bluuebunny/crossref_metadata_2025 huggingface dataset:
Technical Note: Simulation of detailed aerosol chemistry on the global scale using MECCA-AERO
Authors: Kerkweg A. , Sander R. , Tost H. , Jöckel P. , Lelieveld J.
Published: April 2010

Abstract. We present the MESSy submodel MECCA-AERO, which simulates both aerosol and gas phase chemistry within one comprehensive mechanism. Including the aerosol phase into the chemistry mechanism increases the stiffness of the resulting set of differential equations. The numerical aspects of the approach followed in MECCA-AERO are presented. MECCA-AERO requires input of an aerosol dynamical/microphysical model to provide the aerosol size and particle number information of the modes/bins for which the chemistry is explicitly calculated. Additional precautions are required to avoid the double counting of processes, especially for sulphate in the aerosol dynamical and the chemistry model. This coupling is explained in detail. To illustrate the capabilities of the new aerosol submodel, examples for species usually treated in aerosol dynamical models are shown. The aerosol chemistry as provided by MECCA-AERO is very sumptuous and not readily applicable for long-term simulations, though it provides a reference to evaluate simplified approaches.
Chemical characterization of the inorganic fraction of aerosols and mechanisms of the neutralization of atmospheric acidity in Athens, Greece
Authors: Karageorgos E. T. , Rapsomanikis S.
Published: April 2010

Abstract. The PM10 mass concentration levels and inorganic chemical composition were determined on 12-h resolution sampling during August 2003 and March 2004, in the centre of Athens, Greece. The August 2003 campaign mean PM10 mass concentration, obtained by Beta Attenuation at 5 m above ground in Athinas Street, was 56 μg m−3 while the corresponding value for March 2004 was 92 μg m−3. In both campaigns the E.U. imposed daily limit of 50 μg m−3 was exceeded on several days. During the March campaign, in Athinas Street, additionally obtained DSFU-PM10 (PM10-2.5+PM2.5) gravimetric mass concentrations (mean: 121 μg m−3) in the "breathing zone", at 1.5 m above ground were significantly higher compared to the respective mean PM10 mass concentrations obtained by the same method at 25 m above ground, in a second site (AEDA; mean: 86 μg m−3) also in the centre of the city. The above findings suggest that, for a realistic estimation of the exposure of citizens to particulate matter, PM10 sampling in the "breathing zone" (1.5–3 m above ground) is necessary. Such data are presented for the first time for the centre of Athens. In both campaigns, calcium was found to be the predominant component of the coarse fraction while crust-related aluminosilicates and iron were the other major components. The above elements constitute the most important components of the fine fraction, together with the predominant sulphur. All toxic metals were found in concentrations below the established air quality limits, and most of them in lower concentrations compared to older studies. Lead in particular, appeared mostly in the fine fraction and in very low concentrations compared to studies dating more than a decade back. The predominant ions of the coarse fraction have been found to be Ca2+, NO3−, Na+ and Cl−, while SO42−, Ca2+ and NH4+ were the major ionic components of the fine fraction. In the fine particles, a low molar ratio of NH4+/SO42− indicated an ammonium-poor ambient air, and together with inter-ionic correlations suggested that atmospheric ammonia is the major neutralizing agent of sulfate, while being insufficient to neutralize it to full extend. The formation of NH4NO3 is therefore not favored and additional contribution to the neutralization of acidity has been shown to be provided by Ca2+ and Mg2+. In the coarse particle fraction, the predominantly abundant Ca2+ has been found to correlate well with NO3− and SO42−, indicating its role as important neutralizing agent in this particle size range. The proximity of the location under study to the sea explains the important concentrations of salts with marine origin like NaCl and MgCl2 that were found in the coarse fraction, while chloride depletion in the gaseous phase was found to be limited to the fine particulate fraction. Total analyzed inorganic mass (elemental+ionic) was found to be ranging between approximately 25–33% of the total coarse particle mass and 35–42% of the total fine particle mass.
Understanding the kinetics of the ClO dimer cycle
Authors: von Hobe M. , Salawitch R. J. , Canty T. , Keller-Rudek H. , Moortgat G. K. , Grooß J.-U. , Müller R. , Stroh F.
Published: April 2010

Abstract. Among the major factors controlling ozone loss in the polar vortices in winter/spring is the kinetics of the ClO dimer catalytic cycle. Here, we propose a strategy to test and improve our understanding of these kinetics by comparing and combining information on the thermal equilibrium between ClO and Cl2O2, the rate of Cl2O2 formation, and the Cl2O2 photolysis rate from laboratory experiments, theoretical studies and field observations. Concordant with a number of earlier studies, we find considerable inconsistencies of some recent laboratory results with rate theory calculations and stratospheric observations of ClO and Cl2O2. The set of parameters for which we find the best overall consistency – namely the ClO/Cl2O2 equilibrium constant suggested by Plenge et al. (2005), the Cl2O2 recombination rate constant reported by Nickolaisen et al. (1994) and Cl2O2 photolysis rates based on absorption cross sections in the range between the JPL 2006 assessment and the laboratory study by Burkholder et al. (1990) – is not congruent with the latest recommendations given by the JPL and IUPAC panels and does not represent the laboratory studies currently regarded as the most reliable experimental values. We show that the incorporation of new Pope et al. (2007) Cl2O2 absorption cross sections into several models, combined with best estimates for other key parameters (based on either JPL and IUPAC evaluations or on our study), results in severe model underestimates of observed ClO and observed ozone loss rates. This finding suggests either the existence of an unknown process that drives the partitioning of ClO and Cl2O2, or else some unidentified problem with either the laboratory study or numerous measurements of atmospheric ClO. Our mechanistic understanding of the ClO/Cl2O2 system is grossly lacking, with severe implications for our ability to simulate both present and future polar ozone depletion.
A modeling analysis of a heavy air pollution episode occurred in Beijing
Authors: An X. , Zhu T. , Wang Z. , Li C. , Wang Y.
Published: April 2010

Abstract. The concentrations of fine particulate matter (PM) and ozone in Beijing often exceed healthful levels in recent years, therefore China is to taking steps to improve Beijing's air quality for the 2008 Olympic Games. In this paper, the Models-3 Community Multiscale Air Quality (CMAQ) Modeling System was used to investigate a heavy air pollution episode in Beijing during 3–7 April 2005 to obtain the basic information of how heavy air pollution formed and the contributions of local sources and surround emissions. The modeling domain covered from East Asia with four nested grids with 81 to 3 km horizontal resolution focusing on urban Beijing. This was coupled with a regional emissions inventory with a 10 km resolution and a local 1 km Beijing emissions database. The trend of predicted concentrations of various pollutants agreed reasonably well with the observations and captured the main features of this heavy pollution episode. The simulated column concentration distribution of PM was correlated well with the MODIS remote sensing products. Control runs with and without Beijing emissions were conducted to quantify the contributions of non-Beijing sources (NBS) to the Beijing local air pollution. The contributions of NBS to each species differed spatially and temporally with the order of PM2.5>PM10>SO2> soil for this episode. The percentage contribution of NBS to fine particle (PM2.5) in Beijing was averaged about 39%, up to 53% at the northwest of urban Beijing and only 15% at southwest. The spatial distribution of NBS contributions for PM10 was similar to that for PM2.5, with a slightly less average percentage of about 30%. The average NBS contributions for SO2 and soil (diameter between 2.5 μm and 10 μm) were 18% and 10%. In addition, the pollutant transport flux was calculated and compared at different levels to investigate transport pathway and magnitude. It was found that the NBS contribution correlated with the transport flux, contributing 60% of PM10 concentration in Beijing at the time of transport flux peak during a strong episode with a transport path from southwest to northeast.
The impact of diurnal variations of air traffic on contrail radiative forcing
Authors: Stuber N. , Forster P.
Published: April 2010

Abstract. We combined high resolution aircraft flight data from the EU Fifth Framework Programme project AERO2k with analysis data from the ECMWF's integrated forecast system to calculate diurnally resolved 3-D contrail cover. We scaled the contrail cover in order to match observational data for the Bakan area (eastern-Atlantic/western-Europe). We found that less than 40% of the global distance travelled by aircraft is due to flights during local night time. Yet, due to the cancellation of shortwave and longwave effects during daytime, night time flights contribute a disproportional 60% to the global annual mean forcing. Under clear sky conditions the night flights contribute even more disproportionally at 76%. There are pronounced regional variations in night flying and the associated radiative forcing. Over parts of the North Atlantic flight corridor 75% of air traffic and 84% of the forcing occurs during local night, whereas only 35% of flights are during local night in South-East Asia, yet these contribute 68% of the radiative forcing. In general, regions with a significant local contrail radiative forcing are also regions for which night time flights amount to less than half of the daily total of flights. Therefore, neglecting diurnal variations in air traffic/contrail cover by assuming a diurnal mean contrail cover can over-estimate the global mean radiative forcing by up to 30%.
Reformulating atmospheric aerosol thermodynamics and hygroscopic growth into fog, haze and clouds
Authors: Metzger S. , Lelieveld J.
Published: April 2010

Abstract. Modeling atmospheric aerosol and cloud microphysics is rather complex, even if chemical and thermodynamical equilibrium is assumed. We show, however, that the thermodynamics can be considerably simplified by reformulating equilibrium to consistently include water, and transform laboratory-based concepts to atmospheric conditions. We generalize the thermodynamic principles that explain hydration and osmosis – merely based on solute solubilities – to explicitly account for the water mass consumed by hydration. As a result, in chemical and thermodynamical equilibrium the relative humidity (RH) suffices to determine the saturation molality, including solute and solvent activities (and activity coefficients), since the water content is fixed by RH for a given aerosol concentration and type. As a consequence, gas/liquid/solid aerosol equilibrium partitioning can be solved analytically and non-iteratively. Our new concept enables an efficient and accurate calculation of the aerosol water mass and directly links the aerosol hygroscopic growth to fog, haze and cloud formation. We apply our new concept in the 3rd Equilibrium Simplified Aerosol Model (EQSAM3) for use in regional and global chemistry-transport and climate models. Its input is limited to the species' solubilities from which a newly introduced stoichiometric coefficient for water is derived. Analogously, we introduce effective stoichiometric coefficients for the solutes to account for complete or incomplete dissociation. We show that these coefficients can be assumed constant over the entire activity range and calculated for various inorganic, organic and non-electrolyte compounds, including alcohols, sugars and dissolved gases. EQSAM3 calculates the aerosol composition and gas/liquid/solid partitioning of mixed inorganic/organic multicomponent solutions and the associated water uptake for almost 100 major compounds. It explicitly accounts for particle hygroscopic growth by computing aerosol properties such as single solute molalities, molal based activities, including activity coefficients for volatile compounds, efflorescence and deliquescence relative humidities of single solute and mixed solutions. Various applications and a model inter-comparison indicate that a) the application is not limited to dilute binary solutions, b) sensitive aerosol properties such as hygroscopic growth and the pH of binary and mixed inorganic/organic salt solutions up to saturation can be computed accurately, and c) aerosol water is central in modeling atmospheric chemistry, visibility, weather and climate.
Hygroscopic growth of sub-micrometer and one-micrometer aerosol particles measured during ACE-Asia
Authors: Massling A. , Leinert S. , Wiedensohler A. , Covert D.
Published: April 2010

Abstract. Hygroscopic properties of aerosol particles in the sub-micrometer and one-micrometer size ranges were measured during the ACE-Asia study (Aerosol Characterization Experiment-Asia) in spring 2001. The measurements took place off the coasts of Japan, Korea, and China. All instruments contributing to this study were deployed in a container on the forward deck of the NOAA Research Vessel Ronald H. Brown. Air masses with primarily marine influence and air masses from the Asian continent affected by both anthropogenic sources and by the transport of desert dust aerosol were encountered during the cruise. Results showed very different hygroscopic behavior in the sub-micrometer size range compared to the one-micrometer size range. In general, for all continentally influenced air masses, the one-micrometer particle population was characterized by two different particle groups – a nearly hydrophobic fraction with growth factors around 1.0 representative of dust particles and a sea salt fraction with hygroscopic growth factors around 2.0. The number fraction of dust particles was generally about 60% independent of long-range air mass origin. For sub-micrometer particles, a dominant, more hygroscopic particle fraction with growth factors between 1.5 and 1.9 (depending on dry particle size) consistent with ammonium sulfate or non-neutralized sulfates as major component was always found. In marine air masses and for larger sizes within the sub-micrometer range (Dp=250 and 350 nm), a sea salt fraction with growth factors between 2.0 and 2.1 was also observed. For all other air masses, the more hygroscopic particle fraction in the sub-micrometer size range was mostly accompanied by a less hygroscopic particle fraction with growth factors between 1.20 and 1.55 depending on both the continental sources and the dry particle size. Number fractions of this particle group varied between 4 and 39% depending on dry particle size and air mass type. Nearly hydrophobic particles indicating dust particles in the sub-micrometer size regime were only found for particles with Dp=250 and 350 nm during a time period when the aerosol was influenced by transport from Asian desert regions.
Contribution of mixing to upward transport across the tropical tropopause layer (TTL)
Authors: Konopka P. , Günther G. , Müller R. , dos Santos F. H. S. , Schiller C. , Ravegnani F. , Ulanovsky A. , Schlager H. , Volk C. M. , Viciani S. , Pan L. L. , McKenna D.-S. , Riese M.
Published: April 2010

Abstract. During the second part of the TROCCINOX campaign that took place in Brazil in early 2005, chemical species were measured on-board the high-altitude research aircraft Geophysica (ozone, water vapor, NO, NOy, CH4 and CO) in the altitude range up to 20 km (or up to 450 K potential temperature), i.e. spanning the entire TTL region roughly extending between 350 and 420 K. Here, analysis of transport across the TTL is performed using a new version of the Chemical Lagrangian Model of the Stratosphere (CLaMS). In this new version, the stratospheric model has been extended to the earth surface. Above the tropopause, the isentropic and cross-isentropic advection in CLaMS is driven by meteorological analysis winds and heating/cooling rates derived from a radiation calculation. Below the tropopause, the model smoothly transforms from the isentropic to the hybrid-pressure coordinate and, in this way, takes into account the effect of large-scale convective transport as implemented in the vertical wind of the meteorological analysis. As in previous CLaMS simulations, the irreversible transport, i.e. mixing, is controlled by the local horizontal strain and vertical shear rates. Stratospheric and tropospheric signatures in the TTL can be seen both in the observations and in the model. The composition of air above ≈350 K is mainly controlled by mixing on a time scale of weeks or even months. Based on CLaMS transport studies where mixing can be completely switched off, we deduce that vertical mixing, mainly driven by the vertical shear in the tropical flanks of the subtropical jets and, to some extent, in the the outflow regions of the large-scale convection, offers an explanation for the upward transport of trace species from the main convective outflow at around 350 K up to the tropical tropopause around 380 K.
Global trends in visibility: implications for dust sources
Authors: Mahowald N. M. , Ballantine J. A. , Feddema J. , Ramankutty N.
Published: April 2010

Abstract. There is a large uncertainty in the relative roles of human land use, climate change and carbon dioxide fertilization in changing desert dust source strength over the past 100 years, and the overall sign of human impacts on dust is not known. We used visibility data from meteorological stations in dusty regions to assess the anthropogenic impact on long term trends in desert dust emissions. We did this by looking at time series of visibility derived variables and their correlations with precipitation, drought, winds, land use and grazing. Visibility data are available at thousands of stations globally from 1900 to the present, but we focused on 357 stations with more than 30 years of data in regions where mineral aerosols play a dominant role in visibility observations. We evaluated the 1974 to 2003 time period because most of these stations have reliable records only during this time. We first evaluated the visibility data against AERONET aerosol optical depth data, and found that only in dusty regions are the two moderately correlated. Correlation coefficients between visibility-derived variables and AERONET optical depths indicate a moderate correlation (0.47), consistent with capturing about 20% of the variability in optical depths. Two visibility-derived variables appear to compare the best with AERONET observations: the fraction of observations with visibility less than 5 km (VIS5) and the surface extinction (EXT). Regional trends show that in many dusty places, VIS5 and EXT are statistically significantly correlated with the Palmer drought severity index (based on precipitation and temperature) or surface wind speeds, consistent with dust temporal variability being largely driven by meteorology. This is especially true for North African and Chinese dust sources, but less true in the Middle East, Australia or South America, where there are not consistent patterns in the correlations. Climate indices such as El Nino or the North Atlantic Oscillation are not correlated with visibility-derived variables in this analysis. There are few stations where visibility measures are correlated with cultivation or grazing estimates on a temporal basis, although this may be a function of the very coarse temporal resolution of the land use datasets. On the other hand, spatial analysis of the visibility data suggests that natural topographic lows are not correlated with VIS5 or EXT, but land use is correlated at a moderate level. This analysis is consistent with land use being important in some regions, but meteorology driving interannual variability during 1974–2003.
Hydrocarbon fluxes above a Scots pine forest canopy: measurements and modeling
Authors: Rinne J. , Taipale R. , Markkanen T. , Ruuskanen T. M. , Hellén H. , Kajos M. K. , Vesala T. , Kulmala M.
Published: April 2010

Abstract. We measured the fluxes of several hydrocarbon species above a Scots pine (Pinus sylvestris) stand using disjunct eddy covariance technique with proton transfer reaction – mass spectrometry. The measurements were conducted during four days in July at SMEAR II research station in Hyytiälä, Finland. Compounds which showed significant emission fluxes were methanol, acetaldehyde, acetone, and monoterpenes. A stochastic Lagrangian transport model with simple chemical degradation was applied to assess the sensitivity of the above canopy fluxes to chemistry. According to the model, the chemical degradation had a minor effect on the fluxes measured in this study but may have a major effect on the vertical flux profiles of more reactive compounds, such as sesquiterpenes. The monoterpene fluxes derived using M81 and M137 had a systematic difference with the latter one being higher. These fluxes followed the traditional exponential temperature dependent emission algorithm but were considerably higher than the fluxes measured before at the same site. The normalized monoterpene emission potentials at 30°C, obtained using the temperature dependence coefficient of 0.09°C−1, were 2.0 μg gdw−1 h−1 and 2.5 μg gdw−1 h−1, for fluxes derived using M81 and M137.
Simulation of hurricane response to suppression of warm rain by sub-micron aerosols
Authors: Rosenfeld D. , Khain A. , Lynn B. , Woodley W. L.
Published: April 2010

Abstract. The feasibility of hurricane modification was investigated for hurricane Katrina using the Weather Research and Forecasting Model (WRF). The possible impact of seeding of clouds with submicron cloud condensation nuclei (CCN) on hurricane structure and intensity as measured by nearly halving of the area covered by hurricane force winds was simulated by "turning–off" warm rain formation in the clouds at Katrina's periphery (where wind speeds were less than 22 m s−1). This simplification of the simulation of aerosol effects is aimed at evaluating the largest possible response. This resulted in the weakening of the hurricane surface winds compared to the "non-seeded" simulated storm during the first 24 h within the entire tropical cyclone (TC) area compared to a control simulation without warm rain suppression. Later, the seeding-induced evaporative cooling at the TC periphery led to a shrinking of the eye and hence to some increase in the wind within the small central area of the TC. Yet, the overall strength of the hurricane, as defined by the area covered by hurricane force winds, decreased in response to the suppressed warm rain at the periphery, as measured by a 25% reduction in the radius of hurricane force winds. In a simulation with warm rain suppression throughout the hurricane, the radius of the hurricane force winds was reduced by more than 42%, and although the diameter of the eye shrunk even further the maximum winds weakened. This shows that the main mechanism by which suppressing warm rain weakens the TC is the low level evaporative cooling of the un-precipitated cloud drops and the added cooling due to melting of precipitation that falls from above.
A semi-analytical method for calculating rates of new sulfate aerosol formation from the gas phase
Authors: Kazil J. , Lovejoy E. R.
Published: April 2010

Abstract. The formation of new aerosol from the gas phase is commonly represented in atmospheric modeling with parameterizations of the steady state nucleation rate. Present parameterizations are based on classical nucleation theory or on nucleation rates calculated with a numerical aerosol model. These parameterizations reproduce aerosol nucleation rates calculated with a numerical aerosol model only imprecisely. Additional errors can arise when the nucleation rate is used as a surrogate for the production rate of particles of a given size. We discuss these errors and present a method which allows a more precise calculation of steady state sulfate aerosol formation rates. The method is based on the semi-analytical solution of an aerosol system in steady state and on parameterized rate coefficients for H2SO4 uptake and loss by sulfate aerosol particles, calculated from laboratory and theoretical thermodynamic data.
Characteristics of aerosol and cloud particle size distributions in the tropical tropopause layer measured with optical particle counter and lidar
Authors: Iwasaki S. , Maruyama K. , Hayashi M. , Ogino S.-Y. , Ishimoto H. , Tachibana Y. , Shimizu A. , Matsui I. , Sugimoto N. , Yamashita K. , Saga K. , Iwamoto K. , Kamiakito Y. , Chabangborn A. , Thana B. , Hashizume M. , Koike T. , Oki T.
Published: April 2010

Abstract. An optical particle counter (OPC) is used in conjunction with lidar measurements to examine the characteristics of the particle size distribution in cirrus cloud in the tropical tropopause layer (TTL) over Thailand where the TTL is defined as the height at which temperature is lower than −75°C in this paper. Of 11 OPC launches, cirrus cloud was detected at 10–15 km high on 7 occasions, cirrus was detected in the TTL in 6 cases, and simultaneous OPC and lidar measurements were made on two occasions. Comparison of lidar and OPC measurements reveal that the cloud heights of cirrus in the TTL varies by several hundred meters over distances of tens kilometers; hence the height is not always horizontally uniform. The mode radii of particles constituting the clouds are estimated by lidar and OPC measurements to be less than approximately 10 μm. The regression lines of the particle size distribution with and without cirrus cloud exhibit similar features at equivalent radii of <0.8 μm. Enhancement in the integrated number concentration at radii greater than 0.8 μm indicates that liquid particles tend to be frozen at a radius of 0.8 μm, with cirrus clouds above 10 km exhibiting similar features. On the other hand, enhancement in the particle size distribution at radii greater than 0.9 μm and a peak at around 0.8 μm in the ratio of the standard deviation of count values to that of the Poisson distribution of the averaged count values are common features of cirrus clouds in the TTL, where the ratio shows the vertical homogeneity of the particle number. These typical features suggest that the transition from liquid, sulfuric acid aerosol, to ice is more observable in the TTL and the timing of freezing may vary with height in the TTL.
Technical Note: Interference errors in infrared remote sounding of the atmosphere
Authors: Sussmann R. , Borsdorff T.
Published: April 2010

Abstract. Classical error analysis in remote sounding distinguishes between four classes: "smoothing errors," "model parameter errors," "forward model errors," and "retrieval noise errors". For infrared sounding "interference errors", which, in general, cannot be described by these four terms, can be significant. Interference errors originate from spectral residuals due to "interfering species" whose spectral features overlap with the signatures of the target species. A general method for quantification of interference errors is presented, which covers all possible algorithmic implementations, i.e., fine-grid retrievals of the interfering species or coarse-grid retrievals, and cases where the interfering species are not retrieved. In classical retrieval setups interference errors can exceed smoothing errors and can vary by orders of magnitude due to state dependency. An optimum strategy is suggested which practically eliminates interference errors by systematically minimizing the regularization strength applied to joint profile retrieval of the interfering species. This leads to an interfering-species selective deweighting of the retrieval. Details of microwindow selection are no longer critical for this optimum retrieval and widened microwindows even lead to reduced overall (smoothing and interference) errors. Since computational power will increase, more and more operational algorithms will be able to utilize this optimum strategy in the future. The findings of this paper can be applied to soundings of all infrared-active atmospheric species, which include more than two dozen different gases relevant to climate and ozone. This holds for all kinds of infrared remote sounding systems, i.e., retrievals from ground-based, balloon-borne, airborne, or satellite spectroradiometers.
Source apportionment of the particulate PAHs at Seoul, Korea: impact of long range transport to a megacity
Authors: Lee J. Y. , Kim Y. P.
Published: April 2010

Abstract. Northeast Asia including China, Korea, and Japan is one of the world's largest fossil fuel consumption regions. Seoul, Korea, is a megacity in Northeast Asia. Its emissions of air pollutants can affect the region, and in turn it is also affected by regional emissions. To understand the extent of these influences, major sources of ambient particulate PAHs in Seoul were identified and quantified based on measurements made between August 2002 and December 2003. The chemical mass balance (CMB) model was applied. Seven major emission sources were identified based on the emission data in Seoul and Northeast Asia: Gasoline and diesel vehicles, residential coal use, coke ovens, coal power plants, biomass burning, and natural gas (NG) combustion. The major sources of particulate PAHs in Seoul during the whole measurement period were gasoline and diesel vehicles, together accounted for 31% of the measured particulate PAHs levels. However, the source contributions showed distinct daily and seasonal variations. High contributions of biomass burning and coal (residential and coke oven) were observed in fall and winter, accounting for 63% and 82% of the total concentration of PAHs, respectively. Since these sources were not strong in and around Seoul, they are likely to be related to transport from outside of Seoul, from China and/or North Korea. This implies that the air quality in a mega-city such as Seoul can be influenced by the long range transport of air pollutants such as PAHs.
On the efficiency of rocket-borne particle detection in the mesosphere
Authors: Hedin J. , Gumbel J. , Rapp M.
Published: April 2010

Abstract. Meteoric smoke particles have been proposed as a key player in the formation and evolution of mesospheric phenomena. Despite their apparent importance still very little is known about these particles. Important questions concern the smoke number density and size distribution as a function of altitude as well as the fraction of charged particles. Sounding rockets are used to measure smoke in situ, but aerodynamics has remained a major challenge. Basically, the small smoke particles tend to follow the gas flow around the payload rather than reaching the detector if aerodynamics is not considered carefully in the detector design. So far only indirect evidence for the existence of meteoric smoke has been available from measurements of heavy charge carriers. Quantitative ways are needed that relate these measured particle population to the atmospheric particle population. This requires in particular knowledge about the size-dependent, altitude-dependent and charge-dependent detection efficiency for a given instrument. In this paper, we investigate the aerodynamics for a typical electrostatic detector design. We first quantify the flow field of the background gas, then introduce particles in the flow field and determine their trajectories around the payload structure. We use two different models to trace particles in the flow field, a Continuous motion model and a Brownian motion model. Brownian motion is shown to be of basic importance for the smallest particles. Detection efficiencies are determined for three detector designs, including two with ventilation holes to allow airflow through the detector. Results from this investigation show that rocket-borne smoke detection with conventional detectors is largely limited to altitudes above 75 km. The flow through a ventilated detector has to be relatively large in order to significantly improve the detection efficiency.
Model study of the cross-tropopause transport of biomass burning pollution
Authors: Duncan B. N. , Strahan S. E. , Yoshida Y. , Steenrod S. D. , Livesey N.
Published: April 2010

Abstract. We present a modeling study of the troposphere-to-stratosphere transport (TST) of pollution from major biomass burning regions to the tropical upper troposphere and lower stratosphere (UT/LS). TST occurs predominately through 1) slow ascent in the tropical tropopause layer (TTL) to the LS and 2) quasi-horizontal exchange to the lowermost stratosphere (LMS). We show that biomass burning pollution regularly and significantly impacts the composition of the TTL, LS, and LMS. Carbon monoxide (CO) in the LS in our simulation and data from the Aura Microwave Limb Sounder (MLS) shows an annual oscillation in its composition that results from the interaction of an annual oscillation in slow ascent from the TTL to the LS and seasonal variations in sources, including a semi-annual oscillation in CO from biomass burning. The impacts of CO sources that peak when ascent is seasonally low are damped (e.g. Southern Hemisphere biomass burning) and vice-versa for sources that peak when ascent is seasonally high (e.g. extra-tropical fossil fuels). Interannual variation of CO in the UT/LS is caused primarily by year-to-year variations in biomass burning and the locations of deep convection. During our study period, 1994–1998, we find that the highest concentrations of CO in the UT/LS occurred during the strong 1997–1998 El Niño event for two reasons: i. tropical deep convection shifted to the eastern Pacific Ocean, closer to South American and African CO sources, and ii. emissions from Indonesian biomass burning were higher. This extreme event can be seen as an upper bound on the impact of biomass burning pollution on the UT/LS. We estimate that the 1997 Indonesian wildfires increased CO in the entire TTL and tropical LS (>60 mb) by more than 40% and 10%, respectively, for several months. Zonal mean ozone increased and the hydroxyl radical decreased by as much as 20%, increasing the lifetimes and, subsequently TST, of trace gases. Our results indicate that the impact of biomass burning pollution on the UT/LS is likely greatest during an El Niño event due to favorable dynamics and historically higher burning rates.
On using radon-222 and CO2 to calculate regional-scale CO2 fluxes
Authors: Hirsch A. I.
Published: April 2010

Abstract. Because of its ubiquitous release on land and well-characterized atmospheric loss, radon-222 has been very useful for deducing fluxes of greenhouse gases such as CO2, CH4, and N2O. It is shown here that the radon-tracer method, used in previous studies to calculate regional-scale greenhouse gas fluxes, returns a weighted-average flux (the flux field F weighted by the sensitivity of the measurements to that flux field, f) rather than an evenly-weighted spatial average flux. A synthetic data study using a Lagrangian particle dispersion model and modeled CO2 fluxes suggests that the discrepancy between the sensitivity-weighted average flux and evenly-weighted spatial average flux can be significant in the case of CO2, due to covariance between F and f for biospheric CO2 fluxes during the growing season and also for anthropogenic CO2 fluxes in general. A technique is presented to correct the radon-tracer derived fluxes to yield an estimate of evenly-weighted spatial average CO2 fluxes. A new method is also introduced for correcting the CO2 flux estimates for the effects of radon-222 radioactive decay in the radon-tracer method.
Characteristics and error estimation of stratospheric ozone and ozone-related species over Poker Flat (65° N, 147° W), Alaska observed by a ground-based FTIR spectrometer from 2001 to 2003
Authors: Kagawa A. , Kasai Y. , Jones N. B. , Yamamori M. , Seki K. , Murcray F. , Murayama Y. , Mizutani K. , Itabe T.
Published: April 2010

Abstract. It is important to obtain the year-to-year trend of stratospheric minor species in the context of global changes. An important example is the trend in global ozone depletion. The purpose of this paper is to report the accuracy and precision of measurements of stratospheric chemical species that are made at our Poker Flat site in Alaska (65° N, 147° W). Since 1999, minor atmospheric molecules have been observed using a Fourier-Transform solar-absorption infrared Spectrometer (FTS) at Poker Flat. Vertical profiles of the abundances of ozone, HNO3, HCl, and HF for the period from 2001 to 2003 were retrieved from FTS spectra using Rodgers' formulation of the Optimal Estimation Method (OEM). The accuracy and precision of the retrievals were estimated by formal error analysis. Errors for the total column were estimated to be 5.3%, 3.4%, 5.9%, and 5.3% for ozone, HNO3, HCl, and HF, respectively. The ozone vertical profiles were in good agreement with profiles derived from collocated ozonesonde measurements that were smoothed with averaging kernel functions that had been obtained with the retrieval procedure used in the analysis of spectra from the ground-based FTS (gb-FTS). The O3, HCl, and HF columns that were retrieved from the FTS measurements were consistent with Earth Probe/Total Ozone Mapping Spectrometer (TOMS) and HALogen Occultation Experiment (HALOE) data over Alaska within the error limits of all the respective datasets. This is the first report from the Poker Flat FTS observation site on a number of stratospheric gas profiles including a comprehensive error analysis.
Ozonolysis of α-pinene: parameterization of secondary organic aerosol mass fraction
Authors: Pathak R. K. , Presto A. A. , Lane T. E. , Stanier C. O. , Donahue N. M. , Pandis S. N.
Published: April 2010

Abstract. Existing parameterizations tend to underpredict the α-pinene aerosol mass fraction (AMF) or yield by a factor of 2–5 at low organic aerosol concentrations (<5 µg m−3). A wide range of smog chamber results obtained at various conditions (low/high NOx, presence/absence of UV radiation, dry/humid conditions, and temperatures ranging from 15–40°C) collected by various research teams during the last decade are used to derive new parameterizations of the SOA formation from α-pinene ozonolysis. Parameterizations are developed by fitting experimental data to a basis set of saturation concentrations (from 10−2 to 104 µg m−3) using an absorptive equilibrium partitioning model. Separate parameterizations for α-pinene SOA mass fractions are developed for: 1) Low NOx, dark, and dry conditions, 2) Low NOx, UV, and dry conditions, 3) Low NOx, dark, and high RH conditions, 4) High NOx, dark, and dry conditions, 5) High NOx, UV, and dry conditions. According to the proposed parameterizations the α-pinene SOA mass fractions in an atmosphere with 5 µg m−3 of organic aerosol range from 0.032 to 0.1 for reacted α-pinene concentrations in the 1 ppt to 5 ppb range.
GEM/POPs: a global 3-D dynamic model for semi-volatile persistent organic pollutants – Part 2: Global transports and budgets of PCBs
Authors: Huang P. , Gong S. L. , Zhao T. L. , Neary L. , Barrie L. A.
Published: April 2010

Abstract. Global transports and budgets of three PCBs were investigated with a 3-D dynamic model for semi-volatile persistent organic pollutants – GEM/POPs. Dominant pathways were identified for PCB transports in the atmosphere with a transport flux peaking below 8 km for gaseous and 14 km for particulate PCB28, and peaking below 4 km for gaseous and 6 km for particulate PCB180. The inter-continental transports of PCBs in the Northern Hemisphere (NH) are dominated in the zonal direction with their route changes regulated seasonally by the variation of westerly jet. The transport pathways from Europe and North Atlantic contributed the most PCBs to the Arctic. Inter-hemispheric transports of PCBs originated from the regions of Europe, Asia and North America in three different flow-paths, accompanying with easterly jet, Asian monsoon winds and trade winds. PCBs from the Southern Hemisphere (SH) could also be exported into the NH. According to the PCB emissions of year 2000, Europe, North America and Asia are the three largest sources of the three PCBs, contributing to the global background concentrations in the atmosphere, soil and water. Globally, PCB28 in soil and water has become a comparable source to the anthropogenic emissions while heavier PCBs such as PCB153 and 180 are still transporting into soil and water. For all three congeners, particulate PCBs are concentrated in the higher levels than gaseous PCBs. More than half of the particulate PCB28 could reach up to the stratosphere, while most of the heavier counter-parts (PCB153 and PCB180) are stored in the troposphere including boundary layer with more than 99% gaseous PCB180 below 6 km.
Evaluation of a new convective cloud field model: precipitation over the maritime continent
Authors: Graf H.-F. , Yang J.
Published: April 2010

Abstract. A convective cloud field model (CCFM) is substituted for a standard mass flux parameterisation of convective clouds in a limited area atmospheric model (REMO) and is tested for a whole annual cycle (July 1997 to June 1998) over the West Pacific Maritime Continent. REMO with CCFM is run in 0.5-degree resolution and the model at the lateral boundaries is forced 6-hourly by ECMWF reanalysis data. Simulated precipitation from runs with the standard convection parameterisation and with CCFM is compared against two sets of observations. The use of CCFM clearly improves the simulated precipitation patterns and total rainfall over the whole model domain. The distribution between large-scale and convective precipitation becomes more realistic. CCFM shows to be a useful concept to describe convective cloud spectra in atmospheric models, although there are still similar problems with occasionally extreme precipitation as in the original set-up of REMO.
Comparison and synergy of stratospheric ozone measurements by satellite limb sounders and the ground-based microwave radiometer SOMORA
Authors: Hocke K. , Kämpfer N. , Ruffieux D. , Froidevaux L. , Parrish A. , Boyd I. , von Clarmann T. , Steck T. , Timofeyev Y. M. , Polyakov A. V. , Kyrölä E.
Published: April 2010

Abstract. Stratospheric O3 profiles obtained by the satellite limb sounders Aura/MLS, ENVISAT/MIPAS, ENVISAT/GOMOS, SAGE-II, SAGE-III, UARS/HALOE are compared to coincident O3 profiles of the ground-based microwave radiometer SOMORA in Switzerland. Data from the various measurement techniques are within 10% at altitudes below 45 km. At altitudes 45–60 km, the relative O3 differences are within a range of 50%. Larger deviations at upper altitudes are attributed to larger relative measurement errors caused by lower O3 concentrations. The spatiotemporal characteristics of the O3 differences (satellite – ground station) are investigated by analyzing about 2300 coincident profile pairs of Aura/MLS (retrieval version 1.5) and SOMORA. The probability density function of the O3 differences is represented by a Gaussian normal distribution. The dependence of the O3 differences on the horizontal distance between the sounding volumes of Aura/MLS and SOMORA is derived. While the mean bias (Aura/MLS – SOMORA) is constant with increasing horizontal distance (up to 800 km), the standard deviation of the O3 differences increases from around 8 to 11% in the mid-stratosphere. Geographical maps yield azimuthal dependences and horizontal gradients of the O3 difference field around the SOMORA ground station. Coherent oscillations of O3 are present in the time series of Aura/MLS and SOMORA (e.g., due to traveling planetary waves). Ground- and space-based measurements often complement one another. We discuss the double differencing technique which allows both the cross-validation of two satellites by means of a ground station and the cross-validation of distant ground stations by means of one satellite. Temporal atmospheric noise in the geographical ozone map over Payerne is significantly reduced by combination of the data from SOMORA and Aura/MLS. These analyses illustrate the synergy of ground-based and space-based measurements.
Mixing between a stratospheric intrusion and a biomass burning plume
Authors: Brioude J. , Cooper O. R. , Trainer M. , Ryerson T. B. , Holloway J. S. , Baynard T. , Peischl J. , Warneke C. , Neuman J. A. , De Gouw J. , Stohl A. , Eckhardt S. , Frost G. J. , McKeen S. A. , Hsie E.-Y. , Fehsenfeld F. C. , Nédélec P.
Published: April 2010

Abstract. Ozone, carbon monoxide, aerosol extinction coefficient, acetonitrile, nitric acid and relative humidity measured from the NOAA P3 aircraft during the TexAQS/GoMACCS 2006 experiment, indicate mixing between a biomass burning plume and a stratospheric intrusion in the free troposphere above eastern Texas. Lagrangian-based transport analysis and satellite imagery are used to investigate the transport mechanisms that bring together the tropopause fold and the biomass burning plume originating in southern California, which may affect the chemical budget of tropospheric trace gases.
Mid-winter lower stratosphere temperatures in the Antarctic vortex: comparison between observations and ECMWF and NCEP operational models
Authors: Parrondo M. C. , Yela M. , Gil M. , von der Gathen P. , Ochoa H.
Published: April 2010

Abstract. Radiosonde temperature profiles from Belgrano (78° S) and other Antarctic stations have been compared with European Centre for Medium-Range Weather Forecasting (ECMWF) and National Centers for Environmental Prediction (NCEP) operational analyses during the winter of 2003. Results show good agreement between radiosondes and NCEP and a bias in the ECMWF model which is height and temperature dependent, being up to 3°C too cold at 80 and 25–30 hPa, and hence resulting in an overestimation of the predicted potential PSC areas. Here we show the results of the comparison and discuss the potential implications that this bias might have on the ozone depletion computed by Chemical Transport Models based on ECMWF temperature fields, after rejecting the possibility of a bias in the sondes at extreme low temperatures.
Water-side turbulence enhancement of ozone deposition to the ocean
Authors: Fairall C. W. , Helmig D. , Ganzeveld L. , Hare J.
Published: April 2010

Abstract. A parameterization for the deposition velocity of an ocean-reactive atmospheric gas (such as ozone) is developed. The parameterization is based on integration of the turbulent-molecular transport equation (with a chemical source term) in the ocean. It extends previous work that only considered reactions within the oceanic molecular sublayer. The sensitivity of the ocean-side transport to reaction rate and wind forcing is examined. A more complicated case with a much more reactive thin surfactant layer is also considered. The full atmosphere-ocean deposition velocity is obtained by matching boundary conditions at the interface. For an assumed ocean reaction rate of 103 s−1, the enhancement for ozone deposition by oceanic turbulence is found to be up to a factor of three for meteorological data obtained in a recent cruise off the East Coast of the U.S.