bluuebunny/crossref_metadata_2025 huggingface dataset:
The two-day wave in the Antarctic and Arctic mesosphere and lower thermosphere
Authors: Tunbridge V. M. , Mitchell N. J.
Published: April 2010

Abstract. There have been comparatively few studies reported of the 2-day planetary wave in the middle atmosphere at polar latitudes. Here we report studies made using high-latitude meteor radars at Rothera in the Antarctic (68° S, 68° W) and Esrange in Arctic Sweden (68° N, 21° E). Observations from 2005–2008 are used for Rothera and from 1999–2008 for Esrange. Data were recorded for heights of 80–100 km. The radar data reveal distinct summertime and wintertime 2-day waves. The Antarctic summertime wave occurs with significant amplitudes in January–February at heights between about 88–100 km. Horizontal wind monthly variances associated with the wave exceed 160 m2 s−2 and the zonal component has larger amplitudes than the meridional. In contrast, the Arctic summertime wave occurs for a longer duration, June–August and has meridional amplitudes larger than zonal. The Arctic summertime wave is weaker than that in the Antarctic and maximum monthly variances are typically 60 m2 s−2. In both hemispheres the summertime wave reaches largest amplitudes in the strongly sheared eastward zonal flow above the zero wind line and is largely absent in the westward flow below. The observed differences in the summertime wave is probably due to the differences in the background zonal winds in the two hemispheres. The Antarctic and Arctic wintertime waves have very similar behavior. The Antarctic wave has significant amplitudes in May–August and the Arctic wave in November–February. Both are evident across the full height range observed.
Extensive reduction of surface UV radiation since 1750 in world's populated regions
Authors: Kvalevåg M. M. , Myhre G. , Lund Myhre C. E.
Published: April 2010

Abstract. Human activity influences a wide range of components that affect the surface UV radiation levels, among them ozone at high latitudes. We calculate the effect of human-induced changes in the surface erythemally weighted ultra-violet radiation (UV-E) since 1750. We compare results from a radiative transfer model to surface UV-E radiation for year 2000 derived by satellite observations (from Total Ozone Mapping Spectroradiometer) and to ground based measurements at 14 sites. The model correlates well with the observations; the correlation coefficients are 0.97 and 0.98 for satellite and ground based measurements, respectively. In addition to the effect of changes in ozone, we also investigate the effect of changes in SO2, NO2, the direct and indirect effects of aerosols, albedo changes and aviation-induced contrails and cirrus. The results show an increase of surface UV-E in polar regions, most strongly in the Southern Hemisphere. Furthermore, our study also shows an extensive surface UV-E reduction over most land areas; a reduction up to 20% since 1750 is found in some industrialized regions.
Measurements of total and tropospheric ozone from IASI: comparison with correlative satellite and ozonesonde observations
Authors: Boynard A. , Clerbaux C. , Coheur P.-F. , Hurtmans D. , Turquety S. , George M. , Hadji-Lazaro J. , Keim C. , Meyer-Arnek J.
Published: April 2010

Abstract. In this paper, we present measurements of total and tropospheric ozone, retrieved from infrared radiance spectra recorded by the Infrared Atmospheric Sounding Interferometer (IASI), which was launched on board the MetOp-A European satellite in October 2006. We compare the IASI total ozone columns to observations from the Global Ozone Monitoring Experiment-2 (GOME-2) for one full year of observations (2008). The global distributions are in good agreement, with a correlation coefficient better than 0.9. On average, IASI ozone retrievals exhibit a positive bias compared to GOME-2 of about 4.9 DU (2.9%) to 13 DU (4.4%) depending on the season. In addition to total ozone columns, the good spectral resolution of IASI enables the retrieval of tropospheric ozone concentrations. Comparisons of IASI tropospheric columns to 490 collocated ozone soundings available from several stations around the globe have been performed for the period June 2007–August 2008. IASI tropospheric ozone columns compare well with sonde observations, with correlation coefficients of 0.95 and 0.77 for the [surface – 6 km] and [surface – 12 km] partial columns, respectively. IASI retrievals tend to overestimate the tropospheric ozone columns in comparison with ozonesonde measurements. Positive average biases of 0.15 DU (1.2%) and 3 DU (11%) are found for the [surface – 6 km] and for the [surface – 12 km] partial columns, respectively.
Analytical treatment of ice sublimation and test of sublimation parameterisations in two-moment ice microphysics models
Authors: Gierens K. , Bretl S.
Published: April 2010

Abstract. We derive an analytic solution to the spectral growth/sublimation equation for ice crystals and apply it to idealised cases. The results are used to test parameterisations of the ice sublimation process in two-moment bulk microphysics models. Although it turns out that the relation between number loss fraction and mass loss fraction is not a function since it is not unique, it seems that a functional parameterisation is the best that one can do in a bulk model. Testing a more realistic case with humidity oscillations shows that artificial crystal loss can occur in simulations of mature cirrus clouds with relative humidity fluctuating about ice saturation.
The effects of Forbush decreases on Antarctic climate variability: a re-assessment
Authors: Laken B. A. , Kniveton D. R.
Published: April 2010

Abstract. In an attempt to test the validity of a relationship between Galactic cosmic rays (GCRs) and cloud cover, a range of past studies have performed composite analysis based around Forbush decrease (FD) events. These studies have produced a range of conflicting results, consequently reducing confidence in the existence of a GCR-cloud link. A potential reason why past FD based studies have failed to identify a consistent relationship may be that the FD events themselves are too poorly defined, and require calibration prior to analysis. Drawing from an initial sample of 48 FD events taken from multiple studies this work attempts to isolate a GCR decrease of greater magnitude and coherence than has been demonstrated by past studies. After this calibration composite analysis revealed increases in high level (10–180 mb) cloud cover (of ~20%) occurred over the Antarctic plateau in conjunction with decreases in the rate of GCR flux during austral winter (these results are broadly opposite to those of past studies). The cloud changes occurred in conjunction with locally significant surface level air temperature increases over the Antarctic plateau (~4 K) and temperature decreases over the Ross Ice Sheet (~8 K). These temperature variations appear to be indirectly linked to cloud via anomalous surface level winds rather than a direct radiative forcing. These results provide good evidence of a relationship between daily timescale GCR variations and Antarctic climate variability.
Simulation of particle size distribution with a global aerosol model: contribution of nucleation to aerosol and CCN number concentrations
Authors: Yu F. , Luo G.
Published: April 2010

Abstract. An advanced particle microphysics model with a number of computationally efficient schemes has been incorporated into a global chemistry transport model (GEOS-Chem) to simulate particle number size distributions and cloud condensation nuclei (CCN) concentrations in the atmosphere. Size-resolved microphysics for secondary particles (i.e., those formed from gaseous species) and sea salt has been treated in the present study. The growth of nucleated particles through the condensation of sulfuric acid vapor and equilibrium uptake of nitrate, ammonium, and secondary organic aerosol is explicitly simulated, along with the scavenging of secondary particles by primary particles (dust, black carbon, organic carbon, and sea salt). We calculate secondary particle formation rate based on ion-mediated nucleation (IMN) mechanism and constrain the parameterizations of primary particle emissions with various observations. Our simulations indicate that secondary particles formed via IMN appear to be able to account for the particle number concentrations observed in many parts of troposphere. A comparison of the simulated annual mean concentrations of condensation nuclei larger than 10 nm (CN10) with those measured values show very good agreement (within a factor of two) in near all 22 sites around the globe that have at least one full year of CN10 measurements. Secondary particles appear to dominate the number abundance in most parts of the troposphere. Calculated CCN concentration at supersaturation of 0.4% (CCN0.4) and the fraction of CCN0.4 that is secondary (fCCNsec) have large spatial variations. Over the middle latitude in the Northern Hemisphere, zonally averaged CCN0.4 decreases from ~400–700 cm−3 in the boundary layer (BL) to below 100 cm−3 above altitude of ~4 km, the corresponding fCCNsec values change from 50–60% to above ~70%. In the Southern Hemisphere, the zonally averaged CCN0.4 is below 200 cm−3 and fCCNsec is generally above 60% except in the BL over the Southern Ocean.
Lightning-produced NOx during the Northern Australian monsoon; results from the ACTIVE campaign
Authors: Labrador L. , Vaughan G. , Heyes W. , Waddicor D. , Volz-Thomas A. , Pätz H.-W. , Höller H.
Published: April 2010

Abstract. Measurements of nitrogen oxides onboard a high altitude aircraft were carried out for the first time during the Northern Australian monsoon in the framework of the Aerosol and Chemical Transport in Tropical Convection (ACTIVE) campaign, in the area around Darwin, Australia. During one flight on 22 January 2006, average NOx mixing ratios (mrs) of 723 and 984 parts per trillion volume (pptv) were recorded for both in and out of cloud conditions, respectively. The in-cloud measurements were made in the convective outflow region of a storm 56 km south-west of Darwin, whereas those out of cloud were made due south of Darwin and upwind from the storm sampled. This storm produced a total of only 8 lightning strokes, as detected by an in-situ lightning detection network, ruling out significant lightning-NOx production. 5-day backward trajectories suggest that the sampled airmasses had travelled over convectively-active land in Northern Australia during that period. The low stroke count of the sampled storm, along with the high out-of-cloud NOx concentration, suggest that, in the absence of other major NOx sources during the monsoon season, a combination of processes including regional transport patterns, convective vertical transport and entrainment may lead to accretion of lightning-produced NOx, a situation that contrasts with the pre-monsoon period in Northern Australia, where the high NOx values occur mainly in or in the vicinity of storms. These high NOx concentrations may help start ozone photochemistry and OH radical production in an otherwise NOx-limited environment.
The impact of tropical recirculation on polar composition
Authors: Strahan S. E. , Schoeberl M. R. , Steenrod S. D.
Published: April 2010

Abstract. We derive the tropical modal age of air from an analysis of the water vapor tape recorder. We combine the observationally derived modal age with mean age of air from CO2 and SF6 to create diagnostics for the independent evaluation of the vertical transport rate and horizontal recirculation into the tropics between 16–32 km. These diagnostics are applied to two Global Modeling Initiative (GMI) chemistry and transport model (CTM) age tracer simulations to give new insights into the tropical transport characteristics of the meteorological fields from the GEOS4-GCM and the GEOS4-DAS. Both simulations are found to have modal ages that are in reasonable agreement with the empirically derived age (i.e., transit times) over the entire altitude range. Both simulations show too little horizontal recirculation into the tropics above 22 km, with the GEOS4-DAS fields having greater recirculation. Using CH4 as a proxy for mean age, comparisons between HALOE and model CH4 in the Antarctic demonstrate how the strength of tropical recirculation affects polar composition in both CTM experiments. The better the tropical recirculation is simulated, the better the CH4 simulation is in the Antarctic. Mean age in the Antarctic lower stratosphere can be compromised by poor representation of tropical ascent, tropical recirculation, or vortex barrier strength. The connection between polar and tropical composition shown in this study demonstrates the importance of diagnosing each of these processes separately in order to verify the adequate representation of the processes contributing to polar composition in models.
Tempo-spatial variation of emission inventories of speciated volatile organic compounds from on-road vehicles in China
Authors: Cai H. , Xie S. D.
Published: April 2010

Abstract. Emission inventories of sixty-nine speciated non-methane volatile organic compounds (NMVOC) from on-road vehicles in China were estimated for the period of 1980–2005, using seven NMVOC emission profiles, which were summarized based on local and international measurements from published literatures dealing with specific vehicle categories running under particular modes. Results show an exponential growth trend of China's historical emissions of alkanes, alkenes, alkines, aromatics and carbonyls during the period of 1980–2005, increasing from 63.9, 39.3, 6.9, 36.8 and 24.1 thousand tons, respectively, in 1980 to 2781.4, 1244.9, 178.5, 1350.7 and 403.3 thousand tons, respectively, in 2005, which coincided well with China's economic growth. Emission inventories of alkenes, aromatics and carbonyls were gridded at a high resolution of 40 km×40 km for air quality simulation and health risk evaluation, using the geographic information system (GIS) methodology. Spatial distribution of speciated NMVOC emissions shows a clear difference in emission densities between developed eastern and relatively underdeveloped western and inland China. Besides, the appearance and expansion of high-emission areas was another notable characteristic of spatial distribution of speciated NMVOC emissions during the period. Emission contributions of vehicle categories to speciated NMVOC groups showed annual variation, due to the variance in the provincial emissions and in the relative fractions of the seven emission profiles adopted at the provincial level. Highly reactive and toxic compounds accounted for high proportions of emissions of speciated NMVOC groups. The most abundant compounds were isopentane, pentane and butane from alkanes; ethene, propene, 2-methyl-2-butene and ethyne from alkenes and alkines; benzene, toluene, ethylbenzene, o-xylene, and m,p-xylene (BTEX) and 1,2,4-trimethylbenzene from aromatics and formaldehyde, acetaldehyde, benzaldehyde, acetone and acrolein from carbonyls.
Quantifying atmospheric nitrate formation pathways based on a global model of the oxygen isotopic composition (Δ17O) of atmospheric nitrate
Authors: Alexander B. , Hastings M. G. , Allman D. J. , Dachs J. , Thornton J. A. , Kunasek S. A.
Published: April 2010

Abstract. The oxygen isotopic composition (Δ17O) of atmospheric nitrate is a function of the relative abundance of atmospheric oxidants (O3, HOx=OH +HO2+RO2) and the formation pathway of nitrate from its precursor NOx (=NO+NO2). Coupled observations and modeling of nitrate Δ17O can be used to quantify the relative importance of chemical formation pathways leading to nitrate formation and reduce uncertainties in the budget of reactive nitrogen chemistry in the atmosphere. We present the first global model of atmospheric nitrate Δ17O and compare with available observations. The model shows the best agreement with a global compilation of observations when assuming a Δ17O value of tropospheric ozone equal to 35‰ and preferential oxidation of NOx by the terminal oxygen atoms of ozone. Calculated values of annual-mean nitrate Δ17O in the lowest model layer (0–200 m above the surface) vary from 6‰ in the tropics to 41‰ in the polar-regions. On the global scale, O3 is the dominant oxidant (81% annual-mean) during NOx cycling reactions. The global, annual-mean tropospheric inorganic nitrate burden is dominated by nitrate formation via NO2+OH (76%), followed by N2O5 hydrolysis (18%) and NO3+DMS/HC (4%). Model discrepancies are largest in the polar spring and summer, most likely due to the lack of reactive halogen chemistry in the model. The influence of organic nitrates on observations of nitrate Δ17O needs to be determined, especially for observations in summertime and tropical forested regions where organic nitrates can contribute up to 80% of the total NOy (organic plus inorganic nitrate) budget.
Two years of Ozone radio soundings over Cotonou as part of AMMA: overview
Authors: Thouret V. , Saunois M. , Minga A. , Mariscal A. , Sauvage B. , Solete A. , Agbangla D. , Nédélec P. , Mari C. , Reeves C. E. , Schlager H.
Published: April 2010

Abstract. As part of the African Monsoon Multidisciplinary Analysis (AMMA) program, a total of 98 ozone vertical profiles over Cotonou, Benin, have been measured during a 26 month period (December 2004–January 2007). These regular measurements broadly document the seasonal and inter annual variability of ozone in both the troposphere and the lower stratosphere over West Africa for the first time. This data set is complementary to the MOZAIC observations made from Lagos between 0 and 12 km during the period 1998–2004. Both data sets highlight the unique way in which West Africa is impacted by two biomass burning seasons: in December–February (dry season) due to burning in the Sahelian band and in June–August (wet season) due to burning in southern Africa. High inter annual variabilities between Cotonou and Lagos data sets and within each data set are observed and are found to be a major characteristic of this region. In particular, the dry and wet seasons are discussed in order to set the data of the Special Observing Periods (SOPs) into a climatological context. Compared to other dry and wet seasons, the dry and wet season campaigns took place in rather high ozoneenvironments. During the sampled wet seasons, southern intrusions of biomass burning were particularly frequent with concentrations up to 120 ppbv of ozone in the lower troposphere. An insight into the ozone distribution in the upper troposphere and the lower stratosphere (up to 26 km) is given. The first tropospheric columns of ozone based on in-situ data in this region are assessed. They compare well with satellite products on seasonal and inter annual time-scales, provided that the layer below 850 Pa where the remote instrument is less sensitive to ozone, is removed.
Lightning NOx emissions over the USA investigated using TES, NLDN, LRLDN, IONS data and the GEOS-Chem model
Authors: Jourdain L. , Kulawik S. S. , Worden H. M. , Pickering K. E. , Worden J. , Thompson A. M.
Published: April 2010

Abstract. Knowledge of the lightning source of NOx is required to better understand NOx and ozone distributions and changes in the troposphere, the oxidising capacity of the troposphere as well as some of the feedbacks between chemistry and climate change. In this paper, we use the National Lightning Detection (NLDN) and the Long Range Lightning Detection Network (LRLDN) data as well as the HYPSLIT transport and dispersion model to show the presence of ozone enhanced layers downwind of convective events in the ozone vertical profiles from the Tropospheric Emission Spectrometer (TES) instrument over the USA in July 2006. We use the TES dataset in conjunction with ozonesonde measurements from the Intercontinental Chemical Transport Experiment (INTEX) Ozonesonde Network Study (IONS) 2006 to test the parameterization of the lightning source of NOx in a global chemistry transport model. We find that the global 3-D chemistry transport model GEOS-Chem with a lightning activity calculated with a parameterization based on cloud top height, scaled regionally and monthly to OTD/LIS (Optical Transient Detector/Lightning Imaging Sensor) climatology, and with a production of 260 mol NO/Flash captures the ozone enhancements seen by TES, but underestimates their intensities. We show that the model's ability to reproduce the location of the enhancements is due to the fact that this model reproduces the pattern of the convective events occurrence on a daily basis during the summer of 2006, even though it does not well represent the relative distribution of lightning intensities. By imposing an updated lightning NO production value of 520 mol NO/Flash, we decrease the bias between TES and GEOS-Chem over the US in July 2006 by 40%.
Ice nucleation properties of mineral dust particles: Determination of onset RHi, IN active fraction, nucleation time-lag, and the effect of active sites on contact angles
Authors: Kulkarni G. , Dobbie S.
Published: April 2010

Abstract. A newly developed ice nucleation experimental set up was used to investigate the heterogeneous ice nucleation properties of three Saharan and one Spanish dust particle samples. It was observed that the spread in the onset relative humidities with respect to ice (RHi) for Saharan dust particles varied from 104% to 110%, whereas for the Spanish dust from 106% to 110%. The elemental composition analysis shows a prominent Ca feature in the Spanish dust sample which could potentially explain the differences in nucleation threshold. Although the spread in the onset RHi) for the Saharan dust samples were in agreement, the active fractions and nucleation time-lags calculated at various temperature and RHi) conditions were found to differ. This could be due to the subtle variation in the elemental composition of the dust samples, and surface irregularities like steps, cracks, cavities etc. A combination of classical nucleation theory and active site theory is used to understand the importance of these surface irregularities on the nucleability parameter contact angle that is widely used in the ice cloud modeling. These calculations show that the surface irregularities can reduce the contact angle by approximately 10°.
Microphysical and optical properties of Arctic mixed-phase clouds – the 9 April 2007 case study
Authors: Gayet J.-F. , Mioche G. , Dörnbrack A. , Ehrlich A. , Lampert A. , Wendisch M.
Published: April 2010

Abstract. Airborne measurements in Arctic boundary-layer stratocumulus were carried out near Spitsbergen on 9 April 2007 during the Arctic Study of Tropospheric Aerosol, Clouds and Radiation (ASTAR) campaign. A unique set of co-located observations is used to describe the cloud properties, including detailed in situ cloud microphysical and radiation measurements along with airborne and co-located spaceborne remote sensing data (Lidar on Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations [CALIPSO] and radar on CloudSat satellites). The CALIPSO profiles evidence a cloud top temperature which varies between −24°C and −21°C. The in situ cloud observations reveal that the attenuated backscatter signal from lidar along the aircraft trajectory is linked with the presence of liquid water and therefore confirms a cloud top layer dominated by liquid-water, which is a common feature observed in Arctic mixed-phase stratocumulus clouds. A low concentration of quite large ice crystals are also evidenced up to the cloud top and lead to significant CloudSat radar echo. Since the ratio of the extinction of liquid water droplets and ice crystals is high the broadband radiative effects near the cloud top are mostly dominated by water droplets. CloudSat observations as well as in situ measurements reveal high reflectivity factors (up to 15 dBZ) and precipitation rates (1 mm h−1). This feature is due to efficient ice production processes. About 25% of the theoretically available liquid water is converted into ice water with large ice crystals which precipitate. According to an estimation of the mean cloud cover, a considerable value of 106 m3 h−1 of fresh water could be settled over the Greenland sea pool. European Centre for Medium-Range Weather Forecast (ECMWF) operational analyses reproduces the variation of the boundary layer height along the flight track. However, small-scale features in the observed cloud field cannot be resolved by ECMWF analysis. Furthermore, ECMWF's diagnostic partitioning of the condensed water into ice and liquid reveals serious shortcomings for Arctic mixed-phased clouds. Too much ice is modeled.
Generation of free convection due to changes of the local circulation system
Authors: Eigenmann R. , Metzger S. , Foken T.
Published: April 2010

Abstract. Eddy-covariance and Sodar/RASS experimental measurement data of the COPS (Convective and Orographically-induced Precipitation Study) field campaign 2007 are used to investigate the generation of near-ground free convection events in the Kinzig valley, Black Forest, Southwest Germany. The measured high-quality turbulent flux data revealed free convection to be induced in situations where high buoyancy fluxes and a simultaneously occurring wind speed collapse were present. The minimum in wind speed – observable by the Sodar measurements through the whole vertical extension of the valley atmosphere – is the consequence of a thermally-induced valley wind system, which changes its wind direction from down to up-valley winds in the morning hours. Buoyant forces then dominate over shear forces within turbulence production. These situations are detected by the stability parameter (ratio of the measurement height to the Obukhov length) calculated from directly measured turbulent fluxes. An analysis of the scales of turbulent motions during the free convection event using wavelet transform confirms the large-eddy scale character of the detected plume-like coherent structures. Regarding the entire COPS measurement period, free convection events (FCEs) in the morning hours occur on about 50% of all days.
First multi-year occultation observations of CO2 in the MLT by ACE satellite: observations and analysis using the extended CMAM
Authors: Beagley S. R. , Boone C. D. , Fomichev V. I. , Jin J. J. , Semeniuk K. , McConnell J. C. , Bernath P. F.
Published: April 2010

Abstract. This paper presents the first multi-year global set of observations of CO2 in the mesosphere and lower thermosphere (MLT) obtained by the ACE-FTS instrument on SCISAT-I, a small Canadian satellite launched in 2003. The observations use the solar occultation technique and document the fall-off in the mixing ratio of CO2 in the MLT region. The beginning of the fall-off of the CO2, or "knee" occurs at about 78 km and lies higher than in the CRISTA measurements (~70 km) but lower than in the SABER 1.06 (~82 km) and much lower than in rocket measurements. We also present the measurements of CO obtained concurrently which provide important constraints for analysis. We have compared the ACE measurements with simulations of the CO2 and CO distributions in the vertically extended version of the Canadian Middle Atmosphere Model (CMAM). Applying standard chemistry we find that we cannot get agreement between the model and ACE CO2 observations although the CO observations are adequately reproduced. There appears to be about a 10 km offset compared to the observed ACE CO2, with the model knee occurring too high. In analysing the disagreement, we have investigated the variation of several parameters of interest, photolysis rates, formation rate for CO2, and the impact of uncertainty in eddy diffusion, in order to explore parameter space for this problem. Our conclusions are that there must be a loss process for CO2, about 2–4 times faster than photolysis that will sequester the carbon in some form other than CO and we have speculated on the role of meteoritic dust as a possible candidate. In addition, from this study we have highlighted a possible important role for vertical eddy diffusion in 3-D models in determining the distribution of candidate species in the mesosphere which requires further study.
Investigation of ship-plume chemistry using a newly-developed photochemical ship-plume model
Authors: Kim H. S. , Park R. S. , Song C. H.
Published: April 2010

Abstract. A photochemical ship-plume model, which can consider the ship-plume dynamics and ship-plume chemistry, simultaneously, was developed to gain a better understanding of atmospheric impact of ship emissions. The model performance was then evaluated by a comparison with the observation data measured on a NOAA WP-3D flight during the Intercontinental Transport and Chemical Transformation 2002 (ITCT 2K2) airborne field campaign. The simulation conditions and parameters, such as meteorological conditions, emission rates, and background gas and particulate species concentrations, were obtained directly and/or inferred indirectly from the ITCT 2K2 observation data. The model-predicted concentrations showed good agreement with the observed concentrations of five ambient species (NOx, NOy, O3, HNO3, and H2SO4) at the eight plume transects by the WP-3D flight with strong correlations around the 1:1 line (0.66≤R≤0.85). In addition, a set of tests were carried out to approximate the magnitude of the reaction probability of HNO3 onto sea-salt particles in the model-observation comparison framework. These results suggest that the reaction probability of HNO3 onto sea-salt particles may be in the order of 10−3 or smaller. The equivalent NOx lifetime throughout the "entire" plume was also estimated from ship-plume chemistry modeling. The NOx lifetimes estimated throughout the "entire ship plume" was 3.36 h. The short NOx lifetime over the entire ship plume clearly shows that the ship-plume chemistry shortens the NOx lifetime considerably. Therefore, the ship-plume chemistry model should be used to model the changes in ship-plume chemical compositions and better evaluate the atmospheric impact of ocean-going ship emissions.
Satellite NO2 observations and model simulations of tropospheric columns over South-eastern Europe
Authors: Zyrichidou I. , Koukouli M. E. , Balis D. S. , Katragkou E. , Melas D. , Poupkou A. , Kioutsioukis I. , van der A R. , Boersma F. K. , van Roozendael M. , Richter A.
Published: April 2010

Abstract. Satellite observations of nitrogen dioxide (NO2) tropospheric columns over Southeastern Europe are analyzed to study the characteristics of the spatial and temporal variability of pollution in the area. The interannual variability of the tropospheric NO2 columns is presented over urban, rural and industrial locations based on measurements from four satellite instruments, GOME/ERS-2, SCIAMACHY/Envisat, OMI/Aura and GOME-2/MetOp spanning a period of over twelve years. The consistency between the different datasets over the area is investigated. Two operational algorithms for the retrieval of tropospheric NO2 are considered, the one developed jointly by the Royal Netherlands Meteorological Institute and Belgian Institute for Space Astronomy and the one developed by the University of Bremen. The tropospheric NO2 columns for the area under study have been simulated for the period 1996–2001 with the Comprehensive Air Quality Model (CAMx) and are compared with GOME measurements. Over urban and industrial locations the mean tropospheric NO2 columns range between 3 and 7.0×1015 molecules/cm2, showing a seasonal variability with a peak to peak amplitude of about 6.0×1015 molecules/cm2, while the background values over rural sites are close to 1.1×1015 molecules/cm2. Differences in the overpass time and spatial resolution of the different satellites, as well as differences in the algorithms, introduce significant differences in the estimated columns however the correlation between the different estimates is higher than 0.8. It is found that the model simulations reveal similar spatial patterns as the GOME observations, a result which is consistent with both algorithms. Although the model simulations show a mean bias of −0.1 under clean conditions, the modeled temporal correlation of 0.5 is poor in absence of biogenic and biomass burning emissions.
Comparison of a global-climate model simulation to a cloud-system resolving model simulation for long-term thin stratocumulus clouds
Authors: Lee S. S. , Penner J. E. , Wang M.
Published: April 2010

Abstract. A case of thin, warm marine-boundary-layer (MBL) clouds is simulated by a cloud-system resolving model (CSRM) and is compared to the same case of clouds simulated by a general circulation model (GCM). In this study, the simulation by the CSRM adopts higher resolutions and more advanced microphysics as compared to those by the GCM, enabling the CSRM-simulation to act as a benchmark to assess the simulation by the GCM. Explicitly simulated interactions among the surface latent heat (LH) fluxes, buoyancy fluxes, and cloud-top entrainment lead to the deepening-warming decoupling and thereby the transition from stratiform clouds to cumulus clouds in the CSRM. However, in the simulation by the GCM, these interactions are not resolved and thus the transition to cumulus clouds is not simulated. This leads to substantial differences in cloud mass and radiation between simulations by the CSRM and the GCM. When stratocumulus clouds are dominant prior to the transition to cumulus clouds, interactions between supersaturation and cloud droplet number concentration (CDNC) (controlling condensation) and those between rain evaporation and cloud-base instability (controlling cloud dynamics and thereby condensation) determine cloud mass and thus the radiation budget in the simulation by the CSRM. These interactions result in smaller condensation and thus smaller cloud mass and reflected solar radiation by clouds in the simulation by the CSRM than in the simulation by the GCM where these interactions are not resolved. The resolved interactions (associated with condensation and the transition to cumulus clouds) lead to better agreement between the CSRM-simulation and observation than that between the GCM-simulation and observation.
Photolytic control of the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cycling
Authors: Frey M. M. , Savarino J. , Morin S. , Erbland J. , Martins J. M. F.
Published: April 2010

Abstract. The nitrogen (δ15N) and triple oxygen (δ17/18O) isotopic composition of nitrate (NO3−) was measured year-round in the atmosphere and snow pits at Dome C (DC, 75.1° S, 123.3° E), and in surface snow on a transect between DC and the coast. Snow pit profiles of δ15N (δ18O) in NO3− show significant enrichment (depletion) of >200 (<40) ‰ compared to the isotopic signal in atmospheric NO3−, whereas post-depositional fractionation in Δ17O(NO3−) is small, allowing reconstruction of past shifts in tropospheric oxidation pathways from ice cores. Assuming a Rayleigh-type process we find in the DC04 (DC07) pit fractionation factors ε of −50±10 (−71±12) ‰, 6±3 (9±2) ‰ and 1±0.2 (2±0.6) ‰, for δ15N, δ18O and Δ17O, respectively. A photolysis model reproduces ε for δ15N within the range of uncertainty at DC and for lab experiments reported by Blunier et al. (2005), suggesting that the current literature value for photolytic isotopic fractionation in snow is significantly underestimated. Depletion of oxygen stable isotopes is attributed to photolysis followed by isotopic exchange with water and hydroxyl radicals. Conversely, 15N enrichment of the NO3− fraction in the snow implies 15N depletion of emissions. Indeed, δ15N in atmospheric NO3− shows a strong decrease from background levels (4.4±6.8‰) to −35.1‰ in spring followed by recovery during summer, consistent with significant snow pack emissions of reactive nitrogen. Field and lab evidence therefore suggest that photolysis dominates fractionation and associated NO3− loss from snow in the low-accumulation regions of the East Antarctic Ice Sheet (EAIS). The Δ17O signature confirms previous coastal measurements that the peak of atmospheric NO3− in spring is of stratospheric origin. After sunrise photolysis drives then redistribution of NO3− from the snowpack photic zone to the atmosphere and a snow surface skin layer, thereby concentrating NO3− at the surface. Little NO3− is exported off the EAIS plateau, still snow emissions from as far as 600 km inland can contribute to the coastal NO3− budget.
Vehicular emission of volatile organic compounds (VOCs) from a tunnel study in Hong Kong
Authors: Ho K. F. , Lee S. C. , Ho W. K. , Blake D. R. , Cheng Y. , Li Y. S. , Fung K. , Louie P. K. K. , Park D.
Published: April 2010

Abstract. Vehicle emissions of VOCs were determined in summer and winter of 2003 at the Shing Mun Tunnel, Hong Kong. One hundred and ten VOCs were quantified in this study. The average concentration of the total measured VOCs at the inlet and outlet of the tunnel were 81 250 pptv and 117 850 pptv, respectively. Among the 110 compounds analyzed, ethene, ethyne and toluene were the most abundant species in the tunnel. The total measured VOC emission factors ranged from 67 mg veh−1 km−1 to 148 mg veh−1 km−1, with an average of 115 mg veh−1 km−1. The five most abundant VOCs observed in the tunnel were, in decreasing order, ethene, toluene, n-butane, propane and i-pentane. These five most abundant species contributed over 38% of the total measured VOCs emitted. The high propane and n-butane emissions were found to be associated with LPG-fueled taxi. And fair correlations were observed between marker species (ethene, i-pentane, n-nonane, BTEX) with fractions of gasoline-fueled or diesel-fueled vehicles. Moreover, ethene, ethyne, and propene are the key species that were abundant in the tunnel but not in gasoline vapors or LPG. In order to evaluate the ozone formation potential emissions in Hong Kong, the maximum increment reactivity is calculated. It was found that about 568 mg of O3 is induced by per vehicle per kilometer traveled. Among them, ethene, propene and toluene contribute most to the ozone-formation reactivity.
Impact of tropospheric nitrogen dioxide on the regional radiation budget
Authors: Vasilkov A. P. , Joiner J. , Oreopoulos L. , Gleason J. F. , Veefkind P. , Bucsela E. , Celarier E. A. , Spurr R. J. D. , Platnick S.
Published: April 2010

Abstract. Following the launch of several satellite ultraviolet and visible spectrometers including the Ozone Monitoring Instrument (OMI), much has been learned about the global distribution of nitrogen dioxide (NO2). NO2, which is mostly anthropogenic in origin, absorbs solar radiation at ultraviolet and visible wavelengths. We parameterized NO2 absorption for fast radiative transfer calculations. Using this parameterization with cloud, surface, and NO2 information from different sensors in the NASA A-train constellation of satellites and NO2 profiles from the Global Modeling Initiative (GMI), we compute the global distribution of net atmospheric heating due to tropospheric NO2 for January and July 2005. We assess the impact of clouds and find that because most of N02 is contained in the boundary layer in polluted regions, the cloud shielding effect can significantly reduce the net atmospheric heating due to NO2. We examine the effect of diurnal variations in NO2 emissions and chemistry on net atmospheric heating and find only a small impact of these on the daily-averaged heating. While the impact of NO2 on the global radiative forcing is small, locally it can produce instantaneous net atmospheric heating of 2–4 W/m2 in heavily polluted areas. We also examine the sensitivity of NO2 absorption to various geophysical conditions. Effects of the vertical distributions of cloud optical depth and NO2 on net atmospheric heating and downwelling radiance are simulated in detail for various scenarios including vertically-inhomogeneous convective clouds observed by CloudSat. The maximum effect of NO2 on downwelling radiance occurs when the NO2 is located in the middle part of the cloud where the optical extinction peaks.
VOC measurements within a boreal forest during spring 2005: the role of monoterpenes and sulphuric acid in selected intense nucleation events
Authors: Eerdekens G. , Yassaa N. , Sinha V. , Aalto P. P. , Fiedler V. , Aufmhoff H. , Arnold F. , Kulmala M. , Williams J.
Published: April 2010

Abstract. In this study we present measurements of selected trace gases and aerosol made in a boreal forest during the BACCI-QUEST IV intensive field campaign in Hyytiälä, Finland in April 2005. Several clear aerosol "nucleation events" were observed and characterized. One type of "event" occurred synchronously with huge increases in monoterpenes, while a second event type correlated instead with sulphuric acid. Here we elucidate the origin of these two distinct forms of aerosol production at the Hyytiälä site using the measurement data, airmass back trajectories and the optical stereoisomery of monoterpenes.
Properties of the average distribution of equatorial Kelvin waves investigated by ray tracing techniques
Authors: Ern M. , Cho H.-K. , Preusse P. , Eckermann S. D.
Published: April 2010

Abstract. Kelvin waves excited by tropospheric convection are considered to be one of the main drivers of the stratospheric quasi-biennial oscillation (QBO). In this paper we combine several measured data sets with the Gravity wave Regional Or Global RAy Tracer (GROGRAT) in order to study the forcing and vertical propagation of Kelvin waves. Launch distributions for the ray tracer at tropospheric altitudes are deduced from space-time spectra of European Centre for Medium-Range Weather Forecasts (ECMWF) operational analyses, as well as outgoing longwave radiation (OLR) and rainfall data measured by the Tropical Rainfall Measuring Mission (TRMM) satellite. The resulting stratospheric Kelvin wave spectra are compared to ECMWF operational analyses and temperature measurements of the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) satellite instrument. Questions addressed are: the relative importance of source variability versus wind modulation, the relative importance of radiative and turbulent damping versus wave breaking, and the minimum altitude where freely propagating waves dominate the spectrum.
Different characteristics of char and soot in the atmosphere and their ratio as an indicator for source identification in Xi'an, China
Authors: Han Y. M. , Cao J. J. , Lee S. C. , Ho K. F. , An Z. S.
Published: April 2010

Abstract. Elemental carbon (EC) is a collective term encompassing all thermally altered carbonaceous materials and can be subdivided into two classes: char and soot. Since the different classes of EC have different chemical and physical properties, their optical light-absorbing properties differ, so that it is essential to differentiate them in the environment. One year of observations of the daily and seasonal variations of carbonaceous particles were conducted in Xi'an, China in 2004 to demonstrate the different characteristics of char and soot in the atmosphere. Total carbon (TC), organic carbon (OC), EC and char-EC showed similar seasonal trends, with high concentrations in winter and low concentrations in summer, while soot-EC revealed relatively small seasonal variations, with maximum concentration (1.85 μg m−3) in spring and minimum concentration (1.15 μg m−3) in summer. The strong correlation between EC and char-EC (R2=0.99) indicates that previously reported total EC reflected the characteristics of char only, while overlooking that of soot. However, soot exhibits stronger light-absorbing characteristics than char, and merits greater focus. The small seasonal variation of soot-EC indicates that soot may be the background fraction in total EC, and is likely to have an even longer lifetime in the atmosphere than previously estimated for total EC, which suggests that soot has a greater contribution to global warming. Although char-EC/soot-EC ratio is similar to primary OC/EC ratio as both vary with emission sources, OC/EC ratio is affected by the secondary organic aerosol (SOA) formation. Thus char-EC/soot-EC may be a more effective indicator than OC/EC in source identification of carbonaceous aerosol. Comparison of seasonal variations of OC/EC and char-EC/soot-EC ratios in Xi'an confirms this point. However, wet scavenging by snow and rain was more effective for char than for soot and influenced the char-EC/soot-EC ratio, and this factor should be considered in source identification as well.
Global carbon tetrachloride distributions obtained from the Atmospheric Chemistry Experiment (ACE)
Authors: Allen N. D. C. , Bernath P. F. , Boone C. D. , Chipperfield M. P. , Fu D. , Manney G. L. , Toon G. C. , Weisenstein D. K.
Published: April 2010

Abstract. The first study of the global atmospheric distribution of carbon tetrachloride (CCl4), as a function of altitude and latitude, was performed using solar occultation measurements obtained by the Atmospheric Chemistry Experiment (ACE) mission using Fourier transform spectroscopy. A total of 8703 profile measurements were used in the study taken between February 2004 and August 2007. The zonal distribution of carbon tetrachloride displays a slight hemispheric asymmetry and decreasing concentration with increasing altitude at all latitudes. Maximum carbon tetrachloride concentrations are situated below 10 km in altitude with VMR (Volume Mixing Ratio) values of 100–130 ppt (parts per trillion). The highest concentrations are located about the equator and at mid-latitudes, particularly for latitudes in heavily industrialised regions (20–45° N), with values declining towards the poles. Global distributions obtained from ACE were compared with predictions from three chemistry transport models. The ACE dataset gives unique global and temporal coverage of carbon tetrachloride and its transport through the atmosphere. An estimated lifetime for carbon tetrachloride of 34±5 years was determined through correlation with CFC-11.
UV aerosol indices from SCIAMACHY: introducing the SCattering Index (SCI)
Authors: Penning de Vries M. , Beirle S. , Wagner T.
Published: April 2010

Abstract. The Absorbing Aerosol Index (AAI) is a useful tool for detecting aerosols that absorb UV radiation – especially in cases where other aerosol retrievals fail, such as over bright surfaces (e.g. desert) and in the presence of clouds. The AAI does not, however, consider contributions from "scattering" (hardly absorbing) aerosols and clouds: they cause negative AAI values and are usually discarded. In this paper, we demonstrate the use of the AAI's negative counterpart, the SCattering Index (SCI) to detect "scattering" aerosols. Maps of seasonally averaged SCI show significantly enhanced values in summer in Southeast USA and Southeast Asia, pointing to high production of "scattering" aerosols (presumably mainly sulphate aerosols and organic aerosols) in this season. The application of a cloud filter makes the presence of "scattering" aerosols even more clear. In a comparison of AOT from AERONET and our Aerosol Indices from SCIAMACHY, good agreement was found for two AERONET stations in Southeast USA, and two stations in Africa. This fact confirms the suitability of SCI as a tool to detect "scattering" aerosols. The combination of the UV Aerosol Indices AAI and SCI provides the unique possibility to characterise absorbing properties of aerosols from space. Accurate knowledge about aerosol absorption is crucial for the correct determination of the contribution of aerosols to the radiative budget.