were compared, which differ in the choice of the experimental winds driving the flow simulation. The average emission factor per vehicle was 2.1 (±0.2) · 1014 km−1 for particle number and 0.077 (±0.01) · 1014 cm3 km−1 for particle volume. Regression analysis suggested that lorry-like vehicles emit 123 (±28) times more particle number than passenger car-like vehicles, and lorry-like vehicles account for about 91% of particulate number emissions on weekdays. Our work highlights the increasing applicability of 3-D flow models in urban microscale environments and their usefulness for determining traffic emission factors.
Aerosol indirect forcing in a global model with particle nucleation
Authors: Wang M. , Penner J. E.
Published: April 2010

Abstract. The number concentration of cloud condensation nuclei (CCN) formed as a result of anthropogenic emissions is a key uncertainty in the study of aerosol indirect forcing and global climate change. Here, we use a global aerosol model that includes an empirical boundary layer nucleation mechanism, the use of primary-emitted sulfate particles to represent sub-grid scale nucleation, as well as binary homogeneous nucleation to explore how nucleation affects the CCN concentration and the first aerosol indirect effect (AIE). The inclusion of the boundary layer nucleation scheme increases the global average CCN concentrations in the boundary layer by 31.4% when no primary-emitted sulfate particles are included and by 5.3% when they are included. Particle formation with the boundary layer nucleation scheme decreases the first indirect forcing over ocean, and increases the first indirect forcing over land when primary sulfate particles are included. This suggests that whether particle formation from aerosol nucleation increases or decreases aerosol indirect effects largely depends on the relative change of primary particles and SO2 emissions from the preindustrial to the present day atmosphere. Including primary-emitted sulfate particle significantly increases both the anthropogenic fraction of CCN concentrations and the first aerosol indirect forcing. The forcing from various treatments of aerosol nucleation ranges from −1.22 to −2.03 w/m2. This large variation shows the importance of better quantifying aerosol nucleation mechanisms for the prediction of CCN concentrations and aerosol indirect effects.
Optical characteristics of biomass burning aerosols over Southeastern Europe determined from UV-Raman lidar measurements
Authors: Amiridis V. , Balis D. S. , Giannakaki E. , Stohl A. , Kazadzis S. , Koukouli M. E. , Zanis P.
Published: April 2010

Abstract. The influence of smoke on the aerosol loading in the free troposphere over Thessaloniki, Greece is examined in this paper. Ten cases during 2001–2005 were identified when very high aerosol optical depth values in the free troposphere were observed with a UV-Raman lidar. Particle dispersion modeling (FLEXPART) and satellite hot spot fire detection (ATSR) showed that these high free tropospheric aerosol optical depths are mainly attributed to the advection of smoke plumes from biomass burning regions over Thessaloniki. The biomass burning regions were found to extend across Russia in the latitudinal belt between 45° N–55° N, as well as in Eastern Europe (Baltic countries, Western Russia, Belarus, and the Ukraine). The highest frequency of agricultural fires occurred during the summer season (mainly in August). The data collected allowed the optical characterization of the smoke aerosols that arrived over Greece, where limited information has so far been available. Two-wavelength backscatter lidar measurements showed that the backscatter-related Ångström exponent ranged between 0.5 and 2.4 indicating a variety of particle sizes. UV-Raman lidar measurements showed that for smoke particles the extinction to backscatter ratios (so-called lidar ratios) varied between 40 sr for small particles to 100 sr for large particles. Dispersion model estimations of the carbon monoxide tracer concentration profiles for smoke particles indicate that the variability of the optical parameters is a function of the age of the smoke plumes. This information could be useful on the lidar community for reducing uncertainty in the aerosol backscatter coefficient determination due to the lidar ratio assumption, starting from a simply elastic backscatter lidar as the first satellite-borne lidar CALIPSO.
Development of a global model of mineral dust aerosol microphysics
Authors: Lee Y. H. , Chen K. , Adams P. J.
Published: April 2010

Abstract. A mineral dust module is developed and implemented into the global aerosol microphysics model, GISS-TOMAS. The model is evaluated against long-term measurements of dust surface mass concentrations and deposition fluxes. Predicted mass concentrations and deposition fluxes are in error on average by a factor of 3 and 5, respectively. The comparison shows that the model performs better near the dust source regions but underestimates surface concentrations and deposition fluxes in more remote regions. Including only sites with measured dust concentrations of at least 0.5 μg m−3, the model prediction agrees with observations to within a factor of 2. It was hypothesized that the lifetime of dust, 2.6 days in our base case, is too short and causes the underestimation in remote areas. However, a sensitivity simulation with smaller dust particles and increased lifetime, 3.7 days, does not significantly improve the comparison. These results suggest that the underestimation of mineral dust in remote areas may result from local factors/sources not well described by the global dust source function used here or the GCM meteorology. The effect of dust aerosols on CCN(0.2%) concentrations is negligible in most regions of the globe; however, CCN(0.2%) concentrations change decrease by 10–20% in dusty regions the impact of dust on CCN(0.2%) concentrations in dusty regions is very sensitive to the assumed size distribution of emissions. If emissions are predominantly in the coarse mode, CCN(0.2%) decreases in dusty regions up to 10–20% because dust competes for condensable H2SO4, reducing the condensational growth of ultrafine mode particles to CCN sizes. With significant fine mode emissions, however, CCN(0.2%) doubles in Saharan source regions because the direct emission of dust particles outweighs any microphysical feedbacks. The impact of dust on CCN concentrations active at various water supersaturations is also investigated. Below 0.1%, CCN concentrations increase significantly in dusty regions due to the presence of coarse dust particles. Above 0.2%, CCN concentrations show a similar behavior as CCN(0.2%).
The impact of tropical recirculation on polar composition
Authors: Strahan S. E. , Schoeberl M. R. , Steenrod S. D.
Published: April 2010

Abstract. We derive the tropical modal age of air from an analysis of the water vapor tape recorder. We combine the observationally derived modal age with mean age of air from CO2 and SF6 to create diagnostics for the independent evaluation of the vertical transport rate and horizontal recirculation into the tropics between 16–32 km. These diagnostics are applied to two Global Modeling Initiative (GMI) chemistry and transport model (CTM) age tracer simulations to give new insights into the tropical transport characteristics of the meteorological fields from the GEOS4-GCM and the GEOS4-DAS. Both simulations are found to have modal ages that are in reasonable agreement with the empirically derived age (i.e., transit times) over the entire altitude range. Both simulations show too little horizontal recirculation into the tropics above 22 km, with the GEOS4-DAS fields having greater recirculation. Using CH4 as a proxy for mean age, comparisons between HALOE and model CH4 in the Antarctic demonstrate how the strength of tropical recirculation affects polar composition in both CTM experiments. Better tropical recirculation tends to improve the CH4 simulation in the Antarctic. However, mean age in the Antarctic lower stratosphere can be compromised by poor representation of tropical ascent, tropical recirculation, or vortex barrier strength. The connection between polar and tropical composition shown in this study demonstrates the importance of diagnosing each of these processes separately in order to verify the adequate representation of the processes contributing to polar composition in models.
Springtime warming and reduced snow cover from carbonaceous particles
Authors: Flanner M. G. , Zender C. S. , Hess P. G. , Mahowald N. M. , Painter T. H. , Ramanathan V. , Rasch P. J.
Published: April 2010

Abstract. Boreal spring climate is uniquely susceptible to solar warming mechanisms because it has expansive snow cover and receives relatively strong insolation. Carbonaceous particles can influence snow coverage by warming the atmosphere, reducing surface-incident solar energy (dimming), and reducing snow reflectance after deposition (darkening). We apply a range of models and observations to explore impacts of these processes on springtime climate, drawing several conclusions: 1) Nearly all atmospheric particles (those with visible-band single-scatter albedo less than 0.999), including all mixtures of black carbon (BC) and organic matter (OM), increase net solar heating of the atmosphere-snow column. 2) Darkening caused by small concentrations of particles within snow exceeds the loss of absorbed energy from concurrent dimming, thus increasing solar heating of snowpack as well (positive net surface forcing). Over global snow, we estimate 6-fold greater surface forcing from darkening than dimming, caused by BC+OM. 3) Equilibrium climate experiments suggest that fossil fuel and biofuel emissions of BC+OM induce 95% as much springtime snow cover loss over Eurasia as anthropogenic carbon dioxide, a consequence of strong snow-albedo feedback and large BC+OM emissions from Asia. 4) Of 22 climate models contributing to the IPCC Fourth Assessment Report, 21 underpredict the rapid warming (0.64°C decade−1) observed over springtime Eurasia since 1979. Darkening from natural and anthropogenic sources of BC and mineral dust exerts 3-fold greater forcing on springtime snow over Eurasia (3.9 W m−2) than North America (1.2 W m−2). Inclusion of this forcing significantly improves simulated continental warming trends, but does not reconcile the low bias in rate of Eurasian spring snow cover decline exhibited by all models, likely because BC deposition trends are negative or near-neutral over much of Eurasia. Improved Eurasian warming may therefore relate more to darkening-induced reduction in mean snow cover.
Parameterization of cloud droplet formation for global and regional models: including adsorption activation from insoluble CCN
Authors: Kumar P. , Sokolik I. N. , Nenes A.
Published: April 2010

Abstract. Dust and black carbon aerosol have long been known to exert potentially important and diverse impacts on cloud droplet formation. Most studies to date focus on the soluble fraction of these particles, and overlook interactions of the insoluble fraction with water vapor (even if known to be hydrophilic). To address this gap, we developed a new parameterization that considers cloud droplet formation within an ascending air parcel containing insoluble (but wettable) particles externally mixed with aerosol containing an appreciable soluble fraction. Activation of particles with a soluble fraction is described through well-established Köhler theory, while the activation of hydrophilic insoluble particles is treated by "adsorption-activation" theory. In the latter, water vapor is adsorbed onto insoluble particles, the activity of which is described by a multilayer Frenkel-Halsey-Hill (FHH) adsorption isotherm modified to account for particle curvature. We further develop FHH activation theory to i) find combinations of the adsorption parameters AFHH, BFHH which yield atmospherically-relevant behavior, and, ii) express activation properties (critical supersaturation) that follow a simple power law with respect to dry particle diameter. The new parameterization is tested by comparing the parameterized cloud droplet number concentration against predictions with a detailed numerical cloud model, considering a wide range of particle populations, cloud updraft conditions, water vapor condensation coefficient and FHH adsorption isotherm characteristics. The agreement between parameterization and parcel model is excellent, with an average error of 10% and R2~0.98. A preliminary sensitivity study suggests that the sublinear response of droplet number to Köhler particle concentration is not as strong for FHH particles.
Aerosol hygroscopicity in the marine atmosphere: a closure study using high-time-resolution, multiple-RH DASH-SP and size-resolved C-ToF-AMS data
Authors: Hersey S. P. , Sorooshian A. , Murphy S. M. , Flagan R. C. , Seinfeld J. H.
Published: April 2010

Abstract. We have conducted the first airborne hygroscopic growth closure study to utilize data from an Aerodyne compact Time-of-Flight Aerosol Mass Spectrometer (C-ToF-AMS) coupled with size-resolved, multiple-RH, high-time-resolution hygroscopic growth factor (GF) measurements from the differential aerosol sizing and hygroscopicity spectrometer probe (DASH-SP). These data were collected off the coast of Central California during seven of the 16 flights carried out during the MASE-II field campaign in July 2007. Two of the seven flights were conducted in airmasses characterized by continental origin. These flights exhibited elevated organic volume fractions (VForganic=0.56±0.19, as opposed to 0.39±0.20 for all other flights), corresponding to significantly suppressed GFs at high RH (1.61±0.14 at 92% RH, as compared with 1.91±0.07 for all other flights), more moderate GF suppression at intermediate RH (1.53±0.10 at 85%, compared with 1.58±0.08 for all other flights), and no measurable GF suppression at low RH (1.31±0.06 at 74%, compared with 1.31±0.07 for all other flights). Organic loadings were slightly elevated in above-cloud aerosols, as compared with below-cloud aerosols, and corresponded to a similar trend of significantly suppressed GF at high RH, but more moderate impacts at lower values of RH. A hygroscopic closure based on a volume-weighted mixing rule provided good agreement with DASH-SP measurements (R2=0.78). Minimization of root mean square error between observations and predictions indicated mission-averaged organic GFs of 1.22, 1.45, and 1.48 at 74, 85, and 92% RH, respectively. These values agree with previously reported values for water-soluble organics such as dicarboxylic and multifunctional acids, and correspond to a highly oxidized, presumably water-soluble, organic fraction (mission-averaged O:C=0.92±0.33). Finally, a backward stepwise linear regression revealed that, other than RH, the most important predictor for GF is VForganic, indicating that a simple emperical model relating GF, RH, and the relative abundance of organic material can provide accurate predictions (R2=0.77) of hygroscopic growth for the California coast.
Technical note: a new method for the Lagrangian tracking of pollution plumes from source to receptor using gridded model output
Authors: Owen R. C. , Honrath R. E.
Published: April 2010

Abstract. Lagrangian particle dispersion models (LPDMs) are powerful and popular tools used for the analysis of atmospheric trace gas measurements. However, it can be difficult to determine the transport pathway of emissions from their source to a receptor using the standard gridded model output, particularly during complex meteorological scenarios. In this paper we present a method to clearly and easily identify the pathway taken by only those emissions that arrive at a receptor at a particular time, by combining the standard gridded output from forward (e.g., concentration) and backward (e.g., residence time) LPDM simulations. By comparing the pathway determined from this method with particle trajectories from both the forward and backward models, we show that this method successfully restores much of the Lagrangian information that is lost when the data are gridded. A sample analysis is presented, demonstrating that the source-to-receptor pathway determined from this method is more accurate and easier to use than existing methods using standard LPDM products (gridded fields of, e.g., concentrations and residence time). As demonstrated in an evaluation and an example application, the method requires agreement between the transport described by the forward and backward simulations and thus provides a means to assess the quality and reversibility of the simulation. Finally, we discuss the potential for combining the backward LPDM simulation with gridded data from other sources (e.g., chemical transport models) to obtain a Lagrangian sampling of the air that will eventually arrive at a receptor. Based on the advantages presented here, this new method can complement or even replace many of the standard uses of backward LPDM simulations.
Properties of aerosols and their wet deposition in the arctic spring during ASTAR2004 at Ny-Alesund, Svalbard
Authors: Yamagata S. , Kobayashi D. , Ohta S. , Murao N. , Shiobara M. , Wada M. , Yabuki M. , Konishi H. , Yamanouchi T.
Published: April 2010

Abstract. During the period of scientific campaign "Arctic Study of Tropospheric Aerosols, Clouds and Radiation 2004" (ASTAR2004), precipitation samples were collected in late spring at Ny-Alesund, Svalbard and their ionic components were analyzed in parallel with the measurement of properties of atmospheric aerosol particles at the same place. Backward trajectory analyses indicated that the air mass above the observatory initially dominated by air masses from the Arctic Ocean, then those from western Siberia and later those from Greenland and the Arctic Ocean. In the measurement period, six precipitation samples were obtained and five of them were analyzed their ionic components by ionchromatography. The concentrations of nss-sulphate in precipitations were between 1.8 and 24.6 ppm from which the scavenging ratio and scavenging coefficients were calculated using the data such as the concentrations of nss-sulphate in aerosol particles, amounts of precipitations, and the heights of precipitations obtained from radar echo data. The scavenging ratio ranged from 1.0×106 to 17×106 which are comparable values reported in other areas. A detailed comparison between precipitation events and the number concentration of aerosol particles obtained from optical particle counters suggests that the type of precipitations, i.e. rain or snow, significantly affects the number concentrations of aerosol particles.
Water vapour transport in the tropical tropopause region in coupled Chemistry-Climate Models and ERA-40 reanalysis data
Authors: Kremser Stefanie , Wohltmann Ingo , Rex Markus , Langematz Ulrike , Dameris Martin , Kunze Markus
Published: April 2010

Abstract. In this study backward trajectories from the tropical lower stratosphere were calculated for the Northern Hemisphere (NH) winters 1995–1996, 1997–1998 (El Niño) and 1998–1999 (La Niña) and summers 1996, 1997 and 1999 using both ERA-40 reanalysis data of the European Centre for Medium-Range Weather Forecast (ECMWF) and coupled Chemistry-Climate Model (CCM) data. The calculated trajectories were analysed to determine the distribution of points where individual air masses encounter the minimum temperature and thus minimum water vapour mixing ratio during their ascent through the tropical tropopause layer (TTL) into the stratosphere. The geographical distribution of these dehydration points and the local conditions there determine the overall water vapour entry into the stratosphere. Results of two CCMs are presented: the ECHAM4.L39(DLR)/CHEM (hereafter: E39/C) from the German Aerospace Center (DLR) and the Freie Universität Berlin Climate Middle Atmosphere Model with interactive chemistry (hereafter: FUB-CMAM-CHEM). In the FUB-CMAM-CHEM model the minimum temperatures are overestimated by about 9 K in NH winter and about 3 K in NH summer, resulting in too high water vapour entry values compared to ERA-40. However, the geographical distribution of dehydration points is fairly similar to ERA-40 for NH winter 1995–1996 and 1998–1999. The distribution of dehydration points in the boreal summer 1996 suggests an influence of the Indian monsoon upon the water vapour transport. The E39/C model displays a temperature bias of about +5 K. Hence, the minimum water vapour mixing ratios are higher relative to ERA-40. The geographical distribution of dehydration points is fairly well in NH winter 1995–1996 and 1997–1998 with respect to ERA-40. The distribution is not reproduced for the NH winter 1998–1999 (La Niña event) compared to ERA-40. There is an excessive water vapour flux through warm regions e.g. Africa in the NH winter and summer. The possible influence of the Indian monsoon on the transport is not seen in the boreal summer 1996. Further, the residence times of air parcels in the TTL were derived from the trajectory calculations. The analysis of the residence times reveals that in both CCMs residence times in the TTL are lower compared to ERA-40 and the seasonal variation is hardly present.
Studies of heterogeneous freezing by three different desert dust samples
Authors: Connolly P. J. , Möhler O. , Field P. R. , Saathoff H. , Burgess R. , Choularton T. , Gallagher M.
Published: April 2010

Abstract. We present results of experiments at the aerosol interactions and dynamics in the atmosphere (AIDA) chamber facility looking at the freezing of water by three different types of mineral particles at temperatures between −12°C and −33°C. The three different dusts are Asia Dust-1 (AD1), Sahara Dust-2 (SD2) and Arizona test Dust (ATD). The dust samples used had particle concentrations of sizes that were log-normally distributed with mode diameters between 0.3 and 0.5 μm and standard deviations, σg, of 1.6–1.9. The results from the freezing experiments are consistent with the singular hypothesis of ice nucleation. The dusts showed different nucleation abilities, with ATD showing a rather sharp increase in ice-active surface site density at temperatures less than −24°C. AD1 was the next most efficient freezing nuclei and showed a more gradual increase in activity than the ATD sample. SD2 was the least active freezing nuclei. We used data taken with particle counting probes to derive the ice-active surface site density forming on the dust as a function of temperature for each of the three samples and polynomial curves are fitted to this data. The curve fits are then used independently within a bin microphysical model to simulate the ice formation rates from the experiments in order to test the validity of parameterising the data with smooth curves. Good agreement is found between the measurements and the model for AD1 and SD2; however, the curve for ATD does not yield results that agree well with the observations. The reason for this is that more experiments between −20 and −24°C are needed to quantify the rather sharp increase in ice-active surface site density on ATD in this temperature regime. The curves presented can be used as parameterisations in atmospheric cloud models where cooling rates of approximately 1°C min−1 or more are present to predict the concentration of ice crystals forming by the condensation-freezing mode of ice nucleation. Finally a polynomial is fitted to all three samples together in order to have a parameterisation describing the average ice-active surface site density vs. temperature for an equal mixture of the three dust samples.
Introduction: European Integrated Project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) – integrating aerosol research from nano to global scales
Authors: Kulmala M. , Asmi A. , Lappalainen H. K. , Carslaw K. S. , Pöschl U. , Baltensperger U. , Hov Ø. , Brenquier J.-L. , Pandis S. N. , Facchini M. C. , Hansson H.-C. , Wiedensohler A. , O'Dowd C. D.
Published: April 2010

Abstract. The European Aerosol Cloud Climate and Air Quality Interactions project EUCAARI is an EU Research Framework 6 integrated project focusing on understanding the interactions of climate and air pollution. EUCAARI works in an integrative and multidisciplinary way from nano- to global scale. EUCAARI brings together several leading European research groups, state-of-the-art infrastructure and some key scientists from third countries to investigate the role of aerosol on climate and air quality. Altogether 48 partners from 25 countries are participating in EUCAARI. During the first 16 months EUCAARI has built operational systems, e.g. established pan-European measurement network for Lagrangian studies and four stations in developing countries. Also an improved understanding of nanoscale processes (like nucleation) has been implemented in global models. Here we present the research methods, organisation, operations and first results of EUCAARI.