bluuebunny/crossref_metadata_2025 huggingface dataset:
Technical note: analytical estimation of the optimal parameters for the EOF retrievals of the IASI Level 2 Product Processing Facility and its application using AIRS and ECMWF data
Authors: Calbet X. , Schlüssel P.
Published: April 2010

Abstract. The Empirical Orthogonal Function (EOF) retrieval technique consists of calculating the eigenvectors of the spectra to later perform a linear regression between these and the atmospheric states, this first step is known as training. At a later stage, known as performing the retrievals, atmospheric profiles are derived from measured atmospheric radiances. When EOF retrievals are trained with a statistically different data set than the one used for retrievals two basic problems arise: significant biases appear in the retrievals and differences between the covariances of the training data set and the measured data set degrade them. The retrieved profiles will show a bias with respect to the real profiles which comes from the combined effect of the mean difference between the training and the real spectra projected into the atmospheric state space and the mean difference between the training and the atmospheric profiles. The standard deviations of the difference between the retrieved profiles and the real ones show different behavior depending on whether the covariance of the training spectra is bigger, equal or smaller than the covariance of the measured spectra with which the retrievals are performed. The procedure to correct for these effects is shown both analytically and with a measured example. It consists of first calculating the average and standard deviation of the difference between real observed spectra and the calculated spectra obtained from the real atmospheric state and the radiative transfer model used to create the training spectra. In a later step, measured spectra must be bias corrected with this average before performing the retrievals and the linear regression of the training must be performed adding noise to the spectra corresponding to the aforementioned calculated standard deviation. This procedure is optimal in the sense that to improve the retrievals one must resort to using a different training data set or a different algorithm.
Large-scale atmospheric circulation biases and changes in global climate model simulations and their importance for climate change in Central Europe
Authors: van Ulden A. P. , van Oldenborgh G. J.
Published: April 2010

Abstract. The quality of global sea level pressure patterns has been assessed for simulations by 23 coupled climate models. Most models showed high pattern correlations. With respect to the explained spatial variance, many models showed serious large-scale deficiencies, especially at mid-latitudes. Five models performed well at all latitudes and for each month of the year. Three models had a reasonable skill. We selected the five models with the best pressure patterns for a more detailed assessment of their simulations of the climate in Central Europe. We analysed observations and simulations of monthly mean geostrophic flow indices and of monthly mean temperature and precipitation. We used three geostrophic flow indices: the west component and south component of the geostrophic wind at the surface and the geostrophic vorticity. We found that circulation biases were important, and affected precipitation in particular. Apart from these circulation biases, the models showed other biases in temperature and precipitation, which were for some models larger than the circulation induced biases. For the 21st century the five models simulated quite different changes in circulation, precipitation and temperature. Precipitation changes appear to be primarily caused by circulation changes. Since the models show widely different circulation changes, especially in late summer, precipitation changes vary widely between the models as well. Some models simulate severe drying in late summer, while one model simulates significant precipitation increases in late summer. With respect to the mean temperature the circulation changes were important, but not dominant. However, changes in the distribution of monthly mean temperatures, do show large indirect influences of circulation changes. Especially in late summer, two models simulate very strong warming of warm months, which can be attributed to severe summer drying in the simulations by these models. The models differ also significantly in the simulated warming of cold winter months. Finally, the models simulate rather different changes in North Atlantic sea surface temperature, which is likely to impact on changes in temperature and precipitation. These results imply that several important aspects of climate change in Central Europe are highly uncertain. Other aspects of the simulated climate change appear to be more robust. All models simulate significant warming all year round and an increase in precipitation in the winter half-year.
Constraining the total aerosol indirect effect in the LMDZ and ECHAM4 GCMs using MODIS satellite data
Authors: Quaas J. , Boucher O. , Lohmann U.
Published: April 2010

Abstract. Aerosol indirect effects are considered to be the most uncertain yet important anthropogenic forcing of climate change. The goal of the present study is to reduce this uncertainty by constraining two different general circulation models (LMDZ and ECHAM4) with satellite data. We build a statistical relationship between cloud droplet number concentration and the optical depth of the fine aerosol mode as a measure of the aerosol indirect effect using MODerate Resolution Imaging Spectroradiometer (MODIS) satellite data, and constrain the model parameterizations to match this relationship. We include here "empirical" formulations for the cloud albedo effect as well as parameterizations of the cloud lifetime effect. When fitting the model parameterizations to the satellite data, consistently in both models, the radiative forcing by the combined aerosol indirect effect is reduced considerably, down to −0.5 and −0.3 Wm−2, for LMDZ and ECHAM4, respectively.
Size-segregated aerosol chemical composition at a boreal site in southern Finland, during the QUEST project
Authors: Cavalli F. , Facchini M. C. , Decesari S. , Emblico L. , Mircea M. , Jensen N. R. , Fuzzi S.
Published: April 2010

Abstract. Size-segregated aerosol samples were collected during the QUEST field campaign at Hyytiälä, a boreal forest site in Southern Finland, during spring 2003. Aerosol samples were selectively collected during both particle formation events and periods in which no particle formation occurred. A comprehensive characterisation of the aerosol chemical properties (water-soluble inorganic and organic fraction) and an analysis of the relevant meteorological parameters revealed how aerosol chemistry and meteorology combine to determine a favorable "environment" for new particle formation. The results indicated that all events, typically favored during northerly air mass advection, were background aerosols (total mass concentrations range between 1.97 and 4.31 µg m-3), with an increasingly pronounced marine character as the northerly air flow arrived progressively from the west and, in contrast, with a moderate SO2-pollution influence as the air arrived from more easterly directions. Conversely, the non-event aerosol, transported from the south, exhibited the chemical features of European continental sites, with a marked increase in the concentrations of all major anthropogenic aerosol constituents. The higher non-event mass concentration (total mass concentrations range between 6.88 and 16.30 µg m-3) and, thus, a larger surface area, tended to suppress new particle formation, more efficiently depleting potential gaseous precursors for nucleation. The analysis of water-soluble organic compounds showed that clean nucleation episodes were dominated by aliphatic biogenic species, while non-events were characterised by a large abundance of anthropogenic oxygenated species. Interestingly, a significant content of α-pinene photo-oxidation products was observed in the events aerosol, accounting for, on average, 72% of their WSOC; while only moderate amounts of these species were found in the non-event aerosol. If the organic vapors condensing onto accumulation mode particles are responsible also for the growth of newly formed thermodynamically stable clusters, our finding allows one to postulate that, at the site, α-pinene photo-oxidation products (and probably also photo-oxidation products from other terpenes) are the most likely species to contribute to the growth of nanometer-sized particles.
Direct observations of the atmospheric processing of Asian mineral dust
Authors: Sullivan R. C. , Guazzotti S. A. , Sodeman D. A. , Prather K. A.
Published: April 2010

Abstract. The accumulation of secondary acids and ammonium on individual mineral dust particles during ACE-Asia has been measured with an online single-particle mass spectrometer, the ATOFMS. Changes in the amounts of sulphate, nitrate, and chloride mixed with dust particles correlate with air masses from different source regions. The uptake of secondary acids depended on the individual dust particle mineralogy; high amounts of nitrate accumulated on calcium-rich dust while high amounts of sulphate accumulated on aluminosilicate-rich dust. Oxidation of S(IV) to S(VI) by iron in the aluminosilicate dust is a possible explanation for this enrichment of sulphate, which has important consequences for the fertilization of remote oceans by soluble iron. This study shows the segregation of sulphate from nitrate and chloride in individual aged dust particles for the first time. A transport and aging timeline provides an explanation for the observed segregation. Our data suggests that sulphate became mixed with the dust first. This implies that the transport pathway is more important than the reaction kinetics in determining which species accumulate on mineral dust. Early in the study, dust particles in volcanically influenced air masses were mixed predominately with sulphate. Dust mixed with chloride then dominated over sulphate and nitrate when a major dust front reached the R. V. Ronald Brown. We hypothesize that the rapid increase in chloride on dust was due to mixing with HCl(g) released from acidified sea salt particles induced by heterogeneous reaction with volcanic SO2(g), prior to the arrival of the dust front. The amount of ammonium mixed with dust correlated strongly with the total amount of secondary acid reaction products in the dust. Submicron dust and ammonium sulphate were internally mixed, contrary to frequent reports that they exist as external mixtures. The size distribution of the mixing state of dust with these secondary species validates previous mechanisms of the atmospheric processing of dust and generally agrees with simulated aerosol chemistry from the STEM-2K3 model. This series of novel results has important implications for improving the treatment of dust in global chemistry models and highlights a number of key processes that merit further investigation through laboratory and field studies.
MAX-DOAS detection of glyoxal during ICARTT 2004
Authors: Sinreich R. , Volkamer R. , Filsinger F. , Frieß U. , Kern C. , Platt U. , Sebastián O. , Wagner T.
Published: April 2010

Abstract. The direct detection of glyoxal (CHOCHO), the smallest α-dicarbonyl, in the open atmosphere by active differential optical absorption spectroscopy (DOAS) has recently been demonstrated (Volkamer et al., 2005a) and triggered the very recent successful detection of CHOCHO from space (Kurosu et al., 2005; Wittrock et al., 2006; Beirle et al., 2006). Here we report the first comprehensive analysis of CHOCHO by passive multi axis differential optical absorption spectroscopy (MAX-DOAS). CHOCHO and NO2 slant column measurements were conducted at the Massachusetts Institute of Technology (MIT), Cambridge, USA, and on board the research vessel Ron Brown in the Gulf of Maine as part of the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) 2004 campaign. For a day with nearly clear sky conditions, radiative transfer modeling was employed to derive diurnal CHOCHO mixing ratios in the planetary boundary layer (PBL) for both sites. CHOCHO mixing ratios at MIT varied from 40 to 140 ppt, with peak values observed around noon. Mixing ratios over the Gulf of Maine were found to be up to 2.5 times larger than at MIT. The CHOCHO-to-NO2 ratio at MIT was <0.03, and enhancements of this ratio by up to two orders of magnitude were found over the Gulf of Maine. This paper focuses on the methodological aspects involved with MAX-DOAS measurements of CHOCHO.
Characterizing ozone production in the Mexico City Metropolitan Area: a case study using a chemical transport model
Authors: Lei W. , de Foy B. , Zavala M. , Volkamer R. , Molina L. T.
Published: April 2010

Abstract. An episodic simulation is conducted to characterize midday (12:00–17:00 CDT) ozone (O3) photochemical production and to investigate its sensitivity to emission changes of ozone precursors in the Mexico City Metropolitan Area (MCMA) during an "O3-South" meteorological episode using the Comprehensive Air Quality Model with extensions (CAMx). High Ox (O3+NO2) photochemical production rates of 10–80 ppb/h are predicted due to the high reactivity of volatile organic compounds (VOCs) in which alkanes, alkenes, and aromatics exert comparable contributions. The predicted ozone production efficiency is between 4–10 O3 molecules per NOx molecule oxidized, and increases with VOC-to-NO2 reactivity ratio. Process apportionment analyses indicate significant outflow of pollutants such as O3 and peroxyacetyl nitrate (PAN) from the urban area to the surrounding regional environment. PAN is not in chemical-thermal equilibrium during the photochemically active periods. Sensitivity studies of O3 production suggest that O3 formation in the MCMA urban region with less chemical aging (NOz/NOy<0.3) is VOC-limited. Both the simulated behavior of O3 production and its sensitivities to precursors suggest that midday O3 formation during this episode is VOC-sensitive in the urban region on the basis of the current emissions inventory estimates, and current NOx levels depress the O3 production.
Mesoscale modelling of water vapour in the tropical UTLS: two case studies from the HIBISCUS campaign
Authors: Marécal V. , Durry G. , Longo K. , Freitas S. , Rivière E. D. , Pirre M.
Published: April 2010

Abstract. In this study, we evaluate the ability of the BRAMS (Brazilian Regional Atmospheric Modeling System) mesoscale model compared to ECMWF global analysis to simulate the observed vertical variations of water vapour in the tropical upper troposphere and lower stratosphere (UTLS). The observations are balloon-borne measurements of water vapour mixing ratio and temperature from micro-SDLA (Tunable Diode Laser Spectrometer) instrument. Data from two balloon flights performed during the 2004 HIBISCUS field campaign are used to compare with the mesoscale simulations and to the ECMWF analysis. The observations exhibit fine scale vertical structures of water vapour of a few hundred meters height. The ECMWF vertical resolution (~1 km) is too coarse to capture these vertical structures in the UTLS. With a vertical resolution similar to ECMWF, the mesoscale model performs better than ECMWF analysis for water vapour in the upper troposphere and similarly or slightly worse for temperature. The BRAMS model with 250 m vertical resolution is able to capture more of the observed fine scale vertical variations of water vapour compared to runs with a coarser vertical resolution. This is mainly related to: (i) the enhanced vertical resolution in the UTLS and (ii) to the more detailed microphysical parameterization providing ice supersaturations as in the observations. In near saturated or supersaturated layers, the mesoscale model predicted relative humidity with respect to ice saturation is close to observations provided that the temperature profile is realistic. For temperature, the ECMWF analysis gives good results partly attributed to data assimilation. The analysis of the mesoscale model results showed that the vertical variations of the water vapour profile depends on the dynamics in unsaturated layer while the microphysical processes play a major role in saturated/supersaturated layers. In the lower stratosphere, the ECMWF model and the BRAMS model give very similar water vapour profiles that are significantly drier than micro-SDLA measurements. This similarity comes from the fact that BRAMS is initialised using ECMWF analysis and that no mesoscale process acts in the stratosphere leading to no modification of the BRAMS results with respect to ECMWF analysis.
The role of ozone atmosphere-snow gas exchange on polar, boundary-layer tropospheric ozone – a review and sensitivity analysis
Authors: Helmig D. , Ganzeveld L. , Butler T. , Oltmans S. J.
Published: April 2010

Abstract. Recent research on snowpack processes and atmosphere-snow gas exchange has demonstrated that chemical and physical interactions between the snowpack and the overlaying atmosphere have a substantial impact on the composition of the lower troposphere. These observations also imply that ozone deposition to the snowpack possibly depends on parameters including the quantity and composition of deposited trace gases, solar irradiance, snow temperature and the substrate below the snowpack. Current literature spans a remarkably wide range of ozone deposition velocities (vdO3); several studies even reported positive ozone fluxes out of the snow. Overall, published values range from ~–3<vdO3<2 cm s−1, although most data are within 0<vdO3<0.2 cm s−1. This literature reveals a high uncertainty in the parameterization and the magnitude of ozone fluxes into (and possibly out of) snow-covered landscapes. In this study a chemistry and tracer transport model was applied to evaluate the applicability of the published vdO3 and to investigate the sensitivity of tropospheric ozone towards ozone deposition over Northern Hemisphere snow-covered land and sea-ice. Model calculations using increasing vdO3 of 0.0, 0.01, 0.05 and 0.10 cm s−1 resulted in general ozone sensitivities up to 20–30% in the Arctic surface layer, and of up to 130% local increases in selected Northern Latitude regions. The simulated ozone concentrations were compared with mean January ozone observations from 18 Arctic stations. Best agreement between the model and observations, not only in terms of absolute concentrations but also in the hourly ozone variability, was found by applying an ozone deposition velocity in the range of 0.00–0.01 cm s−1, which is smaller than most literature data and also significantly lower compared to the value of 0.05 cm s−1 that is commonly applied in large-scale atmospheric chemistry models. This sensitivity analysis demonstrates that large errors in the description of the wintertime tropospheric ozone budget stem from the uncertain magnitude of ozone deposition rates and the inability to properly parameterize ozone fluxes to snow-covered landscapes.
Circumpolar transport and air-surface exchange of atmospheric mercury at Ny-Ålesund (79° N), Svalbard, spring 2002
Authors: Sommar J. , Wängberg I. , Berg T. , Gårdfeldt K. , Munthe J. , Richter A. , Urba A. , Wittrock F. , Schroeder W. H.
Published: April 2010

Abstract. Mercury in different environmental compartments has been measured at Ny-Ålesund (78°54' N, 11°53' E) during an intensive campaign, 17 April to 14 May 2002. Time-resolved speciated determination of mercury in the atmosphere and snow was conducted at the Norwegian research station at the Zeppelin mountain, 474 m above the sea level, and at the Italian research facility Dirigibile Italia, 12 m above the sea level. Total Gaseous Mercury (TGM) was present in the range <0.1 to 2.2 ng m−3 during the campaign. Three mercury depletion events, identified as periods with decreased TGM concentrations, were observed. At the lower altitude, TGM concentrations following such events were found to exhibit both higher magnitude and larger variability in comparison to results from the Zeppelin station. Oxidised mercury species in air and fall-out with snow as well as mercury attached to particles were also measured and their concentrations were found to be anti-correlated with TGM in air. concentrations of total Hg in snow (Hg-tot) showed a large (~15×) increase in response to Gaseous Elemental Mercury Depletion Events (GEMDEs, range 1.5–76.5 ng L−1). Solid evidence for photo-stimulated emissions of Hg0(g) from the snow pack in conjunction to depletion events were obtained from gradient measurements as well as from flux chamber measurements. Steep diurnal concentration variations of Hg0(aq) in surface seawater were also found to concur with changing solar radiation. The concentration of Hg0(aq) in seawater was found to be in the range 12.2–70.4 pg L−1, which corresponds to supersaturation. Hence, the seawater surface constituted a source emitting elemental mercury. The concentrations of RGM (reactive gaseous mercury), Hg-p (particulate mercury), and BrO column densities (detected by DOAS) were very low except for a few individual samples during the major Hg0 depletion event. BrO vertical column densities obtained by the remote satellite ESR-2 and trajectory analysis indicate that the air masses exhibiting low Hg0 concentrations originated from areas with high BrO densities.
Technical Note: A new SIze REsolved Aerosol Model (SIREAM)
Authors: Debry E. , Fahey K. , Sartelet K. , Sportisse B. , Tombette M.
Published: April 2010

Abstract. We briefly present in this short paper a new SIze REsolved Aerosol Model (SIREAM) which simulates the evolution of atmospheric aerosol by solving the General Dynamic Equation (GDE). SIREAM segregates the aerosol size distribution into sections and solves the GDE by splitting coagulation and condensation/evaporation-nucleation. A quasi-stationary sectional approach is used to describe the size distribution change due to condensation/evaporation, and a hybrid equilibrium/dynamical mass-transfer method has been developed to lower the computational burden. SIREAM uses the same physical parameterizations as those used in the Modal Aerosol Model, MAM Sartelet et al. (2006). It is hosted in the modeling system Polyphemus Mallet et al., 2007, but can be linked to any other three-dimensional Chemistry-Transport Model.
The T1-T2 study: evolution of aerosol properties downwind of Mexico City
Authors: Doran J. C. , Barnard J. C. , Arnott W. P. , Cary R. , Coulter R. , Fast J. D. , Kassianov E. I. , Kleinman L. , Laulainen N. S. , Martin T. , Paredes-Miranda G. , Pekour M. S. , Shaw W. J. , Smith D. F. , Springston S. R. , Yu X.-Y.
Published: April 2010

Abstract. As part of a major atmospheric chemistry and aerosol field program carried out in March 2006, a study was conducted in the area to the north and northeast of Mexico City to investigate the evolution of aerosols and their associated optical properties in the first few hours after their emission. The focus of the T1-T2 aerosol study was to investigate changes in the specific absorption αABS (absorption per unit mass, with unit of m2 g−1) of black carbon as it aged and became coated with compounds such as sulfate and organic carbon, evolving from an external to an internal mixture. Such evolution has been reported in previous studies. The T1 site was located just to the north of the Mexico City metropolitan area; the T2 site was situated approximately 35 km farther to the northeast. Nephelometers, particle soot absorption photometers, photoacoustic absorption spectrometers, and organic and elemental carbon analyzers were used to measure the optical properties of the aerosols and the carbon concentrations at each of the sites. Radar wind profilers and radiosonde systems helped to characterize the meteorology and to identify periods when transport from Mexico City over T1 and T2 occurred. Organic and elemental carbon concentrations at T1 showed diurnal cycles reflecting the nocturnal and early morning buildup from nearby sources, while concentrations at T2 appeared to be more affected by transport from Mexico City. Specific absorption during transport periods was lower than during other times, consistent with the likelihood of fresher emissions being found when the winds blew from Mexico City over T1 and T2. The specific absorption at T2 was larger than at T1, which is also consistent with the expectation of more aged particles with encapsulated black carbon being found at the more distant location. In situ measurements of single scattering albedo with an aircraft and a ground station showed general agreement with column-averaged values derived from rotating shadowband radiometer data, although some differences were found that may be related to boundary-layer evolution.
Detection of organic compound signatures in infra-red, limb emission spectra observed by the MIPAS-B2 balloon instrument
Authors: Remedios J. J. , Allen G. , Waterfall A. M. , Oelhaf H. , Kleinert A. , Moore D. P.
Published: April 2010

Abstract. Organic compounds play a central role in troposphere chemistry and increasingly are a viable target for remote sensing observations. In this paper, infra-red spectral features of three organic compounds are investigated in thermal emission spectra recorded on a flight on 8 May 1998 near Aire sur l'Adour by a balloon-borne instrument, MIPAS-B2, operating at high spectral resolution. It is demonstrated, for the first time, that PAN and acetone can be detected in infra-red remote sensing spectra of the upper troposphere; detection results are presented at tangent altitudes of 10.4 km and 7.5 km (not acetone). In addition, the results provide the first observation of spectral features of formic acid in thermal emission, as opposed to solar occultation, and confirm that concentrations of this gas are measurable in the mid-latitude upper troposphere, given accurate spectroscopic data. For PAN, two bands are observed centred at 794 cm−1 and 1163 cm−1. For acetone and formic acid, one band has been detected for each so far with band centres at 1218 cm−1 and 1105 cm−1 respectively. Mixing ratios inferred at 10.4 km tangent altitude are 180 pptv and 530 pptv for PAN and acetone respectively, and 200 pptv for formic acid with HITRAN 2000 spectroscopy. Accuracies are on the order of 15 to 40%. The detection technique applied here is verified by examining weak but known signatures of CFC-12 and HCFC-22 in the same spectral regions as those of the organic compounds, with results confirming the quality of both the instrument and the radiative transfer model. The results suggest the possibility of global sensing of the organic compounds studied here which would be a major step forward in verifying and interpreting global tropospheric model calculations.
Characterization of MIPAS elevation pointing
Authors: Kiefer M. , von Clarmann T. , Grabowski U. , De Laurentis M. , Mantovani R. , Milz M. , Ridolfi M.
Published: April 2010

Abstract. Sufficient knowledge of the pointing is essential for analyses of limb emission measurements. The scientific retrieval processor for MIPAS on ENVISAT operated at IMK allows the retrieval of pointing information in terms of tangent altitudes along with temperature. The retrieved tangent altitudes are independent of systematic offsets in the engineering Line-Of-Sight (LOS) information delivered with the ESA Level 1b product. The difference of pointing retrieved from the reprocessed high resolution MIPAS spectra and the engineering pointing information was examined with respect to spatial/temporal behaviour. Among others the following characteristics of MIPAS pointing could be identified: Generally the engineering tangent altitudes are too high by 0–1.8 km with conspicuous variations in this range over time. Prior to December of 2003 there was a drift of about 50–100 m/h, which was due to a slow change in the satellite attitude. A correction of this attitude is done twice a day, which leads to discontinuities in the order of 1–1.5 km in the tangent altitudes. Occasionally discontinuities up to 2.5 km are found, as already reported from MIPAS and SCIAMACHY observations. After an update of the orbit position software in December 2003 values of drift and jumps are much reduced. There is a systematic difference in the mispointing between the poles which amounts to 1.5–2 km, i.e. there is a conspicuous orbit-periodic feature. The analysis of the correlation between the instrument's viewing angle azimuth and differential mispointing supports the hypotheses that a major part of this latter phenomenon can be attributed to an error in the roll angle of the satellite/instrument system of approximately 42 mdeg. One conclusion is that ESA level 2 data should be compared to other data exclusively on tangent pressure levels. Complementary to IMK data, ESA operational LOS calibration results were used to characterize MIPAS pointing. For this purpose MIPAS is used as a radiometer while the passage of infrared bright stars through the instrument's field of view is recorded. Deviation from expected time of passage gives information about mispointing. Results are: a pronounced seasonal variation of the LOS is seen before a correction of on-board software took place in December of 2003. Further a pitch bias of 26 mdeg with respect to the platform attitude information is found, which corresponds to 1.45 km tangent altitude offset towards low altitudes.
The global impact of supersaturation in a coupled chemistry-climate model
Authors: Gettelman A. , Kinnison D. E.
Published: April 2010

Abstract. Ice supersaturation is important for understanding condensation in the upper troposphere. Many general circulation models however do not permit supersaturation. In this study, a coupled chemistry climate model, the Whole Atmosphere Community Climate Model (WACCM), is modified to include supersaturation for the ice phase. Rather than a study of a detailed parameterization of supersaturation, the study is intended as a sensitivity experiment, to understand the potential impact of supersaturation, and of expected changes to stratospheric water vapor, on climate and chemistry. High clouds decrease and water vapor in the stratosphere increases at a similar rate to the prescribed supersaturation (20% supersaturation increases water vapor by nearly 20%). The stratospheric Brewer-Dobson circulation slows at high southern latitudes, consistent with slight changes in temperature likely induced by changes to cloud radiative forcing. The cloud changes also cause an increase in the seasonal cycle of near tropopause temperatures, increasing them in boreal summer over boreal winter. There are also impacts on chemistry, with small increases in ozone in the tropical lower stratosphere driven by enhanced production. The radiative impact of changing water vapor is dominated by the reduction in cloud forcing associated with fewer clouds (~+0.6 Wm−2) with a small component likely from the radiative effect (greenhouse trapping) of the extra water vapor (~+0.2 Wm−2), consistent with previous work. Representing supersaturation is thus important, and changes to supersaturation resulting from changes in aerosol loading for example, might have a modest impact on global radiative forcing, mostly through changes to clouds. There is no evidence of a strong impact of water vapor on tropical tropopause temperatures.
Estimation of a "radiatively correct" black carbon specific absorption during the Mexico City Metropolitan Area (MCMA) 2003 field campaign
Authors: Barnard J. C. , Kassianov E. I. , Ackerman T. P. , Johnson K. , Zuberi B. , Molina L. T. , Molina M. J.
Published: April 2010

Abstract. During the Mexico City Metropolitan Area (MCMA) field campaign of 2003, measurements of the shortwave radiation field allowed the inference of the black carbon (BC) specific absorption, αλ, defined as the monochromatic absorption cross section per unit mass (with units of m2/g). The averaged values of αλ derived from the method here are either 8.9 m2/g or 8.2 m2/g at 500 nm, depending upon the physical and optical parameters assumed for BC. These results are reasonably consistent with those of Schuster et al. (2005), 9.5 m2/g, and Baumgartner et al. (2002), 7.0 m2/g, both measured at 550 nm. The αλ values reported in this paper should only be considered effective, "radiatively correct" values because when used in radiative transfer calculations the calculated irradiances match the measured irradiances at 500 nm. The specific absorption so defined can assume a wide range of values, depending upon: (1) the assumptions made prior to the retrieval (e.g., shell/core aerosol configuration), and (2) values chosen for BC density and refractive index. The range of possible values is large, corresponding to a "worst case" uncertainty of about ±70%, assuming that all errors are additive and of the same sign so that no error cancellation occurs.
Global impact of road traffic emissions on tropospheric ozone
Authors: Matthes S. , Grewe V. , Sausen R. , Roelofs G.-J.
Published: April 2010

Abstract. Road traffic is one of the major anthropogenic emission sectors for NOx, CO and NMHCs (non-methane hydrocarbons). We applied ECHAM4/CBM, a general circulation model coupled to a chemistry module, which includes higher hydrocarbons, to investigate the global impact of 1990 road traffic emissions on the atmosphere. Improving over previous global modelling studies, which concentrated on road traffic NOx and CO emissions only, we assess the impact of NMHC emissions from road traffic. It is revealed that NMHC emissions from road traffic play a key role for the impact on ozone. They are responsible for (indirect) long-range transport of NOx from road traffic via the formation of PAN, which is not found in a simulation without NMHC emissions from road traffic. Long-range transport of NMHC-induced PAN impacts on the ozone distribution in Northern Hemisphere regions far away from the sources, especially in arctic and remote maritime regions. In July total road traffic emissions (NOx, CO and NMHCs) contribute to the zonally averaged ozone distribution by more than 12% near the surface in the Northern Hemisphere midlatitudes and arctic latitudes. In January road traffic emissions contribute near the surface in northern and southern extratropics more than 8%. Sensitivity studies for regional emission show that effective transport of road traffic emissions occurs mainly in the free troposphere. In tropical latitudes of America up to an altitude of 200 hPa, global road traffic emissions contribute about 8% to the ozone concentration. In arctic latitudes NMHC emissions from road transport are responsible for about 90% of PAN increase from road transport, leading to a contribution to ozone concentrations of up to 15%.
A numerical study of tropical cross-tropopause transport by convective overshoots
Authors: Chaboureau J.-P. , Cammas J.-P. , Duron J. , Mascart P. J. , Sitnikov N. M. , Voessing H.-J.
Published: April 2010

Abstract. Observations obtained during the Tropical Convection, Cirrus and Nitrogen Oxides (TROCCINOX) golden day have revealed the presence of ice particles up to 410 K (18.2 km) 2 km above the local tropopause. The case was investigated using a three-dimensional quadruply nested non-hydrostatic simulation and Meteosat Second Generation (MSG) observations. The simulation reproduced the measurements along the flight track fairly well. A reasonable agreement with MSG observations was also achieved: the 10.8-μm brightness temperature (BT) minimum of 187 K was reproduced (a value 6 K colder than the environmental cold-point temperature) as was the positive BT difference between the 6.2- and 10.8-μm bands, an overshoot signature. The simulation produced several overshooting plumes up to 410 K yielding an upward transport of water vapour of a few tons per second across the tropical tropopause. The estimated mass flux agrees with those derived from over tracer budgets, indicating that convection transports mass across the tropopause.
Mesoscale circulations over complex terrain in the Valencia coastal region, Spain – Part 1: Simulation of diurnal circulation regimes
Authors: Pérez-Landa G. , Ciais P. , Sanz M. J. , Gioli B. , Miglietta F. , Palau J. L. , Gangoiti G. , Millán M. M.
Published: April 2010

Abstract. We collected ground-based and aircraft vertical profile measurements of meteorological parameters during a 2-week intensive campaign over the Valencia basin, in order to understand how mesoscale circulations develop over complex terrain and affect the atmospheric transport of tracers. A high-resolution version of the RAMS model was run to simulate the campaign and characterize the diurnal patterns of the flow regime: night-time katabatic drainage, morning sea-breeze development and its subsequent coupling with mountain up-slopes, and evening flow-veering under larger-scale interactions. An application of this mesoscale model to the transport of CO2 is given in a companion paper. A careful evaluation of the model performances against diverse meteorological observations is carried out. Despite the complexity of the processes interacting with each other, and the uncertainties on modeled soil moisture boundary conditions and turbulence parameterizations, we show that it is possible to simulate faithfully the contrasted flow regimes during the course of one day, especially the inland progression and organization of the sea breeze. This gives confidence with respect to future applicability of mesoscale models to establish a reliable link between surface sources of tracers and their atmospheric concentration signals over complex terrain.
Boundary layer concentrations and landscape scale emissions of volatile organic compounds in early spring
Authors: Haapanala S. , Rinne J. , Hakola H. , Hellén H. , Laakso L. , Lihavainen H. , Janson R. , O'Dowd C. , Kulmala M.
Published: April 2010

Abstract. Boundary layer concentrations of several volatile organic compounds (VOC) were measured during two campaigns in springs of 2003 and 2006. The measurements were conducted over boreal landscapes near SMEAR II measurement station in Hyytiälä, Southern Finland. In 2003 the measuremens were performed using a light aircraft and in 2006 using a hot air balloon. Isoprene concentrations were low, usually below detection limit. This can be explained by low biogenic production due to cold weather, phenological stage of the isoprene emitting plants, and snow cover. Monoterpenes were observed frequently. The average total monoterpene concentration in the boundary layer was 33 pptv. Many anthropogenic compounds such as benzene, xylene and toluene, were observed in high amounts. Ecosystem scale surface emissions were estimated using a simple mixed box budget methodology. Total monoterpene emissions varied up to 80 μg m−2 h−1, α-pinene contributing typically more than two thirds of that. These emissions were somewhat higher that those calculated using emission algorithm. The highest emissions of anthropogenic compounds were those of p/m xylene.
Connections between atmospheric sulphuric acid and new particle formation during QUEST III–IV campaigns in Heidelberg and Hyytiälä
Authors: Riipinen I. , Sihto S.-L. , Kulmala M. , Arnold F. , Dal Maso M. , Birmili W. , Saarnio K. , Teinilä K. , Kerminen V.-M. , Laaksonen A. , Lehtinen K. E. J.
Published: April 2010

Abstract. This study investigates the connections between atmospheric sulphuric acid and new particle formation during QUEST III and BACCI/QUEST IV campaigns. The campaigns have been conducted in Heidelberg (2004) and Hyytiälä (2005), the first representing a polluted site surrounded by deciduous forest, and the second a rural site in a boreal forest environment. We have studied the role of sulphuric acid in particle formation and growth by determining 1) the power-law dependencies between sulphuric acid ([H2SO4]), and particle concentrations (N3–6) or formation rates at 1 nm and 3 nm (J1 and J3); 2) the time delays between [H2SO4] and N3–6 or J3, and the growth rates for 1–3 nm particles; 3) the empirical nucleation coefficients A and K in relations J1=A[H2SO4] and J1=K[H2SO4]2, respectively; 4) theoretical predictions for J1 and J3 for the days when no significant particle formation is observed, based on the observed sulphuric acid concentrations and condensation sinks. In both environments, N3–6 or J3 and [H2SO4] were linked via a power-law relation with exponents typically ranging from 1 to 2. The result suggests that the cluster activation theory and kinetic nucleation have the potential to explain the observed particle formation. However, some differences between the sites existed: The nucleation coefficients were about an order of magnitude greater in Heidelberg than in Hyytiälä conditions. The time lags between J3 and [H2SO4] were consistently lower than the corresponding delays between N3–6 and [H2SO4]. The exponents in the J3∝[H2SO4 ]nJ3-connection were consistently higher than or equal to the exponents in the relation N3–6∝[H2SO4 ]nN36. In the J1 values, no significant differences were found between the observed rates on particle formation event days and the predictions on non-event days. The J3 values predicted by the cluster activation or kinetic nucleation hypotheses, on the other hand, were considerably lower on non-event days than the rates observed on particle formation event days. This study provides clear evidence implying that the main process limiting the observable particle formation is the competition between the growth of the freshly formed particles and their loss by scavenging, rather than the initial particle production by nucleation of sulphuric acid. In general, it can be concluded that the simple models based on sulphuric acid concentrations and particle formation by cluster activation or kinetic nucleation can predict the occurence of atmospheric particle formation and growth well, if the particle scavenging is accurately accounted for.
Precision validation of MIPAS-Envisat products
Authors: Piccolo C. , Dudhia A.
Published: April 2010

Abstract. This paper discusses the variation and validation of the precision, or estimated random error, associated with the ESA Level 2 products from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). This quantity represents the propagation of the radiometric noise from the spectra through the retrieval process into the Level 2 profile values. The noise itself varies with time, steadily rising between ice decontamination events, but the Level 2 precision has a greater variation due to the atmospheric temperature which controls the total radiance received. Hence, for all species, the precision varies latitudinally/seasonally with temperature, with a small superimposed temporal structure determined by the degree of ice contamination on the detectors. The precision validation involves comparing two MIPAS retrievals at the intersections of ascending/descending orbits. For 5 days per month of full resolution MIPAS operation, the standard deviation of the matching profile pairs is computed and compared with the precision given in the MIPAS Level 2 data, except for NO2 since it has a large diurnal variation between ascending/descending intersections. Even taking into account the propagation of the pressure-temperature retrieval errors into the VMR retrieval, the standard deviation of the matching pairs is usually a factor 1–2 larger than the precision. This is thought to be due to effects such as horizontal inhomogeneity of the atmosphere and instability of the retrieval.
Nitrogen and oxygen isotopic constraints on the origin of atmospheric nitrate in coastal Antarctica
Authors: Savarino J. , Kaiser J. , Morin S. , Sigman D. M. , Thiemens M. H.
Published: April 2010

Abstract. Throughout the year 2001, aerosol samples were collected continuously for 10 to 15 days at the French Antarctic Station Dumont d'Urville (DDU) (66°40' S, l40°0' E, 40 m above mean sea level). The nitrogen and oxygen isotopic ratios of particulate nitrate at DDU exhibit seasonal variations that are among the most extreme observed for nitrate on Earth. In association with concentration measurements, the isotope ratios delineate four distinct periods, broadly consistent with previous studies on Antarctic coastal areas. During austral autumn and early winter (March to mid-July), nitrate concentrations attain a minimum between 10 and 30 ng m−3 (referred to as Period 2). Two local maxima in August (55 ng m−3) and November/December (165 ng m−3) are used to assign Period 3 (mid-July to September) and Period 4 (October to December). Period 1 (January to March) is a transition period between the maximum concentration of Period 4 and the background concentration of Period 2. These seasonal changes are reflected in changes of the nitrogen and oxygen isotope ratios. During Period 2, which is characterized by background concentrations, the isotope ratios are in the range of previous measurements at mid-latitudes: δ18Ovsmow=(77.2±8.6)‰; Δ17O=(29.8±4.4)‰; δ15Nair=(−4.4±5.4)‰ (mean ± one standard deviation). Period 3 is accompanied by a significant increase of the oxygen isotope ratios and a small increase of the nitrogen isotope ratio to δ18Ovsmow=(98.8±13.9)‰; Δ17O=(38.8±4.7)‰ and δ15Nair=(4.3±8.20‰). Period 4 is characterized by a minimum 15N/14N ratio, only matched by one prior study of Antarctic aerosols, and oxygen isotope ratios similar to Period 2: δ18Ovsmow=(77.2±7.7)‰; Δ17O=(31.1±3.2)‰; δ15Nair=(−32.7±8.4)‰. Finally, during Period 1, isotope ratios reach minimum values for oxygen and intermediate values for nitrogen: δ18Ovsmow=63.2±2.5‰; Δ17O=24.0±1.1‰; δ15Nair=−17.9±4.0‰). Based on the measured isotopic composition, known atmospheric transport patterns and the current understanding of kinetics and isotope effects of relevant atmospheric chemical processes, we suggest that elevated tropospheric nitrate levels during Period 3 are most likely the result of nitrate sedimentation from polar stratospheric clouds (PSCs), whereas elevated nitrate levels during Period 4 are likely to result from snow re-emission of nitrogen oxide species. We are unable to attribute the source of the nitrate during periods 1 and 2 to local production or long-range transport, but note that the oxygen isotopic composition is in agreement with day and night time nitrate chemistry driven by the diurnal solar cycle. A precise quantification is difficult, due to our insufficient knowledge of isotope fractionation during the reactions leading to nitrate formation, among other reasons.
Climatic consequences of regional nuclear conflicts
Authors: Robock A. , Oman L. , Stenchikov G. L. , Toon O. B. , Bardeen C. , Turco R. P.
Published: April 2010

Abstract. We use a modern climate model and new estimates of smoke generated by fires in contemporary cities to calculate the response of the climate system to a regional nuclear war between emerging third world nuclear powers using 100 Hiroshima-size bombs (less than 0.03% of the explosive yield of the current global nuclear arsenal) on cities in the subtropics. We find significant cooling and reductions of precipitation lasting years, which would impact the global food supply. The climate changes are large and long-lasting because the fuel loadings in modern cities are quite high and the subtropical solar insolation heats the resulting smoke cloud and lofts it into the high stratosphere, where removal mechanisms are slow. While the climate changes are less dramatic than found in previous "nuclear winter" simulations of a massive nuclear exchange between the superpowers, because less smoke is emitted, the changes are more long-lasting because the older models did not adequately represent the stratospheric plume rise.