bluuebunny/crossref_metadata_2025 huggingface dataset:
Remote sensing of cloud sides of deep convection: towards a three-dimensional retrieval of cloud particle size profiles
Authors: Zinner T. , Marshak A. , Lang S. , Martins J. V. , Mayer B.
Published: April 2010

Abstract. The cloud scanner sensor is a central part of a recently proposed satellite remote sensing concept – the three-dimensional (3-D) cloud and aerosol interaction mission (CLAIM-3D) combining measurements of aerosol characteristics in the vicinity of clouds and profiles of cloud microphysical characteristics. Such a set of collocated measurements will allow new insights in the complex field of cloud-aerosol interactions affecting directly the development of clouds and precipitation, especially in convection. The cloud scanner measures radiance reflected or emitted by cloud sides at several wavelengths to derive a profile of cloud particle size and thermodynamic phase. For the retrieval of effective size a Bayesian approach was adopted and introduced in a preceding paper. In this paper the potential of the approach, which has to account for the complex three-dimensional nature of cloud geometry and radiative transfer, is tested in realistic cloud observing situations. In a fully simulated environment realistic cloud resolving modelling provides complex 3-D structures of ice, water, and mixed phase clouds, from the early stage of convective development to mature deep convection. A three-dimensional Monte Carlo radiative transfer is used to realistically simulate the aspired observations. A large number of cloud data sets and related simulated observations provide the database for an experimental Bayesian retrieval. An independent simulation of an additional cloud field serves as a synthetic test bed for the demonstration of the capabilities of the developed retrieval techniques. For this test case only a minimal overall bias in the order of 1% as well as pixel-based uncertainties in the order of 1 μm for droplets and 8 μm for ice particles were found for measurements at a high spatial resolution of 250 m.
Basic characteristics of atmospheric particles, trace gases and meteorology in a relatively clean Southern African Savannah environment
Authors: Laakso L. , Laakso H. , Aalto P. P. , Keronen P. , Petäjä T. , Nieminen T. , Pohja T. , Siivola E. , Kulmala M. , Kgabi N. , Molefe M. , Mabaso D. , Phalatse D. , Pienaar K. , Kerminen V.-M.
Published: April 2010

Abstract. We have analyzed one year (July 2006–July 2007) of measurement data from a relatively clean background site located in dry savannah in South Africa. The annual-median trace gas concentrations were equal to 0.7 ppb for SO2, 1.4 ppb for NOx, 36 ppb for O3 and 105 ppb for CO. The corresponding PM1, PM2.5 and PM10 concentrations were 9.0, 10.5 and 18.8 μg m−3, and the annual median total particle number concentration in the size range 10–840 nm was 2340 cm−3. During Easterly winds, influence of industrial sources approximately 150 km away from the measurement site was clearly visible, especially in SO2 and NOx concentrations. Of gases, NOx and CO had a clear annual, and SO2, NOx and O3 clear diurnal cycle. Atmospheric new-particle formation was observed to take place in more than 90% of the analyzed days. The days with no new particle formation were cloudy or rainy days. The formation rate of 10 nm particles varied in the range of 0.1–28 cm−3 s−1 (median 1.9 cm−3 s−1) and nucleation mode particle growth rates were in the range 3–21 nm h−1 (median 8.5 nm h−1). Due to high formation and growth rates, observed new particle formation gives a significant contribute to the number of cloud condensation nuclei budget, having a potential to affect the regional climate forcing patterns.
Multiphase modeling of nitrate photochemistry in the quasi-liquid layer (QLL): implications for NOx release from the Arctic and coastal Antarctic snowpack
Authors: Boxe C. S. , Saiz-Lopez A.
Published: April 2010

Abstract. We utilize a multiphase model, CON-AIR (Condensed Phase to Air Transfer Model), to show that the photochemistry of nitrate (NO3−) in and on ice and snow surfaces, specifically the quasi-liquid layer (QLL), can account for NOx volume fluxes, concentrations, and [NO]/[NO2] (γ=[NO]/[NO2]) measured just above the Arctic and coastal Antarctic snowpack. Maximum gas phase NOx volume fluxes, concentrations and γ simulated for spring and summer range from 5.0×104 to 6.4×105 molecules cm−3 s−1, 5.7×108 to 4.8×109 molecules cm−3, and ~0.8 to 2.2, respectively, which are comparable to gas phase NOx volume fluxes, concentrations and γ measured in the field. The model incorporates the appropriate actinic solar spectrum, thereby properly weighting the different rates of photolysis of NO3− and NO2−. This is important since the immediate precursor for NO, for example, NO2−, absorbs at wavelengths longer than nitrate itself. Finally, one-dimensional model simulations indicate that both gas phase boundary layer NO and NO2 exhibit a negative concentration gradient as a function of height although [NO]/[NO2] are approximately constant. This gradient is primarily attributed to gas phase reactions of NOx with halogens oxides (i.e. as BrO and IO), HOx, and hydrocarbons, such as CH3O2.
The influence of natural and anthropogenic secondary sources on the glyoxal global distribution
Authors: Myriokefalitakis S. , Vrekoussis M. , Tsigaridis K. , Wittrock F. , Richter A. , Brühl C. , Volkamer R. , Burrows J. P. , Kanakidou M.
Published: April 2010

Abstract. Glyoxal, the smallest dicarbonyl, which has recently been observed from space, is expected to provide indications on volatile organic compounds (VOC) oxidation and secondary aerosol formation in the troposphere. Glyoxal (CHOCHO) is known to be mostly of natural origin and is produced during biogenic VOC oxidation. However, a number of anthropogenically emitted hydrocarbons, like acetylene and aromatics, have been positively identified as CHOCHO precursors. The present study investigates the contribution of pollution to the CHOCHO levels by taking into account the secondary chemical formation of CHOCHO from precursors emitted from biogenic, anthropogenic and biomass burning sources. The impact of potential primary land emissions of CHOCHO is also investigated. A global 3-dimensional chemistry transport model of the troposphere (TM4-ECPL) able to simulate the gas phase chemistry coupled with all major aerosol components is used. The secondary anthropogenic contribution from fossil fuel and industrial VOCs emissions oxidation to the CHOCHO columns is found to reach 20–70% in the industrialized areas of the Northern Hemisphere and 3–20% in the tropics. This secondary CHOCHO source is on average three times larger than that from oxidation of VOCs from biomass burning sources. The chemical production of CHOCHO is calculated to equal to about 56 Tg y−1 with 70% being produced from biogenic hydrocarbons oxidation, 17% from acetylene, 11% from aromatic chemistry and 2% from ethene and propene. CHOCHO is destroyed in the troposphere primarily by reaction with OH radicals (23%) and by photolysis (63%), but it is also removed from the atmosphere through wet (8%) and dry deposition (6%). Potential formation of secondary organic aerosol through CHOCHO losses on/in aerosols and clouds is neglected here due to the significant uncertainties associated with the underlying chemistry. The global annual mean CHOCHO burden and lifetime in the model domain are estimated to be 0.02 Tg (equal to the global burden seen by SCIAMACHY over land for the year 2005) and about 3 h, respectively. The model results are compared with satellite observations of CHOCHO columns. When accounting only for the secondary sources of CHOCHO in the model, the model underestimates CHOCHO columns observed by satellites. This is attributed to an overestimate of CHOCHO sinks or a missing global source of about 20 Tg y−1. Using the current primary emissions of CHOCHO from biomass burning together with the anthropogenic combustion sources of about 7 Tg y−1 leads to an overestimate by the model over hot spot areas.
Airborne dust distributions over the Tibetan Plateau and surrounding areas derived from the first year of CALIPSO lidar observations
Authors: Liu Z. , Liu D. , Huang J. , Vaughan M. , Uno I. , Sugimoto N. , Kittaka C. , Trepte C. , Wang Z. , Hostetler C. , Winker D.
Published: April 2010

Abstract. Using an analysis of the first full year of CALIPSO lidar measurements, this paper derives unprecedented, altitude-resolved seasonal distributions of desert dust transported over the Tibetan Plateau (TP) and the surrounding areas. The CALIPSO lidar observations include numerous large dust plumes over the northern slope and eastern part of the TP, with the largest number of dust events occurring in the spring of 2007, and some layers being lofted to altitudes of 11–12 km. Generation of the Tibetan airborne dusts appears to be largely associated with source regions to the north and on the eastern part of the plateau. Examination of the CALIPSO time history reveals an "airborne dust corridor" due to the eastward transport of dusts originating primarily in these source areas. This corridor extends from west to east and shows a seasonality largely modulated by the TP through its dynamical and thermal forcing on the atmospheric flows. On the southern side, desert dust particles originate predominately in Northwest India and Pakistan. The dust transport occurs primarily in dry seasons around the TP western and southern slopes and dust particles become mixed with local polluted aerosols. No significant amount of dust appears to be transported over the Himalayas. Extensive forward trajectory simulations are also conducted to confirm the dust transport pattern from the nearby sources observed by the CALIPSO lidar. Comparisons with the OMI and MODIS measurements show the unique capability of the CALIPSO lidar to provide unambiguous, altitude-resolved dust measurements.
The high Arctic in extreme winters: vortex, temperature, and MLS and ACE-FTS trace gas evolution
Authors: Manney G. L. , Daffer W. H. , Strawbridge K. B. , Walker K. A. , Boone C. D. , Bernath P. F. , Kerzenmacher T. , Schwartz M. J. , Strong K. , Sica R. J. , Krüger K. , Pumphrey H. C. , Lambert A. , Santee M. L. , Livesey N. J. , Remsberg E. E. , Mlynczak M. G. , Russell III J. R.
Published: April 2010

Abstract. The first three Arctic winters of the ACE mission represented two extremes of winter variability: Stratospheric sudden warmings (SSWs) in 2004 and 2006 were among the strongest, most prolonged on record; 2005 was a record cold winter. Canadian Arctic Atmospheric Chemistry Experiment (ACE) Validation Campaigns were conducted at Eureka (80° N, 86° W) during each of these winters. New satellite measurements from ACE-Fourier Transform Spectrometer (ACE-FTS), Sounding of the Atmosphere using Broadband Emission Radiometry (SABER), and Aura Microwave Limb Sounder (MLS), along with meteorological analyses and Eureka lidar temperatures, are used to detail the meteorology in these winters, to demonstrate its influence on transport, and to provide a context for interpretation of ACE-FTS and validation campaign observations. During the 2004 and 2006 SSWs, the vortex broke down throughout the stratosphere, reformed quickly in the upper stratosphere, and remained weak in the middle and lower stratosphere. The stratopause reformed at very high altitude, near 75 km. ACE measurements covered both vortex and extra-vortex conditions in each winter, except in late-February through mid-March 2004 and 2006, when the strong, pole-centered vortex that reformed after the SSWs resulted in ACE sampling only inside the vortex in the middle through upper stratosphere. The 2004 and 2006 Eureka campaigns were during the recovery from the SSWs, with the redeveloping vortex over Eureka. 2005 was the coldest winter on record in the lower stratosphere, but with an early final warming in mid-March. The vortex was over Eureka at the start of the 2005 campaign, but moved away as it broke up. Disparate temperature profile structure and vortex evolution resulted in much lower (higher) temperatures in the upper (lower) stratosphere in 2004 and 2006 than in 2005. Satellite temperatures agree well with lidar data up to 50–60 km, and ACE-FTS, MLS and SABER show good agreement in high-latitude temperatures throughout the winters. Consistent with a strong, cold upper stratospheric vortex and enhanced radiative cooling after the SSWs, MLS and ACE-FTS trace gas measurements show strongly enhanced descent in the upper stratospheric vortex in late January through March 2006 compared to that in 2005.
First atmospheric observations of three chlorofluorocarbons
Authors: Laube J. C. , Engel A.
Published: April 2010

Abstract. We report the first atmospheric observations of the Chlorofluorocarbons (CFCs) trifluorochloroethene, 3-chloropentafluoropropene and 4,4-dichlorohexafluoro-1-butene by means of Gas Chromatography with Electron Capture and Mass Spectrometric detection (GC-ECD-MS) in air samples taken at the Taunus Observatory operated by the University of Frankfurt (Main) and the Jungfraujoch High Altitude Research Station in Switzerland. These substances belong to a class of CFCs containing a double bond and are suspected to originate from the production and thermal degradation of widely used fluoropolymers like polychlorotrifluoroethene (PCTFE). Their atmospheric lifetimes are expected to be rather short. A quantitative calibration could only be derived for trifluorochloroethene but not for the other species by now. Thus, we use a relative sensitivity method to get a first indication of the observed atmospheric abundances. Identification was possible because of an air plume containing high concentrations of these substances. We suggest that the abundances found on this occasion originated from a local source. However, we have also observed the novel CFCs in air masses representative of background conditions, though with much lower concentrations. These species and some of their degradation products are toxic and could also be relevant for stratospheric and tropospheric ozone depletion.
The effect of lightning NOx production on surface ozone in the continental United States
Authors: Kaynak B. , Hu Y. , Martin R. V. , Russell A. G. , Choi Y. , Wang Y.
Published: April 2010

Abstract. Lightning NOx emissions calculated using the US National Lightning Detection Network data were found to account for 30% of the total NOx emissions for July–August 2004, a period chosen both for having higher lightning NOx production and high ozone levels, thus maximizing the likelihood that such emissions could impact peak ozone levels. Including such emissions led to modest, but sometimes significant increases in simulated surface ozone when using the Community Multi-scale Air Quality Model (CMAQ). Three model simulations were performed, two with the addition of lightning NOx emissions, and one without. Domain-wide daily maximum 8-h ozone changes due to lightning NOx were less than 2 ppbv in 71% of the cases with a maximum of 10 ppbv; whereas the difference in 1-h ozone was less than 2 ppbv in 77% of the cases with a maximum of 6 ppbv. Daily maximum 1-h and 8-h ozone for grids containing O3 monitoring stations changed slightly, with more than 43% of the cases differing less than 2 ppbv. The greatest differences were 42 ppbv for both 1-h and 8-h O3, though these tended to be on days of lower ozone. Lightning impacts on the season-wide maximum 1-h and 8-h averaged ozone decreased starting from the 1st to 4th highest values (an average of 4th highest, 8-h values is used for attainment demonstration in the US). Background ozone values from the y-intercept of O3 versus NOz curve were 42.2 and 43.9 ppbv for simulations without and with lightning emissions, respectively. Results from both simulations with lightning NOx suggest that while North American lightning production of NOx can lead to significant local impacts on a few occasions, they will have a relatively small impact on typical maximum levels and determination of Policy Relevant Background levels.
The total solar eclipse of March 2006: overview
Authors: Gerasopoulos E. , Zerefos C. S. , Tsagouri I. , Founda D. , Amiridis V. , Bais A. F. , Belehaki A. , Christou N. , Economou G. , Kanakidou M. , Karamanos A. , Petrakis M. , Zanis P.
Published: April 2010

Abstract. This paper provides the overview of an integrated, multi-disciplinary effort to study the effects of the 29 March 2006 total solar eclipse on the environment, with special focus on the atmosphere. The eclipse has been visible over the Eastern Mediterranean, and on this occasion several research and academic institutes organised co-ordinated experimental campaigns, at different distances from eclipse totality and at various environments in terms of air quality. Detailed results and findings are presented in a number of component scientific papers included in a Special Issue of Atmospheric Chemistry and Physics. The effects of the eclipse on meteorological parameters, though very clear, were shown to be controlled by local factors rather than the eclipse magnitudes, and the turbulence activity near surface was suppressed causing a decrease in the Planetary Boundary Layer. In addition to the above, the decrease in solar radiation has caused change to the photochemistry of the atmosphere, with night time chemistry dominating. The abrupt "switch off" of the sun, induced changes also in the ionosphere (140 up to 220 km) and the stratosphere. In the ionosphere, both photochemistry and dynamics resulted to changes in the reflection heights and the electron concentrations. Among the most important scientific findings from the experiments undertaken has been the experimental proof of eclipse induced thermal fluctuations in the ozone layer (Gravity Waves), due to the supersonic movement of the moon's shadow, for the first time with simultaneous measurements at three altitudes namely the troposphere, the stratosphere and the ionosphere. Within the challenging topics of the experiments has been the investigation of eclipse impacts on ecosystems (field crops and marine plankton). The rare event of a total solar eclipse provided the opportunity to evaluate 1 dimensional (1-D) and three dimensional (3-D) radiative transfer (in the atmosphere and underwater), mesoscale meteorological, regional air quality and photochemical box models, against measurements.
Model simulations of stratospheric ozone loss caused by enhanced mesospheric NOx during Arctic Winter 2003/2004
Authors: Vogel B. , Konopka P. , Grooß J.-U. , Müller R. , Funke B. , López-Puertas M. , Reddmann T. , Stiller G. , von Clarmann T. , Riese M.
Published: April 2010

Abstract. Satellite observations show that the enormous solar proton events (SPEs) in October–November 2003 had significant effects on the composition of the stratosphere and mesosphere in the polar regions. After the October–November 2003 SPEs and in early 2004, significant enhancements of NOx(=NO+NO2) in the upper stratosphere and lower mesosphere in the Northern Hemisphere were observed by several satellite instruments. Here we present global full chemistry calculations performed with the CLaMS model to study the impact of mesospheric NOx intrusions on Arctic polar ozone loss processes in the stratosphere. Several model simulations are preformed with different upper boundary conditions for NOx at 2000 K potential temperature (≈50 km altitude). In our study we focus on the impact of the non-local production of NOx, which means the downward transport of enhanced NOx from the mesosphere to the stratosphere. The local production of NOx in the stratosphere is neglected. Our findings show that intrusions of mesospheric air into the stratosphere, transporting high burdens of NOx, affect the composition of the Arctic polar region down to about 400 K (≈17–18 km). We compare our simulated NOx and O3 mixing ratios with satellite observations by ACE-FTS and MIPAS processed at IMK/IAA and derive an upper limit for the ozone loss caused by enhanced mesospheric NOx. Our findings show that in the Arctic polar vortex (equivalent lat.>70° N) the accumulated column ozone loss between 350–2000 K potential temperature (≈14–50 km altitude) caused by the SPEs in October–November 2003 in the stratosphere is up to 3.3 DU with an upper limit of 5.5 DU until end of November. Further, we found that about 10 DU, but in any case lower than 18 DU, accumulated ozone loss additionally occurred until end of March 2004 caused by the transport of mesospheric NOx-rich air in early 2004. The solar-proton-produced NOx above 55 km due to the SPEs of October–November 2003 had a negligibly small impact on ozone loss processes through the end of November in the lower stratosphere (350–700 K≈14–27 km). The mesospheric NOx intrusions in early 2004 yielded a lower stratospheric ozone loss of about 3.5 DU, and clearly lower than 6.5 DU through the end of March. Overall, the non-local production of NOx is an additional variability in the existing variations of the ozone loss observed in the Arctic.
Heterogeneous OH oxidation of palmitic acid in single component and internally mixed aerosol particles: vaporization and the role of particle phase
Authors: McNeill V. F. , Yatavelli R. L. N. , Thornton J.  A. , Stipe C. B. , Landgrebe O.
Published: April 2010

Abstract. We studied the OH oxidation of submicron aerosol particles consisting of pure palmitic acid (PA) or thin (near monolayer) coatings of PA on aqueous and effloresced inorganic salt particles. Experiments were performed as a function of particle size and OH exposure using a continuous-flow photochemical reaction chamber coupled to a chemical ionization mass spectrometer (CIMS) system, for detection of gas and particle-bound organics, and a DMA/CPC for monitoring particle size distributions. The loss rate of PA observed for pure PA aerosols and PA on crystalline NaCl aerosols indicates that the OH oxidation of PA at the gas-aerosol interface is efficient. The pure PA oxidation data are well represented by a model consisting of four main processes: 1) surface-only reactions between OH and palmitic acid, 2) secondary reactions between palmitic acid and OH oxidation products, 3) volatilization of condensed-phase mass, and 4) a surface renewal process. Using this model we infer a value of γOH between 0.8 and 1. The oxidation of palmitic acid in thin film coatings of salt particles is also efficient, though the inferred γOH is lower, ranging from ~0.3+0.1/−0.05) for coatings on solid NaCl and ~0.05 (±0.01) on aqueous NaCl particles. These results, together with simultaneous data on particle size change and volatilized oxidation products, provide support for the ideas that oxidative aging of aliphatic organic aerosol is a source of small oxidized volatile organic compounds (OVOCs), and that OH oxidation may initiate secondary condensed-phase reactions.
Measurements of UV irradiance within the area of one satellite pixel
Authors: Weihs P. , Blumthaler M. , Rieder H. E. , Kreuter A. , Simic S. , Laube W. , Schmalwieser A. W. , Wagner J. E. , Tanskanen A.
Published: April 2010

Abstract. A measurement campaign was performed in the region of Vienna and its surroundings from May to July 2007. Within the scope of this campaign erythemal UV was measured at six ground stations within a radius of 30 km. First, the homogeneity of the UV levels within the area of one satellite pixel was studied. Second, the ground UV was compared to ground UV retrieved by the ozone monitoring instrument (OMI) onboard the NASA EOS Aura Spacecraft. During clear-sky conditions the mean bias between erythemal UV measured by the different stations was within the measurement uncertainty of ±5%. Short term fluctuations of UV between the stations were below 3% within a radius of 20 km. For partly cloudy conditions and overcast conditions the discrepancy of instantaneous values between the stations is up to 200% or even higher. If averages of the UV index over longer time periods are compared the difference between the stations decreases strongly. The agreement is better than 20% within a distance of 10 km between the stations for 3 h averages. The comparison with OMI UV showed for clear-sky conditions higher satellite retrieved UV values by, on the average, approximately 15%. The ratio of OMI to ground measured UV lies between 0.9 and 1.5. and strongly depends on the aerosol optical depth. For partly cloudy and overcast conditions the OMI derived surface UV estimates show larger deviation from the ground-based reference data, and even bigger systematic positive bias. Here the ratio OMI to ground data lies between 0.5 and 4.5. The average difference between OMI and ground measurements is +24 to +37% for partly cloudy conditions and more than +50% for overcast conditions.
Size distributions, sources and source areas of water-soluble organic carbon in urban background air
Authors: Timonen H. , Saarikoski S. , Tolonen-Kivimäki O. , Aurela M. , Saarnio K. , Petäjä T. , Aalto P. P. , Kulmala M. , Pakkanen T. , Hillamo R.
Published: April 2010

Abstract. This paper represents the results of one year long measurement period of the size distributions of water-soluble organic carbon (WSOC), inorganic ions and gravimetric mass of particulate matter. Measurements were done at an urban background station (SMEAR III) by using a micro-orifice uniform deposit impactor (MOUDI). The site is located in northern European boreal region in Helsinki, Finland. The WSOC size distribution measurements were completed with the chemical analysis of inorganic ions, organic carbon (OC) and monosaccharide anhydrides from the filter samples (particle aerodynamic diameter smaller than 1 μm, PM1). Gravimetric mass concentration varied during the MOUDI samplings between 3.4 and 55.0 μg m−3 and the WSOC concentrations were between 0.3 and 7.4 μg m−3. On average, water-soluble particulate organic matter (WSPOM, WSOC multiplied by 1.6 to convert the analyzed carbon mass to organic matter mass) comprised 25±7.7% and 7.5±3.4% of aerosol PM1 mass and the PM1–10 mass, respectively. Inorganic ions contributed 33±12% and 28±19% of the analyzed PM1 and PM1–10 aerosol mass. Five different aerosol categories corresponding to different sources or source areas were identified (long-range transport aerosols, biomass burning aerosols from wild land fires and from small-scale wood combustion, aerosols originating from marine areas and from the clean arctic areas). Categories were identified mainly using levoglucosan concentration level for wood combustion and air mass backward trajectories for other groups. Clear differences in WSOC concentrations and size distributions originating from different sources or source areas were observed, although there are also many other factors which might affect the results. E.g. the local conditions and sources of volatile organic compounds (VOCs) and aerosols as well as various transformation processes are likely to have an impact on the measured aerosol composition. Using the source categories, it was identified that especially the oxidation products of biogenic VOCs in summer had a clear effect on WSOC concentrations.
The impact of transport across the polar vortex edge on Match ozone loss estimates
Authors: Grooß J.-U. , Müller R. , Konopka P. , Steinhorst H.-M. , Engel A. , Möbius T. , Volk C. M.
Published: April 2010

Abstract. The Match method for the quantification of polar chemical ozone loss is investigated mainly with respect to the impact of the transport of air masses across the vortex edge. For the winter 2002/03, we show that significant transport across the vortex edge occurred and was simulated by the Chemical Lagrangian Model of the Stratosphere. In-situ observations of inert tracers and ozone from HAGAR on the Geophysica aircraft and balloon-borne sondes, and remote observations from MIPAS on the ENVISAT satellite were reproduced well by CLaMS. The model even reproduced a small vortex remnant that remained a distinct feature until June 2003 and was also observed in-situ by a balloon-borne whole air sampler. We use this CLaMS simulation to quantify the impact of transport across the vortex edge on ozone loss estimates from the Match method. We show that a time integration of the determined vortex average ozone loss rates, as performed in Match, results in a larger ozone loss than the polar vortex average ozone loss in CLaMS. The determination of the Match ozone loss rates is also influenced by the transport of air across the vortex edge. We use the model to investigate how the sampling of the ozone sondes on which Match is based represents the vortex average ozone loss rate. Both the time integration of ozone loss and the determination of ozone loss rates for Match are evaluated using the winter 2002/2003 CLaMS simulation. These impacts can explain the majority of the differences between CLaMS and Match column ozone loss. While the investigated effects somewhat reduce the apparent discrepancy in January ozone loss rates reported earlier, a distinct discrepancy between simulations and Match remains. However, its contribution to the accumulated ozone loss over the winter is not large.
Origin of diversity in falling snow
Authors: Nelson J.
Published: April 2010

Abstract. This paper presents a systematic way to examine the origin of variety in falling snow. First, we define shape diversity as the logarithm of the number of possible distinguishable crystal forms for a given resolution and set of conditions, and then we examine three sources of diversity. Two sources are the range of initial-crystal sizes and variations in the trajectory variables. For a given set of variables, diversity is estimated using a model of a crystal falling in an updraft. The third source is temperature-updraft heterogeneities along each trajectory. To examine this source, centimeter-scale data on cloud temperature and updraft speed are used to estimate the spatial frequency (m−1) of crystal feature changes. For air-temperature heterogeneity, this frequency decays as p−0.66, where p is a measure of the temperature-deviation size. For updraft-speed heterogeneity, the decay is p−0.50. By using these frequencies, the fallpath needed per feature change is found to range from ~0.8 m, for crystals near −15°C, to ~8 m near −19°C – lengths much less than total fallpath lengths. As a result, the third source dominates the diversity, with updraft heterogeneity contributing more than temperature heterogeneity. Plotted against the crystal's initial temperature (−11 to −19°C), the diversity curve is "mitten shaped", having a broad peak near −15.4°C and a sharp subpeak at −14.4°C, both peaks arising from peaks in growth-rate sensitivity. The diversity is much less than previous estimates, yet large enough to explain observations. For example, of all snow crystals ever formed, those that began near −15°C are predicted to all appear unique to 1−μm resolution, but those that began near −11°C are not.
Hygroscopicity of the submicrometer aerosol at the high-alpine site Jungfraujoch, 3580 m a.s.l., Switzerland
Authors: Sjogren S. , Gysel M. , Weingartner E. , Alfarra M. R. , Duplissy J. , Cozic J. , Crosier J. , Coe H. , Baltensperger U.
Published: April 2010

Abstract. Data from measurements of hygroscopic growth of submicrometer aerosol with a hygroscopicity tandem differential mobility analyzer (HTDMA) during four campaigns at the high alpine research station Jungfraujoch, Switzerland, are presented. The campaigns took place during the years 2000, 2002, 2004 and 2005, each lasting approximately one month. Hygroscopic growth factors (GF, i.e. the relative change in particle diameter from dry diameter, D0, to diameter measured at higher relative humidity, RH) are presented for three distinct air mass types, namely for: 1) free tropospheric winter conditions, 2) planetary boundary layer influenced air masses (during a summer period) and 3) Saharan dust events (SDE). The GF values at 85% RH (D0=100 nm) were 1.40±0.11 and 1.29±0.08 for the first two situations while for SDE a bimodal GF distribution was often found. No phase changes were observed when the RH was varied between 10–90%, and the continuous water uptake could be well described with a single-parameter empirical model. The frequency distributions of the average hygroscopic growth factors and the width of the retrieved growth factor distributions (indicating whether the aerosol is internally or externally mixed) are presented, which can be used for modeling purposes. Measurements of size resolved chemical composition were performed with an aerosol mass spectrometer in parallel to the GF measurements. This made it possible to estimate the apparent ensemble mean GF of the organics (GForg) using inverse ZSR (Zdanovskii-Stokes-Robinson) modeling. GForg was found to be ~1.20 at aw=0.85, which is at the upper end of previous laboratory and field data though still in agreement with the highly aged and oxidized nature of the Jungfraujoch aerosol.
Odin stratospheric proxy NOy measurements and climatology
Authors: Brohede S. , McLinden C. A. , Urban J. , Haley C. S. , Jonsson A. I. , Murtagh D.
Published: April 2010

Abstract. Five years of OSIRIS (Optical Spectrograph and InfraRed Imager System) NO2 and SMR (Sub-millimetre and Millimetre Radiometer) HNO3 observations from the Odin satellite, combined with data from a photochemical box model, have been used to construct a stratospheric proxy NOy data set including the gases: NO, NO2, HNO3, 2×N2O5 and ClONO2. This Odin NOy climatology is based on all daytime measurements and contains monthly mean and standard deviation, expressed as mixing ratio or number density, as function of latitude or equivalent latitude (5° bins) on 17 vertical layers (altitude, pressure or potential temperature) between 14 and 46 km. Comparisons with coincident NOy profiles from the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS) instrument were used to evaluate several methods to combine Odin observations with model data. This comparison indicates that the most appropriate merging technique uses OSIRIS measurements of NO2, scaled with model NO/NO2 ratios, to estimate NO. The sum of 2×N2O5 and ClONO2 is estimated from uncertainty-based weighted averages of scaled observations of SMR HNO3 and OSIRIS NO2. Comparisons with ACE-FTS suggest the precision (random error) and accuracy (systematic error) of Odin NOy profiles are about 15% and 20%, respectively. Further comparisons between Odin and the Canadian Middle Atmosphere Model (CMAM) show agreement to within 20% and 2 ppb throughout most of the stratosphere except in the polar vortices. The combination of good temporal and spatial coverage, a relatively long data record, and good accuracy and precision make this a valuable NOy product for various atmospheric studies and model assessments.
Direct SW aerosol radiative forcing over Portugal
Authors: Santos D. , Costa M. J. , Silva A. M.
Published: April 2010

Abstract. In this work, the evaluation of the aerosol radiative forcing at the top of the atmosphere as well as at the surface over the south of Portugal is made, particularly in the regions of Évora (38°34' N, 7°54' W) and of Cabo da Roca (38°46' N, 9°38' W), during years 2004 and 2005. The radiative transfer calculations, using the radiative transfer code Second Simulation of the Satellite Signal in the Solar Spectrum (6S), combine ground-based measurements, from Aerosol Robotic NETwork (AERONET), and satellite measurements, from MODerate Imaging Spectroradiometer (MODIS), to estimate the direct SW aerosol radiative forcing. The method developed to retrieve the surface spectral reflectance is also presented, based on ground-based measurements (AERONET) of the aerosol optical properties combined with the satellite-measured radiances (MODIS). The instantaneous direct SW aerosol radiative forcing values obtained at the top of the atmosphere are, in the majority of the cases, negative, indicating a tendency for cooling the Earth at the top of the atmosphere. For Desert Dust aerosols, over the Évora land region, the average forcing efficiency is estimated to be −25 Wm−2/AOT0.55 whereas for the Cabo da Roca area, the average forcing efficiency is −46 Wm−2/AOT0.55. In the presence of Forest Fire aerosols, both from short and long distances, the average value of forcing efficiency at the top of the atmosphere over Cabo da Roca is found to be −28 Wm−2/AOT0.55 and, over Évora, −27 Wm−2/AOT0.55. For specific situations, discussed in this work, the average surface direct SW aerosol radiative forcing efficiency due to the Desert Dust aerosols, in Évora region, is −66 Wm−2/AOT0.55, whereas in Cabo da Roca region, the corresponding average value is −38 Wm−2/AOT0.55. Considering the Forest Fire aerosols, over Évora region, the average surface direct SW aerosol radiative forcing efficiency can vary between −36 and −113 Wm−2/AOT0.55, the more negative value corresponding to forest fire aerosols coming only from shorter distances.
Size distributions of elemental carbon in the atmosphere of a coastal urban area in South China: characteristics, evolution processes, and implications for the mixing state
Authors: Huang X.-F. , Yu J. Z.
Published: April 2010

Abstract. Elemental carbon (EC), as one of the primary light-absorbing components in the atmosphere, has a significant impact on both regional and global climate. The environmental impacts of EC are strongly dependent on its particle size. Little is known about the size distribution characteristics of EC particles in China's ambient environments. We report size distributions of EC particles in the urban area of Shenzhen in Southern China. In our samples, EC was consistently found in two modes, a fine mode and a coarse mode. The majority of EC mass (~80%) in this coastal metropolitan city resided in particles smaller than 3.2 μm in diameter. The fine mode peaked at around either 0.42 μm or 0.75 μm. While the mode at 0.42 μm could be ascribed to fresh vehicular emissions in the region, the mode at 0.75 μm was likely a result of particle growth from smaller EC particles. We theoretically investigated the particle growth processes that caused the EC particles to grow from 0.42 μm to 0.75 µm in the atmosphere. Our calculations indicate that the EC peak at 0.75 μm was not produced through either coagulation or H2SO4 condensation; both processes are too slow to lead to significant EC growth. Hygroscopic growth was also determined to be insignificant. Instead, addition of sulfate through in-cloud processing was found to cause significant growth of the EC particles and to explain the EC peak at 0.75 μm. We also estimated the mixing state of EC from the EC size distributions. In the droplet size, at least 45–60% of the EC mass in the summer samples and 68% of the EC mass in the winter samples was internally mixed with sulfate as a result of in-cloud processing. This information on EC should be considered in models of the optical properties of aerosols in this region. Our results also suggest that the in-cloud processing of primary EC particles could increase the light absorbing capacities through mixing EC with sulfate.
Consistent simulation of bromine chemistry from the marine boundary layer to the stratosphere – Part 1: Model description, sea salt aerosols and pH
Authors: Kerkweg A. , Jöckel P. , Pozzer A. , Tost H. , Sander R. , Schulz M. , Stier P. , Vignati E. , Wilson J. , Lelieveld J.
Published: April 2010

Abstract. This is the first article of a series presenting a detailed analysis of bromine chemistry simulated with the atmospheric chemistry general circulation model ECHAM5/MESSy. Release from sea salt is an important bromine source, hence the model explicitly calculates aerosol chemistry and phase partitioning for coarse mode aerosol particles. Many processes including chemical reaction rates are influenced by the particle size distribution, and aerosol associated water strongly affects the aerosol pH. Knowledge of the aerosol pH is important as it determines the aerosol chemistry, e.g., the efficiency of sulphur oxidation and bromine release. Here, we focus on the simulated sea salt aerosol size distribution and the coarse mode aerosol pH. A comparison with available field data shows that the simulated aerosol distributions agree reasonably well within the range of measurements. In spite of the small number of aerosol pH measurements and the uncertainty in its experimental determination, the simulated aerosol pH compares well with the observations. The aerosol pH ranges from alkaline aerosol in areas of strong production down to pH-values of 1 over regions of medium sea salt production and high levels of gas phase acids, mostly polluted regions over the oceans in the Northern Hemisphere.
Consistent simulation of bromine chemistry from the marine boundary layer to the stratosphere – Part 2: Bromocarbons
Authors: Kerkweg A. , Jöckel P. , Warwick N. , Gebhardt S. , Brenninkmeijer C. A. M. , Lelieveld J.
Published: April 2010

Abstract. In this second part of a series of articles dedicated to a detailed analysis of bromine chemistry in the atmosphere we address one (out of two) dominant natural sources of reactive bromine. The two main source categories are the release of bromine from sea salt and the decomposition of bromocarbons by photolysis and reaction with OH. Here, we focus on C1-bromocarbons. We show that the atmospheric chemistry general circulation model ECHAM5/MESSy realistically simulates their emission, transport and decomposition from the boundary layer up to the mesosphere. We included oceanic emission fluxes of the short-lived bromocarbons CH2Br2, CH2ClBr, CHClBr2, CHCl2Br, CHBr3 and of CH3Br. The vertical profiles and the surface mixing ratios of the bromocarbons are in general agreement with the (few available) observations, especially in view of the limited information available and the consequent coarseness of the emission fields. For CHBr3, CHCl2Br and CHClBr2 photolysis is the most important degradation process in the troposphere. In contrast to this, tropospheric CH2Br2, CH3Br and CH2ClBr are more efficiently decomposed by reaction with OH. In the free troposphere approximately 40% of the C1-bromocarbons decompose by reaction with OH. Our results indicate that bromoform contributes substantial amounts of reactive bromine to the lower stratosphere and thus should not be neglected in stratospheric simulations.
Effect of explicit urban land surface representation on the simulation of the 26 July 2005 heavy rain event over Mumbai, India
Authors: Lei M. , Niyogi D. , Kishtawal C. , Pielke R. A. , Beltrán-Przekurat A. , Nobis T. E. , Vaidya S. S.
Published: April 2010

Abstract. We investigate whether explicit representation of the urban land surface improves the simulation of the record-breaking 24-h heavy rain event that occurred over Mumbai, India on 26 July 2005 as the event has been poorly simulated by operational weather forecasting models. We conducted experiments using the Regional Atmosphere modeling system (RAMS 4.3), coupled with and without explicit urban energy balance model-town energy budget (TEB) to study the role of urban land – atmosphere interactions in modulating the heavy rain event over the Indian monsoon region. The impact of including an explicit urban energy balance on surface thermodynamic, boundary layer, and circulation changes are analyzed. The results indicate that even for this synoptically active rainfall event, the vertical wind and precipitation are significantly influenced by heterogeneity in surface temperatures due to urbanization, and the effect is more significant during the storm initiation. Interestingly, precipitation in the upwind region of Mumbai city is increased in the simulation, possibly as a feedback from the sea breeze – urban landscape convergence. We find that even with the active monsoon, the representation of urbanization contributes to local heavy precipitation and mesoscale precipitation distribution over the Indian monsoon region. Additional experiments within a statistical dynamical framework show that an urban model by itself is not the dominant factor for the enhanced rainfall for a Mumbai heavy rain event; the combination of updated SST fields using Tropical Rainfall Measurement Mission (TRMM) data with the detailed representation of urban effects simulated by the TEB model created realistic gradients that successfully maintained the convergence zone over Mumbai. Further research will require more detailed morphology data for simulating weather events in such urban regions. The results suggest that urbanization can significantly contribute to extremes in monsoonal rain events that have been reported to be on the rise.
How many carboxyl groups does an average molecule of humic-like substances contain?
Authors: Salma I. , Láng G. G.
Published: April 2010

Abstract. The carboxyl groups of atmospheric humic-like substances (HULIS) are of special interest because they influence the solubility in water, affect the water activity and surface tension of droplets in the air, and allow formation of chelates with biologically active elements. Experimentally determined abundances of the carboxyl group within HULIS by functional group analysis are consistent with our knowledge on the average molecular mass of HULIS if the number of dissociable carboxyl groups is assumed to be rather small. The best agreement between the average molecular mass derived from the existing abundance data and the average molecular mass published earlier occurs for assuming approximately one dissociable carboxyl group only. This implies that HULIS can not be regarded as polycarboxilic acid in diluted solutions. The average molecular mass of HULIS derived from our electrochemical measurements with the assumption of one dissociable carboxyl group or equivalently, one dissociable sulphate ester per molecule ranges from 250 to 310 Da. It was concluded that HULIS are a moderately strong/weak acid with a dissociation constant of about pK=3.4, which fits well into the interval represented by fulvic and humic acids. The mean number of dissociable hydrogen (i.e. of carboxyl groups and sulphate esters jointly) in HULIS molecules was refined to be between 1.1 and 1.4 in acidic solutions.
MATRIX (Multiconfiguration Aerosol TRacker of mIXing state): an aerosol microphysical module for global atmospheric models
Authors: Bauer S. E. , Wright D. L. , Koch D. , Lewis E. R. , McGraw R. , Chang L.-S. , Schwartz S. E. , Ruedy R.
Published: April 2010

Abstract. A new aerosol microphysical module MATRIX, the Multiconfiguration Aerosol TRacker of mIXing state, and its application in the Goddard Institute for Space Studies (GISS) climate model (ModelE) are described. This module, which is based on the quadrature method of moments (QMOM), represents nucleation, condensation, coagulation, internal and external mixing, and cloud-drop activation and provides aerosol particle mass and number concentration and particle size information for up to 16 mixed-mode aerosol populations. Internal and external mixing among aerosol components sulfate, nitrate, ammonium, carbonaceous aerosols, dust and sea-salt particles are represented. The solubility of each aerosol population, which is explicitly calculated based on its soluble and insoluble components, enables calculation of the dependence of cloud drop activation on the microphysical characterization of multiple soluble aerosol populations. A detailed model description and results of box-model simulations of various aerosol population configurations are presented. The box model experiments demonstrate the dependence of cloud activating aerosol number concentration on the aerosol population configuration; comparisons to sectional models are quite favorable. MATRIX is incorporated into the GISS climate model and simulations are carried out primarily to assess its performance/efficiency for global-scale atmospheric model application. Simulation results were compared with aircraft and station measurements of aerosol mass and number concentration and particle size to assess the ability of the new method to yield data suitable for such comparison. The model accurately captures the observed size distributions in the Aitken and accumulation modes up to particle diameter 1 μm, in which sulfate, nitrate, black and organic carbon are predominantly located; however the model underestimates coarse-mode number concentration and size, especially in the marine environment. This is more likely due to oversimplifications of the representation of sea salt emissions – sea salt emissions are only calculated for two size classes – than to inherent limitations of MATRIX.