bluuebunny/crossref_metadata_2025 huggingface dataset:
Size-segregated fluxes of mineral dust from a desert area of northern China by eddy covariance
Authors: Fratini G. , Ciccioli P. , Febo A. , Forgione A. , Valentini R.
Published: April 2010

Abstract. Mineral dust emission accounts for a substantial portion of particles present in the troposphere. It is emitted most from desert areas, mainly through intense storm episodes. The aim of this work was to quantify size-segregated fluxes of mineral dust particles emitted during storm events occurring in desert areas of northern China (Alashan desert, Inner Mongolia), known to act as one of the strongest sources of mineral dust particles in the Asian continent. Long-range transport of mineral dust emitted in this area is responsible for the high particle concentrations reached in densely populated areas, including the city of Beijing. Based on a theoretical analysis, an eddy covariance system was built to get size-segregated fluxes of mineral dust particles with optical diameters ranging between 0.26 and 7.00 μm. The system was optimised to measure fluxes under intense storm event conditions. It was tested in two sites located in the Chinese portion of the Gobi desert. During the field campaign, an intense storm event was recorded in one of them. Data obtained during this event indicate that particle number fluxes were dominated by the finer fraction, whereas in terms of volume, coarser particle accounted for the largest portion. It was found that during the storm event, ratios of size-segregated particle volume fluxes remained substantially constant and a simple parameterization of particle emission from total volume fluxes was possible. A strong correlation was also found between particle volume fluxes and the friction velocity. This relationship is extremely useful to investigate mechanisms of particle formation by wind erosion.
A semi-analytical method for calculating rates of new sulfate aerosol formation from the gas phase
Authors: Kazil J. , Lovejoy E. R.
Published: April 2010

Abstract. The formation of new sulfate aerosol from the gas phase is commonly represented in atmospheric modeling with parameterizations of the steady state nucleation rate. Such parameterizations are based on classical nucleation theory or on aerosol nucleation rate tables, calculated with a numerical aerosol model. These parameterizations reproduce aerosol nucleation rates calculated with a numerical aerosol model only imprecisely. Additional errors can arise when the nucleation rate is used as a surrogate for the production rate of particles of a given size. We discuss these errors and present a method which allows a more precise calculation of steady state sulfate aerosol formation rates. The method is based on the semi-analytical solution of an aerosol system in steady state and on parameterized rate coefficients for H2SO4 uptake and loss by sulfate aerosol particles, calculated from laboratory and theoretical thermodynamic data.
Model study of the cross-tropopause transport of biomass burning pollution
Authors: Duncan B. N. , Strahan S. E. , Yoshida Y.
Published: April 2010

Abstract. We present a modeling study of the troposphere-to-stratosphere transport (TST) of pollution from major biomass burning regions to the tropical tropopause layer (TTL) and lower stratosphere (LS). We show that biomass burning pollution regularly and significantly impacts the composition of the TTL/LS. TST occurs through 1) slow ascent in the TTL and 2) quasi-horizontal exchange in the regions of the subtropical jets; we find both pathways to be important. The seasonal oscillation in CO in the TTL/LS (i.e., the CO "tape recorder") is caused largely by seasonal changes in biomass burning. Another contributing factor is the long-range transport of northern hemispheric pollution (e.g., biofuels and fossil fuels) to the northern tropics in boreal winter. Other tropical sources of CO (e.g., methane oxidation) have insignificant seasonal variation, contributing little to the tape recorder. Interannual variation of CO in the TTL/LS is caused by year-to-year variations in biomass burning and the strength, frequency, and locations of deep convection, which lofts pollution to the upper troposphere. During our study period, 1994–1998, we find that the highest concentrations of CO in the TTL/LS occur during the strong 1997/98 El Niño event for two reasons: i.~tropical deep convection was stronger and ii.~emissions were higher. This extreme event can be seen as an upper bound on the impact of biomass burning pollution on the TTL/LS. We estimate that the 1997 Indonesian wildfires increased CO in the entire TTL and tropical LS (<60 mb) by more than 40% and 10%, respectively, for several months. Zonal mean ozone increased and the hydroxyl radical decreased by as much as 20%, increasing the lifetimes and, subsequently TST, of trace gases. Our results indicate that the impact of biomass burning pollution on the TTL/LS is likely greatest during an El Niño event due to favorable dynamics and historically higher burning rates.
Arctic smoke – aerosol characteristics during a record air pollution event in the European Arctic and its radiative impact
Authors: Treffeisen R. , Turnved P. , Ström J. , Herber A. , Bareiss J. , Helbig A. , Stone R. S. , Hoyningen-Huene W. , Krejci R. , Stohl A. , Neuber R.
Published: April 2010

Abstract. In early May 2006 a record high air pollution event was observed at Ny-Ålesund, Spitsbergen. An atypical weather pattern established a pathway for the rapid transport of biomass burning aerosols from agricultural fires in Eastern Europe to the Arctic. Atmospheric stability was such that the smoke was constrained to low levels, within 2 km of the surface during the transport. A description of this smoke event in terms of transport and main aerosol characteristics can be found in Stohl et al. (2007). This study puts emphasis on the radiative effect of the smoke. The aerosol size distribution was characterized as having an accumulation mode centered at 165–185 nm and almost 1.6 for geometric standard deviation of the mode. Nucleation and small Aitken mode particles were almost completely suppressed within the smoke plume measured at Ny-Ålesund. Chemical and microphysical aerosol information obtained at Mt. Zeppelin (474 m.a.s.l) was used to derive input parameters for a one-dimensional radiation transfer model to explore the radiative effects of the smoke. The daily mean heating rate calculated on 2 May 2006 for the average size distribution and measured chemical composition reached 0.55 K day−1 at 0.5 km altitude for the assumed external mixture of the aerosols but showing much higher heating rates for an internal mixture (1.7 K day−1). In comparison a case study for March 2000 showed that the local climatic effects due to Arctic haze, using a regional climate model, HIRHAM, amounts to a maximum of 0.3 K day−1 of heating at 2 km altitude (Treffeisen et al., 2005).
Hydrocarbon fluxes above a Scots pine forest canopy: Measurements and modeling
Authors: Rinne J. , Taipale R. , Markkanen T. , Ruuskanen T. M. , Hellén H. , Kajos M. K. , Vesala T. , Kulmala M.
Published: April 2010

Abstract. We measured the fluxes of several hydrocarbon species above a Scots pine (Pinus sylvestris) stand using disjunct eddy covariance technique with proton transfer reaction – mass spectrometry. The measurements were conducted during four days in July at SMEAR II research station in Hyytiälä, Finland. Compounds which showed significant emission fluxes were methanol, acetaldehyde, acetone, and monoterpenes. A stochastic Lagrangian transport model with simple chemical degradation was applied to assess the sensitivity of the above canopy fluxes to chemistry. According to the model, the chemical degradation had a minor effect on the fluxes measured in this study but has a major effect on the vertical flux profiles of more reactive compounds, such as sesquiterpenes. The monoterpene fluxes followed the traditional exponential temperature dependent emission algorithm but were considerably higher than the fluxes measured before at the same site. The normalized emission potential (30°C) was 2.5 μg gdw–1 h−1 obtained using the temperature dependence coefficient of 0.09°C−1.
Lightning-produced NOx over Brazil during TROCCINOX: Airborne measurements in tropical and subtropical thunderstorms and the importance of mesoscale convective systems
Authors: Huntrieser H. , Schlager H. , Roiger A. , Lichtenstern M. , Schumann U. , Kurz C. , Brunner D. , Schwierz C. , Richter A. , Stohl A.
Published: April 2010

Abstract. During the TROCCINOX field experiments in February–March 2004 and February 2005, airborne in situ measurements of NO, NOy, CO, and O3 mixing ratios and the J(NO2) photolysis rate were carried out in the anvil outflow of thunderstorms over southern Brazil. Both tropical and subtropical thunderstorms were investigated, depending on the location of the South Atlantic convergence zone. Tropical air masses were discriminated from subtropical ones according to the higher equivalent potential temperature (Θe) in the lower and mid troposphere, the higher CO mixing ratio in the mid troposphere, and the lower wind velocity and proper wind direction in the upper troposphere. During thunderstorm anvil penetrations, typically at 20–40 km horizontal scales, NOx mixing ratios were on average enhanced by 0.2–1.6 nmol mol−1. This enhancement was mainly attributed to NOx production by lightning and partly due to upward transport from the NOx-richer boundary layer. In addition, CO mixing ratios were occasionally enhanced, indicating upward transport from the boundary layer. For the first time, the composition of the anvil outflow from a large, long-lived mesoscale convective system (MCS) advected from northern Argentina and Uruguay was investigated in more detail. Over a horizontal scale of about 400 km, NOx, CO and O3 mixing ratios were significantly enhanced in these air masses in the range of 0.6–1.1, 110–140 and 60–70 nmol mol−1, respectively. Analyses from trace gas correlations and a Lagrangian particle dispersion model indicate that polluted air masses, probably from the Buenos Aires urban area and from biomass burning regions, were uplifted by the MCS. Ozone was distinctly enhanced in the aged MCS outflow, due to photochemical production and entrainment of O3-rich air masses from the upper troposphere – lower stratosphere region. The aged MCS outflow was transported to the north, ascended and circulated, driven by the Bolivian High over the Amazon basin. In the observed case, the O3-rich MCS outflow remained over the continent and did not contribute to the South Atlantic ozone maximum.
The global lightning-induced nitrogen oxides source
Authors: Schumann U. , Huntrieser H.
Published: April 2010

Abstract. The knowledge of the lightning-induced nitrogen oxides (LNOx) source is important for understanding and predicting the nitrogen oxides and ozone distributions in the troposphere and their trends, the oxidising capacity of the atmosphere, and the lifetime of trace gases destroyed by reactions with OH. This knowledge is further required for the assessment of other important NOx sources, in particular from aviation, the stratosphere, and from surface sources, and for understanding the possible feedback between climate changes and lightning. This paper reviews more then 3 decades of research. The review includes laboratory studies as well as surface, airborne and satellite-based observations of lightning and of NOx and related species in the atmosphere. Relevant data available from measurements in regions with strong LNOx influence are identified, including recent observations at midlatitudes and over tropical continents where most lightning occurs. Various methods to model LNOx at cloud scales or globally are described. Previous estimates are re-evaluated using the global annual mean flash frequency of 44±5 s−1 reported from OTD satellite data. From the review, mainly of airborne measurements near thunderstorms and cloud-resolving models, we conclude that a "typical" thunderstorm flash produces 15 (2–40)×1025 NO molecules per flash, equivalent to 250 mol NOx or 3.5 kg of N mass per flash with uncertainty factor from 0.13 to 2.7. Mainly as a result of previous global model studies for various LNOx parameterisations tested with related observations, the best estimate of the annual global LNOx nitrogen mass source and its uncertainty range is (5±3) Tg a−1 in this study. An accuracy of order 1 Tg a−1 or 20%, as necessary in particular for understanding tropical tropospheric chemistry, is still a challenging goal.
Evaluation of a coupled dispersion and aerosol process model against measurements near a major road
Authors: Pohjola M. A. , Pirjola L. , Karppinen A. , Härkönen J. , Ketzel M. , Kukkonen J.
Published: April 2010

Abstract. A field measurement campaign was conducted near a major road "Itäväylä" in an urban area in Helsinki in 17–20 February 2003. Aerosol measurements were conducted using a mobile laboratory "Sniffer" at various distances from the road, and at an urban background location. Measurements included particle size distribution in the size range of 7 nm–10 μm (aerodynamic diameter) by the Electrical Low Pressure Impactor (ELPI) and in the size range of 3–50 nm (mobility diameter) by Scanning Mobility Particle Sizer (SMPS), total number concentration of particles larger than 3 nm detected by an ultrafine condensation particle counter (UCPC), temperature, relative humidity, wind speed and direction, driving route of the mobile laboratory, and traffic density on the studied road. In this study, we have compared measured concentration data with the predictions of the road network dispersion model CAR-FMI used in combination with an aerosol process model MONO32. The vehicular exhaust emissions, and atmospheric dispersion and transformation of fine and ultrafine particles was evaluated within the distance scale of 200 m (corresponding to a time scale of a couple of minutes). We computed the temporal evolution of the number concentrations, size distributions and chemical compositions of various particle size classes. The atmospheric dilution rate of particles is obtained from the roadside dispersion model CAR-FMI. Considering the evolution of total number concentration, dilution was shown to be the most important process. The influence of coagulation and condensation on the number concentrations of particle size modes was found to be negligible at this distance scale. Condensation was found to affect the evolution of particle diameter in the two smallest particle modes. The assumed value of the concentration of condensable organic vapour of 1012 molecules cm−3 was shown to be in a disagreement with the measured particle size evolution, while the modelling runs with the concentration of condensable organic vapour of 109–1010 molecules cm−3 resulted in particle sizes that were closest to the measured values.
Investigation of the formaldehyde differential absorption cross section at high and low spectral resolution in the simulation chamber SAPHIR
Authors: Brauers T. , Bossmeyer J. , Dorn H.-P. , Schlosser E. , Tillmann R. , Wegener R. , Wahner A.
Published: April 2010

Abstract. The results from a simulation chamber study on the formaldehyde (HCHO) absorption cross section in the UV spectral region are presented. We performed 5 experiments at ambient HCHO concentrations with simultaneous measurements of two DOAS instruments in the atmosphere simulation chamber SAPHIR in Jülich. The two instruments differ in their spectral resolution, one working at 0.2 nm (broad-band, BB-DOAS), the other at 2.7 pm (high-resolution, HR-DOAS). Both instruments use dedicated multi reflection cells to achieve long light path lengths of 960 m and 2240 m, respectively, inside the chamber. During three experiments HCHO was injected into the clean chamber by thermolysis of well defined amounts of para-formaldehyde reaching mixing rations of 40 ppbV at maximum. The HCHO concentration calculated from the injection and the chamber volume agrees with the BB-DOAS measured value when the absorption cross section of Meller and Moortgat (2000) was used for data evaluation. In two further experiments we produced HCHO in-situ from the ozone + ethene reaction which was intended to provide an independent way of HCHO calibration through the measurements of ozone and ethene. However, we found an unexpected deviation from the current understanding of the ozone + ethene reaction when CO was added to suppress possible oxidation of ethene by OH radicals. The reaction of the Criegee intermediate with CO could to be 240 times slower than currently assumed. Based on the BB-DOAS measurements we could deduce a high-resolution cross section for HCHO which was not measured directly so far.
Global trends in visibility: implications for dust sources
Authors: Mahowald N. M. , Ballantine J. A. , Feddema J. , Ramankutty N.
Published: April 2010

Abstract. There is a large uncertainty in the relative roles of human land use, climate change and carbon dioxide fertilization in changing desert dust source strength over the past 100 years, and the overall sign of human impacts on dust is not known. We used visibility data from meteorological stations in dusty regions to assess the anthropogenic impact on long term trends in desert dust emissions. Visibility data are available at thousands of stations globally from 1900 to the present, but we focused on 359 stations with more than 30 years of data in regions where mineral aerosols play a dominant role in visibility observations. We evaluated the 1974 to 2003 time period because most of these stations have reliable records only during this time. We first evaluated the visibility data against AERONET aerosol optical depth data, and found that only in dusty regions are the two moderately correlated. Correlation coefficients between visibility derived variables and AERONET optical depths indicate a moderate correlation (~0.47), consistent with capturing about 20% of the variability in optical depths. Two visibility derived variables appear to compare the best with AERONET observations: the fraction of observations with visibility less than 5 km (VIS5) and the surface extinction (EXT). Regional trends show that in many dusty places, VIS5 and EXT are statistically significantly correlated with the palmer drought severity index (based on precipitation and temperature) or surface wind speeds, consistent with dust temporal variability being largely driven by meteorology. This is especially true for North African and Chinese dust sources, but less true in the Middle East, Australia or South America, where there are not consistent patterns in the correlations. Climate indices such as El Nino or the North Atlantic Oscillation are not correlated with visibility derived variables in this analysis. There are few stations where visibility measures are correlated with cultivation or grazing estimates on a temporal basis, although this may be a function of the very coarse temporal resolution of the land use datasets. On the other hand, spatial analysis of the visibility data suggests that natural topographic lows are not correlated with visibility, but land use is correlated at a moderate level. This analysis is consistent with land use being important in some regions, but meteorology driving interannual variability during 1974–2003.
Fine aerosol bulk composition measured on WP-3D research aircraft in vicinity of the Northeastern United States – results from NEAQS
Authors: Peltier R. E. , Sullivan A. P. , Weber R. J. , Brock C. A. , Wollny A. G. , Holloway J. S. , de Gouw J. A. , Warneke C.
Published: April 2010

Abstract. During the New England Air Quality Study (NEAQS) in the summer of 2004, airborne measurements were made of the major inorganic ions and the water-soluble organic carbon (WSOC) of the submicron (PM1.0) aerosol. These and ancillary data are used to describe the overall aerosol chemical characteristics encountered during the study. Fine particle mass was estimated from particle volume and a calculated density based on measured particle composition. Fine particle organic matter (OM) was estimated from WSOC and a mass balance analysis. The aerosol over the northeastern United States (U.S.) and Canada was predominately sulfate and associated ammonium, and organic components, although in unique plumes additional ionic components were also periodically above detection limits. In power generation regions, and especially in the Ohio River Valley region, the aerosol tended to be predominantly sulfate (~60% μg μg−1) and apparently acidic, based on an excess of measured anions compared to cations. In all other regions where sulfate concentrations were lower and a smaller fraction of overall mass, the cations and anions were balanced suggesting a more neutral aerosol. In contrast, the WSOC and estimated OM were more spatially uniform and the fraction of OM relative to PM mass largely influenced by sources of sulfate. The study median OM mass fraction was 40%. Throughout the study region, sulfate and organic aerosol mass were highest near the surface and decreased rapidly with increasing altitude. The relative fraction of organic mass to sulfate was similar within the boundary layer (altitude less than ~2.5 km), but was significantly higher in the free troposphere (above ~2.5 km). A number of distinct biomass burning plumes from fires in Alaska and the Yukon were periodically intercepted, mostly at altitudes between 3 and 4 km. These plumes were associated with highest aerosol concentrations of the study and were largely comprised of organic aerosol components (~60%).
Technical Note: simulation of detailed aerosol chemistry on the global scale using MECCA-AERO
Authors: Kerkweg A. , Sander R. , Tost H. , Jöckel P. , Lelieveld J.
Published: April 2010

Abstract. We present the MESSy submodel MECCA-AERO, which simulates both aerosol and gas phase chemistry with the same mechanism. Including the aerosol phase into the chemistry mechanism increases the stiffness of the resulting set of differential equations. The numerical aspects of the approach followed in MECCA-AERO are presented. MECCA-AERO requires input of an aerosol dynamical/microphysical model to provide the aerosol size and particle number information of the modes/bins for which the chemistry is explicitly calculated. Additional precautions are required to avoid the double counting of processes, especially for sulphate in the aerosol dynamical and the chemistry model. This coupling is explained in detail. To illustrate the capabilities of the new aerosol submodel, examples for species usually treated in aerosol dynamical models are shown. The aerosol chemistry as provided by MECCA-AERO is very sumptuous and not readily applicable for long-term simulations, though it provides a reference to evaluate simplified approaches.
GEM/POPs: a global 3-D dynamic model for semi-volatile persistent organic pollutants – 1. Model description and evaluations
Authors: Gong S. L. , Huang P. , Zhao T. L. , Sahsuvar L. , Barrie L. A. , Kaminski J. W. , Li Y. F. , Niu T.
Published: April 2010

Abstract. GEM/POPs was developed to simulate the transport, deposition and partitioning of semi-volatile persistent organic pollutants (POPs) in the atmosphere within the framework of Canadian weather forecasting model GEM. In addition to the general processes such as anthropogenic emissions, atmosphere/water and atmosphere/soil exchanges, GEM/POPs incorporates a dynamic aerosol module to provide the aerosol surface areas for the semi-volatile POPs to partition between gaseous and particle phases and a mechanism for particle-bound POPs to be removed. Simulation results of three PCBs (28, 153 and 180) for year 2000 indicate that the model captured the main features of global atmospheric PCBs when compared with observations from EMEP, IADN and Alert stations. The annual averaged concentrations and the fractionation of the three PCBs as a function of latitudes are agreed reasonably well with observations. The impacts of atmospheric aerosols on the transports and partitioning of the three PCBs are reasonably simulated. The ratio of particulate to gaseous PCBs ranges from less than 0.1 for PCB28 to as high as 100 for PCB180, increasing from the warm lower latitudes to the cold high latitudes. Application of GEM/POPs in a study of the global transports and budgets of various PCBs accompanies this paper.
Evaluation of ECMWF ERA-40 temperature and wind in the lower tropical stratosphere since 1988 from past long-duration balloon measurements
Authors: Christensen T. , Knudsen B. M. , Pommereau J.-P. , Letrenne G. , Hertzog A. , Vial F. , Ovarlez J. , Piot M.
Published: April 2010

Abstract. The temperature and wind of the ECMWF ERA-40 reanalysis in the tropical lower stratosphere during the period 1988–2001 has been evaluated by comparison with independent in situ measurements of 21 IR Montgolfier and superpressure long-duration balloon flights performed by CNES from Pretoria (26° S) in South Africa in 1988–1989, Latacunga (1° S) in Ecuador in 1991–1998 and Bauru (22° S) in Brazil in 2000–2001. The ERA-40 temperature displays a bias varying progressively from +1.16 K in 1988–1989, to +0.26 K in 1994–1996 and −0.46 K after 1998, the latter being fully consistent with recent evaluations of ECMWF operational analysis from radio occultation and in situ long-duration balloon observations. The amplitude of the bias and its evolution are very similar to the results of a previous evaluation from radiosondes in 1991–2003, suggesting that the origin of the drift of ERA-40 might be mainly due to errors in the series of satellite measurements of MSU, replaced by AMSU in 1998, assimilated in the model. The ERA-40 zonal wind speed in the lower stratosphere appears slightly overestimated by 0.7–1.0 m/s on average in both the tropics and equatorial region, that is by 5–10% compared to the average 10–20 m/s wind speed. This bias, fully consistent with a recent evaluation of ECMWF operational analysis in 2004, is found constant during the whole 1988–2001 period, suggesting that the difference in that case might originate in the model. Finally calculated trajectories using ERA-40, frequently used for analysing field observations, are found in error compared to that of the balloons by ±500 km after 5 days and ±1000 km after 10 days.
Cloud microphysics and aerosol indirect effects in the global climate model ECHAM5-HAM
Authors: Lohmann U. , Stier P. , Hoose C. , Ferrachat S. , Roeckner E. , Zhang J.
Published: April 2010

Abstract. The double-moment cloud microphysics scheme from ECHAM4 has been coupled to the size-resolved aerosol scheme ECHAM5-HAM. ECHAM5-HAM predicts the aerosol mass and number concentrations and the aerosol mixing state. This results in a much better agreement with observed vertical profiles of the black carbon and aerosol mass mixing ratios than with the previous version ECHAM4, where only the different aerosol mass mixing ratios were predicted. Also, the simulated liquid, ice and total water content and the cloud droplet and ice crystal number concentrations as a function of temperature in stratiform mixed-phase clouds between 0 and –35°C agree much better with aircraft observations in the ECHAM5 simulations. ECHAM5 performs better because more realistic aerosol concentrations are available for cloud droplet nucleation and because the Bergeron-Findeisen process is parameterized as being more efficient. The total anthropogenic aerosol effect includes the direct, semi-direct and indirect effects and is defined as the difference in the top-of-the-atmosphere net radiation between present-day and pre-industrial times. It amounts to –1.8 W m−2 in ECHAM5, when a relative humidity dependent cloud cover scheme and present-day aerosol emissions representative for the year 2000 are used. It is larger when either a statistical cloud cover scheme or a different aerosol emission inventory are employed.
Ice nucleation of ammonia gas exposed montmorillonite mineral dust particles
Authors: Salam A. , Lohmann U. , Lesins G.
Published: April 2010

Abstract. The ice nucleation characteristics of montmorillonite mineral dust aerosols with and without exposure to ammonia gas were measured at different atmospheric temperatures and relative humidities with a continuous flow diffusion chamber. The montmorillonite particles were exposed to pure (100%) and diluted ammonia gas (25 ppm) at room temperature in a stainless steel chamber. There was no significant change in the mineral dust particle size distribution due to the ammonia gas exposure. 100% pure ammonia gas exposure enhanced the ice nucleating fraction of montmorillonite mineral dust particles 3 to 8 times at 90% relative humidity with respect to water (RHw) and 5 to 8 times at 100% RHw for 120 min exposure time within our experimental conditions. The percentages of active ice nuclei were 2 to 9 times higher at 90% RHw and 2 to 13 times higher at 100% RHw in 25 ppm ammonia exposed montmorillonite compared to unexposed montmorillonite. All montmorillonite particles are more efficient as ice nuclei with increasing relative humidities and decreasing temperatures. The activation temperature of montmorillonite exposed to 100% pure ammonia was 12°C higher than for unexposed montmorillonite particles at 90% RHw and 10°C higher at 100% RHw. In the 25 ppm ammonia exposed montmorillonite experiments, the activation temperature was 7°C warmer than unexposed montmorillonite at 100% RHw. Degassing does not reverse the ice nucleating ability of ammonia exposed montmorillonite mineral dust particles. This is the first experimental evidence that ammonia gas exposed montmorillonite mineral dust particles can enhance its activation as ice nuclei and that the activation can occur at temperatures warmer than –10°C where natural atmospheric ice nuclei are very scarce.
Elemental and organic carbon in PM10: a one year measurement campaign within the European Monitoring and Evaluation Programme EMEP
Authors: Yttri K. E. , Aas W. , Bjerke A. , Ceburnis D. , Dye C. , Emblico L. , Facchini M. C. , Forster C. , Hanssen J. E. , Hansson H. C. , Jennings S. G. , Maenhaut W. , Putaud J. P. , Tørseth K.
Published: April 2010

Abstract. In the present study, ambient aerosol (PM10) concentrations of elemental carbon (EC), organic carbon (OC), and total carbon (TC) are reported for 12 European rural background sites and two urban background sites following a one-year (1 July 2002–1 July 2003) sampling campaign within the European Monitoring and Evaluation Programme, EMEP (http://www.emep.int/). The purpose of the campaign was to assess the feasibility of performing EC and OC monitoring on a regular basis and to obtain an overview of the spatial and seasonal variability on a regional scale in Europe. Analyses were performed using the thermal-optical transmission (TOT) instrument from Sunset Lab Inc., operating according to a NIOSH derived temperature program. The annual mean mass concentration of EC ranged from 0.17±0.19 μg m−3 (mean ± SD) at Birkenes (Norway) to 1.83±1.32 μg m−3 at Ispra (Italy). The corresponding range for OC was 1.20±1.29 μg m−3 at Mace Head (Ireland) to 7.79±6.80 μg m−3 at Ispra. On average, annual concentrations of EC, OC, and TC were three times higher for rural background sites in Central, Eastern and Southern Europe compared to those situated in the Northern and Western parts of Europe. Wintertime concentrations of EC and OC were higher than those recorded during summer for the majority of the sites. Moderate to high Pearson correlation coefficients (rp) (0.50–0.94) were observed for EC versus OC for the sites investigated. The lowest correlation coefficients were noted for the three Scandinavian sites: Aspvreten (SE), Birkenes (NO), and Virolahti (FI), and the Slovakian site Stara Lesna, and are suggested to reflect biogenic sources, wild and prescribed fires. This suggestion is supported by the fact that higher concentrations of OC are observed for summer compared to winter for these sites. For the rural background sites, total carbonaceous material accounted for 30±9% of PM10, of which 27±9% could be attributed to organic matter (OM) and 3.4±1.0% to elemental matter (EM). OM was found to be more abundant than SO42− for sites reporting both parameters.
Bias determination and precision validation of ozone profiles from MIPAS-Envisat retrieved with the IMK-IAA processor
Authors: Steck T. , von Clarmann T. , Fischer H. , Funke B. , Glatthor N. , Grabowski U. , Höpfner M. , Kellmann S. , Kiefer M. , Linden A. , Milz M. , Stiller G. P. , Wang D. Y. , Allaart M. , Blumenstock Th. , van der Gathen P. , Hansen G. , Hase F. , Hochschild G. , Kopp G. , Kyrö E. , Oelhaf H. , Raffalski U. , Redondas Marrero A. , Remsberg E. , Russell J. , Stebel K. , Steinbrecht W. , Wetzel G. , Yela M. , Zhang G.
Published: April 2010

Abstract. This paper characterizes vertical ozone profiles retrieved with the IMK-IAA (Institute for Meteorology and Climate Research, Karlsruhe – Instituto de Astrofisica de Andalucia) science-oriented processor from spectra measured by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) aboard the environmental satellite Envisat. Bias determination and precision validation is performed on the basis of correlative measurements by ground-based lidars, Fourier transform infrared spectrometers, and microwave radiometers as well as balloon-borne ozonesondes, the balloon-borne version of MIPAS, and two satellite instruments (Halogen Occultation Experiment and Polar Ozone and Aerosol Measurement III). Percentage mean differences between MIPAS and the comparison instruments for stratospheric ozone are within ±10%. The precision in this altitude region is estimated at values between 5 and 10% which gives an accuracy of 15 to 20%. Below 18 km, the spread of the percentage mean differences is larger and the precision increases to values of more than 20% depending on altitude and latitude. The main reason for the degraded precision at low altitudes is attributed to undetected thin clouds which affect MIPAS retrievals, and to the influence of uncertainties in the water vapor concentration.
Long range transport and fate of a stratospheric volcanic cloud from Soufriere Hills volcano, Montserrat
Authors: Prata A. J. , Carn S. A. , Stohl A. , Kerkmann J.
Published: April 2010

Abstract. Volcanic eruptions emit gases, ash particles and hydrometeors into the atmosphere, occasionally reaching great heights to reside in the stratospheric overworld where they affect the radiative balance of the atmosphere and the earth's climate. Here we use satellite measurements and a Lagrangian particle dispersion model to determine the mass loadings, vertical penetration, horizontal extent, dispersion and transport of volcanic gases and particles in the stratosphere from the volcanic cloud emitted during the 20 May 2006 eruption of Soufriere Hills volcano, Montserrat, West Indies. Infrared, ultraviolet and microwave radiation measurements from two polar orbiters are used to quantify the gases and particles, and track the movement of the cloud for 23 days, over a distance of ~18 000 km. Approximately, 0.1±0.01 Tg(S) was injected into the stratosphere in the form of SO2: the largest single sulfur input to the stratosphere in 2006. Microwave Limb Sounder measurements indicate an enhanced mass of HCl of ~0.003–0.01 Tg. Geosynchronous satellite data reveal the rapid nature of the stratospheric injection and indicate that the eruption cloud contained ~2 Tg of ice, with very little ash reaching the stratosphere. These new satellite measurements of volcanic gases and particles can be used to test the sensitivity of climate to volcanic forcing and assess the impact of stratospheric sulfates on climate cooling.
Chemistry, transport and dry deposition of trace gases in the boundary layer over the tropical Atlantic Ocean and the Guyanas during the GABRIEL field campaign
Authors: Stickler A. , Fischer H. , Bozem H. , Gurk C. , Schiller C. , Martinez-Harder M. , Kubistin D. , Harder H. , Williams J. , Eerdekens G. , Yassaa N. , Ganzeveld L. , Sander R. , Lelieveld J.
Published: April 2010

Abstract. We present a comparison of different Lagrangian and steady state box model runs with measurement data obtained during the GABRIEL campaign over the tropical Atlantic Ocean and the rainforest in the Guyanas, October 2005. Lagrangian modelling of boundary layer (BL) CO constrained by measurements of reactive trace gases and radiation is used to derive a horizontal gradient (≈5.6 pmol/mol km−1) of this compound from the ocean to the rainforest (east to west). This is significantly smaller than that derived from the measurements (16–48 pmol/mol km−1), indicating that photochemical production from organic precursors alone cannot explain the observed strong gradient. It appears that HCHO is overestimated by the Lagrangian and "steady state" models, which include dry deposition but not exchange with the free troposphere (FT). The relatively short lifetime of HCHO (50–100 min) implies substantial BL-FT exchange. The mixing-in of FT air affected by African and South American biomass burning at an estimated rate of 0.12 h−1 increases the CO and lowers the HCHO mixing ratios, leading to a better agreement with measurements. A 24 h mean deposition velocity of 1.35 cm/s for H2O2 over the ocean as well as over the rainforest is deduced assuming BL-FT exchange adequate to the results for CO. The measured increase of the organic peroxides from the ocean to the rainforest (≈0.66 nmol/mol d−1) is significantly overestimated by the Lagrangian model, even when using high values for the deposition velocity and the entrainment rate. Our results point at either heterogeneous loss of organic peroxides and/or their radical precursors or a missing reaction path of peroxy radicals not forming peroxides in isoprene chemistry. We calculate a mean integrated daytime net ozone production (NOP) in the BL of (0.2±5.9) nmol/mol (ocean) and (2.4±2.1) nmol/mol (rainforest). The NOP strongly correlates with NO and shows a positive tendency in the boundary layer over the rainforest.
Physical controls on orographic cirrus inhomogeneity
Authors: Kay J. E. , Baker M. , Hegg D.
Published: April 2010

Abstract. Optical depth distributions (P(σ)) are a useful measure of radiatively important cirrus (Ci) inhomogeneity. Using a parcel model with binned ice microphysics and kinematic trajectories from a mesoscale weather model (MM5), we assess physical controls on Ci P(σ) during an orographic Ci case study. On 19 April 2001, satellite imagery revealed Ci formation in the lee of the Southern Rocky Mountains and Ci advection along a broad upper level ridge. Above Lamont, Oklahoma (USA), lidar observations indicated a broad Ci P(σ). Along MM5 trajectories associated with the observed Ci, homogeneous freezing and mesoscale variability in vertical velocities led to broad modeled P(σ) and variability in modeled Ci cloud lifetimes. The addition of background ice nuclei concentrations (NIN=0.03 cm−3) to air parcels had little impact on modeled Ci σ variability. The presence of background NIN did increase cloud cover by increasing the frequency of small σ Ci. These results highlight the importance of homogeneous freezing and mesoscale vertical velocity variability in controlling Ci P(σ) shapes along realistic upper tropospheric trajectories.
Simulation of solar radiation during a total solar eclipse: a challenge for radiative transfer
Authors: Emde C. , Mayer B.
Published: April 2010

Abstract. A solar eclipse is a rare but spectacular natural phenomenon and furthermore it is a challenge for radiative transfer modeling. Whereas a simple one-dimensional radiative transfer model with reduced solar irradiance at the top of the atmosphere can be used to calculate the brightness during partial eclipses a much more sophisticated model is required to calculate the brightness (i.e. the diffuse radiation) during the total eclipse. The reason is that radiation reaching a detector in the shadow gets there exclusively by horizontal (three-dimensional) transport of photons in a spherical shell atmosphere. In this study the first accurate simulations are presented examplified by the solar eclipse at 29 March 2006. Using a backward Monte Carlo model we calculated the diffuse radiation in the umbra and simulated the changing colors of the sky. Radiance and irradiance are decreased by 3 to 4 orders of magnitude, depending on wavelength. We found that aerosol has a comparatively small impact on the radiation in the umbra. We also estimated the contribution of the solar corona to the radiation under the umbra and found that it is negligible compared to the diffuse solar radiation in most parts of the spectrum. Spectrally resolved measurements in the umbra are not yet available. They are challenging due to the low intensity and therefore need careful planning. The new model may be used to support measurements during future solar eclipses.
Twenty-five years of continuous sulphur dioxide emission reduction in Europe
Authors: Vestreng V. , Myhre G. , Fagerli H. , Reis S. , Tarrasón L.
Published: April 2010

Abstract. During the last twenty-five years European emission data have been compiled and reported under the Cooperative Programme for Monitoring and Evaluation of the Long-range Transmission of Air Pollutants in Europe (EMEP) as part of the work under the UNECE Convention on Long-range Transboundary Air Pollution (LRTAP). This paper presents emission trends of SO2 reported to EMEP and validated within the programme for the period 1980–2004. These European anthropogenic sulphur emissions have been steadily decreasing over the last twenty-five years, amounting from about 55 Tg SO2 in 1980 to 15 Tg SO2 in 2004. The uncertainty in sulphur emission estimates for individual countries and years are documented to range between 3% and 25%. The relative contribution of European emissions to global anthropogenic sulphur emissions has been halved during this period. Based on annual emission reports from European countries, three emission reduction regimes have been identified. The period 1980–1989 is characterized by low annual emission reductions (below 5% reduction per year and 20% for the whole period) and is dominated by emission reductions in Western Europe. The period 1990–1999 is characterised by high annual emission reductions (up to 11% reduction per year and 54% for the whole period), most pronounced in Central and Eastern Europe. The annual emission reductions in the period 2000–2004 are medium to low and reflect the unified Europe, with equally large reductions in both East and West. The sulphur emission reduction has been largest in the sector Combustion in energy and transformation industries, but substantial decreases are also seen in the Non-industrial combustion plants together with the sectors Industrial Combustion and Industrial Production Processes. The majority of European countries have reduced their emissions by more than 60% between 1990 and 2004, and one quarter have already achieved sulphur emission reductions higher than 80%. At European level, the total sulphur target for 2010 set in the Gothenburg Protocol (16 Tg) has apparently already been met by 2004. However, still half of the Parties to the Gothenburg Protocol have to reduce further their sulphur emissions in order to attain their individual country total emission targets for 2010. It is also noteworthy that, contrasting the Gothenburg Protocol requirements, a growing number of countries have recently been reporting increasing sulphur emissions, while others report only minor further decreases. The emission trends presented here are supported by different studies of air concentrations and depositions carried out within and outside the framework of the LRTAP Convention.
A fate for organic acids, formaldehyde and methanol in cloud water: their biotransformation by micro-organisms
Authors: Amato P. , Demeer F. , Melaouhi A. , Fontanella S. , Martin-Biesse A.-S. , Sancelme M. , Laj P. , Delort A.-M.
Published: April 2010

Abstract. The interactions between microbial and chemical contents of cloud water were investigated. First, we observe that the bulk cloud water solution provides a substantial environment where bacteria can develop significantly. Then, a total number of 60 microbial strains originating from seven distinct samples of cloud water and affiliated to various taxonomic groups were looked for their ability to degrade some of the main atmospheric carboxylic compounds: formate, acetate, lactate, succinate, formaldehyde and methanol. Biodegradation tests show that all these compounds can be transformed when used as single carbonaceous substrates, with activities depending on both the strain and the compound. The highest capacities of biodegradation are observed towards formaldehyde, formate and acetate, which are also the more concentrated compounds typically measured in cloud water. Hence, analyses by 1H NMR permitted to establish for instance that compounds like pyruvate or fumarate can be produced and released in the media in relation to the transformation of lactate or succinate. In addition, utilization of 13C labelled formaldehyde showed that it can be transformed through many metabolic pathways, similar to those induced by photochemistry and leading to the production of formate and/or methanol. These results suggest that microorganisms of cloud water can have various behaviours towards the chemical compounds present in the atmosphere: they can represent either a sink or source for organic carbon, and may have to be considered as actors of cloud chemistry.
Nine years of UV aerosol optical depth measurements at Thessaloniki, Greece
Authors: Kazadzis S. , Bais A. , Amiridis V. , Balis D. , Meleti C. , Kouremeti N. , Zerefos C. S. , Rapsomanikis S. , Petrakakis M. , Kelesis A. , Tzoumaka P. , Kelektsoglou K.
Published: April 2010

Abstract. Spectral measurements of the aerosol optical depth (AOD) and the Angstrom coefficient were conducted at Thessaloniki, Greece (40.5° N, 22.9° E) between January 1997 and December 2005 with a Brewer MKIII double-monochromator spectroradiometer. The dataset was compared with collocated measurements of a second spectroradiometer (Brewer MKII) and a CIMEL sun-photometer, showing correlations of 0.93 and 0.98 respectively. A seasonal variation of the AOD was observed at Thessaloniki, with AOD values at 340 nm of 0.52 and 0.28 for August and December respectively. Back trajectories of air masses for up to 4 days were used to assess the influence of long-range transport from various regions to the aerosol load over Thessaloniki. It is shown that part of the observed seasonality can be attributed to air masses with high AOD originating from North-Eastern and Eastern directions during summertime. The analysis of the long-term record (9 years) of AOD showed a downward tendency. A similar decreasing tendency was found in the record of the PM-10 aerosol measurements, which are conducted near the surface at 4 air-quality monitoring stations in the area of the city of Thessaloniki.