bluuebunny/crossref_metadata_2025 huggingface dataset:
A model study of ozone in the eastern Mediterranean free troposphere during MINOS (August 2001)
Authors: Roelofs G. J. , Scheeren H. A. , Heland J. , Ziereis H. , Lelieveld J.
Published: April 2010

Abstract. A coupled tropospheric chemistry-climate model is used to analyze tropospheric ozone distributions observed during the MINOS campaign in the eastern Mediterranean region (August, 2001). Modeled ozone profiles are generally in good agreement with the observations. Our analysis shows that the atmospheric dynamics in the region are strongly influenced by the occurrence of an upper tropospheric anti-cyclone, associated with the Asian summer monsoon and centered over the Tibetan Plateau. The anti-cyclone affects the chemical composition of the upper troposphere, where ozone concentrations of about 50 ppbv were measured, through advection of boundary layer air from South-East Asia. A layer between 4-6 km thickness was present beneath, containing up to 120 ppbv of ozone with substantial contributions by transport from the stratosphere and through lightning NOx. Additionally, pollutant ozone from North America was mixed in. Ozone in the lower troposphere originated mainly from the European continent. The stratospheric influence may be overestimated due to too strong vertical diffusion associated with the relatively coarse vertical resolution. The estimated tropospheric ozone column over the eastern Mediterranean is ~50 DU in summer, to which ozone from recent stratospheric origin contributes about 30%, ozone from lightning 13%, and from South-East Asia, North America and Europe about 7%, 8% and 14%, respectively, adding to a long-term hemispheric background of 25% of the column.
GC×GC measurements of C7-C11 aromatic and n-alkane hydrocarbons on Crete, in air from Eastern Europe during the MINOS campaign
Authors: Xu X. , Williams C. , Plass-Dülmer H. , Berresheim H. , Salisbury G. , Lange L. , Lelieveld J.
Published: April 2010

Abstract. During the Mediterranean Intensive Oxidant Study (MINOS) campaign in August 2001 gas-phase organic compounds were measured using comprehensive two-dimensional gas chromatography (GCxGC) at the Finokalia ground station, Crete. In this paper, C7-C11 aromatic and n-alkane measurements are presented and interpreted. The mean mixing ratios of the hydrocarbons varied from 1±1 pptv (i-propylbenzene) to 43±36 pptv (toluene). The observed mixing ratios showed strong day-to-day variations and generally higher levels during the first half of the campaign. Mean diel profiles showed maxima at local midnight and late morning, and minima in the early morning and evening. Results from analysis using a simplified box model suggest that both the chemical sink (i.e. reaction with OH) and the variability of source strengths were the causes of the observed variations in hydrocarbon mixing ratios. The logarithms of hydrocarbon concentrations were negatively correlated with the OH concentrations integral over a day prior to the hydrocarbon measurements. Slopes of the regression lines derived from these correlations for different compounds are compared with literature rate constants for their reactions with OH. The slopes for most compounds agree reasonably well with the literature rate constants. A sequential reaction model has been applied to the interpretation of the relationship between ethylbenzene and two of its potential products, i.e. acetophenone and benzeneacetaldehyde. The model can explain the good correlation observed between [acetophenone]/[ethylbenzene] and [benzeneacetaldehyde]/[ethylbenzene]. The model results and field measurements suggest that the reactivity of benzeneacetaldehyde may lie between those of acetophenone and ethylbenzene and that the ratio between yields of acetophenone and benzeneacetaldehyde may be up to 28:1. Photochemical ages of trace gases sampled at Finokalia during the campaign are estimated using the sequential reaction model and related data. They lie in the range of about 0.5-2.5 days.
An evaluation of the performance of chemistry transport models by comparison with research aircraft observations. Part 1: Concepts and overall model performance
Authors: Brunner D. , Staehelin J. , Rogers H. L. , Köhler M. O. , Pyle J. A. , Hauglustaine D. , Jourdain L. , Berntsen T. K. , Gauss M. , Isaksen I. S. A. , Meijer E. , van Velthoven P. , Pitari G. , Mancini E. , Grewe G. , Sausen R.
Published: April 2010

Abstract. A rigorous evaluation of five global Chemistry-Transport and two Chemistry-Climate Models operated by several different groups in Europe, was performed. Comparisons were made of the models with trace gas observations from a number of research aircraft measurement campaigns during the four-year period 1995-1998. Whenever possible the models were run over the same four-year period and at each simulation time step the instantaneous tracer fields were interpolated to all coinciding observation points. This approach allows for a very close comparison with observations and fully accounts for the specific meteorological conditions during the measurement flights. This is important considering the often limited availability and representativity of such trace gas measurements. A new extensive database including all major research and commercial aircraft measurements between 1995 and 1998, as well as ozone soundings, was established specifically to support this type of direct comparison. Quantitative methods were applied to judge model performance including the calculation of average concentration biases and the visualization of correlations and RMS errors in the form of so-called Taylor diagrams. We present the general concepts applied, the structure and content of the database, and an overall analysis of model skills over four distinct regions. These regions were selected to represent various atmospheric conditions and to cover large geographical domains such that sufficient observations are available for comparison. The comparison of model results with the observations revealed specific problems for each individual model. This study suggests the further improvements needed and serves as a benchmark for re-evaluations of such improvements. In general all models show deficiencies with respect to both mean concentrations and vertical gradients of important trace gases. These include ozone, CO and NOx at the tropopause. Too strong two-way mixing across the tropopause is suggested to be the main reason for differences between simulated and observed CO and ozone values. The generally poor correlations between simulated and measured NOx values suggest that in particular the NOx input by lightning and the convective transport from the polluted boundary layer are still not well described by current parameterizations, which may lead to significant differences in the spatial and seasonal distribution of NOx in the models. Simulated OH concentrations, on the other hand, were found to be in surprisingly good agreement with measured values.
FTIR spectroscopic studies of the simultaneous condensation of HCl and H2O at 190 K – Atmospheric applications
Authors: Xueref I. , Dominé F.
Published: April 2010

Abstract. Type II polar stratospheric cloud particles are made up of ice that forms by water vapor condensation in the presence of numerous trace gases, including HCl. These gaseous species can co-condense with water molecules and perturb ice structure and reactivity. In order to investigate the effect of co-condensing dopants on the structure of ice, we have designed an experimental system where ice films can be stabilized at 190 K, a temperature relevant to the polar stratosphere. We have co-condensed different HCl:H2O gaseous mixtures, with ratios 5:1, 1:10, 1:50 and 1:200 and studied the solids formed by infrared spectroscopy. The IR spectra obtained show that: (1) HCl is likely undergoing ionic dissociation when it is incorporated by co-condensation into the ice at 190 K; (2) this dissociation is done by several water molecules per HCl molecule; and (3) significant differences between our spectra and those of crystalline solids were always detected, and indicated that in all cases the structure of our solids retained some disorganized character. Considering the major impact of HCl on ice structure observed here, and the well known impact of the structure of solids on their reactivity, we conclude that the actual reactivity of stratospheric ice particles, that catalyze reactions involved in ozone depletion, may be different from what has been measured in laboratory experiments that used pure ice.
Impact of large solar zenith angles on lower stratospheric dynamical and chemical processes in a coupled chemistry-climate model
Authors: Lamago D. , Dameris M. , Schnadt C. , Eyring V. , Brühl C.
Published: April 2010

Abstract. Actinic fluxes at large solar zenith angles (SZAs) are important for atmospheric chemistry, especially under twilight conditions in polar winter and spring. The results of a sensitivity experiment employing the fully coupled 3D chemistry-climate model ECHAM4.L39(DLR)/CHEM have been analysed to quantify the impact of SZAs larger than 87.5º on dynamical and chemical processes in the lower stratosphere, in particular their influence on the ozone layer. Although the actinic fluxes at SZAs larger than 87.5º are small, ozone concentrations are significantly affected because daytime photolytic ozone destruction is switched on earlier, especially at the end of polar night the conversion of Cl2 and Cl2O2 into ClO in the lower stratosphere. Comparing climatological mean ozone column values of a simulation considering SZAs up to 93º with those of the sensitivity run with SZAs confined to 87.5º total ozone is reduced by about 20% in the polar Southern Hemisphere, i.e., the ozone hole is "deeper'' if twilight conditions are considered in the model because there is about 4 weeks more time for ozone destruction. This causes an additional cooling of the polar lower stratosphere (50 hPa) up to -4 K with obvious consequences for chemical processes. In the Northern Hemisphere the impact of large SZAs cannot be determined on the basis of climatological mean values due to the pronounced dynamic variability of the stratosphere in winter and spring. This study clearly shows the necessity of considering large SZAs for the calculation of photolysis rates in atmospheric models.
DRIFTS and Knudsen cell study of the heterogeneous reactivity of SO2 and NO2 on mineral dust
Authors: Ullerstam M. , Johnson M. S. , Vogt R. , Ljungström E.
Published: April 2010

Abstract. The heterogeneous oxidation of SO2 by NO2 on mineral dust was studied using Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) and a Knudsen cell. This made it possible to characterise, kinetically, both the formation of sulfate and nitrate as surface products and the gas phase loss of the reactive species. The gas phase loss rate was determined to be first order in both SO2 and NO2. From the DRIFTS experiment the uptake coefficient, g, for the formation of sulfate was determined to be of the order of 10-10 using the BET area as the reactive surface area. No significant formation of sulfate was seen in the absence of NO2. The Knudsen cell study gave uptake coefficients of the order of 10-6 and 10-7 for SO2 and NO2 respectively. There was no significant difference in uptake when SO2 or NO2 were introduced individually compared to experiments in which SO2 and NO2 were present at the same time.
The isotopic fingerprint of the pre-industrial and the anthropogenic N2O source
Authors: Röckmann T. , Kaiser J. , Brenninkmeijer C. A. M.
Published: April 2010

Abstract. We have performed high-precision measurements of the 18O and position dependent 15N isotopic composition of N2O from Antarctic firn air samples. By comparing these data to simulations carried out with a firn air diffusion model, we have reconstructed the temporal evolution of the N2O isotope signatures since pre-industrial times. The heavy isotope content of atmospheric N2O is presently decreasing for all signatures at rates of about -0.038 %o yr -1 for 1d15N, -0.046 %o yr -1 for 2d 15N and -0.025 %o yr -1 for d18O. The total decrease since pre-industrial times is estimated to be about -1.8%o for 1d15N at both positions and -2.2%o for 2d15N. Isotope budget calculations using these trends and recent stratospheric measurements allow to isotopically characterize the present and the pre-industrial global average N2O source, as well as the additional N2O emissions that have caused the global N2O increase since pre-industrial times. The increased fluxes from the depleted surface sources alone are insufficient to explain the inferred temporal isotope changes. In addition, the global average N2O source signature is calculated to be significantly depleted today relative to the pre-industrial value, in agreement with recent indications from soil emission measurements.
Emission of ions and charged soot particles by aircraft engines
Authors: Sorokin A. , Vancassel X. , Mirabel P.
Published: April 2010

Abstract. In this article, a model which examines the formation and evolution of chemiions in an aircraft engine is proposed. This model which includes chemiionisation, electron thermo-emission, electron attachment to soot particles and to neutral molecules, electron-ion and ion-ion recombination, ion-soot interaction, allows the determination of the ion concentration at the exit of the combustor and at the nozzle exit of the engine. It also allows the determination of the charge of the soot particles. For the engine considered, the upper limit for the ion emission index EIi is of the order of (2-5) x1016 ions/kg-fuel if ion-soot interactions are ignored and the introduction of ion-soot interactions lead about to a 50% reduction. The results also show that most of the soot particles are either positively or negatively charged, the remaining neutral particles representing approximately 20% of the total particles. A comparison of the model results with the available ground-based experimental data obtained on the ATTAS research aircraft engines during the SULFUR experiments (Schumann, 2002) shows an excellent agreement.
The Hohenpeissenberg aerosol formation experiment (HAFEX): a long-term study including size-resolved aerosol, H2SO4, OH, and monoterpenes measurements
Authors: Birmili W. , Berresheim H. , Plass-Dülmer C. , Elste T. , Gilge S. , Wiedensohler A. , Uhrner U.
Published: April 2010

Abstract. Ambient aerosol size distributions (>3 nm) and OH, H2SO4, and terpene concentrations were measured from April 1998 to August 2000 at a rural continental site in southern Germany. New particle formation (NPF) events were detected on 18% of all days, typically during midday hours under sunny and dry conditions. The number of newly formed particles correlated significantly with solar irradiance and ambient levels of H2SO4. A pronounced anti-correlatation of NPF events with the pre-existing particle surface area was identified in the cold season, often associated with the advection of dry and relatively clean air masses from southerly directions (Alps). Estimates of the particle formation rate based on observations were around 1 cm-3 s-1, being in agreement with the predictions of ternary homogeneous H2SO4-NH3-H2O nucleation within a few orders of magnitude. The experimentally determined nucleation mode particle growth rates were on average 2.6 nm h-1, with a fraction of 0.7 nm h-1 being attributed to the co-condensation of H2SO4-H2O-NH3. The magnitude of nucleation mode particle growth was neither significantly correlated to H2SO4, nor to the observed particle formation rate. Turn-over rate calculations of measured monoterpenes and aromatic hydrocarbons suggest that especially the oxidation products of monoterpenes have the capacity to contribute to the growth of nucleation mode particles. Although a large number of precursor gases, aerosol and meteorological parameters were measured, the ultimate key factors controlling the occurence of NPF events could not be identified.
The potential of polarization measurements from space at mm and sub-mm wavelengths for determining cirrus cloud parameters
Authors: Miao J. , Johnsen K.-P. , Buehler S. , Kokhanovsky A.
Published: April 2010

Abstract. The millimeter and sub-millimeter waves have been attracting a lot of attention recently in the cloud remote sensing community. This is largely because of their potential use in measuring cirrus cloud parameters with airborne or space-borne radiometers. In this study, we examine the possibility of using polarization measurements in this frequency range to get information on the microphysical properties of cirrus clouds. By using a simple radiative transfer model, we calculated the brightness temperature differences at the vertical and horizontal polarization channels for the following seven frequencies: 90, 157, 220, 340, 463, 683, and 874 GHz. The ice crystals in cirrus clouds are modeled with nearly spherical particles, circular cylinder, and circular plate, as well as with mixtures of these types. We found that the polarization difference signal shows a unique "resonance'' feature with the change of ice particle characteristic size: it has a strong response only in a certain range of ice particle size, beyond that range it approaches zero. The size range where this resonance happens depends to a large extent on particle shape and aspect ratio, but to a much less extent on particle orientation. This resonance feature appears even when ice clouds are composed of a mixture of ice crystals in different shapes, although the magnitude and the position of the resonance peak may change, depending on how the mixture is made. Oriented particles generally show larger polarization difference than randomly oriented ones, and plates have larger polarization difference than cylinders. However, the state of particle orientation has a significantly stronger effect on the polarization difference than the particle shape (cylinder or plate). This makes it difficult to distinguish particle shapes using millimeter and sub-millimeter radiometric measurements, if there is no information available on particle orientations. However, if the state of particle shape mixture can be predetermined by other approaches, polarization measurements can help to determine ice particle characteristic size and orientation. This information, in turn, will benefit our retrieval of the ice water path of cirrus clouds.
On the use of mass-conserving wind fields in chemistry-transport models
Authors: Bregman B. , Segers A. , Krol M. , Meijer E. , van Velthoven P.
Published: April 2010

Abstract. A new method has been developed that provides mass-conserving wind fields for global chemistry-transport models. In previous global Eulerian modeling studies a mass-imbalance was found between the model mass transport and the surface pressure tendencies. Several methods have been suggested to correct for this imbalance, but so far no satisfactory solution has been found. Our new method solves these problems by using the wind fields in a spherical harmonical form (divergence and vorticity) by mimicing the physics of the weather forecast model as closely as possible. A 3-D chemistry-transport model was used to show that the calculated ozone fields with the new processing method agree remarkably better with ozone observations in the upper troposphere and lower stratosphere. In addition, the calculated age of air in the lower stratosphere show better agreement with observations, although the air remains still too young in the extra-tropical stratosphere.
Heterogeneous conversion of NO2 on secondary organic aerosol surfaces: A possible source of nitrous acid (HONO) in the atmosphere?
Authors: Bröske R. , Kleffmann J. , Wiesen P.
Published: April 2010

Abstract. The heterogeneous conversion of NO2 on different secondary organic aerosols (SOA) was investigated with the focus on a possible formation of nitrous acid (HONO). In one set of experiments different organic aerosols were produced in the reactions of O3 with alpha-pinene, limonene or catechol and OH radicals with toluene or limonene, respectively. The aerosols were sampled on filters and exposed to humidified NO2  mixtures under atmospheric conditions. The estimated upper limits for the uptake coefficients of NO2  and the reactive uptake coefficients NO2  -> HONO are in the range of 10-6 and 10-7, respectively. The integrated HONO formation for 1 h reaction time was <1013 cm-2 geometrical surface and <1017 g-1 particle mass. In a second set of experiments the conversion of NO2 into HONO in the presence of organic particles was carried out in an aerosol flow tube under atmospheric conditions. In this case the aerosols were produced in the reaction of O3 with beta-pinene, limonene or catechol, respectively. The upper limits for the reactive uptake coefficients NO2 -> HONO were in the range of 7 x 10-7 - 9 x 10-6. The results from the present study show that heterogeneous formation of nitrous acid on secondary organic aerosols (SOA) is unimportant for the atmosphere.
Spatial variation of aerosol properties over Europe derived from satellite observations and comparison with model calculations
Authors: Robles González C. , Schaap M. , de Leeuw G. , Builtjes P. J. H. , van Loon M.
Published: April 2010

Abstract. Aerosol optical depths (AOD) and Angström coefficients over Europe were retrieved using data from the ATSR-2 radiometer on board the ESA satellite ERS-2, for August 1997. Taking advantage of the nadir and forward view of the ATSR-2, the dual view algorithm was used over land to eliminate the influence of the surface reflection. Over sea the AOD was retrieved using only the forward observations. Retrieved aerosol optical properties are in good agreement with those from ground-based sunphotometers. The AOD and Angström coefficients together yield information on the column integrated effective aerosol distribution.  Observed regional variations of the AOD and Angström coefficient are related to anthropogenic emissions of aerosol precursors such as SO2 and NOx in the major European industrial and urban areas, and their subsequent transformation into the aerosol phase. The influence of anthropogenic aerosols such as ammonium sulphate and ammonium nitrate on the total AOD is estimated using a regional chemistry transport model. Sulphate is estimated to contribute from 15% in very clean areas to 70% in polluted areas, the contribution of nitrate is between 5% and 25% over most of Europe. This paper shows the great importance of nitrate in summer over The Netherlands.
Long term measurements of submicrometer urban aerosols: statistical analysis for correlations with meteorological conditions and trace gases
Authors: Wehner B. , Wiedensohler A.
Published: April 2010

Abstract. Long-term measurements (over 4 years) of particle number size distributions (submicrometer particles, 3-800 nm in diameter), trace gases (NO, NO2, and O3), and meteorological parameters (global radiation, wind speed and direction, atmospheric pressure, etc.) were taken in a moderately polluted site in the city of Leipzig (Germany). The resulting complex data set was analyzed with respect to seasonal, weekly, and diurnal variation of the submicrometer aerosol. Car traffic produced a peak in the number size distribution at around 20 nm particle diameter during morning rush hour on weekdays. A second peak at 10-15 nm particle diameter occurred around noon during summer, confirmed by high correlation between concentration of particles less than 20 nm and the global radiation. This new-particle formation at noon was correlated with the amount of global radiation. A high concentration of accumulation mode particles (between 100 and 800 nm), which are associated with large particle-surface area, might prevent this formation. Such high particle concentration in the ultrafine region (particles smaller than 20 nm in diameter) was not detected in the particle mass, and thus, particle mass concentration is not suitable for determining the diurnal patterns of particles. In summer, statistical time series analysis showed a cyclic pattern of ultrafine particles with a period of one day and confirmed the correlation with global radiation. Principal component analysis (PCA) revealed a strong correlation between the particle concentration for 20-800 nm particles and the NO- and NO2-concentrations, indicating the influence of combustion processes on this broad size range, in particular during winter. In addition, PCA also revealed that particle concentration depended on meteorological conditions such as wind speed and wind direction, although the dependence differed with particle size class.
Modelling of the photooxidation of toluene: conceptual ideas for validating detailed mechanisms
Authors: Wagner V. , Jenkin M. E. , Saunders S. M. , Stanton J. , Wirtz K , Pilling M. J.
Published: April 2010

Abstract. Toluene photooxidation is chosen as an example to examine how simulations of smog-chamber experiments can be used to unravel shortcomings in detailed mechanisms and to provide information on complex reaction systems that will be crucial for the design of future validation experiments. The mechanism used in this study is extracted from the Master Chemical Mechanism Version 3 (MCM v3) and has been updated with new modules for cresol and g-dicarbonyl chemistry. Model simulations are carried out for a toluene-NOx experiment undertaken at the European Photoreactor (EUPHORE). The comparison of the simulation with the experimental data reveals two fundamental shortcomings in the mechanism: OH production is too low by about 80%, and the ozone concentration at the end of the experiment is over-predicted by 55%. The radical budget was analysed to identify the key intermediates governing the radical transformation in the toluene system. Ring-opening products, particularly conjugated g-dicarbonyls, were identified as dominant radical sources in the early stages of the experiment. The analysis of the time evolution of radical production points to a missing OH source that peaks when the system reaches highest reactivity. First generation products are also of major importance for the ozone production in the system. The analysis of the radical budget suggests two options to explain the concurrent under-prediction of OH and over-prediction of ozone in the model: 1) missing oxidation processes that produce or regenerate OH without or with little NO to NO2 conversion or 2) NO3 chemistry that sequesters reactive nitrogen oxides into stable nitrogen compounds and at the same time produces peroxy radicals. Sensitivity analysis was employed to identify significant contributors to ozone production and it is shown how this technique, in combination with ozone isopleth plots, can be used for the design of validation experiments.
Physical properties and concentration of aerosol particles over the Amazon tropical forest during background and biomass burning conditions
Authors: Guyon P. , Graham B. , Beck J. , Boucher O. , Gerasopoulos E. , Mayol-Bracero O. L. , Roberts G. C. , Artaxo P. , Andreae M. O.
Published: April 2010

Abstract. We investigated the size distribution, scattering and absorption properties of Amazonian aerosols and the optical thickness of the aerosol layer under the pristine background conditions typical of the wet season, as well as during the biomass-burning-influenced dry season. The measurements were made during two campaigns in 1999 as part of the European contribution to the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA-EUSTACH). In moving from the wet to the dry season, median particle numbers were observed to increase from values comparable to those of the remote marine boundary layer (~400 cm-3) to values more commonly associated with urban smog (~4000 cm-3), due to a massive injection of submicron smoke particles. Aerosol optical depths at 500 nm increased from 0.05 to 0.8 on average, reaching a value of 2 during the dry season. Scattering and absorption coefficients, measured at 550 nm, showed a concomitant increase from average values of 6.8 and 0.4 Mm-1 to values of 91 and 10 Mm-1, respectively, corresponding to an estimated decrease in single-scattering albedo from ca. 0.97 to 0.91. The roughly tenfold increase in many of the measured parameters attests to the dramatic effect that extensive seasonal biomass burning (deforestation, pasture cleaning) is having on the composition and properties of aerosols over Amazonia. The potential exists for these changes to impact on regional and global climate through changes to the extinction of solar radiation as well as the alteration of cloud properties.
Ice condensation on sulfuric acid tetrahydrate: Implications for polar stratospheric ice clouds
Authors: Fortin T. J. , Drdla K. , Iraci L. T. , Tolbert M. A.
Published: April 2010

Abstract. The mechanism of ice nucleation to form Type 2 PSCs is important for controlling the ice particle size and hence the possible dehydration in the polar winter stratosphere. This paper probes heterogeneous ice nucleation on sulfuric acid tetrahydrate (SAT). Laboratory experiments were performed using a thin-film, high-vacuum apparatus in which the condensed phase is monitored via Fourier transform infrared spectroscopy and water pressure is monitored with the combination of an MKS baratron and an ionization gauge. Results show that SAT is an efficient ice nucleus with a critical ice saturation ratio of S*ice = 1.3 to 1.02 over the temperature range 169.8-194.5 K. This corresponds to a necessary supercooling of 0.1-1.3 K below the ice frost point. The laboratory data is used as input for a microphysical/photochemical model to probe the effect that this heterogeneous nucleation mechanism could have on Type 2 PSC formation and stratospheric dehydration. In the model simulations, even a very small number of SAT particles (e.g., 10-3 cm-3) result in ice nucleation on SAT as the dominant mechanism for Type 2 PSC formation. As a result, Type 2 PSC formation is more widespread, leading to larger-scale dehydration. The characteristics of the clouds are controlled by the assumed number of SAT particles present, demonstrating that a proper treatment of SAT is critical for correctly modeling Type 2 PSC formation and stratospheric dehydration.
Radar and optical leonids
Authors: Brosch N. , Polishook D. , Helled R. , Schijvarg S. , Rosenkrantz M.
Published: April 2010

Abstract. We present joint optical-radar observations of meteors collected near the peak of the Leonid activity in 2002. We show four examples of joint detections with a large, phased array L-band radar and with intensified video cameras. The general characteristic of the radar-detected optical meteors is that they show the radar detection below the termination of the optical meteor. Therefore, at least some radar events associated with meteor activity are neither head echoes nor trail echoes, but probably indicate the formation of "charged clouds" after the visual meteor is extinguished.
Modelling atmospheric transport of α-hexachlorocyclohexane in the Northern Hemispherewith a 3-D dynamical model: DEHM-POP
Authors: Hansen K. M. , Christensen J. H. , Brandt J. , Frohn L. M. , Geels C.
Published: April 2010

Abstract. The Danish Eulerian Hemispheric Model (DEHM) is a 3-D dynamical atmospheric transport model originally developed to describe the atmospheric transport of sulphur into the Arctic. A new version of the model, DEHM-POP, developed to study the atmospheric transport and environmental fate of persistent organic pollutants (POPs) is presented. During environmental cycling, POPs can be deposited and re-emitted several times before reaching a final destination. A description of the exchange processes between the land/ocean surfaces and the atmosphere is included in the model to account for this multi-hop transport. The α-isomer of the pesticide hexachlorocyclohexane (α-HCH) is used as tracer in the model development. The structure of the model and processes included are described in detail. The results from a model simulation showing the atmospheric transport for the years 1991 to 1998 are presented and evaluated against measurements. The annual averaged atmospheric concentration of α-HCH for the 1990s is well described by the model; however, the shorter-term average concentration for most of the stations is not well captured. This indicates that the present simple surface description needs to be refined to get a better description of the air-surface exchange processes of POPs.
A climatological study of rural surface ozone in central Greece
Authors: Kalabokas P. D. , Repapis C. C.
Published: April 2010

Abstract. Recent studies show that surface ozone levels at rural sites in Greece are generally high when compared with rural ozone measurements at northern European sites. The area of SE Europe, including Greece, is not very well monitored regarding rural ozone in comparison to central and northern Europe. In order to have the best possible picture of the rural surface ozone climatology in the area, based on the available data-sets of long-term continuous monitoring stations, the 10-year measurement records (1987-1996) of the Athens peripheral station of Liossia, (12 km N of the city center) and the urban background station of Geoponiki (3 km W) as well as the 4-year record (1996-1999) of the rural station of Aliartos (100 km NW of Athens), are analyzed in this paper. The data for Liossia and Geoponiki stations are screened for cases of strong airflow from rural areas (N-NE winds stronger than 5 m/s). The variation characteristics of the average rural ozone afternoon levels (12:00-18:00), with the best vertical atmospheric mixing, are mainly examined since these measurements are expected to be representative of the broader area. In all three stations there is a characteristic seasonal variation of rural ozone concentrations with lowest winter afternoon values at about 50 μg/m3 in December-January and average summer afternoon values at about 120 μg/m3 in July-August, indicating that high summer values are observed all over the area. The rural summer afternoon ozone values are very well correlated between the three stations, implying spatial homogeneity all over the area but also temporal homogeneity, since during the 13-year period 1987-1999 the rural afternoon ozone levels remained almost constant around the value of 120 μg/m3.
Polycyclic aromatic hydrocarbons (PAHs) in the atmospheres of two French alpine valleys: sources and temporal patterns
Authors: Marchand N. , Besombes J. L. , Chevron N. , Masclet P. , Aymoz G. , Jaffrezo J. L.
Published: April 2010

Abstract. Alpine valleys represent some of the most important crossroads for international heavy-duty traffic in Europe, but the full impact of this traffic on air quality is not known due to a lack of data concerning these complex systems. As part of the program "Pollution des Vallées Alpines" (POVA), we performed two sampling surveys of polycyclic aromatic hydrocarbons (PAHs) in two sensitive valleys: the Chamonix and Maurienne Valleys, between France and Italy. Sampling campaigns were performed during the summer of 2000 and the winter of 2001, with both periods taking place during the closure of the "Tunnel du Mont-Blanc". The first objective of this paper is to describe the relations between PAH concentrations, external parameters (sampling site localization, meteorological parameters, sources), and aerosol characteristics, including its carbonaceous fraction (OC and EC). The second objective is to study the capacity of PAH profiles to accurately distinguish the different emission sources. Temporal evolution of the relative concentration of an individual PAH (CHR) and the PAH groups BghiP+COR and BbF+BkF is studied in order to differentiate wood combustion, gasoline, and diesel emissions, respectively. The results show that the total particulate PAH concentrations were higher in the Chamonix valley during both seasons, despite the cessation of international traffic. Seasonal cycles, with higher concentrations in winter, are also stronger in this valley. During winter, particulate PAH concentration can reach very high levels (up to 155 ng.m-3) in this valley during cold anticyclonic periods. The examination of sources shows the impact during summer of heavy-duty traffic in the Maurienne valley and of gasoline vehicles in the Chamonix valley. During winter, Chamonix is characterized by the strong influence of wood combustion in residential fireplaces, even if the temporal evolution of specific PAH ratios are difficult to interpret. Information on sources given by PAH profiles can only be considered in qualitative terms.
Remote sensing of water cloud droplet size distributions using the backscatter glory: a case study
Authors: Mayer B. , Schröder M. , Preusker R. , Schüller L.
Published: April 2010

Abstract. Cloud single scattering properties are mainly determined by the effective radius of the droplet size distribution. There are only few exceptions where the shape of the size distribution affects the optical properties, in particular the rainbow and the glory directions of the scattering phase function. Using observations by the Compact Airborne Spectrographic Imager (CASI) in 180° backscatter geometry, we found that high angular resolution aircraft observations of the glory provide unique new information which is not available from traditional remote sensing techniques: Using only one single wavelength, 753nm, we were able to determine not only optical thickness and effective radius, but also the width of the size distribution at cloud top. Applying this novel technique to the ACE-2 CLOUDYCOLUMN experiment, we found that the size distributions were much narrower than usually assumed in radiation calculations which is in agreement with in-situ observations during this campaign. While the shape of the size distribution has only little relevance for the radiative properties of clouds, it is extremely important for understanding their formation and evolution.
Around the world in 17 days - hemispheric-scale transport of forest fire smoke from Russia in May 2003
Authors: Damoah R. , Spichtinger N. , Forster C. , James P. , Mattis I. , Wandinger U. , Beirle S. , Wagner T. , Stohl A.
Published: April 2010

Abstract. In May 2003, severe forest fires in southeast Russia resulted in smoke plumes extending widely across the Northern Hemisphere. This study combines satellite data from a variety of platforms (Moderate Resolution Imaging Spectroradiometer (MODIS), Sea-viewing Wide Field-of-view Sensor (SeaWiFS), Earth Probe Total Ozone Mapping Spectrometer (TOMS) and Global Ozone Monitoring Experiment (GOME)) and vertical aerosol profiles derived with Raman lidar measurements with results from a Lagrangian particle dispersion model to understand the transport processes that led to the large haze plumes observed over North America and Europe. The satellite images provided a unique opportunity for validating model simulations of tropospheric transport on a truly hemispheric scale. Transport of the smoke occurred in two directions: Smoke travelling northwestwards towards Scandinavia was lifted over the Urals and arrived over the Norwegian Sea. Smoke travelling eastwards to the Okhotsk Sea was also lifted, it then crossed the Bering Sea to Alaska from where it proceeded to Canada and was later even observed over Scandinavia and Eastern Europe on its way back to Russia. Not many events of this kind, if any, have been observed, documented and simulated with a transport model comprehensively. The total transport time was about 17 days. We compared transport model simulations using meteorological analysis data from both the European Centre for Medium-Range Weather Forecast (ECMWF) and the National Center for Environmental Prediction (NCEP) in order to find out how well this event could be simulated using these two datasets. Although differences between the two simulations are found on small scales, both agree remarkably well with each other and with the observations on large scales. On the basis of the available observations, it cannot be decided which simulation was more realistic.
Investigation of Arctic ozone depletion sampled over midlatitudes during the Egrett campaign of spring/summer 2000
Authors: Ross D. E. M. , Pyle J. A. , Harris N. R. P. , McIntyre J. D. , Millard G. A. , Robinson A. D. , Busen R.
Published: April 2010

Abstract. A unique halocarbon dataset has been obtained using the Australian high altitude research aircraft, the Grob G520T Egrett, during May-June 2000 with GC instrument (DIRAC), which has been previously deployed on balloon platforms. The halocarbon data generally shows a good anticorrelation with ozone data obtained simultaneously from commercial sensors. On 5 June 2000, at 380K, the Egrett entered a high latitude tongue of air over the U.K. CFC-11 and O3 data obtained on the flight show evidence of this feature. The dataset has been used, in conjunction with a 3D chemical transport model, to infer ozone depletion encountered in the midlatitude lower stratosphere during the flight. We calculate that ozone is depleted by 20% relative to its winter value in the higher latitude airmass. A suite of ozone loss tracers in the model have been used to track ozone depletion according to location relative to the vortex and chemical cycle responsible. The model, initialised on 9 December, indicates that 50% of the total chemical ozone destruction encountered in June in the middle latitudes occurred in the 90-70°N equivalent latitude band and that 70% was due to halogen chemistry.
On the decadal increase in the tropical mean outgoing longwave radiation for the period 1984-2000
Authors: Hatzidimitriou D. , Vardavas I. , Pavlakis K. G. , Hatzianastassiou N. , Matsoukas C. , Drakakis E.
Published: April 2010

Abstract. In the present paper, we have calculated the outgoing longwave radiation at the top of the atmosphere (OLR at TOA) using a deterministic radiation transfer model, cloud data from ISCCP-D, and atmospheric temperature and humidity data from NCEP/NCAR reanalysis, for the seventeen-year period 1984-2000. We constructed anomaly time-series of the OLR at TOA, as well as of all of the key input climatological data, averaged in the tropical region between 20°N and 20°S. We compared the anomaly time-series of the model calculated OLR at TOA with that obtained from the ERBE S-10N (WFOV NF edition 2) non-scanner measurements. The model results display very similar seasonal and inter-annual variability as the ERBS data, and indicate a decadal increase of OLR at TOA of 1.9±0.2Wm-2/decade, which is lower than that displayed by the ERBS time-series (3.5±0.3Wm-2). Analysis of the inter-annual and long-term variability of the various parameters determining the OLR at TOA, showed that the most important contribution to the observed trend comes from a decrease in high-level cloud cover over the period 1984-2000, followed by an apparent drying of the upper troposphere and a decrease in low-level cloudiness. Opposite but small trends are introduced by a decrease in low-level cloud top pressure, an apparent cooling of the lower stratosphere (at the 50mbar level) and a small decadal increase in mid-level cloud cover.
Evaluated kinetic and photochemical data for atmospheric chemistry: Volume I - gas phase reactions of Ox, HOx, NOx and SOx species
Authors: Atkinson R. , Baulch D. L. , Cox R. A. , Crowley J. N. , Hampson R. F. , Hynes R. G. , Jenkin M. E. , Rossi M. J. , Troe J.
Published: April 2010

Abstract. This article, the first in the series, presents kinetic and photochemical data evaluated by the IUPAC Subcommittee on GasKinetic Data Evaluation for Atmospheric Chemistry. It covers the gas phase and photochemical reactions of Ox, HOx, NOx and SOx species, which were last published in 1997, and were updated on the IUPAC website in late 2001. The article consists of a summary sheet, containing the recommended kinetic parameters for the evaluated reactions, and five appendices containing the data sheets, which provide information upon which the recommendations are made.
Role of the NO3 radicals in oxidation processes in the eastern Mediterranean troposphere during the MINOS campaign
Authors: Vrekoussis M. , Kanakidou M. , Mihalopoulos N. , Crutzen P. J. , Lelieveld J. , Perner D. , Berresheim H. , Baboukas E.
Published: April 2010

Abstract. During the MINOS campaign (28 July-18 August 2001) the nitrate (NO3) radical was measured at Finokalia station, on the north coast of Crete in South-East Europe using a long path (10.4 km) Differential Optical Absorption Spectroscopy instrument (DOAS). Hydroxyl (OH) radical was also measured by a Chemical Ionization Mass-Spectrometer (Berresheim et al., 2003). These datasets represent the first simultaneous measurements of OH and NO3 radicals in the area. NO3 radical concentrations ranged from less than 3x107 up to 9x108 radicals· cm-3 with an average nighttime value of 1.1x108 radicals· cm-3. The observed NO3 mixing ratios are analyzed on the basis of the corresponding meteorological data and the volatile organic compound (VOC) observations which were measured simultaneously at Finokalia station. The importance of the NO3 radical chemistry relatively to that of OH in the dimethylsulfide (DMS) and nitrate cycles is also investigated. The observed NO3 levels regulate the nighttime variation of DMS. The loss of DMS by NO3 during night is about 75% of that by OH radical during day. NO3 and nitrogen pentoxide (N2O5) reactions account for about 21% of the total nitrate (HNO3(g)+NO-3(g)) production.
A quantitative analysis of grid-related systematic errors in oxidising capacity and ozone production rates in chemistry transport models
Authors: Esler J. G. , Roelofs G. J. , Köhler M. O. , O'Connor F. M.
Published: April 2010

Abstract. Limited resolution in chemistry transport models (CTMs) is necessarily associated with systematic errors in the calculated chemistry, due to the artificial mixing of species on the scale of the model grid (grid-averaging). Here, the errors in calculated hydroxyl radical (OH) concentrations and ozone production rates 3 are investigated quantitatively using both direct observations and model results. Photochemical steady-state models of radical chemistry are exploited in each case to examine the effect on both OH and 3 of averaging relatively long-lived precursor species, such as O3, NOx, CO, H2O, etc. over different spatial scales. Changes in modelled 3 are estimated, independently of other model errors, by calculating the systematic effect of spatial averaging on the ozone production efficiency 1, defined as the ratio of ozone molecules produced per NOx molecule destroyed. Firstly, an investigation of in-flight measurements suggests that, at least in the northern midlatitude upper-troposphere/lower stratosphere, averaging precursor species on the scale of a T42 grid (2.75° x 2.75°) leads to a 15-20% increase in OH concentrations and a 5-10% increase in 1. Secondly, results from CTM model experiments are compared at different horizontal resolutions. Low resolution experiments are found to have significantly higher [OH] and 3 compared with high resolution experiments. The extent to which these differences may be explained by the systematic error in the model chemistry associated with grid size is estimated by degrading the high resolution data onto a low resolution grid and then recalculating 1 and [OH]. The change in calculated 1 is found to be significant and can account for much of the difference in 3 between the high and low resolution experiments. The calculated change in [OH] is less than the difference in [OH] found between the experiments, although the shortfall is likely to be due to the indirect effect of the change in modelled NOx, which is not accounted for in the calculation. It is argued that systematic errors caused by limited resolution need to be considered when evaluating the relative impacts of different pollutant sources on tropospheric ozone.