bluuebunny/crossref_metadata_2025 huggingface dataset:
An elevated large-scale dust veil from the Taklimakan Desert: Intercontinental transport and three-dimensional structure as captured by CALIPSO and regional and global models
Authors: Yumimoto K. , Eguchi K. , Uno I. , Takemura T. , Liu Z. , Shimizu A. , Sugimoto N.
Published: April 2010

Abstract. An intense dust storm occurred during 19–20 May 2007 over the Taklimakan Desert in northwestern China. Over the following days, the space-borne lidar CALIOP tracked an optically thin, highly elevated, horizontally extensive dust veil that was transported intercontinentally over eastern Asia, the Pacific Ocean, North America, and the Atlantic Ocean. A global aerosol transport model (SPRINTARS) simulated the dust veil quite well and provided a three-dimensional view of the intercontinental dust transport. The SPRINTARS simulation revealed that the dust veil traveled at 4–10 km altitudes with a thickness of 1–4 km along the isentropic surface between 310 and 340 K. The transport speed was about 1500 km/day. The estimated dust amount exported to the Pacific was 30.8 Gg, of which 65% was deposited in the Pacific and 18% was transported to the North Atlantic. These results imply that dust veils can fertilize open oceans, add to background dust, and affect the radiative budget at high altitudes through scattering and absorption. The injection mechanism that lifts dust particles into the free atmosphere is important for understanding the formation of the dust veil and subsequent long-range transport. We used a regional dust transport model (RC4) to analyze the dust emission and injection over the source region. The RC4 analysis revealed that strong northeasterly surface winds associated with low pressures invaded the Taklimakan Desert through the eastern corridor. These winds then formed strong upslope wind along the high, steep mountainsides of the Tibetan Plateau and blew large amounts of dust into the air. The updraft lifted the dust particles farther into the upper troposphere (about 9 km above mean sea level, MSL), where westerlies are generally present. The unusual terrain surrounding the Taklimakan Desert played a key role in the injection of dust to the upper troposphere to form the dust veil.
Hydrogen soil deposition at an urban site in Finland
Authors: Lallo M. , Aalto T. , Hatakka J. , Laurila T.
Published: April 2010

Abstract. Hydrogen deposition velocities (vd) were estimated by field chamber measurements and model simulations. A closed-chamber method was used for soil deposition studies in Helsinki, Finland, at an urban park inhabited by broad-leaved trees. Radon tracer method was used to estimate the vd in nighttime when photochemical reactions were minimal and radon gas was concentrated in the shallow boundary layer due to exhalation from soil. A two-dimensional atmospheric model was used for the calculation of respective vd values and radon exhalation rates. The vd and radon exhalation rates were lower in winter than in summer according to all methods. The radon tracer method and the two-dimensional model results for hydrogen deposition velocity were in the range of 0.13 mm s−1 to 0.93 mm s−1 (radon tracer) and 0.12 mm s−1 to 0.61 mm s−1 (two-dimensional). The soil chamber results for vd were 0.00 mm s−1 to 0.70 mm s−1. Both models and chamber measurements revealed a relation between one week cumulative rain sum and deposition velocity. When precipitation events occurred a few days before the chamber measurements, lower vd values were observed. A snow cover also lowered vd.
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 conditions (FCCs) in the Kinzig valley, Black Forest, Southwest Germany. The measured high-quality turbulent flux data revealed that FCCs are initiated near the ground in situations where moderate to high buoyancy fluxes and a simultaneously occurring drop of the wind speed 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. Buoyancy then dominates over shear within the production of turbulence kinetic energy near the ground. These situations are detected by the stability parameter (ratio of the measurement height to the Obukhov length) when the level of free convection, which starts above the Obukhov length, drops below that of the sonic anemometer. An analysis of the scales of turbulent motions during FCCs using wavelet transform shows the occurrence of large-scale turbulence structures. Regarding the entire COPS measurement period, FCCs in the morning hours occur on about 50% of all days. Enhanced surface fluxes of latent and sensible heat are found on these days.
Cold oceans enhance terrestrial new-particle formation in near-coastal forests
Authors: Suni T. , Sogacheva L. , Lauros J. , Hakola H. , Bäck J. , Kurtén T. , Cleugh H. , van Gorsel E. , Briggs P. , Sevanto S. , Kulmala M.
Published: April 2010

Abstract. The world's forests produce atmospheric aerosol by emitting volatile organic compounds (VOC) which, after being oxidized in the atmosphere, readily condense on the omnipresent nanometer-sized nuclei and grow them to climatically relevant sizes. The cooling effect of aerosols is the greatest uncertainty in current climate models and estimates of radiative forcing. Therefore, identifying the environmental factors influencing the biogenic formation of aerosols is crucial. In this paper, we connected biogenic aerosol formation events observed in a Eucalypt forest in South-East Australia during July 2005–December 2006 to air mass history using 96-h back trajectories. Formation of new particles was most frequent in the dry westerly and south-westerly air masses. According to NDVI (Normalized Difference Vegetation Index) measurements, photosynthesis was not significantly higher in this direction compared to the north-east direction. It is unlikely, therefore, that differences in photosynthesis-derived organic precursor emissions would have been significant enough to lead to the clear difference in NPF frequency between these two directions. Instead, the high evaporation rates above the Pacific Ocean resulted in humid winds from the north-east that effectively suppressed new-particle formation in the forest hundreds of kilometers inland. No other factor varied as significantly in tune with new-particle formation as humidity and we concluded that, in addition to local meteorological factors in the forest, the magnitude of evaporation from oceans hundreds of kilometers upwind can effectively suppress or enhance new-particle formation. Our findings indicate that, unlike warm waters, the cold polar oceans provide excellent clean and dry background air that enhances aerosol formation above near-coastal forests in Fennoscandia and South-East Australia.
Quantification of the impact of climate uncertainty on regional air quality
Authors: Liao K.-J. , Tagaris E. , Manomaiphiboon K. , Wang C. , Woo J.-H. , Amar P. , He S. , Russell A. G.
Published: April 2010

Abstract. Uncertainties in calculated impacts of climate forecasts on future regional air quality are investigated using downscaled MM5 meteorological fields from the NASA GISS and MIT IGSM global models and the CMAQ model in 2050 in the continental US. Differences between three future scenarios: high-extreme, low-extreme and base case, are used for quantifying effects of climate uncertainty on regional air quality. GISS, with the IPCC A1B scenario, is used for the base case simulations. IGSM results, in the form of probabilistic distributions, are used to perturb the base case climate to provide the high- and low-extreme scenarios. Impacts of the extreme climate scenarios on concentrations of summertime fourth-highest daily maximum 8-h average ozone are predicted to be up to 10 ppbV (about one-seventh of the current US ozone standard of 75 ppbV) in urban areas of the Northeast, Midwest and Texas due to impacts of meteorological changes, especially temperature and humidity, on the photochemistry of tropospheric ozone formation and increases in biogenic VOC emissions, though the differences in average peak ozone concentrations are about 1–2 ppbV on a regional basis. Differences between the extreme and base scenarios in annualized PM2.5 levels are very location dependent and predicted to range between −1.0 and +1.5 μg m−3. Future annualized PM2.5 is less sensitive to the extreme climate scenarios than summertime peak ozone since precipitation scavenging is only slightly affected by the extreme climate scenarios examined. Relative abundances of biogenic VOC and anthropogenic NOx lead to the areas that are most responsive to climate change. Overall, planned controls for decreasing regional ozone and PM2.5 levels will continue to be effective in the future under the extreme climate scenarios. However, the impact of climate uncertainties may be substantial in some urban areas and should be included in assessing future regional air quality and emission control requirements.
The comprehensive model system COSMO-ART – Radiative impact of aerosol on the state of the atmosphere on the regional scale
Authors: Vogel B. , Vogel H. , Bäumer D. , Bangert M. , Lundgren K. , Rinke R. , Stanelle T.
Published: April 2010

Abstract. A new fully online coupled model system developed for the evaluation of the interaction of aerosol particles with the atmosphere on the regional scale is described. The model system is based on the operational weather forecast model of the Deutscher Wetterdienst. Physical processes like transport, turbulent diffusion, and dry and wet deposition are treated together with photochemistry and aerosol dynamics using the modal approach. Based on detailed calculations we have developed parameterisations to examine the impact of aerosol particles on photolysis and on radiation. Currently the model allows feedback between natural and anthropogenic aerosol particles and the atmospheric variables that are initialized by the modification of the radiative fluxes. The model system is applied to two summer episodes, each lasting five days, with a model domain covering Western Europe and adjacent regions. The first episode is characterised by almost cloud free conditions and the second one by cloudy conditions. The simulated aerosol concentrations are compared to observations made at 700 stations distributed over Western Europe. For each episode two model runs are performed; one where the feedback between the aerosol particles and the atmosphere is taken into account and a second one where the feedback is neglected. Comparing these two sets of model runs, the radiative feedback on temperature and other variables is evaluated. In the cloud free case a clear correlation between the aerosol optical depth and changes in global radiation and temperature is found. In the case of cloudy conditions the pure radiative effects are superposed by changes in the liquid water content of the clouds due to changes in the thermodynamics of the atmosphere. In this case the correlation between the aerosol optical depth and its effects on temperature is low. However, on average a decrease in the 2 m temperature is still found. For the area of Germany we found on average for both cases a reduction in the global radiation of about 6 W m2, a decrease of the 2 m temperature of 0.1 K, and a reduction in the daily temperature range of −0.13 K.
Explicit calculation of indirect global warming potentials for halons using atmospheric models
Authors: Youn D. , Patten K. O. , Lin J.-T. , Wuebbles D. J.
Published: April 2010

Abstract. The concept of Global Warming Potentials (GWPs) has been extensively used in policy consideration as a relative index for comparing the climate impact of an emitted greenhouse gas (GHG), relative to carbon dioxide with equal mass emissions. Ozone depletion due to emission of chlorinated or brominated halocarbons leads to cooling of the climate system in the opposite direction to the direct warming contribution by halocarbons as GHGs. This cooling is a key indirect effect of the halocarbons on climatic radiative forcing, which is accounted for by indirect GWPs. With respect to climate, it is critical to understand net influences considering direct warming and indirect cooling effects especially for Halons due to the greater ozone-depleting efficiency of bromine over chlorine. Until now, the indirect GWPs have been calculated using a parameterized approach based on the concept of Equivalent Effective Stratospheric Chlorine (EESC) and the observed ozone depletion over the last few decades. As a step towards obtaining indirect GWPs through a more robust approach, we use atmospheric models to explicitly calculate the indirect GWPs of Halon-1211 and Halon-1301 for a 100-year time horizon. State-of-the-art global chemistry-transport models (CTMs) were used as the computational tools to derive more realistic ozone depletion changes caused by an added pulse emission of the two major Halons at the surface. The radiative forcings on climate from the ozone changes have been calculated for indirect GWPs using an atmospheric radiative transfer model (RTM). The simulated temporal variations of global average total column Halons after a pulse perturbation follow an exponential decay with an e-folding time which is consistent with the expected chemical lifetimes of the Halons. Our calculated indirect GWPs for the two Halons are much smaller than those from past studies but are within a single standard deviation of WMO (2007) values and the direct GWP values derived agree with the published values. Our model-based assessment of the Halon indirect GWPs thus confirms the significant importance of indirect effects on climate.
Can gravity waves significantly impact PSC occurrence in the Antarctic?
Authors: McDonald A. J. , George S. E. , Woollands R. M.
Published: April 2010

Abstract. A combination of POAM III aerosol extinction and CHAMP RO temperature measurements are used to examine the role of atmospheric gravity waves in the formation of Antarctic Polar Stratospheric Clouds (PSCs). POAM III aerosol extinction observations and quality flag information are used to identify Polar Stratospheric Clouds using an unsupervised clustering algorithm. A PSC proxy, derived by thresholding Met Office temperature analyses with the PSC Type Ia formation temperature (TNAT), shows general agreement with the results of the POAM III analysis. However, in June the POAM III observations of PSC are more abundant than expected from temperature threshold crossings in five out of the eight years examined. In addition, September and October PSC identified using temperature thresholding is often significantly higher than that derived from POAM III; this observation probably being due to dehydration and denitrification. Comparison of the Met Office temperature analyses with corresponding CHAMP observations also suggests a small warm bias in the Met Office data in June. However, this bias cannot fully explain the differences observed. Analysis of CHAMP data indicates that temperature perturbations associated with gravity waves may partially explain the enhanced PSC incidence observed in June (relative to the Met Office analyses). For this month, approximately 40% of the temperature threshold crossings observed using CHAMP RO data are associated with small-scale perturbations. Examination of the distribution of temperatures relative to TNAT shows a large proportion of June data to be close to this threshold, potentially enhancing the importance of gravity wave induced temperature perturbations. Inspection of the longitudinal structure of PSC occurrence in June 2005 also shows that regions of enhancement are geographically associated with the Antarctic Peninsula; a known mountain wave "hotspot". The latitudinal variation of POAM III observations means that we only observe this region in June–July, and thus the true pattern of enhanced PSC production may continue operating into later months. The analysis has shown that early in the Antarctic winter stratospheric background temperatures are close to the TNAT threshold (and PSC formation), and are thus sensitive to temperature perturbations associated with mountain wave activity near the Antarctic peninsula (40% of PSC formation). Later in the season, and at latitudes away from the peninsula, temperature perturbations associated with gravity waves contribute to about 15% of the observed PSC (a value which corresponds well to several previous studies). This lower value is likely to be due to colder background temperatures already achieving the TNAT threshold unaided. Additionally, there is a reduction in the magnitude of gravity waves perturbations observed as POAM III samples poleward of the peninsula.
An intensive study of aerosol optical properties in Beijing urban area
Authors: He X. , Li C. C. , Lau A. K. H. , Deng Z. Z. , Mao J. T. , Wang M. H. , Liu X. Y.
Published: April 2010

Abstract. In order to quantify the aerosol impact on climate, a range of aerosol parameters are required. In this paper, two-year of ground-based observations of aerosol optical properties from an urban site in Beijing of China are assessed. The aerosol absorption coefficient (σa), scattering coefficient (σs), as well as single scattering albedo (ω) are analyzed to aid in characterizing Beijing's urban aerosol. Two-year averages (and standard deviations) for σa at 532 nm, σs at 525 nm and ω at 525 nm are 56±49 Mm−1, 288±281 Mm−1 and 0.80±0.09, respectively. Meanwhile, there is a distinct diurnal variation for σa, with its minimum occurring at approximately 14:00 to 15:00 and maximum at midnight. σs peaks in the late morning and the minimum occurs in the evening. σs in summer is higher than that in winter. ω is also higher in summer than that in winter, except before 07:00 a.m., and peaks in the early afternoon. Both σa and σs show strong dependence on local wind in all four seasons. When the wind blows from the north with low speed (0–2 m/s), the values of σa are high, and in contrast, very low with wind speeds higher than 4 m/s. When the wind blows from south with low speed (0–4 m/s), σa is intermediate. The patterns of the wind dependence of σa indicates that σa is mainly dominated by local emissions. σs displays a similar dependence on wind speed and direction to σa, except in summer. In summer, the σs value is highest when wind is from southeast with speed of 0–6 m/s. This indicates that the particle pollution resulting from regional transport is only significant in the summer season. ω also shows wind dependence to some extent though not as strong as σa or σs. Overall, the wind dependence results provide valuable information about the locations of aerosol pollution sources and suggest that the air pollution in summer is a regional problem but in other seasons it is mainly affected by local urban emissions.
Sensitivity studies of different aerosol indirect effects in mixed-phase clouds
Authors: Lohmann U. , Hoose C.
Published: April 2010

Abstract. Aerosols affect the climate system by changing cloud characteristics. Using the global climate model ECHAM5-HAM, we investigate different aerosol effects on mixed-phase clouds: The glaciation effect, which refers to a more frequent glaciation due to anthropogenic aerosols, versus the de-activation effect, which suggests that ice nuclei become less effective because of an anthropogenic sulfate coating. The glaciation effect can partly offset the indirect aerosol effect on warm clouds and thus causes the total anthropogenic aerosol effect to be smaller. It is investigated by varying the parameterization for the Bergeron-Findeisen process and the threshold coating thickness of sulfate (SO4-crit), which is required to convert an externally mixed aerosol particle into an internally mixed particle. Differences in the net radiation at the top-of-the-atmosphere due to anthropogenic aerosols between the different sensitivity studies amount up to 0.5 W m−2. This suggests that the investigated mixed-phase processes have a major effect on the total anthropogenic aerosol effect.
Northern winter stratospheric temperature and ozone responses to ENSO inferred from an ensemble of Chemistry Climate Models
Authors: Cagnazzo C. , Manzini E. , Calvo N. , Douglass A. , Akiyoshi H. , Bekki S. , Chipperfield M. , Dameris M. , Deushi M. , Fischer A. M. , Garny H. , Gettelman A. , Giorgetta M. A. , Plummer D. , Rozanov E. , Shepherd T. G. , Shibata K. , Stenke A. , Struthers H. , Tian W.
Published: April 2010

Abstract. The connection between the El Niño Southern Oscillation (ENSO) and the Northern polar stratosphere has been established from observations and atmospheric modeling. Here a systematic inter-comparison of the sensitivity of the modeled stratosphere to ENSO in Chemistry Climate Models (CCMs) is reported. This work uses results from a number of the CCMs included in the 2006 ozone assessment. In the lower stratosphere, the mean of all model simulations reports a warming of the polar vortex during strong ENSO events in February–March, consistent with but smaller than the estimate from satellite observations and ERA40 reanalysis. The anomalous warming is associated with an anomalous dynamical increase of column ozone north of 70° N that is accompanied by coherent column ozone decrease in the Tropics, in agreement with that deduced from the NIWA column ozone database, implying an increased residual circulation in the mean of all model simulations during ENSO. The spread in the model responses is partly due to the large internal stratospheric variability and it is shown that it crucially depends on the representation of the tropospheric ENSO teleconnection in the models.
Reduction in biomass burning aerosol light absorption upon humidification: roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer
Authors: Lewis K. A. , Arnott W. P. , Moosmüller H. , Chakrabarty R. K. , Carrico C. M. , Kreidenweis S. M. , Day D. E. , Malm W. C. , Laskin A. , Jimenez J. L. , Ulbrich I. M. , Huffman J. A. , Onasch T. B. , Trimborn A. , Liu L. , Mishchenko M. I.
Published: April 2010

Abstract. Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used were Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients revealed a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: (1) shielding of inner monomers after particle consolidation or collapse with water uptake; (2) the lower case contribution of mass transfer through evaporation and condensation at high relative humidity (RH) to the usual heat transfer pathway for energy release by laser-heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.
Global temperature estimates in the troposphere and stratosphere: a validation study of COSMIC/FORMOSAT-3 measurements
Authors: Kishore P. , Namboothiri S. P. , Jiang J. H. , Sivakumar V. , Igarashi K.
Published: April 2010

Abstract. This paper mainly focuses on the validation of temperature estimates derived with the newly launched Constellation Observing System for Meteorology Ionosphere and Climate (COSMIC)/Formosa Satellite 3 (FORMOSAT-3) system. The analysis is based on the radio occultation (RO) data samples collected during the first year observation from April 2006 to April 2007. For the validation, we have used the operational stratospheric analyses including the National Centers for Environmental Prediction - Reanalysis (NCEP), the Japanese 25-year Reanalysis (JRA-25), and the United Kingdom Met Office (MetO) data sets. Comparisons done in different formats reveal good agreement between the COSMIC and reanalysis outputs. Spatially, the largest deviations are noted in the polar latitudes, and height-wise, the tropical tropopause region noted the maximum differences (2–4 K). We found that among the three reanalysis data sets the NCEP data sets have the best resemblance with the COSMIC measurements.
Initial fate of fine ash and sulfur from large volcanic eruptions
Authors: Niemeier U. , Timmreck C. , Graf H.-F. , Kinne S. , Rast S. , Self S.
Published: April 2010

Abstract. Large volcanic eruptions emit huge amounts of sulfur and fine ash into the stratosphere. These products cause an impact on radiative processes, temperature and wind patterns. In simulations with a General Circulation Model including detailed aerosol microphysics, the relation between the impact of sulfur and fine ash is determined for different eruption strengths and locations, one in the tropics and one in high Northern latitudes. Fine ash with effective radii between 1 μm and 15 μm has a lifetime of several days only. Nevertheless, the strong absorption of shortwave and long-wave radiation causes additional heating and cooling of ±20 K/day and impacts the evolution of the volcanic cloud. Depending on the location of the volcanic eruption, transport direction changes due to the presence of fine ash, vortices develop and temperature anomalies at ground increase. The results show substantial impact on the local scale but only minor impact on the evolution of sulfate in the stratosphere in the month after the simulated eruptions.
Exploring the relation between aerosol optical depth and PM2.5 at Cabauw, the Netherlands
Authors: Schaap M. , Apituley A. , Timmermans R. M. A. , Koelemeijer R. B. A. , de Leeuw G.
Published: April 2010

Abstract. Estimates of PM2.5 distributions based on satellite data depend critically on an established relation between AOD and ground level PM2.5. In this study we performed an experiment at Cabauw to establish a relation between AOD and PM2.5 for the Netherlands. A first inspection of the AERONET L1.5 AOD and PM2.5 data showed a low correlation between the two properties. The AERONET L1.5 showed relatively many observations of high AOD values paired to low PM2.5 values, which hinted cloud contamination. Various methods were used to detect cloud contamination in the AERONET data to substantiate this hypothesis. A cloud screening method based on backscatter LIDAR observations was chosen to detect cloud contaminated observations in the AERONET L1.5 AOD. A later evaluation of AERONET L2.0 showed that the most data that are excluded in the update from L1.5 to L2.0 were also excluded by our cloud screening, which provides confidence in both our cloud-screening method as well as the final screening in the AERONET procedure. The use of LIDAR measurements in conjunction with the CIMEL AOD data is regarded highly beneficial. Contra-intuitively, the AOD to PM2.5 relationship was shown to be insensitive to inclusion of the mixed layer height. The robustness of the relation improves dependent on the time window during the day towards noon. The final relation found for Cabauw is PM2.5=124.5×AOD−0.34 and is valid for fair weather conditions. The relationship found between bias corrected MODIS AOD and PM2.5 at Cabauw is very similar to the analysis based on the much larger dataset from ground based data only. We applied the relationship to a MODIS composite map to assess the PM2.5 distribution over the Netherlands for the first time. The verification of the derived map is difficult because ground level artefact free PM2.5 data are lacking. The validity and utility of our proposed mapping methodology should be further investigated.
Increase of upper troposphere/lower stratosphere wave baroclinicity during the second half of the 20th century
Authors: Castanheira J. M. , Añel J. A. , Marques C. A. F. , Antuña J. C. , Liberato M. L. R. , de la Torre L. , Gimeno L.
Published: April 2010

Abstract. A strengthening of the equatorward temperature gradient in the upper troposphere/lower stratosphere (UTLS), at subtropics and midlatitudes, is consistently reproduced in several modelling studies of the atmospheric response to the increase of greenhouse gas radiative forcing. Some of those studies suggest an increase of the baroclinicity in the UTLS region because of the enhanced meridional temperature gradient. This study presents observational evidence of an increase of the baroclinic wave components of UTLS circulation (UTLS wave baroclinicity), during the second half of the 20th century. The evidence is given by significant positive trends in the energy of baroclinic normal modes of the NCEP/NCAR reanalysis, and significant positive trends in the UTLS eddy available potential energy of the NCEP/NCAR, ERA-40, NCEP-2 and JRA-25 reanalyses. Significant positive trends in the frequency of double tropopause events in radiosonde data are also interpreted as a manifestation of an increase of the UTLS wave baroclinicity.
A novel downscaling technique for the linkage of global and regional air quality modeling
Authors: Lam Y. F. , Fu J. S.
Published: April 2010

Abstract. Recently, downscaling global atmospheric model outputs (GCTM) for the USEPA Community Multiscale Air Quality (CMAQ) Initial (IC) and Boundary Conditions (BC) have become practical because of the rapid growth of computational technologies that allow global simulations to be completed within a reasonable time. The traditional method of generating IC/BC by profile data has lost its advocates due to the weakness of the limited horizontal and vertical variations found on the gridded boundary layers. Theoretically, high quality GCTM IC/BC should yield a better result in CMAQ. Unfortunately, several researchers have found that the outputs from GCTM IC/BC are not necessarily better than profile IC/BC due to the excessive transport of O3 aloft in GCTM IC/BC. In this paper, we intend to investigate the effects of using profile IC/BC and global atmospheric model data. In addition, we are suggesting a novel approach to resolve the existing issue in downscaling. In the study, we utilized the GEOS-Chem model outputs to generate time-varied and layer-varied IC/BC for year 2002 with the implementation of tropopause determining algorithm in the downscaling process (i.e., based on chemical (O3) tropopause definition). The comparison between the implemented tropopause approach and the profile IC/BC approach is performed to demonstrate improvement of considering tropopause. It is observed that without using tropopause information in the downscaling process, unrealistic O3 concentrations are created at the upper layers of IC/BC. This phenomenon has caused over-prediction of surface O3 in CMAQ. In addition, the amount of over-prediction is greatly affected by temperature and latitudinal location of the study domain. With the implementation of the algorithm, we have successfully resolved the incompatibility issues in the vertical layer structure between global and regional chemistry models to yield better surface O3 predictions than profile IC/BC for both summer and winter conditions. At the same time, it improved the vertical O3 distribution of CMAQ outputs. It is strongly recommended that the tropopause information should be incorporated into any two-way coupled global and regional models, where the tropospheric regional model is used, to solve the vertical incompatibility that exists between global and regional models.
Constraining the concentration of the hydroxyl radical in a stratocumulus-topped marine boundary layer from sea-to-air eddy covariance flux measurements of dimethylsulfide
Authors: Yang M. , Blomquist B. W. , Huebert B. J.
Published: April 2010

Abstract. The hydroxyl radical (OH) is an important oxidant in the troposphere due to its high reactivity and relative abundance. Measuring the concentration of OH in situ, however, is technically challenging. Here we present a simple method of estimating an OH-equivalent oxidant concentration ("effective OH") in the marine boundary layer (MBL) from the mass balance of dimethylsulfide (DMS). We use shipboard eddy covariance measurements of the sea-to-air DMS flux from the Vamos Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) in October and November of 2008. The persistent stratocumulus cloud-cover off the west coast of South America and the associated strong inversion between MBL and the free troposphere (FT) greatly simplify the dynamics in this region and make our budget estimate possible. From the observed diurnal cycle in DMS concentration, the nighttime entrainment velocity at the inversion is estimated to be 4 mm s−1. We calculate 1.4(±0.2)×106 OH molecules cm−3 from the DMS budget, which represents a monthly effective concentration and is well within the range of previous estimates. Furthermore, when linearly proportioned according to the intensity of solar flux, the resultant diel OH profile, together with DMS surface and entrainment fluxes, enables us to accurately replicate the observed diurnal cycle in DMS (correlation coefficient over 0.9). The nitrate radical (NO3) is found to have little contribution to DMS oxidation during VOCALS-REx. An upper limit estimate of 1 pptv of bromine oxide radical (BrO) would account for 30% of DMS oxidation and lower the OH concentration to 1.0)×106 OH molecules cm−3. Our effective OH estimate includes the oxidation of DMS by such radicals.
Wildfire smoke in the Siberian Arctic in summer: source characterization and plume evolution from airborne measurements
Authors: Paris J.-D. , Stohl A. , Nédélec P. , Arshinov M. Yu. , Panchenko M. V. , Shmargunov V. P. , Law K. S. , Belan B. D. , Ciais P.
Published: April 2010

Abstract. We present airborne measurements of carbon dioxide (CO2), carbon monoxide (CO), ozone (O3), equivalent black carbon (EBC) and ultra fine particles over North-Eastern Siberia in July 2008 performed during the YAK-AEROSIB/POLARCAT experiment. During a "golden day" (11 July 2008) a number of biomass burning plumes were encountered with CO mixing ratio enhancements of up to 500 ppb relative to a background of 90 ppb. Number concentrations of aerosols in the size range 3.5–200 nm peaked at 4000 cm−3 and the EBC content reached 1.4 μg m−3. These high concentrations were caused by forest fires in the vicinity of the landing airport in Yakutsk where measurements in fresh smoke could be made during the descent. We estimate a combustion efficiency of 90 ± 3% based on CO and CO2 measurements and a CO emission factor of 65.5 ± 10.8 g CO per kilogram of dry matter burned. This suggests a potential increase in the average northern hemispheric CO mixing ratio of 3.0–7.2 ppb per million hectares of Siberian forest burned. For BC, we estimate an emission factor of 0.52 ± 0.07 g BC kg−1, comparable to values reported in the literature. The emission ratio of ultra-fine particles (3.5–200 nm) was 26 cm−3 (ppb CO)−1, consistent with other airborne studies. The transport of identified biomass burning plumes was investigated using the FLEXPART Lagrangian model. Based on sampling of wildfire plumes from the same source but with different atmospheric ages derived from FLEXPART, we estimate that the e-folding lifetimes of EBC and ultra fine particles (between 3.5 and 200 nm in size) against removal and growth processes are 5.1 and 5.5 days respectively, supporting lifetime estimates used in various modelling studies.
Evidence of ice crystals at cloud top of Arctic boundary-layer mixed-phase clouds derived from airborne remote sensing
Authors: Ehrlich A. , Wendisch M. , Bierwirth E. , Gayet J.-F. , Mioche G. , Lampert A. , Mayer B.
Published: April 2010

Abstract. The vertical distribution of ice crystals in Arctic boundary-layer mixed-phase (ABM) clouds was investigated by airborne remote-sensing and in situ measurements during the Arctic Study of Tropospheric Aerosol, Clouds and Radiation (ASTAR) campaign in March and April 2007. Information on the spectral absorption of solar radiation by ice and liquid water cloud particles is derived from airborne measurements of solar spectral radiation reflected by these clouds. It is shown by calculation of the vertical weighting function of the measurements that the observed absorption of solar radiation is dominated by the upper cloud layers (50% within 200 m from cloud top). This vertical weighting function is shifted even closer to cloud top for wavelengths where absorption by ice dominates. On this basis an indicator of the vertical distribution of ice crystals in ABM clouds is designed. Applying in situ measured microphysical properties, the cloud-top reflectivity was calculated by radiative transfer simulations and compared to the measurements. It is found that ice crystals near cloud top (mixed-phase cloud top layer) are necessary to reproduce the measurements at wavelengths where absorption by ice dominates. The observation of backscatter glories on the cloud top generally indicating liquid water droplets does not contradict the postulated presence of ice crystals. Radiative transfer simulations reproduce the observed glories even if the cloud top layer is of mixed-phase character.
Ground-based FTIR and MAX-DOAS observations of formaldehyde at Réunion Island and comparisons with satellite and model data
Authors: Vigouroux C. , Hendrick F. , Stavrakou T. , Dils B. , De Smedt I. , Hermans C. , Merlaud A. , Scolas F. , Senten C. , Vanhaelewyn G. , Fally S. , Carleer M. , Metzger J.-M. , Müller J.-F. , Van Roozendael M. , De Mazière M.
Published: April 2010

Abstract. Formaldehyde (HCHO) columns have been retrieved from ground-based Fourier transform infrared (FTIR) campaign measurements in 2004 and 2007 and from UV-Visible MAX-DOAS measurements in 2004–2005 at the NDACC site of Réunion Island (21° S, 55° E). The FTIR and MAX-DOAS daily mean formaldehyde total columns are intercompared in their common measurement period, from August to October 2004. The ground-based data are also compared to correlative SCIAMACHY data. The comparisons account for the vertical sensitivity differences of the data sets, by including their respective averaging kernels. Complete error budgets are also presented. The FTIR and MAX-DOAS daily mean total columns agree very well: no significant bias is observed and the standard deviation of the comparisons is only 8%. Both FTIR and MAX-DOAS HCHO total columns are in good agreement with SCIAMACHY values in the 2004–2005 period, with standard deviations of 21% and 31%, respectively. The same seasonal cycle is observed by the different instruments, with a minimum in austral winter and a maximum in February–March. The FTIR and MAX-DOAS data are confronted with HCHO columns calculated by a global CTM, the IMAGES model. The model underestimates the HCHO columns by 23–29% in comparison with FTIR, and by 15% in comparison with DOAS. This bias might have multiple causes, including an underestimation of OH concentrations in the model (as indicated by a sensitivity study using prescribed OH fields) and/or an underestimated contribution of large-scale transport of HCHO precursors from Madagascar. The latter hypothesis is comforted by the large observed day-to-day variability of HCHO columns, and by the observation that the peak values of FTIR columns can often be associated with free tropospheric transport patterns from source regions over Madagascar to Réunion Island, according to simulations performed with the Lagrangian particle dispersion model FLEXPART.
BrO measurements over the Eastern North-Atlantic
Authors: Martin M. , Pöhler D. , Seitz K. , Sinreich R. , Platt U.
Published: April 2010

Abstract. The aim of the work presented here was to detect BrO in the marine boundary layer over the Eastern North-Atlantic by Multi AXis-Differential Optical Absorption Spectroscopy (MAX-DOAS) of scattered sunlight. With this technique, information about the concentration and the vertical profile of trace gases in the atmosphere can be gained. BrO can be formed in the marine atmosphere by degradation of biogenic organohalogens or by oxidation of bromide in sea salt aerosol. BrO influences the chemistry in marine air in many ways, e.g. since it catalytically destroys ozone, changes the NO2/NO-ratio as well as the OH/HO2-ratio and oxidises DMS. However, the abundance and the significance of BrO in the marine atmosphere is not yet fully understood. We report on data collected during a ship cruise, which took place along the West African Coast in February 2007, within the framework of the Surface Ocean PRocesses in the ANthropocene project (SOPRAN). Tropospheric BrO could be detected during this cruise at peak mixing ratios of (10.2±3.7) ppt at an assumed layer height of 1 km on 18 February 2007. Furthermore, it was found that the mean BrO concentrations increased when cruising close to the African Coast suggesting that at least part of the BrO might have originated from there.
UV Aerosol Indices from SCIAMACHY: introducing the SCattering Index (SCI)
Authors: Penning de Vries M. J. 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 disregarded. In this paper, we demonstrate the use of the AAI's negative counterpart, the SCattering Index (SCI) to detect scattering aerosols. Consideration of the full UV Aerosol Index scale is of importance if the Aerosol Index is to be used for the quantification of aerosol absorption in the future. Maps of seasonally averaged SCI show significantly enhanced values in summer in Southeast USA and Southeast Asia, pointing to a high production of scattering aerosols (presumably mainly sulphate aerosols and secondary organic aerosols) in this season. The application of a cloud filter makes the presence of scattering aerosols even more clear. Radiative transfer calculations were performed to investigate the sensitivity of AAI and SCI to cloud parameters, and it is demonstrated that clouds cause significant SCI, in some special cases even small AAI values. The results from cloud modelling imply that cloud effects need to be taken into account when AAI and SCI are used in a quantitative manner. The paper concludes with a comparison of aerosol parameters from AERONET and our Aerosol Indices (AAI and SCI) from SCIAMACHY, where reasonable agreement was found for six AERONET stations in Southeast USA, Southeast Asia, and Africa. These findings corroborate the suitability of SCI as a tool to detect scattering aerosols.
On the representativeness of coastal aerosol studies to open ocean studies: Mace Head – a case study
Authors: Rinaldi M. , Facchini M. C. , Decesari S. , Carbone C. , Finessi E. , Mircea M. , Fuzzi S. , Ceburnis D. , Ehn M. , Kulmala M. , de Leeuw G. , O'Dowd C. D.
Published: April 2010

Abstract. A unique opportunity arose during the MAP project to compare open ocean aerosol measurements with those undertaken at the Mace Head Global Atmosphere Watch Station, a station used for decades for aerosol process research and long-term monitoring. The objective of the present study is to demonstrate that the key aerosol features and processes observed at Mace Head are characteristic of the open ocean, while acknowledging and allowing for spatial and temporal gradients. Measurements were conducted for a 5-week period at Mace Head and offshore, on the Research Vessel Celtic Explorer, in generally similar marine air masses, albeit not in connected-flow scenarios. The results of the study indicate, in terms of aerosol number size distribution, higher nucleation mode particle concentrations at Mace Head than offshore, pointing to a strong coastal source of new particles that is not representative of the open ocean. The Aitken mode exhibited a large degree of similarity, with no systematic differences between Mace Head and the open ocean, while the accumulation mode showed averagely 35% higher concentrations at Mace Head. The higher accumulation mode concentration can be attributed equally to cloud processing and to a coastal enhancement in concentration. Chemical analysis showed similar or even higher offshore concentrations for dominant species, such as nss-SO4-2, WSOC, WIOC and MSA. Sea salt concentration differences determined a 40% higher supermicron mass at Mace Head, although this difference can be attributed to a higher wind speed at Mace Head during the comparison period. Moreover, the relative chemical composition as a function of size illustrated remarkable similarity. While differences to varying degrees were observed between offshore and coastal measurements, no convincing evidence was found of local coastal effects, apart from nucleation mode aerosol, thus confirming the integrity of previously reported marine aerosol characterisation studies at Mace Head.
Hydration and dehydration at the tropical tropopause
Authors: Schiller C. , Grooß J.-U. , Konopka P. , Plöger F. , Silva dos Santos F. H. , Spelten N.
Published: April 2010

Abstract. High-resolution water measurements from three tropical airborne missions in Northern Australia, Southern Brazil and West Africa in different seasons are analysed to study the transport and transformation of water in the tropical tropopause layer (TTL) and its impact on the stratosphere. The mean profiles are quite different according to the season and location of the campaigns, with lowest mixing ratios below 2 ppmv at the cold point tropopause during the Australian mission in November/December and high TTL mixing ratios during the African measurements in August. We present backward trajectory calculations considering freeze-drying of the air to the minimum saturation mixing ratio and initialised with climatological satellite data. This trajectory-based reconstruction of water agrees well with the observed H2O average profiles and therefore demonstrates that the water vapour set point in the TTL is primarily determined by the Lagrangian saturation history. Deep convection was found to moisten the TTL, in several events even above the cold point up to 420 K potential temperatures. However, our study does not provide evidence for a larger impact of these highly-localised events on global scales.
Thermodynamics of homogeneous nucleation of ice particles in the polar summer mesosphere
Authors: Zasetsky A. Y. , Petelina S. V. , Svishchev I. M.
Published: April 2010

Abstract. We present the hypothesis of homogeneous nucleation of ice nano-particles in the polar summer mesosphere. The nucleation of condensed phase is traced back to the first step on the formation pathway, which is assumed to be the transition of water vapor to amorphous cluster. Amorphous clusters then freeze into water ice, likely metastable cubic ice, when they reach the critical size. The estimates based on the equilibrium thermodynamics give the critical size (radius) of amorphous water clusters as about 1.0 nm. The same estimates for the final transition step, that is the transformation of cubic to hexagonal ice, give the critical size of about 15 nm at typical upper mesospheric conditions during the polar summer (temperature T=150 K, water vapor density ρvapor=109 cm−3).