bluuebunny/crossref_metadata_2025 huggingface dataset:
Relationships between submicrometer particulate air pollution and air mass history in Beijing, China, 2004–2006
Authors: Wehner B. , Birmili W. , Ditas F. , Wu Z. , Hu M. , Liu X. , Mao J. , Sugimoto N. , Wiedensohler A.
Published: April 2010

Abstract. The Chinese capital Beijing is one of the global megacities where the effects of rapid economic growth have led to complex air pollution problems that are not well understood. In this study, ambient particle number size distributions in Beijing between 2004 and 2006 are analysed as a function of regional meteorological transport. An essential result is that the particle size distribution in Beijing depends to large extent on the history of the synoptic scale air masses. A first approach based on manual back trajectory classification yielded differences in particulate matter mass concentration (PM1 and PM10) by a factor of two between four different air mass categories, including three main wind directions plus the case of stagnant air masses. A back trajectory cluster analysis refined these results, yielding a total of six trajectory clusters. Besides the large scale wind direction, the transportation speed of an air mass was found to play an essential role on the PM concentrations in Beijing. Slow-moving air masses were shown to be associated with an effective accumulation of surface-based anthropogenic emissions due to both, an increased residence time over densely populated land, and their higher degree of vertical stability. For the six back trajectory clusters, differences in PM1 mass concentrations by a factor of 3.5, in the mean air mass speed by a factor of 6, and in atmospheric visibility by a factor of 4 were found. The main conclusion is that the air quality in Beijing is not only degraded by anthropogenic aerosol sources from within the megacity, but also by sources across the entire Northwest China plain depending on the meteorological situation.
Spatial and temporal variation of emission inventories for historical anthropogenic NMVOCs in China
Authors: Bo Y. , Cai H. , Xie S. D.
Published: April 2010

Abstract. Multiyear emission inventories of anthropogenic NMVOCs in China for 1980–2005 were compiled based on time-varying statistical data, literature surveyed and model calculated emission factors, and were gridded at a high spatial resolution of 40 km×40 km using the GIS methodology. Chinese NMVOCs emissions had increased by 4.3 times at an annual average rate of 10.7% from 3.92 Tg in 1980 to 16.5 Tg in 2005. Vehicles, biomass burning, industrial processes, fossil fuel combustion, solvent utilization, and storage and transport generated 5.49 Tg, 3.91 Tg, 2.76 Tg, 1.98 Tg, 1.87 Tg, and 0.55 Tg of NMVOCs, respectively. Motorcycles, biofuel burning, heavy-duty vehicles, synthetic fibre production, biomass open burning, and industrial and commercial consumption were primary emission sources. Besides, from 1980 to 2005, vehicle emission increased notably from 6% to 33%, along with a slight increase for fossil fuel combustion from 9% to 12% and for industrial processes from 11% to 17%. Meanwhile, biomass burning emission decreased from 41% to 23%, along with the decrease of storage and transport and solvent utilization from 9% to 3% and from 28% to 11%, respectively. Varieties of NMVOCs emissions coincided well with China's economic growth. Conversions in economic structure and adjustment of fuel consumption structure in China during the period were the reasons for conspicuous variation of source contributions. The developed eastern and coastal regions produced more emissions than the relatively underdeveloped western and inland regions. Particularly, southeastern, northern, and central China covering 35% of China's territory, generated 59% of the total emissions, while the populous capital cities covering merely 4.5% of China's territory, accounted for 25% of the national emissions. Moreover, rural areas also experienced emission growth during the past two and a half decades, the reason of which was transfer of emission-intensive plants from city to county, inefficient fuel utilization, and biomass burning.
Halogenated organic species over the tropical rainforest
Authors: Gebhardt S. , Colomb A. , Hofmann R. , Williams J. , Lelieveld J.
Published: April 2010

Abstract. Airborne measurements of the halogenated trace gases methyl chloride, methyl bromide and chloroform were conducted over the Atlantic Ocean and 1000 km of pristine tropical rainforest in Suriname and French Guyana (3–6° N, 51–59° W) in October 2005. In the boundary layer (0–1.4 km), maritime air masses initially low in forest hydrocarbons, advected over the forest by southeasterly trade winds, were measured at various distances from the coast. Since the organohalogens presented here have relatively long atmospheric lifetimes (0.4–1.0 years) in comparison to the transport times (1–2 days), emissions will accumulate in air traversing the rainforest. The distributions of methyl chloride, methyl bromide and chloroform were analyzed as a function of forest contact time and the respective relationship used to determine fluxes from the rainforest during the long dry season. Emission fluxes have been calculated for methyl chloride and chloroform as 9.4 (±4.0 2σ) and 0.34 (0.14± 2σ) μg m−2 h−1, respectively. No significant flux from the rainforest was observed for methyl bromide within the limits of these measurements. The flux of methyl chloride was in general agreement with the flux measured over the same region in March 1998 during the LBA Claire project using a different analytical system. This confirms that the rainforest is a strong source for methyl chloride and suggests that this emission is relatively uniform throughout the year. In contrast the chloroform flux derived here is a factor of three less than previous measurements made in March 1998 suggesting a pronounced ecosystem variation. The differences in chloroform fluxes could not be attributed to either temperature or rainfall changes. The global extrapolation of the derived fluxes led to 1.5 (±0.6 2σ) Tg yr−1 for methyl chloride, which is in the range of the missing source postulated by previous model studies and 55 (±22 2σ) Gg yr−1 for chloroform.
Redox activity and chemical speciation of size fractioned PM in the communities of the Los Angeles – Long Beach Harbor
Authors: Hu S. , Polidori A. , Arhami M. , Shafer M. M. , Schauer J. J. , Cho A. , Sioutas C.
Published: April 2010

Abstract. In this study, two different types of assays were used to quantitatively measure the redox activity of PM and to examine its intrinsic toxicity: 1) in vitro exposure to rat alveolar macrophage (AM) cells using dichlorofluorescin diacetate (DCFH-DA) as the fluorescent probe (macrophage ROS assay), and: 2) consumption of dithiothreitol (DTT) in a cell-free system (DTT assay). Coarse (PM10–2.5), accumulation (PM2.5–0.25), and quasi-ultrafine (quasi-UF, PM0.25) mode particles were collected weekly at five sampling sites in the Los Angeles-Long Beach Harbor and at one site near the University of Southern California campus (urban site). All PM samples were analyzed for organic (total and water-soluble) and elemental carbon, organic species, inorganic ions, and total and water-soluble elements. Quasi-UF mode particles showed the highest redox activity at all Long Beach sites (on both a per-mass and per-air volume basis). A significant association (R2=0.61) was observed between the two assays, indicating that macrophage ROS and DTT levels are affected at least partially by similar PM species. Relatively small variation was observed for the DTT measurements across all size fractions and sites, whereas macrophage ROS levels showed more significant ranges across the three different particle size modes and throughout the sites (coefficients of variation, or CVs, were 0.35, 0.24 and 0.53 for quasi-UF, accumulation, and coarse mode particles, respectively). Association between the PM constituents and the redox activity was further investigated using multiple linear regression models. The results showed that OC was the most important component influencing the DTT activity of PM samples. The variability of macrophage ROS was explained by changes in OC concentrations and water-soluble vanadium (probably originating from ship emissions – bunker oil combustion). The multiple regression models were used to predict the average diurnal macrophage ROS and DTT levels as a function of the OC concentration at one of the sampling sites.
Saharan dust levels in Greece and received inhalation doses
Authors: Mitsakou C. , Kallos G. , Papantoniou N. , Spyrou C. , Solomos S. , Astitha M. , Housiadas C.
Published: April 2010

Abstract. The desert of Sahara is one of the major sources of mineral dust on Earth, producing around 2×108 tons/yr. Under certain weather conditions, dust particles from Saharan desert get transported over the Mediterranean Sea and most of Europe. The limiting values set by the directive EC/30/1999 of European Union can easily be exceeded by the transport of desert dust particles in all south European areas and especially urban. In this study, the effects of dust transport on air quality in several Greek urban areas are quantified. PM10 concentration values from stationary monitoring stations are compared to dust concentrations for the 4-year period 2003–2006. The dust concentration values in the Greek areas were estimated by the SKIRON modelling system coupled with embedded algorithms describing the dust cycle. The mean annual dust contribution to daily-averaged PM10 concentration values was found to be around or even greater than 10% in the urban areas throughout the years examined. Natural dust transport may contribute by much more than 20% to the annual number of exceedances – PM10 values greater than EU limits – depending on the specific monitoring location. In a second stage of the study, the inhaled lung dose received by the residents in various Greek locations is calculated. The particle deposition efficiency of mineral dust at the different parts of the human respiratory tract is determined by applying a lung dosimetry numerical model, which incorporates inhalation dynamics and aerosol physical processes. The inhalation dose from mineral dust particles was greater in the upper respiratory system (extrathoracic region) and less significant in the lungs, especially in the sensitive alveolar region. However, in cases of dust episodes, the amounts of mineral dust deposited along the human lung are comparable to those received during exposure in heavily polluted urban or smoking areas.
Mechanisms for synoptic transport of atmospheric CO2 in the midlatitudes and tropics
Authors: Parazoo N. , Denning A. , Kawa S. , Corbin K. , Lokupitiya R. , Baker I.
Published: April 2010

Abstract. Synoptic variations of CO2 mixing ratio produced by interactions between weather and surface fluxes are investigated mechanistically and quantitatively in midlatitude and tropical regions using continuous in-situ CO2 observations in North America, South America and Europe and forward chemical transport model simulations with the Parameterized Chemistry Transport Model. Frontal CO2 climatologies show consistently strong, characteristic frontal CO2 signals throughout the midlatitudes of North America and Europe. Transitions between synoptically identifiable CO2 air masses or transient spikes along the frontal boundary typically characterize these signals. One case study of a summer cold front shows that CO2 gradients organize with deformational flow along weather fronts producing strong and spatially coherent variations. A boundary layer budget equation is constructed in order to determine contributions to boundary layer CO2 tendencies by horizontal and vertical advection, moist convection, and biological and anthropogenic surface fluxes. Analysis of this equation suggests that, in midlatitudes, advection is responsible for 50–90% of the amplitude of frontal variations in the summer, depending on upstream influences, and 50% of all day-to-day variations throughout the year. Simulations testing sensitivity to local cloud and surface fluxes further suggest that horizontal advection is a major source of CO2 variability in midlatitudes. In the tropics, coupling between convective transport and surface CO2 flux is most important. Due to the scarcity of tropical observations available at the time of this study, future work should extend such mechanistic analysis to additional tropical locations.
Emissions and photochemistry of oxygenated VOCs in urban plumes in the Northeastern United States
Authors: Sommariva R. , de Gouw J. A. , Trainer M. , Atlas E. , Goldan P. D. , Kuster W. C. , Warneke C. , Fehsenfeld F. C.
Published: April 2010

Abstract. Photochemical processes inside urban plumes in the Northeast of the United States have been studied using a highly detailed chemical model, based upon the Master Chemical Mechanism (MCM). The model results have been compared to measurements of oxygenated VOCs (acetone, methyl ethyl ketone, acetaldehyde, acetic acid and methanol) obtained during several flights of the NOAA WP-3D aircraft, which sampled plumes from the New York City area during the ICARTT campaign in 2004. The agreement between the model and the measurements was within 40–60% for all species, except acetic acid. The model results have been used to study the formation and photochemical evolution of acetone, methyl ethyl ketone and acetaldehyde. Under the conditions encountered during the ICARTT campaign, acetone is produced from the oxidation of propane (24–28%) and i-propanol (<15%) and from a number of products of i-pentane oxidation. Methyl ethyl ketone (MEK) is mostly produced from the oxidation of n-butane (20–30%) and 3-methylpentane (<40%). Acetaldehyde is formed from several precursors, mostly small alkenes, >C5 alkanes, propanal and MEK. Ethane and ethanol oxidation account, respectively, for 6–23% and 5–25% of acetaldehyde photochemical formation. The results highlight the importance of long-chain alkanes for the photochemical production of ketones and the role of hydroperoxides in sustaining their formation far from the emission sources.
Using 3DVAR data assimilation system to improve ozone simulations in the Mexico City basin
Authors: Bei N. , de Foy B. , Lei W. , Zavala M. , Molina L. T.
Published: April 2010

Abstract. This study investigates the improvement of ozone (O3) simulations in the Mexico City basin using a three-dimensional variational (3DVAR) data assimilation system in meteorological modeling during the MCMA-2003 campaign. Meteorological simulations from the Penn State/NCAR mesoscale model (MM5) are used to drive photochemical modeling with the Comprehensive Air Quality Model with extensions (CAMx) during a four-day episode on 13–16 April 2003. The calculated wind circulation, temperature, and humidity fields in the basin with the data assimilation are found to be more consistent with the observations than those from the reference deterministic forecast. This leads to improved calculations of plume position, peak O3 timing, and peak O3 concentrations in the photochemical model. The improvement of O3 simulations is especially strong during the daytime. The results demonstrate the importance of applying data assimilation in meteorological simulations for air quality studies in the Mexico City basin.
Flux estimates of isoprene, methanol and acetone from airborne PTR-MS measurements over the tropical rainforest during the GABRIEL 2005 campaign
Authors: Eerdekens G. , Ganzeveld L. , Vilà-Guerau de Arellano J. , Klüpfel T. , Sinha V. , Yassaa N. , Williams J. , Harder H. , Kubistin D. , Martinez M. , Lelieveld J.
Published: April 2010

Abstract. Tropical forests are a strong source of biogenic volatile organic compounds (BVOCs) to the atmosphere and such emissions can impact the atmospheric oxidation capacity. Here we present airborne and ground-based BVOC measurements performed during the long dry season in October 2005 during the GABRIEL (Guyanas Atmosphere-Biosphere exchange and Radicals Intensive Experiment with the Learjet) project, which covered a large area of the northern Amazonian rainforest (6–3° N, 50–59° W). The vertical (35 m to 10 km) and diurnal (09:00–16:00) profiles of selected BVOCs like isoprene, its oxidation products methacrolein and methyl vinyl ketone, methanol and acetone, measured by PTRMS (Proton Transfer Reaction Mass Spectrometry), have been used to empirically estimate their emission fluxes from the forest canopy on a regional scale. The mixed layer isoprene emission flux, inferred from the airborne measurements above 300 m, is 4.1 mg isoprene m−2 h−1 whereas the surface flux is 7.3 mg isoprene m−2 h−1 after compensating for chemistry. This surface flux is in general agreement with previous tropical forest studies. Mixed layer fluxes of 0.8 mg methanol m−2 h−1 and 0.35 mg acetone m−2 h−1 were found. The BVOC measurements were compared with fluxes and mixing ratios simulated with a single-column model (SCM). The isoprene flux inferred from the measurements is substantially smaller than that simulated with an SCM implementation of MEGAN (Model of the Exchange of Gases between the Atmosphere and Nature) though consistent with global emission estimates. The exchanges of methanol and acetone can be reasonably well described using a compensation point approach.
Comparison of CMAM simulations of carbon monoxide (CO), nitrous oxide (N2O), and methane (CH4) with observations from Odin/SMR, ACE-FTS, and Aura/MLS
Authors: Jin J. J. , Semeniuk K. , Beagley S. R. , Fomichev V. I. , Jonsson A. I. , McConnell J. C. , Urban J. , Murtagh D. , Manney G. L. , Boone C. D. , Bernath P. F. , Walker K. A. , Barret B. , Ricaud P. , Dupuy E.
Published: April 2010

Abstract. Simulations of CO, N2O and CH4 from a coupled chemistry-climate model (CMAM) are compared with satellite measurements from Odin Sub-Millimeter Radiometer (Odin/SMR), Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), and Aura Microwave Limb Sounder (Aura/MLS). Pressure-latitude cross-sections and seasonal time series demonstrate that CMAM reproduces the observed global distributions and the polar winter time evolutions of the CO, N2O, and CH4 measurements quite well. Generally, excellent agreement with measurements is found in CO monthly zonal mean profiles in the stratosphere and mesosphere for various latitudes and seasons. The difference between the simulations and the observations are generally within 30%, which is comparable with the difference between the instruments in the upper stratosphere and mesosphere. In general, the CO measurements also show an excellent agreement between themselves although MLS retrievals are noisier than other retrievals above 10 hPa (~32 km). The measurements also show large difference in the lower stratosphere and upper troposphere. Comparisons of N2O show that CMAM results usually have a less than 15% difference to the measurements in the lower and middle stratosphere, and the observations are consistent as well. However, the standard version of CMAM has a serious low bias in the upper stratosphere. The CMAM CH4 distribution is also close to the observations in the lower stratosphere, but has a similar but smaller negative bias in the upper stratosphere. These negative biases can be reduced by introducing a vertical diffusion coefficient related to gravity wave drag. CO measurements from 2004 and 2006 show evidence of enhanced descent of air from the mesosphere into the stratosphere in the Arctic after strong stratospheric sudden warmings (SSWs). CMAM also shows strong descent of air after SSWs, but further investigation is needed. In the tropics, CMAM captures the "tape recorder" (or annual oscillation) in the lower stratosphere and the semiannual oscillations (SAO) at the stratopause and mesopause shown in MLS CO and SMR N2O observations. The inter-annual variation of the SAO at the stratopause in SMR N2O observations also shows a biennial oscillation, but CMAM cannot does not reproduce this feature. However, this study confirms that CMAM is able to simulate middle atmospheric transport processes reasonably well.
Regional-scale modeling of near-ground ozone in the Central East China, source attributions and an assessment of outflow to East Asia – The role of regional-scale transport during MTX2006
Authors: Li J. , Wang Z. , Akimoto H. , Yamaji K. , Takigawa M. , Pochanart P. , Liu Y. , Kanaya Y.
Published: April 2010

Abstract. A 3-D regional chemical transport model, the Nested Air Quality Prediction Model System (NAQPMS), with an on-line tracer tagging module was applied to study the source of the near-ground (<1.5 km above ground level) ozone at Mt. Tai (36.25°N, 117.10°E, 1534 m a.s.l.) in Central East China (CEC) during the Mount Tai eXperiment 2006 (MTX2006): regional ozone photochemistry and aerosol studies in Central East China in June, 2006. The model reproduced the temporal and spatial variations of near-ground ozone and other pollutants. In particular, the model captured highly polluted and clean cases well. The simulated near-ground ozone over CEC is 60–85 ppbv (parts per billion by volume), higher than those (20–50 ppbv) in Japan and over the North Pacific. The simulated tagged tracer indicates that the regional-scale transport of chemically produced ozone over other areas in CEC contributes to the most fractions (49%) of the near-ground mean ozone at Mt. Tai in June, rather than the in-situ photochemistry (12%). Due to high anthropogenic and biomass burning emissions, the contributions of the ground ozone from the southern part of CEC plays the most important role (32.4 ppbv, 37.9% of total ozone) in the monthly mean ozone concentration at Mt. Tai, which even reached 59 ppbv (62%) on 6–7 June 2006. The monthly mean horizontal distribution of chemically produced ozone from various source regions indicates that the spatial distribution of O3 over CEC is controlled by the photochemical reactions. In addition, the regional-scale transport of pollutants also plays an important role in the spatial and temporal distribution of ozone over CEC. The chemically produced ozone from the southern part of the study region can be transported northeastwardly to the northern rim of CEC. The mean contribution is 5–10 ppbv, and it can reach 25 ppbv during high ozone events. This work also studied the outflow of CEC ozone and its precursors, as well as their influences and contributions to the ozone level over adjacent regions/countries. It shows that the contribution of CEC ozone to mean ozone mixing ratios over Korea Peninsula and Japan is 5–15 ppbv, of which about half was due to the direct transport of ozone from CEC and half was contributed by the ozone produced locally by the transported ozone precursors from CEC.
Simulation of aerosol optical properties over Europe with a 3-D size-resolved aerosol model: comparisons with AERONET data
Authors: Tombette M. , Chazette P. , Sportisse B.
Published: April 2010

Abstract. This paper aims at presenting a model-to-data comparison of the Aerosol Optical Thickness (AOT) and of a few sparse data for Single Scattering Albedo (SSA) over Europe for one year. The optical parameters are computed from a size-resolved aerosol model embedded in the POLYPHEMUS system described in Mallet et al. (2007). The methodology is first described, showing that several hypothesis can be made for several microphysical aerosol properties. The simulation is made over one year (2001); statistics and monthly time series for the simulation and AERONET data are used to evaluate the ability of the model to reproduce AOT and vertically averaged SSA fields and their variability. The relation with the uncertainties of measurements is discussed. Then a sensitivity study with respect to the mixing state of the particle, the way to compute the Aerosol Complex Refractive Index (ACRI) of a mixture and the way to take into account water uptake is carried out. The results indicate that the computation of AOT is relatively stable, while the computation of the single scattering albedo is much more uncertain.
Classification of Northern Hemisphere stratospheric ozone and water vapor profiles by meteorological regime
Authors: Follette M. B. , Hudson R. D. , Nedoluha G. E.
Published: April 2010

Abstract. The subtropical and polar upper troposphere fronts serve as the boundaries to divide the Northern Hemisphere into four meteorological regimes. These regimes are defined as (1) the arctic regime – within the polar vortex, (2) the polar regime – between the polar front and the polar vortex, or when the latter is not present, the pole, (3) the midlatitude regime – between the subtropical and polar fronts, and (4) the tropical regime – between the equator and the subtropical front. Data from the Halogen Occultation Experiment (HALOE) and the Stratospheric Aerosol and Gas Experiment II (SAGE II) were used to show that within each meteorological regime, ozone and water profiles are characterized by unique ozonepause and hygropause heights. In addition, both constituents exhibited distinct profile shapes up to approximately 25 km. This distinction was most pronounced in the winter and spring months, and less in the summer and fall. Both daily measurements and seven-year (1997–2003) monthly climatologies were analyzed. Daily measurements and seven-year (1997–2003) monthly climatologies showed that, within each meteorological regime, both constituents exhibited distinct profile shapes from the tropopause up to approximately 25 km. This distinction was most pronounced in the winter and spring months, and less in the summer and fall. Despite differences in retrieval techniques and sampling between the SAGE and HALOE instruments, the seven-year monthly climatologies calculated for each regime agreed well for both species below ~25 km. Above this altitude ozone and water vapor profiles were more clearly distinct when binned by latitude rather than by regime. Given that profiles of ozone and water vapor exhibit unique profiles shapes within each regime in the UTLS, trends in this region will therefore be the result of both changes within each meteorological regime, and changes in the relative contribution of each regime to a given zonal band over time.
The ASSET intercomparison of stratosphere and lower mesosphere humidity analyses
Authors: Thornton H. E. , Jackson D. R. , Bekki S. , Bormann N. , Errera Q. , Geer A. J. , Lahoz W. A. , Rharmili S.
Published: April 2010

Abstract. This paper presents results from the first detailed intercomparison of stratosphere-lower mesosphere water vapour analyses; it builds on earlier results from the "Assimilation of ENVISAT Data" (ASSET) project. With the availability of high resolution, good quality Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) water vapour profiles, the ability of four different atmospheric models to assimilate these data is tested. MIPAS data have been assimilated over September 2003 into the models of the European Centre for Medium Range Weather Forecasts (ECMWF), the Belgian Institute for Space and Aeronomy (BIRA-IASB), the French Service d'Aéronomie (SA-IPSL) and the UK Met Office. The resultant middle atmosphere humidity analyses are compared against independent satellite data from the Halogen Occultation Experiment (HALOE), the Polar Ozone and Aerosol Measurement (POAM III) and the Stratospheric Aerosol and Gas Experiment (SAGE II). The MIPAS water vapour profiles are generally well assimilated in the ECMWF, BIRA-IASB and SA systems, producing stratosphere-mesosphere water vapour fields where the main features compare favourably with the independent observations. However, the models are less capable of assimilating the MIPAS data where water vapour values are locally extreme or in regions of strong humidity gradients, such as the Southern Hemisphere lower stratosphere polar vortex. Differences in the analyses can be attributed to the choice of humidity control variable, how the background error covariance matrix is generated, the model resolution and its complexity, the degree of quality control of the observations and the use of observations near the model boundaries. Due to the poor performance of the Met Office analyses the results are not included in the intercomparison, but are discussed separately. The Met Office results highlight the pitfalls in humidity assimilation, and provide lessons that should be learnt by developers of stratospheric humidity assimilation systems. In particular, they underline the importance of the background error covariances in generating a realistic troposphere to mesosphere water vapour analysis.
Water vapor transport in the lower mesosphere of the subtropics: a trajectory analysis
Authors: Flury T. , Müller S. C. , Hocke K. , Kämpfer N.
Published: April 2010

Abstract. The Institute of Applied Physics operates an airborne microwave radiometer that measures the rotational transition line of water vapor at 183.3 GHz. Measurements were acquired on board a Learjet once a year in the period 1998 to 2006. Water vapor profiles are retrieved for the altitude range from 15 to 75 km along the flight track. We report on a water vapor enhancement in the lower mesosphere above India and the Arabic Sea measured on our flight mission in November 2005 conducted during EC-project SCOUT-O3. The flight led from Switzerland to Australia and back. We find an enhancement of up to 25% in the lower mesospheric H2O volume mixing ratio measured on the return flight one week after the outward flight. The origin of the air is traced back by means of a trajectory model in the lower mesosphere. During the outward flight the air came from the Carribean and crossed the Atlantic Ocean. On the return flight the air came from China and orginated from mid latitudes. Thus the large variability of H2O VMR during our flight is explained by a change of the winds in the lower mesosphere.
Detection of reactive nitrogen containing particles in the tropopause region – evidence for a tropical nitric acid trihydrate (NAT) belt
Authors: Voigt C. , Schlager H. , Roiger A. , Stenke A. , de Reus M. , Borrmann S. , Jensen E. , Schiller C. , Konopka P. , Sitnikov N.
Published: April 2010

Abstract. The detection of nitric acid trihydrate (NAT, HNO3×3H2O) particles in the tropical transition layer (TTL) harmonizes our understanding of polar stratospheric cloud formation. Large reactive nitrogen (NOy) containing particles were observed on 8 August 2006 by instruments onboard the high altitude research aircraft M55-Geophysica near and below the tropical tropopause. The particles, most likely NAT, have diameters less than 6 μm and concentrations below 10−4 cm−3. The NAT particle layer was repeatedly detected at altitudes between 15.1 and 17.5 km over extended areas of 9.5 to 17.2° N and 1.5° W to 2.7° E above the African continent. Satellite observations suggest that the NAT particles could have nucleated on ice fed by convective activity. Once nucleated, the NAT particles can slowly grow within the TTL for days, while being transported over long distances. Their in-situ detection combined with global model simulations of the NAT supersaturation near the tropical tropopause indicate the potential for a tropical tropopause NAT particle belt.
Quality assurance of the Brewer UV measurements in Finland
Authors: Lakkala K. , Arola A. , Heikkilä A. , Kaurola J. , Koskela T. , Kyrö E. , Lindfors A. , Meinander O. , Tanskanen A. , Gröbner J. , Hülsen G.
Published: April 2010

Abstract. The quality assurance of the two Brewer spectrophotometers of the Finnish Meteorological Institute is discussed in this paper. The complete data processing chain from raw signal to high quality spectra is presented. The quality assurance includes daily maintenance, laboratory characterizations, calculation of long term spectral responsivity, data processing and quality assessment. The cosine correction of the measurements is based on a new method, and included in the data processing software. The results showed that the actual cosine correction factor of the Finnish Brewers can vary between 1.08–1.13 and 1.08–1.12, respectively, depending on the sky radiance distribution and wavelength. The temperature characterization showed a linear temperature dependence between the internal temperature and the photon counts per cycle, and a temperature correction was used for correcting the measurements. The long term spectral responsivity was calculated using time series of several lamps using two slightly different methods. The long term spectral responsivity was scaled to the irradiance scale of the Helsinki University of Technology (HUT) for the whole measurement time periods 1990–2006 and 1995–2006 for Sodankylä and Jokioinen, respectively. Both Brewers have participated in many international spectroradiometer comparisons, and have shown good stability. The differences between the Brewers and the portable reference spectroradiometer QASUME have been within 5% during 2002–2007.
Parameterizing ice nucleation rates for cloud modeling using contact angle and activation energy derived from laboratory data
Authors: Chen J.-P. , Hazra A. , Levin Z.
Published: April 2010

Abstract. The rate of ice nucleation in clouds is not easily determined and large discrepancies exist between model predictions and actual ice crystal concentration measured in clouds. In an effort to improve the parameterization of ice nucleating in cloud models, we investigate the rate of heterogeneous ice nucleation under specific ambient conditions by knowing the sizes as well as two thermodynamic parameters of the ice nuclei – contact angle and activation energy. Laboratory data of freezing and deposition nucleation modes were analyzed to derive inversely the two thermodynamic parameters for a variety of ice nuclei, including mineral dusts, bacteria, pollens, and soot particles. The analysis considered the Zeldovich factor for the adjustment of ice germ formation, as well as the solute and curvature effects on surface tension, the latter effects have strong influence on the contact angle. Contact angle turns out to be a more important factor than the activation energy in discriminating the nucleation capabilities of various ice nuclei species. By extracting these thermodynamic parameters, laboratory results can be converted into a formulation that follows classical nucleation theory, which then has the flexibility of incorporating factors such as the solute effect and curvature effect that were not considered in the experiments.
Size-dependent activation of aerosols into cloud droplets at a subarctic background site during the second Pallas Cloud Experiment (2nd PaCE): method development and data evaluation
Authors: Anttila T. , Vaattovaara P. , Komppula M. , Hyvärinen A.-P. , Lihavainen H. , Kerminen V.-M. , Laaksonen A.
Published: April 2010

Abstract. In situ measurements of aerosol water uptake and activation of aerosols into cloud droplets provide information on how aerosols influence the microphysical properties of clouds. Here we present a computational scheme that can be used in connection with such measurements to assess the influence of the particle chemical composition and mixing state (in terms of the water uptake) on the cloud nucleating ability of particles. Additionally, it provides an estimate for the peak supersaturation of water vapour reached during the formation of the observed cloud(s). The method was applied in interpreting results of a measurement campaign that focused on aerosol-cloud interactions taking place at a subarctic background site located in northern Finland (second Pallas Cloud Experiment, 2nd PaCE). A set of case studies was conducted, and the observed activation behavior could be successfully explained by a maximum supersaturation that varied between 0.18 and 0.26% depending on the case. In these cases, the diameter corresponding to the activated fraction of 50% was in the range of 110–140 nm, and the particles were only moderately water soluble with hygroscopic growth factors varying between 1.1 and 1.4. The conducted analysis showed that the activated fractions and the total number of particles acting as CCN are expected to be highly sensitive to the particle hygroscopicity. For example, the latter quantity varied over a factor between 1.8 and 3.1, depending on the case, when the mean hygroscopic growth factors were varied by 10%. Another important conclusion is that size-dependent activation profiles carries information on the mixing state of particles.
The aerosol distribution in Europe derived with the Community Multiscale Air Quality (CMAQ) model: comparison to near surface in situ and sunphotometer measurements
Authors: Matthias V.
Published: April 2010

Abstract. The aerosol distribution in Europe was simulated with the Community Multiscale Air Quality (CMAQ) model system for the years 2000 and 2001. The results were compared with daily averages of PM10 measurements taken in the framework of EMEP and with aerosol optical depth (AOD) values measured within Aeronet. The modelled total aerosol mass is typically about 30–60% lower than the corresponding measurements. However a comparison of the chemical composition of the aerosol revealed a considerably better agreement between the modelled and the measured aerosol components for ammonium, nitrate and sulfate, which are on average only 15–20% underestimated. Sligthly worse agreement was determined for sea salt, that was only avaliable at two sites. The largest discrepancies result from the aerosol mass which was not chemically specified by the measurements. The agreement between measurements and model is better in winter than in summer. The modelled organic aerosol mass is higher in summer than in winter but it is significantly underestimated by the model. This could be the main reason for the discrepancies between measurements and model results. The probability distribution function of the PM10 measurements follows a log-normal distribution at most sites. The model is only able to reproduce this distribution function at non-coastal low altitude stations. The AOD derived from the model results is 20–70% lower than the values observed within Aeronet. This is mainly attributed to the missing aerosol mass in the model. The day-to-day variability of the AOD and the log-normal distribution functions are quite well reproduced by the model. The seasonality on the other hand is underestimated by the model results because better agreement is achieved in winter.
Detection of ship tracks in ATSR2 satellite imagery
Authors: Campmany E. , Grainger R. G. , Dean S. M.
Published: April 2010

Abstract. Ships modify cloud microphysics by adding cloud condensation nuclei (CCN) to a developing or existing cloud. These create lines of larger reflectance in cloud fields that are observed in satellite imagery. Ship tracks are most frequently seen off the west coast of California, and the Atlantic coast of both west Africa and south-western Europe. In order to automate their detection within the Along Track Scanning Radiometer 2 (ATSR2) data set an algorithm was developed and integrated with the Global Retrieval of ATSR Cloud Parameters and Evaluation (GRAPE) processing chain. The algorithm firstly identifies intensity ridgelets in clouds which have the potential to be part of a ship track. This identification is done by comparing each pixel with its surrounding ones. If the intensity of three adjacent pixels is greater than the intensity of its neighbours, then it is classified as a ridgelet. These ridgelets are then connected together, according to a set of connectivity rules, to form tracks which are classed as ship tracks if they are long enough. The algorithm has been applied to two years of ATSR2 data. A month of results have been compared with other satellite datasets to validate the algorithm. There is a high ratio of false detections. Nevertheless the global distribution of ship tracks shows a similar pattern to the ship emissions distribution.
Applying the CPCB setup to study the hygroscopicity and composition of freshly-formed 2–9 nm particles in boreal forest
Authors: Riipinen I. , Manninen H. E. , Yli-Juuti T. , Boy M. , Sipilä M. , Ehn M. , Junninen H. , Petäjä T. , Kulmala M.
Published: April 2010

Abstract. Measurements on the composition of nanometer-sized atmospheric particles are the key to understand which vapors participate in the secondary aerosol formation processes. Knowledge on these processes is crucial in assessing the climatic effects of secondary aerosol formation. We present data of >2 nm particle concentrations and their hygroscopicity measured with the Condensation Particle Counter Battery (CPCB) at a boreal forest site in Hyytiälä, Finland, during spring 2006. This is the first time such results on the hygroscopicity and composition of the freshly formed atmospheric clusters as small as 2 nm have been reported – bringing us closer to online measurements of the compounds participating in atmospheric particle formation. The data reveal that during new particle formation events, the smallest particles activate for growth at clearly smaller sizes in water than in butanol vapor. However, even at 2–4 nm, the particles are less hygroscopic than ammonium sulfate or sulfuric acid, which are often referred to as the most likely compounds present in atmospheric nucleation. This observation points to the presence of water-soluble organics, even at the very first steps on particle formation. The water-affinity of the particles decreases with size, indicating that the vapors that participate in the first steps of the particle formation and growth are more hygroscopic than the vapors contributing to the later stages of the growth. This suggests that the relative role of less hygroscopic organics in atmospheric particle growth increases as a function of particle size.
Mass concentrations of black carbon measured by four instruments in the middle of Central East China in June 2006
Authors: Kanaya Y. , Komazaki Y. , Pochanart P. , Liu Y. , Akimoto H. , Gao J. , Wang T. , Wang Z.
Published: April 2010

Abstract. Mass concentrations of black carbon (BC) were determined in June 2006 at the top of Mount Tai (36.26° N, 117.11° E, 1534 m a.s.l.), located in the middle of Central East China, using four different instruments: a multi-angle absorption photometer (5012 MAAP, Thermo), a particle soot absorption photometer (PSAP, Radiance Research), an ECOC semi-continuous analyzer (Sunset Laboratory) and an Aethalometer (AE-21, Magee Scientific). High correlation coefficients (R2>0.88) were obtained between the measurements of the BC mass concentrations by the different instruments. From the range of the slopes of the linear least-square fittings, we concluded that the BC concentrations regionally-representative of the area were measured in a range with a maximum-to-minimum ratio of 1.5 (an exception was that the BC (PM2.5) concentrations derived from MAAP were ~2 times higher than the optical measurements (PM2.5) derived from the ECOC analyzer). This range is significant, but is still sufficiently narrow to better constrain the large and highly uncertain emission rate of BC from China. In detail, two optical instruments (the MAAP instrument and the PSAP instrument equipped with a heated inlet (400°C)) tended to give higher concentrations than the thermal EC concentrations observed by the ECOC analyzer. The ratios of optical BC to thermal EC showed a positive correlation with the OC/EC ratio reported by the ECOC analyzer, suggesting two possibilities. One is that the optical instruments overestimated BC concentrations in spite of careful cancellation of the scattering effect in the MAAP instrument and the expected evaporation of volatile species by heating the inlet of the PSAP instrument. The other is that the determined split points between OC and EC were too late when a large amount of OC underwent charring during the analysis, resulting in an underestimation of EC by the ECOC analyzer. High ratios of optical BC to thermal EC were recorded when the NOx/NOy ratio was low, implying the coating of the particles became thicker in the aged air mass and resulted in the optical instruments overestimating BC concentrations owing to the lensing effect.
Hydroxyl radicals in the tropical troposphere over the Suriname rainforest: airborne measurements
Authors: Martinez M. , Harder H. , Kubistin D. , Rudolf M. , Bozem H. , Eerdekens G. , Fischer H. , Gurk C. , Klüpfel T. , Königstedt R. , Parchatka U. , Schiller C. L. , Stickler A. , Williams J. , Lelieveld J.
Published: April 2010

Abstract. Direct measurements of OH and HO2 over a tropical rainforest were made for the first time during the GABRIEL campaign in October 2005, deploying the custom-built HORUS instrument (HydrOxyl Radical measurement Unit based on fluorescence Spectroscopy), adapted to fly in a Learjet wingpod. Biogenic hydrocarbon emissions were expected to strongly reduce the OH and HO2 mixing ratios as the air is transported from the ocean over the forest. However, surprisingly high mixing ratios of both OH and HO2 were encountered in the boundary layer over the rainforest. The HORUS instrumentation and calibration methods are described in detail and the measurement results obtained are discussed. The extensive dataset collected during GABRIEL, including measurements of many other trace gases and photolysis frequencies, has been used to quantify the main sources and sinks of OH. Comparison of these measurement-derived formation and loss rates of OH indicates strong previously overlooked recycling of OH in the boundary layer over the tropical rainforest, occurring in chorus with isoprene emission.
Effects of sea surface winds on marine aerosols characteristics and impacts on longwave radiative forcing over the Arabian Sea
Authors: Nair Vijayakumar S. , Suresh Babu S. , Satheesh S. K. , Krishna Moorthy K.
Published: April 2010

Abstract. Collocated measurements of spectral aerosol optical depths (AODs), total and BC mass concentrations, and number size distributions of near surface aerosols, along with sea surface winds, made onboard a scientific cruise over southeastern Arabian Sea, are used to delineate the effects of changes in the wind speed on aerosol properties and its implication on the shortwave and longwave radiative forcing. The results indicated that an increase in the sea-surface wind speed from calm to moderate (<1 to 8 m s−1) values results in a selective increase of the particle concentrations in the size range 0.5 to 5 μm, leading to significant changes in the size distribution, increase in the mass concentration, decrease in the BC mass fraction, a remarkable increase in AODs in the near infrared and a flattening of the AOD spectrum. The consequent increase in the longwave direct radiative forcing almost entirely offsets the corresponding increase in the short wave direct radiative forcing (or even overcompensates) at the top of the atmosphere; while the surface forcing is offset by about 50%.