bluuebunny/crossref_metadata_2025 huggingface dataset:
A one dimensional model study of the mechanism of halogen liberation and vertical transport in the polar troposphere
Authors: Lehrer E. , Hönninger G. , Platt U.
Published: April 2010

Abstract. Sudden depletions of tropospheric ozone during spring were reported from the Arctic and also from Antarctic coastal sites. Field studies showed that those depletion events are caused by reactive halogen species, especially bromine compounds. However the source and seasonal variation of reactive halogen species is still not completely understood. There are several indications that the halogen mobilisation from the sea ice surface of the polar oceans may be the most important source for the necessary halogens. Here we present a one dimensional model study aimed at determining the primary source of reactive halogens. The model includes gas phase and heterogeneous bromine and chlorine chemistry as well as vertical transport between the surface and the top of the boundary layer. The autocatalytic Br release by photochemical processes (bromine explosion) and subsequent rapid bromine catalysed ozone depletion is well reproduced in the model and the major source of reactive bromine appears to be the sea ice surface. The sea salt aerosol alone is not sufficient to yield the high levels of reactive bromine in the gas phase necessary for fast ozone depletion. However, the aerosol efficiently "recycles" less reactive bromine species (e.g. HBr) and feeds them back into the ozone destruction cycle. Isolation of the boundary layer air from the free troposphere by a strong temperature inversion was found to be critical for boundary layer ozone depletion to happen. The combination of strong surface inversions and presence of sunlight occurs only during polar spring.
Improved sky imaging for studies of enhanced UV irradiance
Authors: Sabburg J. M. , Long C. N.
Published: April 2010

Abstract. A recent World Meteorological Organisation report discussed the importance of continued study of the effect of clouds on the solar UV radiation reaching the earth's surface. The report mentions that the use of all-sky imagery offers the potential to understand and quantify cloud effects more accurately. There are an increasing number of studies investigating the enhancement of surface solar, UV irradiance, and UV actinic flux, using automated CCD and sky imagers. This paper describes new algorithms applicable to a commercially available all-sky imager (TSI-440), for research investigating cloud enhanced spectral UV irradiance. Specifically, these include three new algorithms relating to cloud amount at different spatial positions from 1) zenith and 2) from the solar position and 3) the visible brightness of clouds surrounding the sun. A possible relationship between UV enhancement and the occurrence of near-sun cloud brightness is reported based on this preliminary data. It is found that a range of wavelength dependent intensities, from 306 to 400 nm, can occur in one day for UV enhancements. Evidence for a possible decreasing variation of intensity with longer wavelengths is also presented.
Initial steps of aerosol growth
Authors: Kulmala M. , Laakso L. , Lehtinen K. E. J. , Riipinen I. , Dal Maso M. , Anttila T. , Kerminen V.-M. , Hõrrak U. , Vana M. , Tammet H.
Published: April 2010

Abstract. The formation and growth of atmospheric aerosols depend on several steps, namely nucleation, initial steps of growth and subsequent – mainly condensational – growth. This work focuses on the initial steps of growth, meaning the growth right after nucleation, where the interplay of curvature effects and thermodynamics has a significant role on the growth kinetics. More specifically, we investigate how ion clusters and aerosol particles grow from 1.5 nm to 20 nm (diameter) in atmospheric conditions using experimental data obtained by air ion and aerosol spectrometers. The measurements have been performed at a boreal forest site in Finland. The observed trend that the growth rate seems to increase as a function of size can be used to investigate possible growth mechanisms. Such a growth rate is consistent with a recently suggested nano-Köhler mechanism, in which growth is activated at a certain size with respect to condensation of organic vapors. The results also imply that charge-enhanced growth associated with ion-mediated nucleation plays only a minor role in the initial steps of growth, since it would imply a clear decrease of the growth rate with size. Finally, further evidence was obtained on the earlier suggestion that atmospheric nucleation and the subsequent growth of fresh nuclei are likely to be uncoupled phenomena via different participating vapors.
Mass balance inverse modelling of methane in the 1990s using a Chemistry Transport Model
Authors: Butler T. M. , Simmonds I. , Rayner P. J.
Published: April 2010

Abstract. A mass balance inverse modelling procedure is applied with a time-dependent methane concentration boundary condition and a chemical transport model to relate observed changes in the surface distribution of methane mixing ratios during the 1990s to changes in its surface sources. The model reproduces essential features of the global methane cycle, such as the latitudinal distribution and seasonal cycle of fluxes, without using a priori knowledge of methane fluxes. A detailed description of the temporal and spatial variability of the fluxes diagnosed by the inverse procedure is presented, and compared with previously hypothesised changes in the methane budget, and previous inverse modelling studies. The sensitivity of the inverse results to the forcing data supplied by surface measurements of methane from the NOAA CMDL cooperative air sampling network is also examined. This work serves as an important starting point for future inverse modelling work examining changes in both the source and sink terms in the methane budget together.
An investigation of processes controlling the evolution of the boundary layer aerosol size distribution properties at the Swedish background station Aspvreten
Authors: Tunved P. , Ström J. , Hansson H.-C.
Published: April 2010

Abstract. Aerosol size distributions have been measured at the Swedish background station Aspvreten (58.8° N, 17.4° E). Different states of the aerosol were determined using a novel application of cluster analysis. The analysis resulted in eight different clusters capturing different stages of the aerosol lifecycle. The atmospheric aerosol size distributions were interpreted as belonging to fresh, intermediate and aged types of size distribution. With aid of back trajectory analysis we present statistics concerning the relation of source area and different meteorological parameters using a non-Lagrangian approach. Source area is argued to be important although not sufficient to describe the observed aerosol properties. Especially processing by clouds and precipitation is shown to be crucial for the evolution of the aerosol size distribution. As much as 60% of the observed size distributions present features that are likely to be related to cloud processes or wet deposition. The lifetime properties of different sized aerosols are discussed by means of measured variability of the aerosol size distribution. Processing by clouds and precipitation is shown to be especially crucial in the size range 100 nm and larger. This indicates an approximate limit for activation in clouds to 100 nm in this type of environment. The aerosol lifecycle is discussed. Size distributions indicating signs of recent new particle formation (~30% of the observed size distributions) represent the first stage in the lifecycle. Aging of the aerosol size distribution may follow two branches: either growth by condensation and coagulation or processing by non-precipitating clouds. In both cases mass is accumulated. Wet removal is the main process capable of removing aerosol mass. Wet deposition is argued to be an important mechanism in reaching a state where nucleation may occur (i.e. sufficiently low aerosol surface area) in environments similar to the one studied.
Formation of binary ion clusters from polar vapours: effect of the dipole-charge interaction
Authors: Nadykto A. B. , Yu F.
Published: April 2010

Abstract. Formation of binary cluster ions from polar vapours is considered. The effect of vapour polarity on the size and composition of the critical clusters is investigated theoretically and a corrected version of classical Kelvin-Thomson theory of binary ion-induced nucleation is derived. The model predictions of the derived theory are compared to the results given by classical binary homogeneous nucleation theory and ion-induced nucleation theory. The calculations are performed in wide range of the ambient conditions for a system composed of sulfuric acid and water vapour. It is shown that dipole-charge interaction significantly decreases the size of the critical clusters, especially under the atmospheric conditions when the size of critical clusters is predicted to be small.
Source-receptor matrix calculation with a Lagrangian particle dispersion model in backward mode
Authors: Seibert P. , Frank A.
Published: April 2010

Abstract. The possibility to calculate linear-source receptor relationships for the transport of atmospheric trace substances with a Lagrangian particle dispersion model (LPDM) running in backward mode is shown and presented with many tests and examples. This mode requires only minor modifications of the forward LPDM. The derivation includes the action of sources and of any first-order processes (transformation with prescribed rates, dry and wet deposition, radioactive decay, etc.). The backward mode is computationally advantageous if the number of receptors is less than the number of sources considered. The combination of an LPDM with the backward (adjoint) methodology is especially attractive for the application to point measurements, which can be handled without artificial numerical diffusion. Practical hints are provided for source-receptor calculations with different settings, both in forward and backward mode. The equivalence of forward and backward calculations is shown in simple tests for release and sampling of particles, pure wet deposition, pure convective redistribution and realistic transport over a short distance. Furthermore, an application example explaining measurements of Cs-137 in Stockholm as transport from areas contaminated heavily in the Chernobyl disaster is included.
Canadian Meteor Orbit Radar (CMOR)
Authors: Webster A. R. , Brown P. G. , Jones J. , Ellis K. J. , Campbell-Brown M.
Published: April 2010

Abstract. The radar system described here (CMOR) comprises a basic 5-element receiving system, co-located with a pulsed transmitter, specifically designed to observe meteor echoes and to determine their position in space with an angular resolution of ~1° and a radial resolution of ~3 km. Two secondary receiving sites, a few km distant and arranged to form approximately a right angle with the base station, allow the determination of the velocity (speed and direction) of the meteor that, together with the time of occurrence, lead to an estimate of the orbit of the original meteoroid. Some equipment details are presented along with a method used to determine the orbits. Representative echoes are shown and observations on the 2002 Leonid shower presented.
Multicomponent aerosol dynamics model UHMA: model development and validation
Authors: Korhonen H. , Lehtinen K. E. J. , Kulmala M.
Published: April 2010

Abstract. A size-segregated aerosol dynamics model UHMA (University of Helsinki Multicomponent Aerosol model) was developed for studies of multicomponent tropospheric aerosol particles. The model includes major aerosol microphysical processes in the atmosphere with a focus on new particle formation and growth; thus it incorporates particle coagulation and multicomponent condensation, applying a revised treatment of condensation flux onto free molecular regime particles and the activation of nanosized clusters by organic vapours (Nano-Köhler theory), as well as recent parameterizations for binary H2SO4-H2O and ternary H2SO4-NH3-H2O homogeneous nucleation and dry deposition. The representation of particle size distribution can be chosen from three sectional methods: the hybrid method, the moving center method, and the retracking method in which moving sections are retracked to a fixed grid after a certain time interval. All these methods can treat particle emissions and atmospheric transport consistently, and are therefore suitable for use in large scale atmospheric models. In a test simulation against an accurate high resolution solution, all the methods showed reasonable treatment of new particle formation with 20 size sections although the hybrid and the retracking methods suffered from artificial widening of the distribution. The moving center approach, on the other hand, showed extra dents in the particle size distribution and failed to predict the onset of detectable particle formation. In a separate test simulation of an observed nucleation event, the model captured the key qualitative behaviour of the system well. Furthermore, its prediction of the organic volume fraction in newly formed particles, suggesting values as high as 0.5 for 3–4 nm particles and approximately 0.8 for 10 nm particles, agrees with recent indirect composition measurements.
Temperature lidar measurements from 1 to 105 km altitude using resonance, Rayleigh, and Rotational Raman scattering
Authors: Alpers M. , Eixmann R. , Fricke-Begemann C. , Gerding M. , Höffner J.
Published: April 2010

Abstract. For the first time, three different temperature lidar methods are combined to obtain time-resolved complete temperature profiles with high altitude resolution over an altitude range from the planetary boundary layer up to the lower thermosphere (about 1–105 km). The Leibniz-Institute of Atmospheric Physics (IAP) at Kühlungsborn, Germany (54° N, 12° E) operates two lidar instruments, using three different temperature measurement methods, optimized for three altitude ranges: (1) Probing the spectral Doppler broadening of the potassium D1 resonance lines with a tunable narrow-band laser allows atmospheric temperature profiles to be determined at metal layer altitudes (80–105 km). (2) Between about 20 and 90 km, temperatures were calculated from Rayleigh backscattering by air molecules, where the upper start values for the calculation algorithm were taken from the potassium lidar results. Correction methods have been applied to account for, e.g. Rayleigh extinction or Mie scattering of aerosols below about 32 km. (3) At altitudes below about 25 km, backscattering in the Rotational Raman lines is strong enough to obtain temperatures by measuring the temperature dependent spectral shape of the Rotational Raman spectrum. This method works well down to about 1 km. The instrumental configurations of the IAP lidars were optimized for a 3–6 km overlap of the temperature profiles at the method transition altitudes. We present two night-long measurements with clear wave structures propagating from the lower stratosphere up to the lower thermosphere.
Stratospheric age of air computed with trajectories based on various 3D-Var and 4D-Var data sets
Authors: Scheele M. P. , Siegmund P. C. , Velthoven P. F. J.
Published: April 2010

Abstract. The age of stratospheric air is computed with a trajectory model, using ECMWF ERA-40 3D-Var and operational 4D-Var winds. Analysis as well as forecast data are used. In the latter case successive forecast segments are put together to get a time series of the wind fields. This is done for different forecast segment lengths. The sensitivity of the computed age to the forecast segment length and assimilation method are studied, and the results are compared with observations and with results from a chemistry transport model that uses the same data sets. A large number of backward trajectories are started in the stratosphere, and from the fraction of these trajectories that has passed the tropopause the age of air is computed. First, for ten different data sets 50-day backward trajectories starting in the tropical lower stratosphere are computed. The results show that in this region the computed cross-tropopause transport decreases with increasing forecast segment length. Next, for three selected data sets (3D-Var 24-h and 4D-Var 72-h forecast segments, and 4D-Var analyses) 5-year backward trajectories are computed that start all over the globe at an altitude of 20km. For all data sets the computed ages of air in the extratropics are smaller than the observation-based age. For 4D-Var forecast series they are closest to the observation-based values, but still 0.5-1.5 year too small. Compared to the difference in age between the results for the different data sets, the difference in age between the trajectory and the chemistry transport model results is small.
Validation of SCIAMACHY tropospheric NO2-columns with AMAXDOAS measurements
Authors: Heue K.-P. , Richter A. , Bruns M. , Burrows J. P. , v. Friedeburg C. , Platt U. , Pundt I. , Wang P. , Wagner T.
Published: April 2010

Abstract. Tropospheric NO2 vertical and slant columns from the new satellite instrument SCIAMACHY on ENVISAT are validated by measurements of the Airborne Multi AXis DOAS (AMAXDOAS) instrument on board the DLR Falcon. The results presented here were obtained in February 2003 on a flight over the Alps, the Po-Valley and the Mediterranean. The tropospheric vertical column measured by AMAXDOAS varied between 16.2 and 35.2*1015molec/cm2 over the Po-Valley where SCIAMACHY data resulted in 19.9 to 37*1015molec/cm2. Over less polluted areas a similarly good agreement was found. The linear correlation between the two datasets results in a slope of 0.93. The slight differences observed can be attributed to the different spatial resolution and the temporal mismatch between the measurements over the Po-Valley.
The aerosol-climate model ECHAM5-HAM
Authors: Stier P. , Feichter J. , Kinne S. , Kloster S. , Vignati E. , Wilson J. , Ganzeveld L. , Tegen I. , Werner M. , Balkanski Y. , Schulz M. , Boucher O. , Minikin A. , Petzold A.
Published: April 2010

Abstract. The aerosol-climate modelling system ECHAM5-HAM is introduced. It is based on a flexible microphysical approach and, as the number of externally imposed parameters is minimised, allows the application in a wide range of climate regimes. ECHAM5-HAM predicts the evolution of an ensemble of microphysically interacting internally- and externally-mixed aerosol populations as well as their size-distribution and composition. The size-distribution is represented by a superposition of log-normal modes. In the current setup, the major global aerosol compounds sulfate (SU), black carbon (BC), particulate organic matter (POM), sea salt (SS), and mineral dust (DU) are included. The simulated global annual mean aerosol burdens (lifetimes) for the year 2000 are for SU: 0.80 Tg(S) (3.9 days), for BC: 0.11 Tg (5.4 days), for POM: 0.99 Tg (5.4 days), for SS: 10.5 Tg (0.8 days), and for DU: 8.28 Tg (4.6 days). An extensive evaluation with in-situ and remote sensing measurements underscores that the model results are generally in good agreement with observations of the global aerosol system. The simulated global annual mean aerosol optical depth (AOD) is with 0.14 in excellent agreement with an estimate derived from AERONET measurements (0.14) and a composite derived from MODIS-MISR satellite retrievals (0.16). Regionally, the deviations are not negligible. However, the main patterns of AOD attributable to anthropogenic activity are reproduced.
A curved multi-component aerosol hygroscopicity model framework: Part 1 – Inorganic compounds
Authors: Topping D. O. , McFiggans G. B. , Coe H.
Published: April 2010

Abstract. A thermodynamic modelling framework to predict the equilibrium behaviour of mixed inorganic salt aerosols is developed, and then coupled with a technique for finding a solution to the Kohler equation in order to create a diameter dependent hygroscopic aerosol model (Aerosol Diameter Dependent Equilibrium Model – ADDEM). The model described here provides a robust and accurate inorganic basis using a mole fraction based activity coefficient model and adjusted energies of formation for treating solid precipitation. The model framework can accommodate organic components, though this added complexity is considered in a companion paper, this paper describes the development of the modelling architecture to be used and predictions of an inorganic model alone. The modelling framework has been developed to flexibly use a combination of mixing rules and other potentially more accurate techniques where available to calculate the water content. Comparisons with other state-of-the-art general equilibrium models and experimental data are presented and show excellent agreement. The Kelvin effect can be considered in this scheme using a variety of surface tension models. Comparison of predicted diameter dependent phenomena, such as the increased relative humidity for onset of deliquescence with decreasing diameter, with another diameter dependent model is very good despite the different approach used. The model is subject to various sensitivities. For the inorganic systems studied here, the model is sensitive to choice of surface tension scheme used, which decreases for larger aerosol. Large sensitivities are found for the value of dry density used. It is thus likely that the history of the aerosol studied in a hygroscopic tandem differential mobility analyser (HTDMA), specifically the nature of the drying process that will influence the final crystalline form, will create systematic uncertainties upon comparisons with theoretical predictions. However, the magnitudes of all of the above sensitivities are potentially less than those introduced when using a semi ideal growth factor analogue for certain conditions.
A curved multi-component aerosol hygroscopicity model framework: Part 2 – Including organic compounds
Authors: Topping D. O. , McFiggans G. B. , Coe H.
Published: April 2010

Abstract. This paper describes the inclusion of organic particulate material within the Aerosol Diameter Dependent Equilibrium Model (ADDEM) framework described in the companion paper applied to inorganic aerosol components. The performance of ADDEM is analysed in terms of its capability to reproduce the behaviour of various organic and mixed inorganic/organic systems using recently published bulk data. Within the modelling architecture already described two separate thermodynamic models are coupled in an additive approach and combined with a method for solving the Kohler equation in order to develop a tool for predicting the water content associated with an aerosol of known inorganic/organic composition and dry size. For development of the organic module, the widely used group contribution method UNIFAC is employed to explicitly deal with the non-ideality in solution. The UNIFAC predictions for components of atmospheric importance were improved considerably by using revised interaction parameters derived from electro-dynamic balance studies. Using such parameters, the model was found to adequately describe mixed systems including 5–6 dicarboxylic acids, down to low relative humidity conditions. By comparison with electrodynamic balance data, it was also found that the model was capable of capturing the behaviour of aqueous aerosols containing Suwannee River Fulvic acid, a structure previously used to represent the functionality of complex oxidised macromolecules often found in atmospheric aerosols. The additive approach for modelling mixed inorganic/organic systems worked well for a variety of mixtures. As expected, deviations between model predictions and measurements increase with increasing concentration. Available surface tension models, used in evaluating the Kelvin term, were found to reproduce measured data with varying success. Deviations from experimental data increased with increased organic compound complexity. For components only slightly soluble in water, significant deviations from measured surface tension depression behaviour were predicted with both model formalisms tested. A Sensitivity analysis showed that such variation is likely to lead to predicted growth factors within the measurement uncertainty for growth factor taken in the sub-saturated regime. Greater sensitivity was found for the value of dry density used in the assumed form of the dried out aerosol. Comparison with a coupled thermodynamic approach showed that assumed values for interactions parameters may lead to erroneous results where a simple additive approach may provide more accurate results. However, where available, the use of coupled thermodynamics can better reproduce measured behaviour. Further work (and laboratory data) is required to assess whether this difference lies within the experimental uncertainty of observed hygroscopic behaviour for a variety of systems.
Analysis of water vapor LIDAR measurements during the MAP campaign: evidence of sub-structures of stratospheric intrusions
Authors: D'Aulerio P. , Fierli F. , Congeduti F. , Redaelli G.
Published: April 2010

Abstract. This paper presents two case studies of transport of dry air in the free troposphere measured by a ground based Raman LIDAR in the Northern-Italy, during the Mesoscale Alpine Programme (MAP). Two observations characterized by the presence of anomalously dry layers, below 6 km height, were analyzed using Lagrangian techniques. These events are related to upper-tropospheric, high Potential Vorticity (PV) streamers crossing the Alpine region. These are interpreted as small-scale features of stratospheric intrusions associated with the PV ridge during its phase of dissipation. One of the measurements also shows the presence of two distinct dehydrated structures associated with the same event. The water vapor concentration also suggests dilution processes of dry stratospheric air in the troposphere. Lagrangian simulations allowed to successfully reproduce the observed water vapor distribution and the air parcel histories confirmed the stratospheric origin of the dry layers.
Evaluation of SHADOZ sondes, HALOE and SAGE II ozone profiles at the tropics from SAOZ UV-Vis remote measurements onboard long duration balloons
Authors: Borchi F. , Pommereau J.-P. , Garnier A. , Pinharanda M.
Published: April 2010

Abstract. Ozone profiles from 10 to 26km have been obtained at almost constant latitude (20 ± 5° S) in the tropics using SAOZ UV-vis spectrometers flown onboard long duration balloons in 2001 and 2003. The precision of the measurements is estimate to be better than 2% in the stratosphere (3.5% accuracy) and 5-6% in the troposphere (12% and 25% accuracy at 15km and 10km respectively) with an altitude uncertainty of -30 ± 25m. The variability of ozone concentration along a latitudinal circle at 20° S in the SH summer is found smaller than 3-4% above 20km, but increasing rapidly below in the Tropical Tropopause Layer (TTL). The high correlation between PV and ozone suggests that most of this variability can be attributed to quasi-horizontal exchange with the mid-latitude stratosphere. The performances of the SHADOZ ozonesonde network, HALOE and SAGE II in the tropics have been studied by comparison with SAOZ measurements. In the stratosphere, the main discrepancies arise from differences in altitude registration, particularly sensitive between 20 and 26km in the tropics because of the strong gradient of ozone concentration. In the upper troposphere, the SAOZ measurements are consistent with those of the sondes and the lidar in cloud free conditions, but biased high by 60% on average compared to ozonesondes over the Western Pacific, at American Samoa and Fiji. The likely explanation is the frequent occurrence of near zero ozone layers in the convective clouds of the South Pacific Convergence Zone which cannot be seen by SAOZ as well as all ground-based and space borne remote sensing instruments. Compared to SAOZ, SAGE II displays a 50-60% low bias similar to that already known with the ozonesondes, and a larger zonal variability. However, the significant correlation with PV suggests that useful information on tropospheric ozone could be derived from SAGE II. Finally, the unrealistic large offsets and variability in the HALOE data compared to all others, indicates that the measurements of this instrument are of limited use below 17km.
Three-dimensional model study of the Arctic ozone loss in 2002/2003 and comparison with 1999/2000 and 2003/2004
Authors: Feng W. , Chipperfield M. P. , Davies S. , Sen B. , Toon G. , Blavier J. F. , Webster C. R. , Volk C. M. , Ulanovsky A. , Ravegnani F. , von der Gathen P. , Jost H. , Richard E. C. , Claude H.
Published: April 2010

Abstract. We have used the SLIMCAT 3-D off-line chemical transport model (CTM) to quantify the Arctic chemical ozone loss in the year 2002/2003 and compare it with similar calculations for the winters 1999/2000 and 2003/2004. Recent changes to the CTM have improved the model's ability to reproduce polar chemical and dynamical processes. The updated CTM uses σ-θ as a vertical coordinate which allows it to extend down to the surface. The CTM has a detailed stratospheric chemistry scheme and now includes a simple NAT-based denitrification scheme in the stratosphere. In the model runs presented here the model was forced by ECMWF ERA40 and operational analyses. The model used 24 levels extending from the surface to ~55km and a horizontal resolution of either 7.5° x 7.5° or 2.8° x 2.8°. Two different radiation schemes, MIDRAD and the CCM scheme, were used to diagnose the vertical motion in the stratosphere. Based on tracer observations from balloons and aircraft, the more sophisticated CCM scheme gives a better representation of the vertical transport in this model which includes the troposphere. The higher resolution model generally produces larger chemical O3 depletion, which agrees better with observations. The CTM results show that very early chemical ozone loss occurred in December 2002 due to extremely low temperatures and early chlorine activation in the lower stratosphere. Thus, chemical loss in this winter started earlier than in the other two winters studied here. In 2002/2003 the local polar ozone loss in the lower stratosphere was ~40% before the stratospheric final warming. Larger ozone loss occurred in the cold year 1999/2000 which had a persistently cold and stable vortex during most of the winter. For this winter the current model, at a resolution of 2.8° x 2.8°, can reproduce the observed loss of over 70% locally. In the warm and more disturbed winter 2003/2004 the chemical O3 loss was generally much smaller, except above 620K where large losses occurred due to a period of very low minimum temperatures at these altitudes.
Ozone loss derived from balloon-borne tracer measurements in the 1999/2000 Arctic winter
Authors: Robinson A. D. , Millard G. A. , Danis F. , Guirlet M. , Harris N. R. P. , Lee A. M. , McIntyre J. D. , Pyle J. A. , Arvelius J. , Dagnesjo S. , Kirkwood S. , Nilsson H. , Toohey D. W. , Deshler T. , Goutail F. , Pommereau J.-P. , Elkins J. W. , Moore F. , Ray E. , Schmidt U. , Engel A. , Müller M.
Published: April 2010

Abstract. Balloon-borne measurements of CFC11 (from the DIRAC in situ gas chromatograph and the DESCARTES grab sampler), ClO and O3 were made during the 1999/2000 Arctic winter as part of the SOLVE-THESEO 2000 campaign, based in Kiruna (Sweden). Here we present the CFC11 data from nine flights and compare them first with data from other instruments which flew during the campaign and then with the vertical distributions calculated by the SLIMCAT 3D CTM. We calculate ozone loss inside the Arctic vortex between late January and early March using the relation between CFC11 and O3 measured on the flights. The peak ozone loss (~1200ppbv) occurs in the 440-470K region in early March in reasonable agreement with other published empirical estimates. There is also a good agreement between ozone losses derived from three balloon tracer data sets used here. The magnitude and vertical distribution of the loss derived from the measurements is in good agreement with the loss calculated from SLIMCAT over Kiruna for the same days.
One-year record of organic and elemental carbon in fine particles in downtown Beijing and Shanghai
Authors: Yang F. , He K. , Ye B. , Chen X. , Cha L. , Cadle S. H. , Chan T. , Mulawa P. A.
Published: April 2010

Abstract. Weekly PM2.5 samples were collected for one year (1999-2000) in Beijing and Shanghai and the carbonaceous species analyzed to investigate and compare their time series patterns and possible sources in the two biggest cities of China. Weekly carbonaceous concentrations varied in wide ranges with 8.6-59µg m-3 for OC and 1.5-25.4µg m-3 for EC in Beijing, and with 5.1-38.4µg m-3 for OC and 2.3-13.0µg m-3 for EC in Shanghai. Similar weekly and seasonal variations of OC and EC concentrations were found in each city though major combustion sources presented source-dependent emission characteristics and seasonal differences in emission amount for carbonaceous species. Both OC and EC maintained much higher concentrations in late fall through winter, probably due to enhanced emissions coupled with unfavorable meteorological conditions. In Beijing, the 14C analysis of limited samples suggested there was a significant contribution (33-48%) of modern carbon to the total fine carbonaceous PM burden with higher fractions in the harvest seasons. The high mass ratios of excessive potassium to EC in both Beijing and Shanghai also indicated that biomass burning had important contribution to fine carbonaceous particles.
GPS radio occultation with CHAMP and SAC-C: global monitoring of thermal tropopause parameters
Authors: Schmidt T. , Heise S. , Wickert J. , Beyerle G. , Reigber C.
Published: April 2010

Abstract. In this study the global lapse-rate tropopause (LRT) pressure, temperature, potential temperature, and sharpness are discussed based on Global Positioning System (GPS) radio occultations (RO) from the German CHAMP (CHAllenging Minisatellite Payload) and the U.S.-Argentinian SAC-C (Satelite de Aplicaciones Cientificas-C) satellite missions. Results with respect to seasonal variations are compared with operational radiosonde data and ECMWF (European Centre for Medium-Range Weather Forecast) operational analyses. Results on the tropical quasi-biennial oscillation (QBO) are updated from an earlier study. CHAMP RO data are available continuously since May 2001 with on average 150 high resolution temperature profiles per day. SAC-C data are available for several periods in 2001 and 2002. In this study temperature data from CHAMP for the period May 2001-December 2004 and SAC-C data from August 2001-October 2001 and March 2002-November 2002 were used, respectively. The bias between GPS RO temperature profiles and radiosonde data was found to be less than 1.5K between 300 and 10hPa with a standard deviation of 2-3K. Between 200-20hPa the bias is even less than 0.5K (2K standard deviation). The mean deviations based on 167699 comparisons between CHAMP/SAC-C and ECMWF LRT parameters are (-2.1±37.1)hPa for pressure and (0.1±4.2)K for temperature. Comparisons of LRT pressure and temperature between CHAMP and nearby radiosondes (13230) resulted in (5.8±19.8)hPa and (-0.1±3.3)K, respectively. The comparisons between CHAMP/SAC-C and ECMWF show on average the largest differences in the vicinity of the jet streams with up to 700m in LRT altitude and 3K in LRT temperature, respectively. The CHAMP mission generates the first long-term RO data set. Other satellite missions will follow (GRACE, COSMIC, MetOp, TerraSAR-X, EQUARS) generating together some thousand temperature profiles daily.
Initial validation of ENVISAT/SCIAMACHY columnar CO by FTIR profile retrievals at the Ground-Truthing Station Zugspitze
Authors: Sussmann R. , Buchwitz M.
Published: April 2010

Abstract. Carbon monoxide vertical profile retrievals from ground-based solar FTIR measurements at the Permanent Ground-Truthing Station Zugspitze (47.42° N, 10.98° E, 2964m a.s.l.), Germany are used to validate columnar CO retrieved from ENVISAT/SCIAMACHY spectra (WFM-DOAS version 0.4). The WFM-DOAS retrievals of CO include an empirical column scaling factor of 0.5. Therefore, not absolute column levels are validated, but the proper response of the SCIAMACHY retrievals to the atmospheric inter-annual variability is quantitatively assessed in comparison to the Zugspitze FTIR results. Although CO WFM-DOAS data for only 33 days were available for this study (data covering January-October 2003), it is possible to retrieve information on the CO annual cycle (≈10% amplitude) in a statistically significant fit out of the scatter of the SCIAMACHY WFM-DOAS data. To obtain this, all pixels within a minimum radius of 2000km around Zugspitze had to be averaged for each day.
Midlatitude ClO during the maximum atmospheric chlorine burden: in situ balloon measurements and model simulations
Authors: Vogel B. , Müller R. , Engel A. , Grooß J.-U. , Toohey D. , Woyke T. , Stroh F.
Published: April 2010

Abstract. Chlorine monoxide (ClO) plays a key role in stratospheric ozone loss processes at midlatitudes. We present two balloon-borne in situ measurements of ClO conducted in northern hemisphere midlatitudes during the period of the maximum of total inorganic chlorine loading in the atmosphere. Both ClO measurements were conducted on board the TRIPLE balloon payload, launched in November 1996 in León, Spain, and in May 1999 in Aire sur l'Adour, France. For both flights a ClO daylight and night-time vertical profile was derived over an altitude range of approximately 15-35 km. ClO mixing ratios are compared to model simulations performed with the photochemical box model version of the Chemical Lagrangian Model of the Stratosphere (CLaMS). Simulations along 24-hour backward trajectories were performed to study the diurnal variation of ClO in the midlatitude lower stratosphere. Model simulations for the flight launched in Aire sur l'Adour 1999 show an excellent agreement with the ClO measurements. For the flight launched in León 1996, an overall good agreement is found, whereas the flight is characterized by a more complex dynamical situation due to a possible mixture of vortex and non-vortex air. We note that for both flights at solar zenith angles greater than 86°-87° simulated ClO mixing ratios are higher than observed ClO mixing ratios. However, the present findings indicate that no substantial uncertainties exist in midlatitude chlorine chemistry of the stratosphere.
Halogens and the chemistry of the free troposphere
Authors: Lary D. J.
Published: April 2010

Abstract. The role of halogens in both the marine boundary layer and the stratosphere has long been recognized, while their role in the free troposphere is often not considered in global chemical models. However, a careful examination of free-tropospheric chemistry constrained by observations using a full chemical data assimilation system shows that halogens do play a significant role in the free troposphere. In particular, the chlorine initiation of methane oxidation in the free troposphere can contribute more than 10%, and in some regions up to 50%, of the total rate of initiation. The initiation of methane oxidation by chlorine is particularly important below the polar vortex and in northern mid-latitudes. Likewise, the hydrolysis of alone can contribute more than 35% of the production rate in the free-troposphere.
Emergence of a tracer source from air concentration measurements, a new strategy for linear assimilation
Authors: Issartel J.-P.
Published: April 2010

Abstract. The measurement of atmospheric concentrations by a monitoring network is a promising tool for the identification of the widespread sources of trace species. The paper addresses the case of the species scattered linearly by a known meteorology. The question is classical: what can be said about the source from a set of measurements? Is it possible to guess from the values observed by the measurements that the source is spread close to the detectors, or that the tracer comes from a remote region? And, if the source was a point source, would it be possible to understand it by just considering these values? A part of the answers is a matter of practical sense: the resolution with which an emission can be retrieved will always be limited and probably lower for a remote region, even if the detectors and dispersion model are error free. The paper proposes a linear strategy of inference: to any set of values taken by the observed concentrations is associated linearly an estimate of the source. Doubled values lead to a doubled estimate. The method, based on adjoint techniques, is intended to optimise the resolution by quantifying, with the concept of illumination, which regions are well, poorly or not seen at all. The illumination tied to ordinary adjoint functions becomes excessive close to the detectors thus leading to inversion artefacts. This may be corrected by attributing each point of the space time domain a geometric and statistical weight. The adjoint functions are transformed. The choice of this renormalising function is constrained by an unambiguous entropic criterion preventing any overestimation of the available information that would lead to artefacts. It amounts to evenly distribute the information between the points organised with their weights as a "known domain". The theory is illustrated by calculations performed with the experimental source ETEX1.
Density changes of aerosol particles as a result of chemical reaction
Authors: Katrib Y. , Martin S. T. , Rudich Y. , Davidovits P. , Jayne J. T. , Worsnop D. R.
Published: April 2010

Abstract. This paper introduces the capability to study simultaneously changes in the density, the chemical composition, the mobility diameter, the aerodynamic diameter, and the layer thickness of multi-layered aerosol particles as they are being altered by heterogeneous chemical reactions. A vaporization-condensation method is used to generate aerosol particles composed of oleic acid outer layers of 2 to 30nm on 101-nm polystyrene latex cores. The layer density is modified by reaction of oleic acid with ozone for variable exposure times. For increasing ozone exposure, the mobility diameter decreases while the vacuum aerodynamic diameter increases, which, for spherical particles, implies that particle density increases. The aerosol particles are confirmed as spherical based upon the small divergence of the particle beam in the aerosol mass spectrometer. The particle and layer densities are calculated by two independent methods, namely one based on the measured aerodynamic and mobility diameters and the other based on the measured mobility diameter and particle mass. The uncertainty estimates for density calculated by the second method are two to three times greater than those of the first method. Both methods indicate that the layer density increases from 0.89 to 1.12g·cm-3 with increasing ozone exposure. Aerosol mass spectrometry shows that, concomitant with the increase in the layer density, the oxygen content of the reacted layer increases. Even after all of the oleic acid has reacted, the layer density and the oxygen content continue to increase slowly with prolonged ozone exposure, a finding which indicates continued chemical reactions of the organic products either with ozone or with themselves. The results of this paper provide new insights into the complex changes occurring for atmospheric particles during the aging processes caused by gas-phase oxidants.
Refining temperature measures in thermal/optical carbon analysis
Authors: Chow J. C. , Watson J. G. , Chen L.-W. A. , Paredes-Miranda G. , Chang M.-C. O. , Trimble D. , Fung K. K. , Zhang H. , Zhen Yu J.
Published: April 2010

Abstract. Thermal/optical methods have been widely used for quantifying total carbon (TC), organic carbon (OC), and elemental carbon (EC) in ambient and source particulate samples. Thermally defined carbon fractions have been used for source identification. Temperature precision in thermal carbon analysis is critical to the allocation of carbon fractions. The sample temperature is determined by a thermocouple, which is usually located in the oven near the sample. Sample and thermocouple temperature may differ owing to different thermal properties between the sample filter punch and the thermocouple, or inhomogeneities in the heating zone. Quick-drying temperature-indicating liquids (Tempil Inc., South Plainfield, NJ) of different liquefying points are used as temperature calibration standards. These consist of chemicals that change their appearance at specific temperatures and can be optically monitored to determine the sample temperature. Temperature measures were evaluated for three different models of carbon analyzers. Sample temperatures were found to differ from sensor temperatures by 10 to 50°C. Temperature biases of 14 to 22°C during thermal analysis were found to change carbon fraction measurements. The temperature indicators allow calibration curves to be constructed that relate the sample temperature to the temperature measured by a thermocouple.
Tropospheric ozone over Equatorial Africa: regional aspects from the MOZAIC data
Authors: Sauvage B. , Thouret V. , Cammas J.-P. , Gheusi F. , Athier G. , Nédélec P.
Published: April 2010

Abstract. We analyze ozone observations recorded over Equatorial Africa between April 1997 and March 2003 by the MOZAIC programme, providing the first ozone climatology deriving from continental in-situ data over this region. Three-dimensional streamlines strongly suggests connections between the characteristics of the ozone monthly mean vertical profiles, the most persistent circulation patterns in the troposphere over Equatorial Africa (on a monthly basis) such as the Harmattan, the African Easterly Jet, the Trades and the regions of ozone precursors emissions by biomass burning. During the biomass burning season in each hemisphere, the lower troposphere exhibits layers of enhanced ozone (i.e. 70 ppbv over the coast of Gulf of Guinea in December-February and 85 ppbv over Congo in June-August). The characteristics of the ozone monthly mean vertical profiles are clearly connected to the regional flow regime determined by seasonal dynamic forcing. The mean ozone profile over the coast of Gulf of Guinea in the burning season is characterized by systematically high ozone below 650hPa ; these are due to the transport by the Harmattan and the AEJ of the pollutants originating from upwind fires. The confinement of high ozone to the lower troposphere is due to the high stability of the Harmattan and the blocking Saharan anticyclone which prevents efficient vertical mixing. In contrast, ozone enhancements observed over Central Africa during the local dry season (June-August) are not only found in the lower troposphere but throughout the troposphere. Moreover, this study highlights a connection between the regions of the coast of Gulf of Guinea and regions of Congo to the south that appears on a semi annual basis. Vertical profiles in wet-season regions exhibit ozone enhancements in the lower troposphere due to biomass burning products transport from fires situated in the opposite dry-season hemisphere.