bluuebunny/crossref_metadata_2025 huggingface dataset:
Influence of meteorological variability on interannual variations of springtime boundary layer ozone over Japan during 1981–2005
Authors: Kurokawa J. , Ohara T. , Uno I. , Hayasaki M. , Tanimoto H.
Published: April 2010

Abstract. We investigated the influence of meteorological variability on the interannual variation of springtime boundary layer ozone over Japan during 1981–2005 by multiyear simulations with the Models-3 Community Multiscale Air Quality (CMAQ) modeling system and the Regional Emission Inventory in Asia (REAS). CMAQ/REAS generally reproduced the observed interannual variability of springtime ozone over Japan, showing year-to-year variations larger than the annual rate of increase of the long-term trend. We then analyzed the influence of the interannual variation of meteorology in simulated results by using the fixed emissions for 2000 and meteorological fields for each year. As a reference parameter, we calculated the area-weighted surface pressure anomaly over the Pacific Ocean east of Japan. When the anomaly has a large negative value, polluted air masses from continental Asia tend to be transported directly to Japan by westerly winds. In contrast, when the anomaly has a large positive value, influence of the outflow from continental Asia tends to be small because the westerly components of wind fields around Japan are comparatively weak. Instead, southerly winds are relatively strong and transport clean air masses from the Pacific Ocean to Japan. Consequently, springtime ozone over Japan is higher (lower) than in ordinary years when the anomaly has a large negative (positive) value. In general, the interannual variation of springtime ozone over Japan is sensitive to the outflow from continental Asia. We also found some correlation between springtime ozone over Japan and the El Niño-Southern Oscillation, indicating that higher and lower springtime ozone over Japan are related to La Niña and El Niño, respectively. Differences in the meridional displacement and diversity of cyclone tracks near Japan between El Niño and La Niña years may be responsible for interannual variations in the springtime boundary layer ozone over Japan.
Comparison of a global-climate model simulation to a cloud-system resolving model simulation for long-term thin stratocumulus clouds
Authors: Lee S. S. , Penner J. E. , Wang M.
Published: April 2010

Abstract. A case of thin, warm marine-boundary-layer (MBL) clouds is simulated by a cloud-system resolving model (CSRM) and is compared to the same case of clouds simulated by a general circulation model (GCM). In this study, the simulation by the CSRM adopts higher resolutions which are generally used in large-eddy simulations (LES) and more advanced microphysics as compared to those by the GCM, enabling the CSRM-simulation to act as a benchmark to assess the simulation by the GCM. Explicitly simulated interactions among the surface latent heat (LH) fluxes, buoyancy fluxes, and cloud-top entrainment lead to the deepening-warming decoupling and thereby the transition from stratiform clouds to cumulus clouds in the CSRM. However, in the simulation by the GCM, these interactions are not resolved and thus the transition to cumulus clouds is not simulated. This leads to substantial differences in liquid water content (LWC) and radiation between simulations by the CSRM and the GCM. When stratocumulus clouds are dominant prior to the transition to cumulus clouds, interactions between supersaturation and cloud droplet number concentration (CDNC) (controlling condensation) and those between rain evaporation and cloud-base instability (controlling cloud dynamics and thereby condensation) determine LWC and thus the radiation budget in the simulation by the CSRM. These interactions result in smaller condensation and thus smaller LWC and reflected solar radiation by clouds in the simulation by the CSRM than in the simulation by the GCM where these interactions are not resolved. The resolved interactions (associated with condensation and the transition to cumulus clouds) lead to better agreement between the CSRM-simulation and observation than that between the GCM-simulation and observation.
The formation of secondary organic aerosol from the isoprene + OH reaction in the absence of NOx
Authors: Kleindienst T. E. , Lewandowski M. , Offenberg J. H. , Jaoui M. , Edney E. O.
Published: April 2010

Abstract. The reaction of isoprene (C5H8) with hydroxyl radicals has been studied in the absence of nitrogen oxides (NOx) to determine physical and chemical characteristics of the secondary organic aerosol formed. Experiments were conducted using a smog chamber operated in a steady-state mode permitting measurements of moderately low aerosol levels. GC-MS analysis was conducted to measure methyl butenediols in the gas phase and polyols in the aerosol phase. Analyses were made to obtain several bulk aerosol parameters from the reaction including values for the organic mass to organic carbon ratio, the effective enthalpy of vaporization (ΔHvapeff), organic peroxide fraction, and the aerosol yield. The gas phase analysis showed the presence of methacrolein, methyl vinyl ketone, and four isomers of the methyl butenediols. These gas-phase compounds may serve as precursors for one or more of several compounds detected in the aerosol phase including 2-methylglyceric acid, three 2-methyl alkenetriols, and two 2-methyl tetrols. In contrast to most previous studies, the 2-methyl tetrols (and the 2-methyl alkenetriols) were found to form in the absence of acidic sulfate aerosol. However, reaction conditions did not favor the production of HO2 radicals, thus allowing RO2+RO2 reactions to proceed more readily than if higher HO2 levels had been generated. SOA/SOC (i.e. OM/OC) was found to average 1.9 in the absence of NOx. The effective enthalpy of vaporization was measured as 38.6 kJ mol−1, consistent with values used previously in modeling studies. The yields in this work (using an independent technique than used previously) are lower than those of Kroll et al. (2006) for similar aerosol masses. SOC yields reported in this work range from 0.5–1.4% for carbon masses between 17 and 49 μgC m−3.
The sensitivity of CO and aerosol transport to the temporal and vertical distribution of North American boreal fire emissions
Authors: Chen Y. , Li Q. , Randerson J. T. , Lyons E. A. , Kahn R. A. , Nelson D. L. , Diner D. J.
Published: April 2010

Abstract. Forest fires in Alaska and western Canada represent important sources of aerosols and trace gases in North America. Among the largest uncertainties when modeling forest fire effects are the timing and injection height of biomass burning emissions. Here we simulate CO and aerosols over North America during the 2004 fire season, using the GEOS-Chem chemical transport model. We apply different temporal distributions and injection height profiles to the biomass burning emissions, and compare model results with satellite-, aircraft-, and ground-based measurements. We find that averaged over the fire season, the use of finer temporal resolved biomass burning emissions usually decreases CO and aerosol concentrations near the fire source region, and often enhances long-range transport. Among the individual temporal constraints, switching from monthly to 8-day time intervals for emissions has the largest effect on CO and aerosol distributions, and shows better agreement with measured day-to-day variability. Injection height substantially modifies the surface concentrations and vertical profiles of pollutants near the source region. Compared with CO, the simulation of black carbon aerosol is more sensitive to the temporal and injection height distribution of emissions. The use of MISR-derived injection heights improves agreement with surface aerosol measurements near the fire source. Our results indicate that the discrepancies between model simulations and MOPITT CO measurements near the Hudson Bay can not be attributed solely to the representation of injection height within the model. Frequent occurrence of strong convection in North America during summer tends to limit the influence of injection height parameterizations of fire emissions in Alaska and western Canada with respect to CO and aerosol distributions over eastern North America.
Microphysical and optical properties of Arctic mixed-phase clouds. The 9 April 2007 case study.
Authors: Gayet J.-F. , Mioche G. , Dörnbrack A. , Ehrlich A. , Lampert A. , Wendisch M.
Published: April 2010

Abstract. Airborne measurements in Arctic boundary-layer stratocumulus were carried out near Spitsbergen on 9 April 2007 during the Arctic Study of Tropospheric Aerosol, Clouds and Radiation (ASTAR) campaign. A unique set of co-located observations is used to describe the cloud properties, including detailed in situ cloud microphysical and radiation measurements along with airborne and co-located spaceborne remote sensing data (CALIPSO lidar and CloudSat radar). CALIPSO profiles indicate cloud top levels at temperature between −24°C and −21°C. In situ measurements confirm that the cloud-top lidar attenuated backscatter signal along the aircraft trajectory is linked with the presence of liquid water, a common feature observed in Arctic mixed-phase stratocumulus clouds. A low concentration of large ice crystals is also observed up to the cloud top resulting in significant CloudSat radar echoes. Since the ratio of the extinction of liquid water droplets to ice crystals is high, broadband radiative effects near the cloud top are mostly dominated by water droplets. CloudSat observations and in situ measurements reveal high reflectivity factors (up to 15 dBZ) and precipitation rates (1 mm h−1). This feature results from efficient ice growth processes. About 25% of the theoretically available liquid water is converted into ice water with large precipitating ice crystals. Using an estimate of mean cloud cover, a considerable value of 106 m3 h−1 of fresh water could be settled over the Greenland sea pool. European Centre for Medium-Range Weather Forecast (ECMWF) operational analyses reproduces the boundary layer height variation along the flight track. However, small-scale features in the observed cloud field cannot be resolved by ECMWF analysis. Furthermore, ECMWF's diagnostic partitioning of the condensed water into ice and liquid reveals serious shortcomings for Arctic mixed-phased clouds. Too much ice is modelled.
Classifying previously undefined days from eleven years of aerosol-particle-size distribution data from the SMEAR II station, Hyytiälä, Finland
Authors: Buenrostro Mazon S. , Riipinen I. , Schultz D. M. , Valtanen M. , Dal Maso M. , Sogacheva L. , Junninen H. , Nieminen T. , Kerminen V.-M. , Kulmala M.
Published: April 2010

Abstract. Studies of secondary aerosol-particle formation depend on identifying days in which new particle formation occurs and, by comparing them to days with no signs of particle formation, identifying the conditions favourable for formation. Continuous aerosol size distribution data has been collected at the SMEAR II station in a boreal forest in Hyytiälä, Finland, since 1996, making it the longest time series of aerosol size distributions available worldwide. In previous studies, the data have been classified as particle-formation event, nonevent, and undefined days, with almost 40% of the dataset classified as undefined. In the present study, eleven years (1996–2006) of undefined days (1630 days) were reanalyzed and subdivided into three new classes: failed events (37% of all previously undefined days), ultrafine-mode concentration peaks (34%), and pollution-related concentration peaks (19%). Unclassified days (10%) comprised the rest of the previously undefined days. The failed events were further subdivided into tail events (21%), where a tail of a formation event presumed to be advected to Hyytiälä from elsewhere, and quasi events (16%) where new particles appeared at sizes 3–10 nm, but showed unclear growth, the mode persisted for less than an hour, or both. The ultrafine concentration peaks days were further subdivided into nucleation-mode peaks (24%) and Aitken-mode peaks (10%), depending on the size range where the particles occurred. The mean annual distribution of the failed events has a maximum during summer, whereas the two peak classes have maxima during winter. The summer minimum previously found in the seasonal distribution of event days partially offsets a summer maximum in failed-event days. Daily-mean relative humidity and condensation sink values are useful in discriminating the new classes from each other. Specifically, event days had low values of relative humidity and condensation sink relative to nonevent days. Failed-event days possessed intermediate condensation sink and relative humidity values, whereas both ultrafine-mode peaks and, to a greater extent, pollution-related peaks had high values of both, similar to nonevent days. Using 96-h back trajectories, particle-size concentrations were plotted as a function of time the trajectory spent over land. Increases in particle size and number concentration during failed-event days were similar to that during the later stages of event days, whereas the particle size and number concentration for both nonevent and peaks classes did not increase as fast as for event and failed events days.
Isoprene oxidation by nitrate radical: alkyl nitrate and secondary organic aerosol yields
Authors: Rollins A. W. , Kiendler-Scharr A. , Fry J. L. , Brauers T. , Brown S. S. , Dorn H.-P. , Dubé W. P. , Fuchs H. , Mensah A. , Mentel T. F. , Rohrer F. , Tillmann R. , Wegener R. , Wooldridge P. J. , Cohen R. C.
Published: April 2010

Abstract. Alkyl nitrates and secondary organic aerosol (SOA) produced during the oxidation of isoprene by nitrate radicals has been observed in the SAPHIR (Simulation of Atmospheric PHotochemistry In a large Reaction Chamber) chamber. A 16 h dark experiment was conducted with temperatures at 289–301 K, and maximum concentrations of 11 ppb isoprene, 62.4 ppb O3 and 31.1 ppb NOx. We find the yield of nitrates is 70±8% from the isoprene + NO3 reaction, and the yield for secondary dinitrates produced in the reaction of primary isoprene nitrates with NO3 is 40±20%. We find an effective rate constant for reaction of NO3 with the group of first generation oxidation products to be 7×10−14 molecule−1 cm3 s−1. At the low total organic aerosol concentration in the chamber (max=0.52 μg m−3) we observed a mass yield (ΔSOA mass/Δisoprene mass) of 2% for the entire 16 h experiment. However a comparison of the timing of the observed SOA production to a box model simulation of first and second generation oxidation products shows that the yield from the first generation products was <0.7% while the further oxidation of the initial products leads to a yield of 14% (defined as ΔSOA/Δisoprene2x where Δisoprene2x is the mass of isoprene which reacted twice with NO3). The SOA yield of 14% is consistent with equilibrium partitioning of highly functionalized C5 products of isoprene oxidation.
Evidence for ice particles in the tropical stratosphere from in-situ measurements
Authors: de Reus M. , Borrmann S. , Bansemer A. , Heymsfield A. J. , Weigel R. , Schiller C. , Mitev V. , Frey W. , Kunkel D. , Kürten A. , Curtius J. , Sitnikov N. M. , Ulanovsky A. , Ravegnani F.
Published: April 2010

Abstract. In-situ ice crystal size distribution measurements are presented within the tropical troposphere and lower stratosphere. The measurements were performed using a combination of a Forward Scattering Spectrometer Probe (FSSP-100) and a Cloud Imaging Probe (CIP), which were installed on the Russian high altitude research aircraft M55 "Geophysica" during the SCOUT-O3 campaign in Darwin, Australia. One of the objectives of the campaign was to characterise the Hector convective system, which appears on an almost daily basis during the pre-monsoon season over the Tiwi Islands, north of Darwin. In total 90 encounters with ice clouds, between 10 and 19 km altitude were selected from the dataset and were analysed. Six of these encounters were observed in the lower stratosphere, up to 1.4 km above the local tropopause. Concurrent lidar measurements on board "Geophysica" indicate that these ice clouds were a result of overshooting convection. Large ice crystals, with a maximum dimension up to 400 μm, were observed in the stratosphere. The stratospheric ice clouds included an ice water content ranging from 7.7×10−5 to 8.5×10−4 g m−3 and were observed at ambient relative humidities (with respect to ice) between 75 and 157%. Three modal lognormal size distributions were fitted to the average size distributions for different potential temperature intervals, showing that the shape of the size distribution of the stratospheric ice clouds are similar to those observed in the upper troposphere. In the tropical troposphere the effective radius of the ice cloud particles decreases from 100 μm at about 10 km altitude, to 3 μm at the tropopause, while the ice water content decreases from 0.04 to 10−5 g m−3. No clear trend in the number concentration was observed with altitude, due to the thin and inhomogeneous characteristics of the observed cirrus clouds. The ice water content calculated from the observed ice crystal size distribution is compared to the ice water content derived from two hygrometer instruments. This independent measurement of the ice water content agrees within the combined uncertainty of the instruments for ice water contents exceeding 3×10−4g m−3. Stratospheric residence times, calculated based on gravitational settling, and evaporation rates show that the ice crystals observed in the stratosphere over the Hector storm system had a high potential of humidifying the stratosphere locally. Utilizing total aerosol number concentration measurements from a four channel condensation particle counter during two separate campaigns, it can be shown that the fraction of ice particles to the number of aerosol particles remaining ranges from 1:300 to 1:30 000 for tropical upper tropospheric ice clouds with ambient temperatures below −75°C.
Formation of secondary organic aerosol from isoprene oxidation over Europe
Authors: Karl M. , Tsigaridis K. , Vignati E. , Dentener F.
Published: April 2010

Abstract. The role of isoprene as a precursor to secondary organic aerosol (SOA) over Europe is studied with the two-way nested global chemistry transport model TM5. The inclusion of the formation of SOA from isoprene oxidation in our model almost doubles the atmospheric burden of SOA over Europe compared to SOA formation from terpenes and aromatics. The reference simulation, which considers SOA formation from isoprene, terpenes and aromatics, predicts a yearly European production rate of 1.0 Tg SOA yr−1 and an annual averaged atmospheric burden of about 50 Gg SOA over Europe. A fraction of 35% of the SOA produced in the boundary layer over Europe is transported to higher altitudes or to other world regions. Summertime measurements of organic matter (OM) during the extensive EMEP OC/EC campaign 2002/2003 are better reproduced when SOA formation from isoprene is taken into account, reflecting also the strong seasonality of isoprene and other biogenic volatile organic compounds (BVOC) emissions from vegetation. However, during winter, our model strongly underestimates OM, likely caused by missing wood burning in the emission inventories. Uncertainties in the parameterisation of isoprene SOA formation have been investigated. Maximum SOA production is found for irreversible sticking (non-equilibrium partitioning) of condensable vapours on particles, with tropospheric SOA production over Europe increased by a factor of 4 in summer compared to the reference case. Completely neglecting SOA formation from isoprene results in the lowest estimate (0.51 Tg SOA yr−1). The amount and the nature of the absorbing matter are shown to be another key uncertainty when predicting SOA levels. Consequently, smog chamber experiments on SOA formation should be performed with different types of seed aerosols and without seed aerosols in order to derive an improved treatment of the absorption of SOA in the models. Consideration of a number of recent insights in isoprene SOA formation mechanisms reduces the tropospheric production of isoprene derived SOA over Europe from 0.4 Tg yr−1 in our reference simulation to 0.1 Tg yr−1.
Cloud condensation nuclei measurements in the marine boundary layer of the Eastern Mediterranean: CCN closure and droplet growth kinetics
Authors: Bougiatioti A. , Fountoukis C. , Kalivitis N. , Pandis S. N. , Nenes A. , Mihalopoulos N.
Published: April 2010

Abstract. Measurements of cloud condensation nuclei (CCN) concentrations (cm−3) between 0.2 and 1.0% supersaturation, aerosol size distribution and chemical composition were performed at a remote marine site in the eastern Mediterranean, from September to October 2007 during the FAME07 campaign. Most of the particles activate at ~0.6% supersaturation, characteristic of the aged nature of the aerosol sampled. Application of Köhler theory, using measurements of bulk composition, size distribution, and assuming that organics are insoluble resulted in agreement between predicted and measured CCN concentrations within 7±11% for all supersaturations, with a tendency for CCN underprediction (16±6%; r2=0.88) at the lowest supersaturations (0.21%). Including the effects of the water-soluble organic fraction (which represent around 70% of the total organic content) reduces the average underprediction bias at the low supersaturations, resulting in a total closure error of 0.6±6%. Using threshold droplet growth analysis, the growth kinetics of ambient CCN is consistent with NaCl calibration experiments; hence the presence of aged organics does not suppress the rate of water uptake in this environment. The knowledge of the soluble salt fraction is sufficient for the description of the CCN activity in this area.
One year of CNR-IMAA multi-wavelength Raman lidar measurements in coincidence with CALIPSO overpasses: Level 1 products comparison
Authors: Mona L. , Pappalardo G. , Amodeo A. , D'Amico G. , Madonna F. , Boselli A. , Giunta A. , Russo F. , Cuomo V.
Published: April 2010

Abstract. At CNR-IMAA, an aerosol lidar system has operated since May 2000 in the framework of EARLINET (European Aerosol Research Lidar Network), the first lidar network for tropospheric aerosol study on a continental scale. High quality multi-wavelength measurements make this system a reference point for the validation of data products provided by CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations), the first satellite-borne lidar specifically designed for aerosol and cloud study. Since 14 June 2006, dedicated measurements have been performed at CNR-IMAA in coincidence with CALIPSO overpasses. For the first time, results on 1-year comparisons between ground-based multi-wavelength Raman lidar measurements and corresponding CALIPSO lidar Level 1 profiles are presented. A methodology for the comparison is presented and discussed in detail. Night-time cases are considered to take advantage from Raman capability of the ground based lidar. Cases with the detection of cirrus clouds in CALIPSO data are separately analysed for taking into account multiple scattering effects. For cirrus cloud cases, few cases are available to draw any conclusions. For clear sky conditions, the comparison shows good performances of the CALIPSO on-board lidar: the mean relative difference between the ground-based and CALIPSO Level 1 measurements is always within its standard deviation at all altitudes, with a mean difference in the 3–8 km altitude range of (−2±12)%. At altitude ranges corresponding to the typical PBL height observed at CNR-IMAA, a mean difference of (−24±20)% is observed in CALIPSO data, probably due to the difference in the aerosol content at the location of PEARL and CALIPSO ground-track location. Finally, the mean differences are on average lower at all altitude ranges for the closest overpasses (at about 40 km) respect to the 80-km overpasses.
Ship emitted NO2 in the Indian Ocean: comparison of model results with satellite data
Authors: Franke K. , Richter A. , Bovensmann H. , Eyring V. , Jöckel P. , Hoor P. , Burrows J. P.
Published: April 2010

Abstract. The inventory of NOx emission from international shipping has been evaluated by comparing NO2 tropospheric columns derived from the satellite instruments SCIAMACHY (January 2003 to February 2008), GOME (January 1996 to June 2003), and GOME-2 (March 2007 to February 2008) to NO2 columns calculated with the atmospheric chemistry general circulation model ECHAM5/MESSy1 (January 2000 to October 2005). For both measurements and model consistently the tropospheric excess method was used to obtain mean NO2 columns over the shipping lane from India to Indonesia, and over two ship free regions, the Bay of Bengal and the central Indian Ocean. The long-term data set from SCIAMACHY yields the first monthly analysis of ship induced NO2 enhancements in the Indian Ocean. Comparison of data from the three instruments and in addition OMI reveals differences between the datasets which are discussed with respect to the diurnal cycle of NO2 and the increase in shipping traffic over the time period studied. In general, the model simulates the differences between the regions affected by ship pollution and ship free regions reasonably well. Minor discrepancies between model results and satellite data were identified during biomass burning seasons in March to May over India and the Indochinese Peninsula and August to October over Indonesia. We conclude that the NOx ship emission inventory used in this study is a good approximation of NOx ship emissions in the Indian Ocean for the years 2002 to 2007. It assumes that around 6 Tg(N) yr−1 are emitted by international shipping globally, resulting in 90 Gg(N) yr−1 in the region of interest when using Automated Mutual Assistance Vessel Rescue System (AMVER) as spatial proxy. A second model run using lower ship emissions estimates of 3–4 Tg(N) yr−1 globally results in poorer agreement with the satellite data.
Sulfuric acid and OH concentrations in a boreal forest site
Authors: Petäjä T. , Mauldin, III R. L. , Kosciuch E. , McGrath J. , Nieminen T. , Paasonen P. , Boy M. , Adamov A. , Kotiaho T. , Kulmala M.
Published: April 2010

Abstract. As demonstrated in a number of investigations, gaseous sulfuric acid plays a central role in atmospheric aerosol formation. Using chemical ionization mass spectrometer the gas-phase sulfuric acid and OH concentration were measured in Hyytiälä, SMEAR II station, Southern Finland during 24 March to 28 June 2007. Clear diurnal cycles were observed as well as differences between new particle formation event days and non-event days. Typically, the daily maximum concentrations of gas phase sulfuric acid varied from 3×105 to 2×106 molec cm−3 between non-event and event days. Noon-time OH concentrations varied from 3-6×105 molec cm−3 and not a clear difference between event and non-events was detected. The measured time series were also used as a foundation to develop reasonable proxies for sulfuric acid concentration. The proxies utilized source and sink terms, and the simplest proxy is radiation times sulfur dioxide divided by condensation sink. Since it is still challenging to measure sulfuric acid in ambient concentrations, and due to its significant role in atmospheric particle formation, reasonable proxies are needed. We use all together three different proxies and one chemical box model and compared their results to the measured data. The proxies for the sulfuric acid concentration worked reasonably well, and will be used to describe sulfuric acid concentrations in SMEAR II station, when no measured sulfuric acid data is available. With caution the proxies could be applied to other environments as well.
New particle formation and growth at a remote, sub-tropical coastal location
Authors: Modini R. L. , Ristovski Z. D. , Johnson G. R. , He C. , Surawski N. , Morawska L. , Suni T. , Kulmala M.
Published: April 2010

Abstract. A month-long intensive measurement campaign was conducted in March/April 2007 at Agnes Water, a remote coastal site just south of the Great Barrier Reef on the east coast of Australia. Particle and ion size distributions were continuously measured during the campaign. Coastal nucleation events were observed in clean, marine air masses coming from the south-east on 65% of the days. The events usually began at ~10:00 local time and lasted for 1–4 h. They were characterised by the appearance of a nucleation mode with a peak diameter of ~10 nm. The freshly nucleated particles grew within 1–4 h up to sizes of 20–50 nm. The events occurred when solar intensity was high (~1000 W m−2) and RH was low (~60%). Interestingly, the events were not related to tide height. The volatile and hygroscopic properties of freshly nucleated particles (17–22.5 nm), simultaneously measured with a volatility-hygroscopicity-tandem differential mobility analyser (VH-TDMA), were used to infer chemical composition. The majority of the volume of these particles was attributed to internally mixed sulphate and organic components. After ruling out coagulation as a source of significant particle growth, we conclude that the condensation of sulphate and/or organic vapours was most likely responsible for driving particle growth at sizes greater than 10 nm during the nucleation events. Although there was a possibility that the precursor vapours responsible for particle formation and growth had continental sources, on the balance of available data we would suggest that the precursors were most likely of marine/coastal origin. Furthermore, a unique and particularly strong nucleation event was observed during northerly wind. The event began early one morning (08:00) and lasted almost the entire day resulting in the production of a large number of ~80 nm particles (average modal concentration during the event was 3200 cm−3). The Great Barrier Reef was the most likely source of precursor vapours responsible for this event.
Extensive reduction of surface UV radiation since 1750 in world's populated regions
Authors: Kvalevåg M. M. , Myhre G. , Lund Myhre C. E.
Published: April 2010

Abstract. Human activity influences a wide range of components that affect the surface UV radiation levels, among them ozone at high latitudes. We calculate the effect of human-induced changes in the surface erythemally weighted ultra-violet radiation (UV-E) since 1750. We compare results from a radiative transfer model to surface UV-E radiation for year 2000 derived by satellite observations (from Total Ozone Mapping Spectroradiometer) and to ground based measurements at 14 sites. The model correlates well with the observations; the correlation coefficients are 0.97 and 0.98 for satellite and ground based measurements, respectively. In addition to the effect of changes in ozone, we also investigate the effect of changes in SO2, NO2, the direct and indirect effects of aerosols, albedo changes and aviation-induced contrails and cirrus. The results show an increase of surface UV-E in polar regions, most strongly in the Southern Hemisphere. Furthermore, our study also shows an extensive surface UV-E reduction over most land areas; a reduction up to 20% since 1750 is found in some industrialized regions. This reduction in UV-E over the industrial period is particularly large in highly populated regions.
Rapid formation of isoprene photo-oxidation products observed in Amazonia
Authors: Karl T. , Guenther A. , Turnipseed A. , Tyndall G. , Artaxo P. , Martin S.
Published: April 2010

Abstract. Isoprene represents the single most important reactive hydrocarbon for atmospheric chemistry in the tropical atmosphere. It plays a central role in global and regional atmospheric chemistry and possible climate feedbacks. Photo-oxidation of primary hydrocarbons (e.g. isoprene) leads to the formation of oxygenated VOCs (OVOCs). The evolution of these intermediates affects the oxidative capacity of the atmosphere (by reacting with OH) and can contribute to secondary aerosol formation, a poorly understood process. An accurate and quantitative understanding of VOC oxidation processes is needed for model simulations of regional air quality and global climate. Based on field measurements conducted during the Amazonian Aerosol Characterization Experiment (AMAZE-08) we show that the production of certain OVOCs (e.g. hydroxyacetone) from isoprene photo-oxidation in the lower atmosphere is significantly underpredicted by standard chemistry schemes. Recently reported fast secondary production could explain 50% of the observed discrepancy with the remaining part possibly produced via a novel primary production channel, which has been proposed theoretically. The observations of OVOCs are also used to test a recently proposed HOx recycling mechanism via degradation of isoprene peroxy radicals. If generalized our observations suggest that prompt photochemical formation of OVOCs and other uncertainties in VOC oxidation schemes could result in uncertainties of modelled OH reactivity, potentially explaining a fraction of the missing OH sink over forests which has previously been largely attributed to a missing source of primary biogenic VOCs.
Annual particle flux observations over a heterogeneous urban area
Authors: Järvi L. , Rannik Ü. , Mammarella I. , Sogachev A. , Aalto P. P. , Keronen P. , Siivola E. , Kulmala M. , Vesala T.
Published: April 2010

Abstract. Long-term eddy covariance particle number flux measurements for the diameter range 6 nm to 5 μm were performed at the SMEAR III station over an urban area in Helsinki, Finland. The heterogeneity of the urban measurement location allowed us to study the effect of different land-use classes in different wind directions on the measured fluxes. The particle number fluxes were highest in the direction of a local road on weekdays, with a daytime median flux of 0.8×109 m−2 s−1. The particle fluxes showed a clear dependence on traffic rates and on the mixing conditions of the boundary layer. The measurement footprint was estimated by the use of both numerical and analytical models. Using the crosswind integrated form of the footprint function, we estimated the emission factor for the mixed vehicle fleet, yielding a median particle number emission factor per vehicle of 3.0×1014 # km−1. Particle fluxes from the vegetated area were the lowest with daytime median fluxes below 0.2×109 m−2 s−1. During weekends and nights, the particle fluxes were low from all land use sectors being in the order of 0.02–0.1×109 m−2 s−1. On an annual scale the highest fluxes were measured in winter, when emissions from stationary combustion sources are also highest. Particle number fluxes were compared with the simultaneously measured CO2 fluxes and similarity in their sources was distinguishable. For CO2, the median emission factor of vehicles was estimated to be 370 g km−1.
An investigation of nucleation events in a coastal urban environment in the Southern Hemisphere
Authors: Mejía J. F. , Morawska L.
Published: April 2010

Abstract. Ambient aerosols play an important role in atmospheric processes affecting the human and natural environments. They affect air quality, reduce visibility, and induce climate change by directly scattering and/or absorbing the incoming solar radiation (Charlson et al., 1992; Kim et al., 2006), or indirectly by acting as cloud condensation nuclei (Hobbs, 1993). Aerosol particles are emitted from a variety of anthropogenic and natural sources either directly into the atmosphere or as secondary particles by gas-to-particle formation process. There is growing interest in studying and analysing the mechanisms of formation of secondary particles. The development of new instruments during the 1990s to measure the particle size distribution of nanoparticles (<50 nm) has enabled scientists to observe the formation and growth of new particles (see Kulmala et al. (2004) for review). Nucleation events, that is, the appearance of a mode below 25–30 nm in the particle number size distribution, known as "nucleation mode" (e.g. Dal Maso et al., 2007; Tunved et al., 2003), usually in very large numbers, have been observed around the world. For example, they have been reported in remote (e.g. Tunved et al., 2003), urban (e.g. Jeong et al., 2004; Zhang et al., 2004) and coastal areas (e.g. Vaattovaara et al., 2006) and at various latitudes in the upper troposphere and the lower stratosphere (Lee et al., 2003). It has been shown that the probability of nucleation was increased by elevated sulphur dioxide (SO2) concentrations (Stanier et al., 2004). This gas is mainly emitted from anthropogenic sources such as the combustion of sulphur-containing fossil fuel (Stern, 2005). Therefore, aerosol nucleation in the atmosphere would be expected to be enhanced by human activities (see also Curtius (2006) for discussion). In urban air, morning nucleation events have been found to be consistent with peaks in traffic (Jeong et al., 2004). In contrast, in coastal environments, higher concentrations of nucleation mode particles have been observed during entries of clean air rather than of polluted air (O'Dowd et al., 2002). This is also confirmed by a Finish study (Spracklen et al., 2006), which found that particle concentrations in remote continental regions are dominated by nucleated particles whereas in polluted continental regions are dominated by primary particles. This paper aims to analyse the frequency of and the atmospheric conditions favourable for nucleation events at coastal urban location in Brisbane, Australia, with a focus on the contribution of vehicle emissions. Monitoring was conducted during four campaigns of two weeks duration each, and a campaign of four weeks duration, covering a total period of 13 months. The objective was to investigate which meteorological conditions enhanced the probability of nucleation and to investigate any patterns in gaseous concentrations leading to the events to determine whether the local traffic was a major source of secondary particles in the study area.
A new transport mechanism of biomass burning from Indochina as identified by modeling studies
Authors: Lin C.-Y. , Hsu H.-m. , Lee Y. H. , Kuo C. H. , Sheng Y.-F. , Chu D. A.
Published: April 2010

Abstract. Biomass burning in the Indochina Peninsula (Indochina) is one of the important ozone sources in the low troposphere over East Asia in springtime. Moderate Resolution Imaging Spectroradiometer (MODIS) data show that 20 000 or more active fire detections occurred annually in spring only from 2000 to 2007. In our tracer modeling study, we identify a new mechanism transporting the tracer over Indochina that is significantly different from the vertical transport mechanism over the equatorial areas such as Indonesia and Malaysia. Simulation results demonstrate that the leeside troughs over Indochina play a dominant role in the uplift of the tracer below 3 km, and that the strong westerlies prevailing above 3 km transport the tracer. These fundamental mechanisms have a major impact on the air quality downwind from Indochina over East Asia. The climatological importance of such a leeside trough is also discussed.
Technical Note: A SAGE-corrected SBUV zonal-mean ozone data set
Authors: McLinden C. A. , Tegtmeier S. , Fioletov V.
Published: April 2010

Abstract. A stratospheric vertically resolved, monthly, zonal-mean ozone data set based on Satellite Aerosol and Gas Experiment (SAGE) and Solar Backscatter UltraViolet (SBUV) data spanning 1979–2005 is presented. Drifts in individual SBUV instruments and inter-SBUV biases are corrected using SAGE I and II by calculating differences between coincident SAGE-SBUV measurements. In this way the daily, near-global coverage of SBUV(/2) is combined with the stability and precision of SAGE to provide a homogeneous ozone record suitable for trend analysis. The resultant SAGE-corrected SBUV data set, shows, for example, a more realistic Quasi-Biennial Oscillation signal compared to the one derived from SBUV data alone. Furthermore, this methodology can be used to extend the present data set beyond the lifetime of SAGE II.
Properties of the average distribution of equatorial Kelvin waves investigated with the GROGRAT ray tracer
Authors: Ern M. , Cho H.-K. , Preusse P. , Eckermann S. D.
Published: April 2010

Abstract. Kelvin waves excited by tropospheric convection are considered to be one of the main drivers of the stratospheric quasi-biennial oscillation (QBO). In this paper we combine several measured data sets with the Gravity wave Regional Or Global RAy Tracer (GROGRAT) in order to study the forcing and vertical propagation of Kelvin waves. Launch distributions for the ray tracer at tropospheric altitudes are deduced from space-time spectra of European Centre for Medium-Range Weather Forecasts (ECMWF) operational analyses, as well as outgoing longwave radiation (OLR) and rainfall data measured by the Tropical Rainfall Measuring Mission (TRMM) satellite. The resulting stratospheric Kelvin wave spectra are compared to ECMWF operational analyses and temperature measurements of the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) satellite instrument. Questions addressed are: the relative importance of source variability versus wind modulation, the relative importance of radiative and turbulent damping versus wave breaking, and the minimum altitude where freely propagating waves dominate the spectrum.
Vertical structure of aerosols and water vapor over West Africa during the African monsoon dry season
Authors: Kim S.-W. , Chazette P. , Dulac F. , Sanak J. , Johnson B. , Yoon S.-C.
Published: April 2010

Abstract. We present observations of tropospheric aerosol and water vapor transport over West Africa and the associated meteorological conditions during the AMMA SOP-0 dry season experiment, which was conducted in West Africa in January–February 2006. This study combines data from ultra-light aircraft (ULA)-based lidar, airborne in-situ aerosol and gas measurements, standard meteorological measurements, satellite-based aerosol measurements, airmass trajectories, and radiosonde measurements. At Niamey (13.5° N, 2.2° E) the prevailing surface wind (i.e. Harmattan) was from the northeast bringing dry dusty air from the Sahara desert. High concentrations of mineral dust aerosol were typically observed from the surface to 1.5 or 2 km associated with the Saharan airmasses. At higher altitudes the prevailing wind veered to the south or southeast bringing relatively warm and humid airmasses from the biomass burning regions to the Sahel (<10° N). These elevated layers had high concentrations of biomass burning aerosol and were typically observed between altitudes of 2–5 km. Meteorological analyses show these airmasses were advected upwards over the biomass burning regions through ascent in Inter-Tropical Discontinuity (ITD) zone. Aerosol vertical profiles obtained from the space-based lidar CALIOP onboard CALIPSO during January 2007 also showed the presence of dust particles (particle depolarization (δ)~30%, lidar Ångström exponent (LAE)<0, aerosol backscatter to extinction ratio (BER): 0.026~0.028 sr−1) at low levels (<1.5 km) and biomass burning smoke aerosol (δ<10%, LAE: 0.6~1.1, BER: 0.015~0.018 sr−1) between 2 and 5 km. CALIOP data indicated that these distinct continental dust and biomass burning aerosol layers likely mixed as they advected further south over the tropical Atlantic Ocean, as indicated an intermediate values of δ (10~17%), LAE (0.16~0.18) and BER (0.0021~0.0022 sr−1).
Using ground-based solar and lunar infrared spectroscopy to study the diurnal trend of carbon monoxide in the Mexico City boundary layer
Authors: Stremme W. , Ortega I. , Grutter M.
Published: April 2010

Abstract. Carbon monoxide (CO) is an important pollutant in urban agglomerations. Quantifying the total burden of this pollutant in a megacity is challenging because not only its surface concentration but also its vertical dispersion present different behaviours and high variability. The diurnal trend of columnar CO in the boundary layer of Mexico City has been measured during various days with ground-based infrared absorption spectroscopy. Daytime CO total columns are retrieved from solar spectra and for the first time, nocturnal CO total columns using moonlight have been retrieved within a megacity. The measurements were taken at the Universidad Nacional Autónoma de México (UNAM) campus located in Mexico City (19.33° N, 99.18° W, 2260 m a.s.l.) from October 2007 until February 2008 with a Fourier-transform infrared spectrometer at 0.5 cm−1 resolution. The atmospheric CO background column was measured from the high altitude site Altzomoni (19.12° N, 98.65° W, 4010 m a.s.l.) located 60 km southeast of Mexico City. The total CO column within the city presents large variations. Fresh CO emissions at the surface, the transport of cleaner or more polluted air masses within the field-of-view of the instrument and other processes contribute to this variability. The mean background value above the boundary mixing layer was found to be (8.4±0.5)×1017 molecules/cm2, while inside the city, the late morning mean on weekdays and Sundays was found to be (2.73±0.41)×1018 molecules/cm2 and (2.04±0.57)×1018 molecules/cm2, respectively. Continuous CO column retrieval during the day and night (when available), in conjunction with surface CO measurements, allow for a reconstruction of the effective mixing layer height. The limitations from this simplified approach, as well as the potential of using continuous column measurements in order to derive top-down CO emissions from a large urban area, are discussed. Also, further monitoring will provide more insight in daily and weekly emission patterns and a usable database for the quantitative validation of CO from satellite observations in a megacity.
Evaluation of tropospheric ozone columns derived from assimilated GOME ozone profile observations
Authors: de Laat A. T. J. , van der A R. J. , van Weele M.
Published: April 2010

Abstract. Tropospheric O3 column estimates are produced and evaluated from spaceborne O3 observations by the subtraction of assimilated O3 profile observations from total column observations, the so-called Tropospheric O3 ReAnalysis or TORA method. Here we apply the TORA method to six years (1996–2001) of ERS-2 GOME/TOMS total O3 and ERS-2 GOME O3 profile observations using the TM5 global chemistry-transport model with a linearized O3 photochemistry parameterization scheme. Free running TM5 simulations show good agreement with O3 sonde observations in the upper-tropospheric and lower stratospheric region (UTLS), both for short day-to-day variability as well as for monthly means. The assimilation of GOME O3 profile observations counteracts the mid-latitude stratospheric O3 drift caused by the overstrong stratospheric meridional circulation in TM5. Assimilation of GOME O3 profile observations also improves the bias and correlations in the tropical UTLS region but slightly degrades the model-to-sonde correlations and bias of extra-tropical UTLS. We suggest that this degradation is related to the large ground pixel size of the GOME O3 measurements (960×100 km) in combination with retrieval and calibration errors. The added value of the assimilation of GOME O3 profiles compared to stand-alone model simulations lays in the long term variations of stratospheric O3, not in short term synoptic variations. The evaluation of daily and monthly tropospheric O3 columns obtained from total column observations and using the TORA methodology shows that the use of GOME UV-VIS nadir O3 profiles in combination with the spatial resolution of the model does not result in satisfactory residual tropospheric ozone columns.