bluuebunny/crossref_metadata_2025 huggingface dataset:
An improved criterion for new particle formation in diverse atmospheric environments
Authors: Kuang C. , Riipinen I. , Sihto S.-L. , Kulmala M. , McCormick A. V. , McMurry P. H.
Published: April 2010

Abstract. A dimensionless theory for new particle formation (NPF) was developed, using an aerosol population balance model incorporating recent developments in nucleation rates and measured particle growth rates. Based on this theoretical analysis, it was shown that a dimensionless parameter LΓ, characterizing the ratio of the particle scavenging loss rate to the particle growth rate, exclusively determined whether or not NPF would occur on a particular day. This parameter determines the probability that a nucleated particle will grow to a detectable size before being lost by coagulation with the pre-existing aerosol. Cluster-cluster coagulation was shown to contribute negligibly to this survival probability under conditions pertinent to the atmosphere. Data acquired during intensive measurement campaigns in Tecamac (MILAGRO), Atlanta (ANARChE), Boulder, and Hyytiälä (QUEST II, QUEST IV, and EUCAARI) were used to test the validity of LΓ as an NPF criterion. Measurements included aerosol size distributions down to 3 nm and gas-phase sulfuric acid concentrations. The model was applied to seventy-seven NPF events and nineteen non-events (characterized by growth of pre-existing aerosol without NPF) measured in diverse environments with broad ranges in sulfuric acid concentrations, ultrafine number concentrations, aerosol surface areas, and particle growth rates (nearly two orders of magnitude). Across this diverse data set, a nominal value of LΓ=0.7 was found to determine the boundary for the occurrence of NPF, with NPF occurring when LΓ<0.7 and being suppressed when LΓ> 0.7. Moreover, nearly 45% of measured LΓ values associated with NPF fell in the relatively narrow range of 0.1<LΓ<0.3.
Historical (1850–2000) gridded anthropogenic and biomass burning emissions of reactive gases and aerosols: methodology and application
Authors: Lamarque J.-F. , Bond T. C. , Eyring V. , Granier C. , Heil A. , Klimont Z. , Lee D. , Liousse C. , Mieville A. , Owen B. , Schultz M. G. , Shindell D. , Smith S. J. , Stehfest E. , Van Aardenne J. , Cooper O. R. , Kainuma M. , Mahowald N. , McConnell J. R. , Naik V. , Riahi K. , van Vuuren D. P.
Published: April 2010

Abstract. We present and discuss a new dataset of gridded emissions covering the historical period (1850–2000) in decadal increments at a horizontal resolution of 0.5° in latitude and longitude. The primary purpose of this inventory is to provide consistent gridded emissions of reactive gases and aerosols for use in chemistry model simulations needed by climate models for the Climate Model Intercomparison Program #5 (CMIP5) in support of the Intergovernmental Panel on Climate Change (IPCC) Fifth Assessment Report (AR5). Our best estimate for the year 2000 inventory represents a combination of existing regional and global inventories to capture the best information available at this point; 40 regions and 12 sectors are used to combine the various sources. The historical reconstruction of each emitted compound, for each region and sector, is then forced to agree with our 2000 estimate, ensuring continuity between past and 2000 emissions. Simulations from two chemistry-climate models is used to test the ability of the emission dataset described here to capture long-term changes in atmospheric ozone, carbon monoxide and aerosol distributions. The simulated long-term change in the Northern mid-latitudes surface and mid-troposphere ozone is not quite as rapid as observed. However, stations outside this latitude band show much better agreement in both present-day and long-term trend. The model simulations indicate that the concentration of carbon monoxide is underestimated at the Mace Head station; however, the long-term trend over the limited observational period seems to be reasonably well captured. The simulated sulfate and black carbon deposition over Greenland is in very good agreement with the ice-core observations spanning the simulation period. Finally, aerosol optical depth and additional aerosol diagnostics are shown to be in good agreement with previously published estimates and observations.
Remote sensing of the tropical rain forest boundary layer using pulsed Doppler lidar
Authors: Pearson G. , Davies F. , Collier C.
Published: April 2010

Abstract. Within the framework of the Natural Environment Research Council (NERC) Oxidant and Particle Photochemical Processes (OP3) project, a pulsed Doppler lidar was deployed for a 3 month period in the tropical rain forest of Borneo to remotely monitor vertical and horizontal transport, aerosol distributions and clouds in the lower levels of the atmosphere. These data are presented with a view to elucidating the scales and structures of the transport processes, which effect the chemical and particulate concentrations in and above the forest canopy, for applications in the parameterisation of climate models. Analysis of the clear-air vertical velocity data set is shown to enable direct characterisation of the diurnal variations in the boundary layer mixing processes.
Chemically aged and mixed aerosols over the Central Atlantic Ocean – potential impacts
Authors: Astitha M. , Kallos G. , Spyrou C. , O'Hirok W. , Lelieveld J. , Denier van der Gon H. A. C.
Published: April 2010

Abstract. Detailed information on the chemical and physical properties of aerosols is important for assessing their role in air quality and climate. This work explores the origin and fate of continental aerosols transported over the Central Atlantic Ocean, in terms of chemical composition, number and size distribution, using chemistry-transport models, satellite data and in situ measurements. We focus on August 2005, a period with intense hurricane and tropical storm activity over the Atlantic Ocean. A mixture of anthropogenic (sulphates, nitrates), natural (desert dust, sea salt) and chemically aged (sulphate and nitrate on dust) aerosols is found entering the hurricane genesis region, most likely interacting with clouds in the area. Results from our modelling study suggest rather small amounts of accumulation mode desert dust, sea salt and chemically aged dust aerosols in this Atlantic Ocean region. Aerosols of smaller size (Aitken mode) are more abundant in the area and in some occasions sulphates of anthropogenic origin and desert dust are of the same magnitude in terms of number concentrations. Typical aerosol number concentrations are derived for the vertical layers near shallow cloud formation regimes, designating that the aerosol number concentration can reach several thousand particles per cubic centimetre. The vertical distribution of the aerosols indicates that the desert dust particles are often transported near the top of the marine cloud layer as they enter into the region where deep convection is initiated. The anthropogenic sulphate aerosol can be transported within a thick layer and enter the cloud deck through multiple ways (from the top, the base of the cloud and entrainment). The sodium (sea salt related) aerosol is mostly found below the cloud base. The results of this work may provide insights relevant for studies that consider aerosol influences on cloud processes and storm development in the Central Atlantic region.
Inter-comparison of source apportionment models for the estimation of wood burning aerosols during wintertime in an Alpine city (Grenoble, France)
Authors: Favez O. , El Haddad I. , Piot C. , Boréave A. , Abidi E. , Marchand N. , Jaffrezo J.-L. , Besombes J.-L. , Personnaz M.-B. , Sciare J. , Wortham H. , George C. , D'Anna B.
Published: April 2010

Abstract. The emission of organic aerosols (OA) in the ambient air by residential wood burning is nowadays a subject of great scientific concern and a growing number of studies aim at apportioning the influence of such emissions on urban air quality. In the present study, results obtained using two commonly-used source apportionment models, i.e., Chemical Mass Balance (CMB, performed with off-line filter measurements) and Positive Matrix Factorization (PMF, applied to aerosol mass spectrometer measurements), as well as using the recently-proposed aethalometer model (based on the measurement of the aerosol light absorption at different wavelengths) are inter-compared. This work is performed using field data obtained during the winter season (14 to 30 January 2009) at an urban background site of a French Alpine city (Grenoble). Converging results from the different models indicate a major contribution of wood burning organic aerosols (OMwb) to the organic fraction, with mean OMwb contributions to total OA of about 67%, 60% and 38% for the CMB, the aethalometer and the AMS-PMF models, respectively. Quantitative discrepancies might notably be due to the overestimation of OMwb calculated by the CMB due to the loss of semi-volatile compounds from sources to receptor site, as well as to the accounting of oxidized primary wood burning organic (OPOAwb) aerosols within the Oxygenated Organic Aerosol (OOA) PMF-factor. This OOA factor accounts on average for about 50% of total OM, while non-combustion sources contribute to about 25% and 28% of total OM according to the CMB and aethalometer models, respectively. Each model suggests a mean contribution of fossil fuel emissions to total OM of about 10%. A good agreement is also obtained for the source apportionment of elemental carbon (EC) by both the CMB and aethalometer models, with fossil fuel emissions representing on average more than 80% of total EC.
Short-term variation in near-highway air pollutant gradients on a winter morning
Authors: Durant J. L. , Ash C. A. , Wood E. C. , Herndon S. C. , Jayne J. T. , Knighton W. B. , Canagaratna M. R. , Trull J. B. , Brugge D. , Zamore W. , Kolb C. E.
Published: April 2010

Abstract. Quantification of exposure to traffic-related air pollutants near highways is hampered by incomplete knowledge of the scales of temporal variation of pollutant gradients. The goal of this study was to characterize short-term temporal variation of vehicular pollutant gradients within 200–400 m of a major highway (>150 000 vehicles/d). Monitoring was done near Interstate 93 in Somerville (Massachusetts) from 06:00 to 11:00 on 16 January 2008 using a mobile monitoring platform equipped with instruments that measured ultrafine and fine particles (6–1000 nm, particle number concentration (PNC)); particle-phase (>30 nm) NO3−, SO42−, and organic compounds; volatile organic compounds (VOCs); and CO2, NO, NO2, and O3. We observed rapid changes in pollutant gradients due to variations in highway traffic flow rate, wind speed, and surface boundary layer height. Before sunrise and peak traffic flow rates, downwind concentrations of particles, CO2, NO, and NO2 were highest within 100-250 m of the highway. After sunrise pollutant levels declined sharply (e.g., PNC and NO were more than halved) and the gradients became less pronounced as wind speed increased and the surface boundary layer rose allowing mixing with cleaner air aloft. The levels of aromatic VOCs and NO3−, SO42− and organic aerosols were generally low throughout the morning, and their spatial and temporal variations were less pronounced compared to PNC and NO. O3 levels increased throughout the morning due to mixing with O3-enriched air aloft and were generally lowest near the highway reflecting reaction with NO. There was little if any evolution in the size distribution of 6–225 nm particles with distance from the highway. These results suggest that to improve the accuracy of exposure estimates to near-highway pollutants, short-term (e.g., hourly) temporal variations in pollutant gradients must be measured to reflect changes in traffic patterns and local meteorology.
Nitrogen oxides in the boundary layer and free troposphere at the Mt. Bachelor Observatory
Authors: Reidmiller D. R. , Jaffe D. A. , Fischer E. V. , Finley B.
Published: April 2010

Abstract. Nitrogen oxide (NOx = NO + NO2) observations were made at the Mt. Bachelor Observatory in central Oregon, USA (MBO; 2.73 km above sea level) during one autumn and three springtime (15 April–20 May) periods. This is the first study to discuss interannual variability in NOx for this region. NOx concentrations (mean ±1σ) for spring 2007, 2008 and 2009 were 119±65, 117±65, and 91±54 pptv, respectively. The difference in mean mixing ratios between 2007 and 2008 is not statistically significant, whereas the difference between these years and 2009 is significant (p<0.01). We attribute the decline in NOx from 2007–2008 to 2009 to changes in free tropospheric synoptic conditions over the Northeast Pacific and trans-Pacific transport pathways during spring 2009. In 2009, there were: (1) higher geopotential heights over the Gulf of Alaska, (2) warmer temperatures over the Aleutian Islands/Gulf of Alaska and (3) much weaker winds throughout the North Pacific. During the autumn 2008 campaign, NOx concentrations (mean ±1σ) were 175±548 pptv. The highly non-normal distribution of data (skewness coefficient of 19.1 vs. 2.5, 2.8 and 2.4 in spring 2007, 2008 and 2009, respectively) resulted from periods of very high NOx levels. Using MODIS Rapid Response (Aqua and Terra) results, we show that during autumn our site can be heavily influenced by wildfires in western North America. This is in contrast to springtime, when the smaller positive (i.e., right) tail of the NOx distribution is driven largely by Asian long-range transport (ALRT) events. We developed a novel means of segregating boundary layer (BL)-influenced vs. free tropospheric (FT) air. During spring 2008 we collected "chairlift soundings" of temperature, relative humidity and pressure in an effort to better understand the diurnal pattern of a BL influence at our summit station. Results from this experiment revealed that, on average, a BL influence begins around 10:00 PDT (UTC – 7 h) in spring. Using this information to isolate FT air, we characterize probable pollution sources and synoptic conditions for the top 20 FT NOx events over three spring campaigns. Half (n = 10) of these 20 events were determined to be "Imported" events characterized by anomalously: (1) high geopotential heights off the west coast of North America, (2) warm temperatures stretching from the Aleutian Islands to Baja California, and (3) strong southwesterly winds in the Asian outflow region. Five events exhibited an influence from the North American continent. These events are characterized by very strong cyclonic behavior off the northwestern USA coast.
Impacts of mechanistic changes on HOx formation and recycling in the oxidation of isoprene
Authors: Archibald A. T. , Cooke M. C. , Utembe S. R. , Shallcross D. E. , Derwent R. G. , Jenkin M. E.
Published: April 2010

Abstract. Recently reported model-measurement discrepancies for the concentrations of the HOx radical species (OH and HO2) in locations characterized by high emission rates of isoprene have indicated possible deficiencies in the representation of OH recycling and formation in isoprene mechanisms currently employed in numerical models; particularly at low levels of NOx. Using version 3.1 of the Master Chemical Mechanism (MCM v3.1) as a base mechanism, the sensitivity of the system to a number of detailed mechanistic changes is examined for a wide range of NOx levels, using a simple box model. These studies place emphasis on processes for which experimental or theoretical evidence has been reported in the peer-reviewed literature, in addition to examining the impact of an intrinsic simplification in the MCM v3.1 chemistry. Although all the considered mechanistic changes lead to simulated increases in the concentrations of OH at low NOx levels, the greatest impact is achieved by implementation of a recently postulated mechanism involving isomerisation of the δ-hydroxyalkenyl peroxy radical isomers, formed from the sequential addition of OH and O2 to isoprene. In conjunction with necessary rapid photolysis of the resultant hydroperoxyaldehyde products, this mechanism yields approximately a factor of three increase in the simulated OH concentration at low NOx, and is the only considered mechanism which achieves enhancements which approach those necessary to explain the reported model-measurement discrepancies. Combination of all the considered mechanistic changes has an effect which is approximately additive, yielding an overall enhancement of about a factor of 3.2 in the simulated OH concentration at the lowest NOx input rate considered, with the simulated mean NOx mixing ratios at this input rate being 42 ppt and 29 ppt with the base case and modified mechanisms respectively. A parameterized representation of the mechanistic changes is optimized and implemented into a reduced variant of the Common Representative Intermediates mechanism (CRI v2-R5), for use in the STOCHEM global chemistry-transport model. The impacts of the modified chemistry in the global model are shown to be consistent with those observed in the box model sensitivity studies, and the results are illustrated and discussed with a particular focus on the tropical forested regions of the Amazon and Borneo where unexpectedly elevated concentrations of OH have recently been reported.
Sensitivity tests for an ensemble Kalman filter for aerosol assimilation
Authors: Schutgens N. A. J. , Miyoshi T. , Takemura T. , Nakajima T.
Published: April 2010

Abstract. We present sensitivity tests for a global aerosol assimilation system utilizing AERONET observations of AOT (aerosol optical thickness) and AAE (aerosol Ångström exponent). The assimilation system employs an ensemble Kalman filter which requires optimization of three numerical parameters: ensemble size nens, local patch size npatch and inflation factor ρ. In addition, experiments are performed to test the impact of various implementations of the system. For instance, we use a different prescription of the emission ensemble or a different combination of observations. The various experiments are compared against one-another and against independent AERONET andMODIS/Aqua observations. The assimilation leads to significant improvements in modelled AOT and AAE fields. Moreover remaining errors are mostly random while they are mostly systematic for an experiment without assimilation. In addition, these results do not depend much on our parameter or design choices. It appears that the value of the local patch size has by far the biggest impact on the assimilation, which has sufficiently converged for an ensemble size of nens=20. Assimilating AOT and AAE is clearly preferential to assimilating AOT at two different wavelengths. In contrast, initial conditions or a description of aerosol beyond two modes (coarse and fine) have only little effect. We also discuss the use of the ensemble spread as an error estimate of the analysed AOT and AAE fields. We show that a very common prescription of the emission ensemble (independent random modification in each grid cell) can have trouble generating sufficient spread in the forecast ensemble.
The challenge of improving visibility in Beijing
Authors: Zhang Q. , Zhang J. , Xue H.
Published: April 2010

Abstract. The "Blue Sky Project" was proposed in 1998 to investigate by how much emissions should be reduced to increase blue sky frequency in Beijing, which hosted the Summer Olympics in 2008. This paper focuses on the temporal variation of visibility and its dependence on meteorological conditions and suspended particles at Beijing using the hourly observed visibility data in Beijing Capital International Airport (BCIA) from 1999 to 2007. It has been found that about 47.8% (24.2%) of the hours in Beijing are "bad" ("good") hours with visibility below 10 km (equal or higher than 20 km) between 1999 and 2007. Due to the high Relative Humidity (RH), summer is the season with the lowest mean visibility in a year. Although PM10 index was reported in a decreasing trend, the increase of RH has resulted in a decreasing trend of visibility over BCIA in the summer from 1999 to 2007. To ensure blue sky ("good" visibility) for Olympics 2008, daily mean PM10 index should be reduced to 44 from 86.5. This requires that not only vehicle emissions, but also other emissions should be limited. Observations during Olympics 2008 verify that blue-sky-hour rate has been increased significantly after mean PM10 index was reduced to 56, however, the visibility during the same period of 2009 has returned to the mean standard before 2008.
Aerosol effects on deep convective clouds: impact of changes in aerosol size distribution and aerosol activation parameterization
Authors: Ekman A. M. L. , Engström A. , Söderberg A.
Published: April 2010

Abstract. A cloud-resolving model including explicit aerosol physics and chemistry is used to study the impact of aerosols on deep convective strength. More specifically, by conducting six sensitivity series we examine how the complexity of the aerosol model, the size of the aerosols and the aerosol activation parameterization influence the aerosol-induced deep convective cloud sensitivity. Only aerosol effects on liquid droplet formation are considered. We find that an increased aerosol concentration generally results in stronger convection, which for the simulated case is in agreement with the conceptual model presented by Rosenfeld et al. (2008). However, there are two sensitivity series that do not display a monotonic increase in updraft velocity with increasing aerosol concentration. These exceptions illustrate the need to: 1) account for changes in evaporation processes and subsequent cooling when assessing aerosol effects on deep convective strength, 2) better understand graupel impaction scavenging of aerosols which may limit the number of CCN at a critical stage of cloud development and thereby dampen the convection, 3) increase our knowledge of aerosol recycling due to evaporation of cloud droplets. Furthermore, we find a significant difference in the aerosol-induced deep convective cloud sensitivity when using different complexities of the aerosol model and different aerosol activation parameterizations. For the simulated case, a 100% increase in aerosol concentration results in a difference in average updraft between the various sensitivity series which is as large as the average updraft increase itself. The model simulations also show that the change in graupel and rain formation is not necessarily directly proportional to the change in updraft velocity. For example, several of the sensitivity series display a decrease of the rain amount at the lowest model level with increasing updraft velocity. Finally, an increased number of aerosols in the Aitken mode (here defined by 23 nm≤d≤100.0 nm) may result in a larger impact on the convective strength compared to an increased number of aerosols in the accumulation mode (here defined by 100 nm≤d≤900.0 nm). When accumulation mode aerosols are activated and grow at the beginning of the cloud cycle, the supersaturation near the cloud base is lowered which to some extent limits further aerosol activation.
Laboratory study on new particle formation from the reaction OH + SO2: influence of experimental conditions, H2O vapour, NH3 and the amine tert-butylamine on the overall process
Authors: Berndt T. , Stratmann F. , Sipilä M. , Vanhanen J. , Petäjä T. , Mikkilä J. , Grüner A. , Spindler G. , Lee Mauldin III R. , Curtius J. , Kulmala M. , Heintzenberg J.
Published: April 2010

Abstract. Nucleation experiments starting from the reaction of OH radicals with SO2 have been performed in the IfT-LFT flow tube under atmospheric conditions at 293±0.5 K for a relative humidity of 13–61%. The presence of different additives (H2, CO, 1,3,5-trimethylbenzene) for adjusting the OH radical concentration and resulting OH levels in the range (4–300)·105 molecule cm−3 did not influence the nucleation process itself. The number of detected particles as well as the threshold H2SO4 concentration needed for nucleation was found to be strongly dependent on the counting efficiency of the used counting devices. High-sensitivity particle counters allowed the measurement of freshly nucleated particles with diameters down to about 1.5 nm. A parameterization of the experimental data was developed using power law equations for H2SO4 and H2O vapour. The exponent for H2SO4 from different measurement series was in the range of 1.7–2.1 being in good agreement with those arising from analysis of nucleation events in the atmosphere. For increasing relative humidity, an increase of the particle number was observed. The exponent for H2O vapour was found to be 3.1 representing a first estimate. Addition of 1.2·1011 molecule cm−3 or 1.2·1012 molecule cm−3 of NH3 (range of atmospheric NH3 peak concentrations) revealed that NH3 has a measureable, promoting effect on the nucleation rate under these conditions. The promoting effect was found to be more pronounced for relatively dry conditions. NH3 showed a contribution to particle growth. Adding the amine tert-butylamine instead of NH3, the enhancing impact for nucleation and particle growth appears to be stronger.
A closer look at Arctic ozone loss and polar stratospheric clouds
Authors: Harris N. R. P. , Lehmann R. , Rex M. , von der Gathen P.
Published: April 2010

Abstract. The empirical relationship found between column-integrated Arctic ozone loss and the volume of polar stratospheric clouds inferred from meteorological analyses is updated and examined in more detail. The relationship is found to hold at different altitudes as well as in the column. Analysis of the photochemistry leading to the ozone loss shows that the early winter activation is limited by the photolysis of nitric acid. This step produces nitrogen dioxide which is converted to chlorine nitrate which in turn reacts with hydrogen chloride on any polar stratospheric clouds to form active chlorine. The rate-limiting step is the photolysis of nitric acid: this occurs at the same rate every year and so the interannual variation in the ozone loss is caused by the extent and persistence of the polar stratospheric clouds. In early spring the ozone loss rate increases as the solar insolation increases the photolysis of the chlorine monoxide dimer. However the length of the ozone loss period is determined by the photolysis of nitric acid which also occurs in the near ultraviolet. As a result of these compensating effects, the amount of the ozone loss is principally limited by the extent of original activation rather than its timing. In addition a number of factors, including the vertical changes in pressure and total inorganic chlorine as well as denitrification and renitrification, offset each other. As a result the extent of original activation is the most important factor influencing ozone loss. These results indicate that relatively simple parameterisations of Arctic ozone loss could be developed for use in coupled chemistry climate models.
GOMOS data characterization and error estimation
Authors: Tamminen J. , Kyrölä E. , Sofieva V. F. , Laine M. , Bertaux J.-L. , Hauchecorne A. , Dalaudier F. , Fussen D. , Vanhellemont F. , Fanton-d'Andon O. , Barrot G. , Mangin A. , Guirlet M. , Blanot L. , Fehr T. , Saavedra de Miguel L. , Fraisse R.
Published: April 2010

Abstract. The Global Ozone Monitoring by Occultation of Stars (GOMOS) instrument uses stellar occultation technique for monitoring ozone and other trace gases in the stratosphere and mesosphere. The self-calibrating measurement principle of GOMOS together with a relatively simple data retrieval where only minimal use of a priori data is required, provides excellent possibilities for long term monitoring of atmospheric composition. GOMOS uses about 180 brightest stars as the light source. Depending on the individual spectral characteristics of the stars, the signal-to-noise ratio of GOMOS is changing from star to star, resulting also varying accuracy to the retrieved profiles. We present the overview of the GOMOS data characterization and error estimation, including modeling errors, for ozone, NO2, NO3 and aerosol profiles. The retrieval error (precision) of the night time measurements in the stratosphere is typically 0.5–4% for ozone, about 10–20% for NO2, 20–40% for NO3 and 2–50% for aerosols. Mesospheric O3, up to 100 km, can be measured with 2–10% precision. The main sources of the modeling error are the incompletely corrected atmospheric turbulence causing scintillation, inaccurate aerosol modeling, uncertainties in cross sections of the trace gases and in the atmospheric temperature. The sampling resolution of GOMOS varies depending on the measurement geometry. In the data inversion a Tikhonov-type regularization with pre-defined target resolution requirement is applied leading to 2–3 km resolution for ozone and 4 km resolution for other trace gases.
HULIS in emissions of fresh rice straw burning and in ambient aerosols in the pearl river delta region, China
Authors: Lin P. , Engling G. , Yu J. Z.
Published: April 2010

Abstract. HUmic-LIke Substances (HULIS) are an abundant unresolved mixture of organic compounds present in atmospheric samples. Biomass burning (BB) has been recognized as an important primary source of HULIS, but measurements of HULIS in various fresh BB particles are lacking. In this work, HULIS in emissions of rice straw burning in a number of field and chamber experiments was measured. The HULIS/OC ratio was 0.34±0.05 in μg/μgC, showing small variance among emissions under different burning conditions. The influence of BB on ambient HULIS levels was investigated by examining the spatial and temporal variation of HULIS and other aerosol constituents and interspecies relations in ambient PM2.5 collected at an urban and a suburban location in the Pearl River Delta (PRD), China over a period of one year. The HULIS concentrations in the ambient PM2.5 were significantly higher in air masses originating from regions influenced by BB. Significant correlations between HULIS and water-soluble K+ concentrations at both sites further support that BB was an important source of HULIS. HULIS also correlated well with sulfate, oxalate, and oxidant (the sum of O3 and NO2). The HULIS/OC ratios in BB-influenced ambient aerosols (~0.6) were much higher than those in the fresh BB emissions (0.34), implying that secondary formation was also an important source of HULIS in the atmosphere. The annual average HULIS concentrations were 4.9 μg m−3 at the urban site and 7.1 μg m−3 at the suburban site while the annual average concentrations of elemental carbon were 3.3 μg m−3 and 2.4 μg m−3, respectively. The urban-suburban spatial gradient of HULIS was opposite to that of elemental carbon, negating vehicular emissions as a significant source of HULIS.
Combining visible and infrared radiometry and lidar data to test ice clouds optical properties
Authors: Bozzo A. , Maestri T. , Rizzi R.
Published: April 2010

Abstract. Measurements taken during the 2003 Pacific THORPEX Observing System Test (P-TOST) by the MODIS Airborne Simulator (MAS), the Scanning High-resolution Interferometer Sounder (S-HIS) and the Cloud Physics Lidar (CPL) are compared to simulations performed with a line-by-line and multiple scattering modeling methodology (LBLMS). Formerly used for infrared hyper-spectral data analysis, LBLMS has been extended to the visible and near infrared with the inclusion of surface bi-directional reflectance properties. A number of scenes are evaluated: two clear scenes, one with nadir geometry and one cross-track encompassing sun glint, and three cloudy scenes, all with nadir geometry. CPL data is used to estimate the particulate optical depth at 532 nm for the clear and cloudy scenes. Cloud optical depth is also retrieved from S-HIS infrared window radiances, and it agrees with CPL values, to within natural variability. MAS data are simulated convolving high resolution radiances. The paper discusses the results of the comparisons for the clear cases and for the three cloudy cases. LBLMS clear simulations agree with MAS data to within 20% in the shortwave (SW) and near infrared (NIR) spectrum and within 2 K in the infrared (IR) range. It is shown that cloudy sky simulations using cloud parameters retrieved from IR radiances systematically underestimate the measured radiance in the SW and NIR by nearly 50%, although the IR retrieved optical thickness agree with same measured by CPL. MODIS radiances measured from Terra are also compared to LBLMS simulations in cloudy conditions using retrieved cloud optical depth and effective radius from MODIS, to understand the origin for the observed discrepancies. It is shown that the simulations agree, to within natural variability, with measurements in selected MODIS SW bands. The paper dwells on a possible explanation of these contraddictory results, involving the phase function of ice particles in the shortwave.
Black carbon absorption effects on cloud cover, review and synthesis
Authors: Koch D. , Del Genio A.
Published: April 2010

Abstract. Absorbing aerosols (AA's) such as black carbon (BC) or dust absorb incoming solar radiation, perturb the temperature structure of the atmosphere, and influence cloud cover. Previous studies have described conditions where AA's either increase or decrease cloud cover. The effect depends on several factors, including the altitude of the AA relative to the cloud and on the cloud type. Cloud cover is decreased if the AA's are embedded in the cloud layer. AA's below cloud may enhance convection and cloud cover. AA's over cloud-level stabilize the underlying layer and tend to enhance stratocumulus clouds but may reduce cumulus clouds. AA's can also promote cloud cover in convergent regions as they enhance deep convection and low level convergence as it draws in moisture from ocean to land regions. Most global model studies indicate a regional variation in the cloud response but generally increased cloud cover over oceans and some land regions, with net increased low-level and/or reduced upper level cloud cover. The result is net negative radiative forcing from cloud response to AA's. In some of these climate model studies, the cooling effect of BC due to cloud changes was strong enough to essentially cancel the warming direct effects.
Long-term record of aerosol optical properties and chemical composition from a high-altitude site (Manora Peak) in Central Himalaya
Authors: Ram K. , Sarin M. M. , Hegde P.
Published: April 2010

Abstract. This MS reports on a long-term study of aerosol optical properties and chemical composition, conducted during February 2005–July 2008, from a high-altitude site (Manora Peak, ~2000 m a.s.l.) in the central Himalaya. The chemical analyses suggest that, on average, total carbonaceous aerosols (TCA) and water-soluble inorganic species (WSIS) contribute nearly 25% and 10% of the total suspended particulate (TSP) mass, respectively. Both, TSP and aerosol optical depth (AOD) exhibit significant increase during summer months, with simultaneous increase in the abundance of mineral dust under the prevailing south-westerly winds and long-range transport from desert regions (from middle-East and Thar Desert in western India). The temporal variability in the abundance pattern of carbonaceous species (EC, OC) is also significantly pronounced, with lower concentrations occurring during summertime (April–June) and monsoon (July–August) and relatively high during post-monsoon (September–November) and wintertime (December–March). The WSOC/OC ratios (range: 0.32 to 0.83) during summer and post-monsoon suggest significant contribution from secondary organic aerosols. The mass fraction of absorbing EC (elemental carbon) ranges from less than a percent (during summer and monsoon) to as high as 7.6% (during winter) and absorption coefficient (babs, at 678 nm) varied as 0.9–33.9 Mm−1 (1 Mm−1=10−6 m−1). The linear regression analysis between (babs and EC concentration (μgC m−3) yields a slope of 12.2(±2.3) m2 g−1, referred as mass absorption efficiency (σabs) of EC. However, temporal data suggests lower σabs values during winter and higher in summer and post-monsoon. The change in the mixing state of aerosols and/or variability in the emission sources could be a plausible reason for the variability in σabs at this high-altitude site (Manora Peak).
Optical closure experiments for biomass smoke aerosols
Authors: Mack L. E. , Levin E. J. T. , Kreidenweis S. M. , Obrist D. , Moosmüller H. , Lewis K. A. , Arnott W. P. , McMeeking G. R. , Sullivan A. P. , Wold C. E. , Hao W.-M. , Collett J. L. , Malm W. C.
Published: April 2010

Abstract. The FLAME experiments were a series of laboratory studies of the chemical, physical, and optical properties of fresh smokes from the combustion of wildland fuels that are burned annually in the western and southeastern US. The burns were conducted in the combustion chamber of the USFS Fire Sciences Laboratory in Missoula, Montana. Here we discuss the retrieval of optical properties for a variety of fuels burned in FLAME 2, using nephelometer-measured scattering coefficients, photoacoustically-measured aerosol absorption coefficients, and size distribution measurements. Uncertainties are estimated from the various instrument characteristics and from instrument calibration studies. Our estimates of single scattering albedo for different dry smokes varied from 0.43–0.99, indicative of the wide variations in smoke aerosol chemical composition that were observed. In selected case studies, we retrieved the complex refractive index from the measurements, but show that these are highly sensitive to the uncertainties in measured size distributions.
Feedback between dust particles and atmospheric processes over West Africa in March 2006 and June 2007
Authors: Stanelle T. , Vogel B. , Vogel H. , Bäumer D. , Kottmeier Ch.
Published: April 2010

Abstract. We used the comprehensive model system COSMO-ART to quantify the impact of mineral dust on the radiative fluxes, the temperature and the feedback between dust particles and their emissions. We simulated two dust storms over West Africa in March 2006 and in June 2007. Simulations with and without coupling of the actual dust concentration with the radiative fluxes and the thermodynamics were carried out for each case. The model results for the 2006 case were compared with observations of the AMMA campaign. At the surface the shortwave radiative effect of mineral dust can be described by a linear relation between the changes in net surface radiation and the aerosol optical depth. For an aerosol optical depth (AOD) at 450 nm of 1 the average shortwave radiation reduction amounts −130 W m−2 during noon. The longwave radiative effect of mineral dust is nonlinear, with an average increase of +70 W m−2 for an AOD (450 nm) of 1. At the top of the atmosphere the effect of the dust layer with an AOD of 1 on radiative fluxes is not as significant as at the surface. It is slightly positive for the shortwave and approximately 26 W m−2 for the longwave radiation. The height range and the extension of the dust layer determine the effect of dust particles on the 2 m temperature. When the dust layer is attached to the surface and lasts for several days it leads to an increase of the surface temperature even during daytime. In case of an elevated dust layer there is a decrease in 2 m temperature of up to 4 K during noon. It is shown, that the temperature changes caused by mineral dust may result in horizontal temperature gradients which also modify near surface winds. Since surface wind thresholds decide the uptake of dust from the surface, a feedback on total emission fluxes is established. The coupled model provides an increase in the total emission fluxes of dust particles by about 16% during the dust storm in March 2006 and 25% during the dust episode in June 2007.
Brown carbon and water-soluble organic aerosols over the southeastern United States
Authors: Hecobian A. , Zhang X. , Zheng M. , Frank N. , Edgerton E. S. , Weber R. J.
Published: April 2010

Abstract. Fine particle (PM2.5) light absorption characteristics of aqueous extracts over wavelengths of 250 to 700 nm were investigated based on two data sets; 24-h Federal Reference Method (FRM) filter extracts from 15 southeastern US monitoring sites over the year of 2007 (900 filters), and online measurements from a Particle-Into-Liquid Sampler deployed from July to mid-August 2009 in Atlanta, Georgia. Three main sources of soluble chromophores were identified, biomass burning, mobile source emissions, and compounds linked to Secondary Organic Aerosol (SOA) formation. Absorption spectra of aerosol solutions from different sources were similar. Angstrom exponents were ~7±1 for biomass burning and non-biomass burning-impacted samples (delineated by a levoglucosan concentration of 50 ng m−3) at both rural and urban sites. The absorption coefficient from measurements averaged between wavelength 360 and 370 nm (Abs365, in units m−1) was used as a measure of overall brown carbon absorptivity. Biomass-burning-impacted samples were highest during colder months and Abs365 was correlated with levoglucosan at all sites. During periods of little biomass burning in summer, light absorbing compounds were still ubiquitous and correlated with fine particle Water-Soluble Organic Carbon (WSOC), but comprised a much smaller fraction of the WSOC, where Abs365/WSOC (i.e., mass absorption efficiency) was typically ~3 times higher in biomass burning-impacted samples. Factor analysis attributed 50% of the yearly average Abs365 to biomass burning sources. Brown carbon from primary urban emissions (mobile sources) was also observed and accounted for ~10% of the regional yearly average Abs365. Summertime diurnal profiles of Abs365 and WSOC showed that morning to midday increases in WSOC from photochemical production were associated with a decrease in Abs365/WSOC. After noon this ratio substantially increased, indicating that either some fraction of the non-light absorbing fresh SOA was rapidly (within hours) converted to chromophores heterogeneously, or that SOA from gas-particle partitioning later in the day was more light-absorbing. Factor analysis associated ~20 to 30% of Abs365 over 2007 with a secondary source that was highest in summer and also the main source for oxalic acid, suggesting that aqueous phase reactions may account for the light-absorbing fraction of WSOC observed throughout the southeastern US in summer.
African biomass burning plumes over the Atlantic: aircraft based measurements and implications for H2SO4 and HNO3 mediated smoke particle activation
Authors: Fiedler V. , Arnold F. , Ludmann S. , Minikin A. , Pirjola L. , Dörnbrack A. , Schlager H.
Published: April 2010

Abstract. Airborne measurements of trace gases and aerosol particles have been made in two aged biomass burning (BB) plumes over the East Atlantic (Gulf of Guinea). The plumes originated from BB in the Southern Hemisphere African savanna belt. On the day of our measurements (13 August 2006), the plumes had ages of about 10 days and were respectively located in the middle troposphere (MT) at about 3000–5500 m altitude and in the upper troposphere (UT) at about 10 800–11 200 m. In the more polluted MT-plume, numerous measured trace species had markedly elevated abundances, particularly HNO3 (5000–8000 pmol/mol), SO2 (up to 1400 pmol/mol), and smoke particles with diameters larger than 250 nm (up to 2000 cm−3). Our MT-plume measurements indicate that SO2 released by BB had not experienced significant loss by deposition and cloud processes but rather had experienced OH-induced conversion to gas-phase sulfuric acid. By contrast, a large fraction of the released NOx had experienced loss, most likely as HNO3, by cloud processes and deposition. In the UT-plume, loss of NOy and SO2 by cloud processes and deposition was more pronounced compared to the MT-plume. Building on our measurements and accompanying model simulations, we have investigated trace gas transformations in the ageing and diluting plumes and their role in smoke particle processing and activation. Emphasis was placed upon the formation of sulfuric acid, nitric acid, and ammonium nitrate, and their influence on the activation potential of smoke particles. Our model simulations reveal that, after 13 August, the lower plume traveled across the Atlantic and descended to 1300 m and hereafter ascended again. During the travel across the Atlantic, the smoke particle mean diameter and sulfuric acid mass fraction increased sufficiently to allow the processed smoke particles to act as water vapor condensation nuclei already at very low water vapor supersaturations of only about 0.04%. Thereby, aged smoke particles had developed a potential to act as water vapor condensation nuclei in the formation of maritime clouds, including not only cumulus but even stratiform clouds.
Novel method of generation of Ca(HCO3)2 and CaCO3 aerosols and first determination of hygroscopic and cloud condensation nuclei activation properties
Authors: Zhao D. F. , Buchholz A. , Mentel Th. F. , Müller K.-P. , Borchardt J. , Kiendler-Scharr A. , Spindler C. , Tillmann R. , Trimborn A. , Zhu T. , Wahner A.
Published: April 2010

Abstract. Atmospheric mineral aerosols contain CaCO3 as a reactive component. A novel method to produce CaCO3 aerosol was developed by spraying Ca(HCO3)2 solutions, which were generated from CaCO3 suspensions and CO2. By aerosol mass spectrometry the freshly sprayed aerosol was characterized to be Ca(HCO3)2 which under annealing in a tube furnace transformed into CaCO3. Transmission Electron Microscopy demonstrated that the particles produced were spherical. The method is easy to operate and was able to generate aerosol of sufficient concentration and proper size for the study of physiochemical properties as was demonstrated for hygroscopicity and CCN activity measurements, and investigations of heterogeneous reactions of mineral aerosol. Fresh Ca(HCO3)2 particles are somewhat more hygroscopic than CaCO3 particles although both have small growth factors of 1.03 and 1.01, respectively, at 95% relative humidity. The CCN activity of Ca(HCO3)2 aerosol is remarkably higher than that of CaCO3 aerosol and only slightly less than that of Ca(NO3)2. Experiments in the Large Jülich Aerosol Chamber showed that Ca(HCO3)2 can exist for several hours under dry atmospheric conditions which is in contrast to the current believe that Ca(HCO3)2 is unstable in the atmosphere. We conclude that Ca(HCO3)2 maybe be formed in the atmosphere in cloud droplets of activated mineral dust by reaction of CaCO3 with CO2 and H2O. The presence of Ca(HCO3)2 and as a consequence an enhanced CCN activity may alter the influence of mineral aerosol on global climate.