bluuebunny/crossref_metadata_2025 huggingface dataset:
Technical Note: Formal blind intercomparison of OH measurements: results from the international campaign HOxComp
Authors: Schlosser E. , Brauers T. , Dorn H.-P. , Fuchs H. , Häseler R. , Hofzumahaus A. , Holland F. , Wahner A. , Kanaya Y. , Kajii Y. , Miyamoto K. , Nishida S. , Watanabe K. , Yoshino A. , Kubistin D. , Martinez M. , Rudolf M. , Harder H. , Berresheim H. , Elste T. , Plass-Dülmer C. , Stange G. , Schurath U.
Published: April 2010

Abstract. Hydroxyl radicals (OH) are the major oxidizing species in the troposphere. Because of their central importance, absolute measurements of their concentrations are needed to validate chemical mechanisms of atmospheric models. The extremely low and highly variable concentrations in the troposphere, however, make measurements of OH difficult. Three techniques are currently used worldwide for tropospheric observations of OH after about 30~years of technical developments: Differential Optical Laser Absorption Spectroscopy (DOAS), Laser-Induced Fluorescence Spectroscopy (LIF), and Chemical Ionisation Mass Spectrometry (CIMS). Even though many measurement campaigns with OH data were published, the question of accuracy and precision is still under discussion. Here, we report results of the first formal, blind intercomparison of these techniques. Six OH instruments (4~LIF, 1~CIMS, 1~DOAS) participated successfully in the ground-based, international HOxComp campaign carried out in Jülich, Germany, in summer 2005. Comparisons were performed for three days in ambient air (3~LIF, 1 CIMS) and for six days in the atmosphere simulation chamber SAPHIR (3~LIF, 1~DOAS). All instruments were found to measure tropospheric OH concentrations with high sensitivity and good time resolution. The pairwise correlations between different data sets were linear and yielded high correlation coefficients (r2=0.75−0.96). Excellent absolute agreement was observed for the instruments at the SAPHIR chamber, yielding slopes between 1.01 and 1.13 in the linear regressions. In ambient air, the slopes deviated from unity by factors of 1.06 to 1.69, which can partly be explained by the stated instrumental accuracies. In addition, sampling inhomogeneities and calibration problems have apparently contributed to the discrepancies. The absolute intercepts of the linear regressions did not exceed 0.6×106 cm−3, mostly being insignificant and of minor importance for daytime observations of OH. No relevant interferences with respect to ozone, water vapour, NOx and peroxy radicals could be detected. The HOxComp campaign has demonstrated that OH can be measured reasonably well by current instruments, but also that there is still room for improvement of calibrations.
A new parametrization for ambient particle formation over coniferous forests and its potential implications for the future
Authors: Bonn B. , Boy M. , Kulmala M. , Groth A. , Trawny K. , Borchert S. , Jacobi S.
Published: April 2010

Abstract. Atmospheric new particle formation is a general phenomenon observed over coniferous forests. So far nucleation is either parameterised as a function of gaseous sulphuric acid concentration only, which is unable to explain the observed seasonality of nucleation events at different measurement sites, or as a function of sulphuric acid and organic molecules. Here we introduce different nucleation parameters based on the interaction of sulphuric acid and terpene oxidation products and elucidate the individual importance. They include basic trace gas and meteorological measurements such as ozone and water vapour concentrations, temperature (for terpene emission) and UV B radiation as a proxy for OH radical formation. We apply these new parameters to field studies conducted at conducted at Finnish and German measurement sites and compare these to nucleation observations on a daily and annual scale. General agreement was found, although the specific compounds responsible for the nucleation process remain speculative. This can be interpreted as follows: During cooler seasons the emission of biogenic terpenes and the OH availability limits the new particle formation while towards warmer seasons the ratio of ozone and water vapour concentration seems to dominate the general behaviour. Therefore, organics seem to support ambient nucleation besides sulphuric acid or an OH-related compound. Using these nucleation parameters to extrapolate the current conditions to prognosed future concentrations of ozone, water vapour and organic concentrations leads to a significant potential increase in the nucleation event number.
Airborne measurements of the nitric acid partitioning in persistent contrails
Authors: Schäuble D. , Voigt C. , Kärcher B. , Stock P. , Schlager H. , Krämer M. , Schiller C. , Bauer R. , Spelten N. , de Reus M. , Szakáll M. , Borrmann S. , Weers U. , Peter Th.
Published: April 2010

Abstract. This study reports the first systematic measurements of nitric acid (HNO3) uptake in contrail ice particles at typical aircraft cruise altitudes. During the CIRRUS-III campaign cirrus clouds and almost 40 persistent contrails were probed with in situ instruments over Germany and Northern Europe in November 2006. Besides reactive nitrogen, water vapor, cloud ice water content, ice particle size distributions, and condensation nuclei were measured during 6 flights. Contrails with ages up to 12 h were detected at altitudes 10–11.5 km and temperatures 211–220 K. These contrails had a larger ice phase fraction of total nitric acid (HNO3ice/HNO3tot = 6%) than the ambient cirrus layers (3%). On average, the contrails contained twice as much HNO3ice as the cirrus clouds, 14 pmol/mol and 6 pmol/mol, respectively. Young contrails with ages below 1 h had a mean HNO3ice of 21 pmol/mol. The contrails had higher nitric acid to water molar ratios in ice and slightly higher ice water contents than the cirrus clouds under similar meteorological conditions. The differences in ice phase fractions and molar ratios between developing contrails and cirrus are likely caused by high plume concentrations of HNO3 prior to contrail formation. The location of the measurements in the upper region of frontal cirrus layers might account for slight differences in the ice water content between contrails and adjacent cirrus clouds. The observed dependence of molar ratios as a function of the mean ice particle diameter suggests that ice-bound HNO3 concentrations are controlled by uptake of exhaust HNO3 in the freezing plume aerosols in young contrails and subsequent trapping of ambient HNO3 in growing ice particles in older (age > 1 h) contrails.
Satellite measurements of formaldehyde linked to shipping emissions
Authors: Marbach T. , Beirle S. , Platt U. , Hoor P. , Wittrock F. , Richter A. , Vrekoussis M. , Grzegorski M. , Burrows J. P. , Wagner T.
Published: April 2010

Abstract. International shipping is recognized as a pollution source of growing importance, in particular in the remote marine boundary layer. Nitrogen dioxide originating from ship emissions has previously been detected in satellite measurements. This study presents the first satellite measurements of formaldehyde (HCHO) linked to shipping emissions as derived from observations made by the Global Ozone Monitoring Experiment (GOME) instrument. We analyzed enhanced HCHO tropospheric columns from shipping emissions over the Indian Ocean between Sri Lanka and Sumatra. This region offers good conditions in term of plume detection with the GOME instrument as all ship tracks follow a single narrow track in the same east-west direction as used for the GOME pixel scanning. The HCHO signal alone is weak but could be clearly seen in the high-pass filtered data. The line of enhanced HCHO in the Indian Ocean as seen in the 7-year composite of cloud free GOME observations clearly coincides with the distinct ship track corridor from Sri Lanka to Indonesia. The observed mean HCHO column enhancement over this shipping route is about 2.0×1015 molec/cm2. Compared to the simultaneously observed NO2 values over the shipping route, those of HCHO are substantially higher; also the HCHO peaks are found at larger distance from the ship routes. These findings indicate that direct emissions of HCHO or degradation of emitted NMHC cannot explain the observed enhanced HCHO values. One possible reason might be increased CH4 degradation due to enhanced OH concentrations related to the ship emissions, but this source is probably too weak to fully explain the observed values. The observed HCHO pattern also agrees qualitatively well with results from the coupled earth system model ECHAM5/MESSy applied to atmospheric chemistry (EMAC). However, the modelled HCHO values over the ship corridor are two times lower than in the GOME high-pass filtered data. This might indicate uncertainties in the satellite data and used emission inventories and/or that the in-plume chemistry taking place in the narrow path of the shipping lanes are not well represented at the rather coarse model resolution.
The continental source of glyoxal estimated by the synergistic use of spaceborne measurements and inverse modelling
Authors: Stavrakou T. , Müller J.-F. , De Smedt I. , Van Roozendael M. , Kanakidou M. , Vrekoussis M. , Wittrock F. , Richter A. , Burrows J. P.
Published: April 2010

Abstract. Tropospheric glyoxal and formaldehyde columns retrieved from the SCIAMACHY satellite instrument in 2005 are used with the IMAGESv2 global chemistry-transport model and its adjoint in a two-compound inversion scheme designed to estimate the continental source of glyoxal. The formaldehyde observations provide an important constraint on the production of glyoxal from isoprene in the model, since the degradation of isoprene constitutes an important source of both glyoxal and formaldehyde. Current modelling studies underestimate largely the observed glyoxal satellite columns, pointing to the existence of an additional land glyoxal source of biogenic origin. We include an extra glyoxal source in the model and we explore its possible distribution and magnitude through two inversion experiments. In the first case, the additional source is represented as a direct glyoxal emission, and in the second, as a secondary formation through the oxidation of an unspecified glyoxal precursor. Besides this extra source, the inversion scheme optimizes the primary glyoxal and formaldehyde emissions, as well as their secondary production from other identified non-methane volatile organic precursors of anthropogenic, pyrogenic and biogenic origin. In the first inversion experiment, the additional direct source, estimated at 36 Tg/yr, represents 38% of the global continental source, whereas the contribution of isoprene is equally important (30%), the remainder being accounted for by anthropogenic (20%) and pyrogenic fluxes. The inversion succeeds in reducing the underestimation of the glyoxal columns by the model, but it leads to a severe overestimation of glyoxal surface concentrations in comparison with in situ measurements. In the second scenario, the inferred total global continental glyoxal source is estimated at 108 Tg/yr, almost two times higher than the global a priori source. The extra secondary source is the largest contribution to the global glyoxal budget (50%), followed by the production from isoprene (26%) and from anthropogenic NMVOC precursors (14%). A better performance is achieved in this case, as the updated emissions allow for a satisfactory agreement of the model with both satellite and in situ glyoxal observations.
Impact of nucleation on global CCN
Authors: Merikanto J. , Spracklen D. V. , Mann G. W. , Pickering S. J. , Carslaw K. S.
Published: April 2010

Abstract. Cloud condensation nuclei (CCN) are derived from particles emitted directly into the atmosphere (primary emissions) or from the growth of nanometer-sized particles nucleated in the atmosphere. It is important to separate these two sources because they respond in different ways to gas and particle emission control strategies and environmental changes. Here, we use a global aerosol microphysics model to quantify the contribution of primary and nucleated particles to global CCN. The model considers primary emissions of sea spray, sulfate and carbonaceous particles, and nucleation processes appropriate for the free troposphere and boundary layer. We estimate that 45% of global low-level cloud CCN at 0.2% supersaturation are secondary aerosol derived from nucleation (ranging between 31–49% taking into account uncertainties in primary emissions and nucleation rates), with the remainder from primary emissions. The model suggests that 35% of CCN (0.2%) in global low-level clouds were created in the free and upper troposphere. In the marine boundary layer 55% of CCN (0.2%) are from nucleation, with 45% entrained from the free troposphere and 10% nucleated directly in the boundary layer. Combinations of model runs show that primary and nucleated CCN are non-linearly coupled. In particular, boundary layer nucleated CCN are strongly suppressed by both primary emissions and entrainment of particles nucleated in the free troposphere. Elimination of all primary emissions reduces global CCN (0.2%) by only 20% and elimination of upper tropospheric nucleation reduces CCN (0.2%) by only 12% because of the increased contribution from boundary layer nucleation.
Assessment of vertically-resolved PM10 from mobile lidar observations
Authors: Raut J.-C. , Chazette P.
Published: April 2010

Abstract. We investigate in this study the vertical PM10 distributions from mobile measurements carried out from locations along the Paris Peripherique (highly trafficked beltway around Paris), examine distinctions in terms of aerosol concentrations between the outlying regions of Paris and the inner city and eventually discuss the influence of aerosol sources, meteorology, and dynamics on the retrieved PM10 distributions. To achieve these purposes, we combine in situ surface measurements with active remote sensing observations obtained from a great number of research programs in Paris area since 1999. Two approaches, devoted to the conversion of vertical profiles of lidar-derived extinction coefficients into PM10, have been set up. A very good agreement is found between the theoretical and empirical methods with a discrepancy of 3%. Hence, specific extinction cross-sections at 355 nm are provided with a reasonable relative uncertainty lower than 12% for urban (4.5 m2 g−1) and periurban (5.9 m2 g−1) aersols, lower than 26% for rural (7.1 m2 g−1) aerosols, biomass burning (2.6 m2 g−1) and dust (1.1 m2 g−1) aerosols The high spatial and temporal resolutions of the mobile lidar (respectively 1.5 m and 1 min) enable to follow the spatiotemporal variability of various layers trapping aerosols in the troposphere. Appropriate specific extinction cross-sections are applied in each layer detected in the vertical heterogeneities from the lidar profiles. The standard deviation (rms) between lidar-derived PM10 at 200 m above ground and surface network stations measurements was ~14μg m−3. This difference is particularly ascribed to a decorrelation of mass concentrations in the first meters of the boundary layer, as highlighted through multiangular lidar observations. Lidar signals can be used to follow mass concentrations with an uncertainty lower than 25% above urban areas and provide useful information on PM10 peak forecasting that affect air quality.
Coastal measurements of short-lived reactive iodocarbons and bromocarbons at Roscoff, Brittany during the RHaMBLe campaign
Authors: Jones C. E. , Hornsby K. E. , Dunk R. M. , Leigh R. J. , Carpenter L. J.
Published: April 2010

Abstract. Atmospheric concentrations of the volatile reactive iodocarbons C2H5I, 1-C3H7I, 2-C3H7I, CH2ICl, CH2IBr, CH2I2 and bromocarbons CH2Br2 and CHBr3 were determined by GC/MS analysis of marine boundary layer air at Roscoff, Brittany on the northwest coast of France during September 2006. Comparison with other coastal studies suggests that emissions of these trace gases are strongly influenced by site topography, seaweed populations and distribution, as well as wind speed and direction and tide height. Concentrations of the very short-lived dihalomethanes CH2IBr and CH2I2 in particular showed evidence of tidal dependence, with higher concentrations observed at low tide during maximum exposure of seaweed beds. We also present a limited number of halocarbon measurements in surface seawater and estimate sea-air fluxes based on these and simultaneous air measurements. CH2Br2 and CHBr3 were strongly correlated both in air and in seawater, with CH2Br2/CHBr3 ratios of 0.19 in air and 0.06 in water. The combined midday I atom flux from the photolabile diahlomethanes CH2I2, CH2IBr and CH2ICl of ~5×103 molecules cm−3 s−1 is several orders of magnitude lower than the estimated I atom flux from I2 based on coinciding measurements at the same site, which indicates that at Roscoff the major I atom precursor was I2 rather than reactive iodocarbons.
Application of φ-IASI to IASI: retrieval products evaluation and radiative transfer consistency
Authors: Masiello G. , Serio C. , Carissimo A. , Grieco G. , Matricardi M.
Published: April 2010

Abstract. Retrieval products for temperature, water vapour and ozone have been obtained from spectral radiances measured by the Infrared Atmospheric Sounding Interferometer flying onboard the first European Meteorological Operational satellite. These products have been used to check the consistency of the forward model and its accuracy and the expected retrieval performance. The study has been carried out using a research-oriented forward-inverse methodology, called φ-IASI, that the authors have specifically developed for the new sounding interferometer. The performance of the forward-inversion strategy has been assessed by comparing the retrieved profiles to profiles of temperature, water vapour and ozone obtained by co-locating in space and time profiles from radiosonde observations and from the European Centre for Medium-Range Weather Forecasts analysis. Spectral residuals have also been computed and analyzed to assess the quality of the forward model. Two versions of the high-resolution transmission molecular absorption database have been used, which mostly differ for ozone absorption line parameters, line and continuum absorption of both CO2 and H2O molecules. Their performance has been assessed by inter-comparing the results, and a consistent improvement in the spectral residual has been found when using the most updated release.
Possible influence of anthropogenic aerosols on cirrus clouds and anthropogenic forcing
Authors: Penner J. E. , Chen Y. , Wang M. , Liu X.
Published: April 2010

Abstract. Cirrus clouds have a net warming effect on the atmosphere and cover about 30% of the Earth's area. Aerosol particles initiate ice formation in the upper troposphere through modes of action that include homogeneous freezing of solution droplets, heterogeneous nucleation on solid particles immersed in a solution, and deposition nucleation of vapor onto solid particles. Here, we examine the possible change in ice number concentration from anthropogenic soot originating from surface sources of fossil fuel and biomass burning, from anthropogenic sulfate aerosols, and from aircraft that deposit their aerosols directly in the upper troposphere. We use a version of the aerosol model that predicts sulfate number and mass concentrations in 3-modes and includes the formation of sulfate aerosol through homogeneous binary nucleation as well as a version that only predicts sulfate mass. The 3-mode version best represents the Aitken aerosol nuclei number concentrations in the upper troposphere which dominated ice crystal residues in the upper troposphere. Fossil fuel and biomass burning soot aerosols with this version exert a radiative forcing of −0.3 to −0.4 Wm−2 while anthropogenic sulfate aerosols and aircraft aerosols exert a forcing of −0.01 to 0.04 Wm−2 and −0.16 to −0.12 Wm−2, respectively, where the range represents the forcing from two parameterizations for ice nucleation. The sign of the forcing in the mass-only version of the model depends on which ice nucleation parameterization is used and can be either positive or negative. The magnitude of the forcing in cirrus clouds can be comparable to the forcing exerted by anthropogenic aerosols on warm clouds, but this forcing has not been included in past assessments of the total anthropogenic radiative forcing of climate.
Surface ozone trend details and interpretations in Beijing, 2001–2006
Authors: Tang G. , Li X. , Wang Y. , Xin J. , Ren X.
Published: April 2010

Abstract. Beijing is a megacity situated in the rapidly developing Beijing-Tianjin-Hebei region of northern China. In this study, we analyze data on ozone and nitrogen oxide levels obtained at six urban sites in Beijing between the months of July and September. Our goal is to investigate average trends and interpretations over the 2001–2006 period. Average concentrations of NOx (NOx=NO+NO2), O3, and Ox (Ox=O3+NO2) were 49.2±5.9 ppbv, 26.6±2.8 ppbv, and 60.3±1.9 ppbv, respectively. NOx concentrations decreased linearly at a rate of 3.9±0.5 ppbv/yr after 2002, while ozone concentrations increased at a rate of 1.1±0.5 ppbv/yr during 2001–2006, and Ox concentrations remained nearly constant. The reduction of NOx emissions and elevated non-methane hydrocarbon (NMHCs) emissions may have contributed to the increased O3 concentrations in Beijing. When the contributions from Beijing's urban and surrounding areas were disaggregated via trajectory cluster analysis, daily maximum and average Ox concentrations attributable to Beijing's local emissions increased linearly at rates of 1.3±0.6 ppbv/yr and 0.8±0.6 ppbv/yr, while the Ox concentrations attributable to regional areas decreased linearly at rates of 0.6±0.3 ppbv/yr and 0.5±0.3 ppbv/yr, respectively. The decrease in Ox concentrations of the surrounding areas was found to counteract increasing Beijing urban Ox production, leading to nearly constant Ox concentrations in the Beijing region over the study period. Our results may be helpful for redefining government strategies to control the photochemical formation of air pollutants in the Beijing region. Our conclusions have relevance for developing megacities worldwide.
Technical note: Scintillations of the double star α Cru observed by GOMOS/Envisat
Authors: Sofieva V. F. , Dalaudier F. , Kan V. , Gurvich A. S.
Published: April 2010

Abstract. In this paper, we discuss scintillation time-spectra of the double star α Cru, which were measured by the GOMOS/Envisat photometer. The components of α Cru are not resolved by the angular field of view of the detector. The double structure of the light source reveals itself in the modulation of the observed scintillation spectra; this modulation is caused by anisotropic irregularities of the stratospheric air density. We present a qualitative and quantitative explanation of the properties of the double-star scintillation spectra. Possibilities of using double star scintillations for studying atmospheric air density irregularities are also discussed in the paper.
Evaluation of black carbon estimations in global aerosol models
Authors: Koch D. , Schulz M. , Kinne S. , McNaughton C. , Spackman J. R. , Balkanski Y. , Bauer S. , Berntsen T. , Bond T. C. , Boucher O. , Chin M. , Clarke A. , De Luca N. , Dentener F. , Diehl T. , Dubovik O. , Easter R. , Fahey D. W. , Feichter J. , Fillmore D. , Freitag S. , Ghan S. , Ginoux P. , Gong S. , Horowitz L. , Iversen T. , Kirkevåg A. , Klimont Z. , Kondo Y. , Krol M. , Liu X. , Miller R. , Montanaro V. , Moteki N. , Myhre G. , Penner J. E. , Perlwitz J. , Pitari G. , Reddy S. , Sahu L. , Sakamoto H. , Schuster G. , Schwarz J. P. , Seland Ø. , Stier P. , Takegawa N. , Takemura T. , Textor C. , van Aardenne J. A. , Zhao Y.
Published: April 2010

Abstract. We evaluate black carbon (BC) model predictions from the AeroCom model intercomparison project by considering the diversity among year 2000 model simulations and comparing model predictions with available measurements. These model-measurement intercomparisons include BC surface and aircraft concentrations, aerosol absorption optical depth (AAOD) retrievals from AERONET and Ozone Monitoring Instrument (OMI) and BC column estimations based on AERONET. In regions other than Asia, most models are biased high compared to surface concentration measurements. However compared with (column) AAOD or BC burden retreivals, the models are generally biased low. The average ratio of model to retrieved AAOD is less than 0.7 in South American and 0.6 in African biomass burning regions; both of these regions lack surface concentration measurements. In Asia the average model to observed ratio is 0.7 for AAOD and 0.5 for BC surface concentrations. Compared with aircraft measurements over the Americas at latitudes between 0 and 50N, the average model is a factor of 8 larger than observed, and most models exceed the measured BC standard deviation in the mid to upper troposphere. At higher latitudes the average model to aircraft BC ratio is 0.4 and models underestimate the observed BC loading in the lower and middle troposphere associated with springtime Arctic haze. Low model bias for AAOD but overestimation of surface and upper atmospheric BC concentrations at lower latitudes suggests that most models are underestimating BC absorption and should improve estimates for refractive index, particle size, and optical effects of BC coating. Retrieval uncertainties and/or differences with model diagnostic treatment may also contribute to the model-measurement disparity. Largest AeroCom model diversity occurred in northern Eurasia and the remote Arctic, regions influenced by anthropogenic sources. Changing emissions, aging, removal, or optical properties within a single model generated a smaller change in model predictions than the range represented by the full set of AeroCom models. Upper tropospheric concentrations of BC mass from the aircraft measurements are suggested to provide a unique new benchmark to test scavenging and vertical dispersion of BC in global models.
Comment on "Quantitative performance metrics for stratospheric-resolving chemistry-climate models" by Waugh and Eyring (2008)
Authors: Grewe V. , Sausen R.
Published: April 2010

Abstract. This comment focuses on the statistical limitations of a model grading, as applied by D. Waugh and V. Eyring (2008) (WE08). The grade g is calculated for a specific diagnostic, which basically relates the difference of means of model and observational data to the standard deviation in the observational dataset. We performed Monte Carlo simulations, which show that this method has the potential to lead to large 95%-confidence intervals for the grade. Moreover, the difference between two model grades often has to be very large to become statistically significant. Since the confidence intervals were not considered in detail for all diagnostics, the grading in WE08 cannot be interpreted, without further analysis. The results of the statistical tests performed in WE08 agree with our findings. However, most of those tests are based on special cases, which implicitely assume that observations are available without any errors and that the interannual variability of the observational data and the model data are equal. Without these assumptions, the 95%-confidence intervals become even larger. Hence, the case, where we assumed perfect observations (ignored errors), provides a good estimate for an upper boundary of the threshold, below that a grade becomes statistically significant. Examples have shown that the 95%-confidence interval may even span the whole grading interval [0, 1]. Without considering confidence intervals, the grades presented in WE08 do not allow to decide whether a model result significantly deviates from reality. Neither in WE08 nor in our comment it is pointed out, which of the grades presented in WE08 inhibits such kind of significant deviation. However, our analysis of the grading method demonstrates the unacceptably high potential for these grades to be insignificant. This implies that the grades given by WE08 can not be interpreted by the reader. We further show that the inclusion of confidence intervals into the grading approach is necessary, since otherwise even a perfect model may get a low grade.
Impact of Chinese anthropogenic emissions on submicrometer aerosol concentration at Mt. Tateyama, Japan
Authors: Osada K. , Ohara T. , Uno I. , Kido M. , Iida H.
Published: April 2010

Abstract. Rapid Asian economic development might engender secondary impacts of atmospheric aerosol particles over the western Pacific after conversion of gaseous pollutants such as SO2. To elucidate changes in aerosol concentrations in leeward areas undergoing remarkable industrialization, the number-size distributions of submicrometer (0.3–1.0 μm) aerosols were measured at Murododaira (36.6° N, 137.6° E, 2450 m a.s.l.) on the western flank of Mount Tateyama in central Japan during January 1999–February 2009. Nighttime data obtained from 2400 to 0500 were used to analyze free-tropospheric aerosol concentration. Monthly average volume concentrations were calculated for months with >50% daily data coverage. Volume concentrations of submicrometer aerosols were high in spring to early summer and low in winter. Significant increasing trends at 95% confidence levels were found for volume concentrations in winter–spring. Simulated monthly anthropogenic aerosol concentrations at Mt. Tateyama from results of regional aerosol modeling with emission inventory up to 2005 showed seasonal variation and winter–spring increasing trends similar to those of observed aerosol concentration. According to the model analyses, the contribution of anthropogenic aerosol concentrations derived from China was high during winter–spring (60–80% of total anthropogenic aerosols at Mt. Tateyama). This accords with the increasing trend observed for winter–spring. Because SO42− is the dominant component of total anthropogenic aerosols, these results suggest that increasing anthropogenic emissions, especially for SO2, in China, engender enhancement of submicrometer-diameter aerosols over Japan during winter–spring.
On the quality of the Nimbus 7 LIMS Version 6 water vapor profiles and distributions
Authors: Remsberg E. E. , Natarajan M. , Lingenfelser G. S. , Thompson R. E. , Marshall B. T. , Gordley L. L.
Published: April 2010

Abstract. This report describes the quality of the Nimbus 7 Limb Infrared Monitor of the Stratosphere (LIMS) water vapor (H2O) profiles of 1978/79 that were processed with a Version 6 (V6) algorithm and archived in 2002. The V6 profiles incorporate a better knowledge of the instrument attitude for the LIMS measurements along its orbits, leading to improvements for its temperature profiles and for the registration of its water vapor radiances with pressure. As a result, the LIMS V6 zonal-mean distributions of H2O exhibit better hemispheric symmetry than was the case from the original Version 5 (V5) dataset that was archived in 1982. Estimates of the precision and accuracy of the V6 H2O profiles are developed and provided. Individual profiles have a precision of order 5% and an estimated accuracy of about 19% at 3 hPa, 14% at 10 hPa, and 26% at 50 hPa. Profile segments within about 2 km of the tropopause are often affected by emissions from clouds that appear in the finite field-of-view of the detector for the LIMS H2O channel. Zonally-averaged distributions of the LIMS V6 H2O are compared with those from the more recent Microwave Limb Sounder (MLS) satellite experiment for November, February, and May of 2004/05. The patterns and values of their respective distributions are similar in many respects. Effects of a strengthened Brewer-Dobson circulation are indicated in the MLS distributions of the recent decade versus those of LIMS from 1978/79. A tropical tape recorder signal is present in the 7-month time series of LIMS V6 H2O with lowest values in February 1979, and the estimated, annually-averaged "entry-level" H2O is 3.5 to 3.8 ppmv. It is judged that this historic LIMS water vapor dataset is of good quality for studies of the near global-scale chemistry and transport for pressure levels from 3 hPa to about 70 to 100 hPa.
Influence of scintillation on quality of ozone monitoring by GOMOS
Authors: Sofieva V. F. , Kan V. , Dalaudier F. , Kyrölä E. , Tamminen J. , Bertaux J.-L. , Hauchecorne A. , Fussen D. , Vanhellemont F.
Published: April 2010

Abstract. Stellar light passing through the Earth atmosphere is affected by refractive effects, which should be taken into account in retrievals from stellar occultation measurements. Scintillation caused by air density irregularities is a nuisance for retrievals of atmospheric composition. In this paper, we consider the influence of scintillation on stellar occultation measurements and on the quality of ozone retrievals from these measurements, based on experience of the GOMOS (Global Ozone Monitoring by Occultation of Stars) instrument on board the Envisat satellite. In GOMOS retrievals, the scintillation effect is corrected using scintillation measurements by the fast photometer. We present quantitative estimates of the current scintillation correction quality and of the impact of scintillation on ozone retrievals by GOMOS. The analysis has shown that the present scintillation correction efficiently removes the distortion of transmission spectra caused by scintillations, which are generated by anisotropic irregularities of air density. The impact of errors of dilution and anisotropic scintillation correction on the quality of ozone retrievals is negligible. However, the current scintillation correction is not able to remove the wavelength-dependent distortion of transmission spectra caused by isotropic scintillations, which can be present in off-orbital-plane occultations. This distortion may result in ozone retrieval errors of 0.5–1.5% at altitudes 20–40 km. This contribution constitutes a significant percentage of the total error for bright stars. The advanced inversion methods that can minimize the influence of scintillation correction error are also discussed.
Modeling the transport of very short-lived substances into the tropical upper troposphere and lower stratosphere
Authors: Aschmann J. , Sinnhuber B.-M. , Atlas E. L. , Schauffler S. M.
Published: April 2010

Abstract. The transport of very short-lived substances into the tropical upper troposphere and lower stratosphere is investigated by a three-dimensional chemical transport model using archived convective updraft mass fluxes (or detrainment rates) from the European Centre for Medium-Range Weather Forecast's ERA-Interim reanalysis. Large-scale vertical velocities are calculated from diabatic heating rates. With this approach we explicitly model the large scale subsidence in the tropical troposphere with convection taking place in fast and isolated updraft events. The model calculations agree generally well with observations of bromoform and methyl iodide from aircraft campaigns and with ozone and water vapor from sonde and satellite observations. Using a simplified treatment of dehydration and bromine product gas washout we give a range of 1.6 to 3 ppt for the contribution of bromoform to stratospheric bromine, assuming a uniform mixing ratio in the boundary layer of 1 ppt. We show that the most effective region for VSLS transport into the stratosphere is the West Pacific, accounting for about 55% of the bromine from bromoform transported into the stratosphere under the supposition of a uniformly distributed source.
Bacteria in the global atmosphere – Part 2: Modeling of emissions and transport between different ecosystems
Authors: Burrows S. M. , Butler T. , Jöckel P. , Tost H. , Kerkweg A. , Pöschl U. , Lawrence M. G.
Published: April 2010

Abstract. Bacteria are constantly being transported through the atmosphere, which may have implications for human health, agriculture, cloud formation, and the dispersal of bacterial species. We simulate the global transport of bacteria, represented as 1 μm and 3 μm diameter spherical solid particle tracers in a general circulation model. We investigate factors influencing residence time and distribution of the particles, including emission region, cloud condensation nucleus activity and removal by ice-phase precipitation. The global distribution depends strongly on the assumptions made about uptake into cloud droplets and ice. The transport is also affected, to a lesser extent, by the emission region, particulate diameter, and season. We find that the seasonal variation in atmospheric residence time is insufficient to explain by itself the observed seasonal variation in concentrations of particulate airborne culturable bacteria, indicating that this variability is mainly driven by seasonal variations in culturability and/or emission strength. We examine the potential for exchange of bacteria between ecosystems and obtain rough estimates of the flux from each ecosystem by using a maximum likelihood estimation technique, together with a new compilation of available observations described in a companion paper. Globally, we estimate the total emissions of bacteria-containing particles to the atmosphere to be 7.6×1023–3.5×1024 a−1, originating mainly from grasslands, shrubs and crops. We estimate the mass of emitted bacteria- to be 40–1800 Gg a−1, depending on the mass fraction of bacterial cells in the particles. In order to improve understanding of this topic, more measurements of the bacterial content of the air and of the rate of surface-atmosphere exchange of bacteria will be necessary. Future observations in wetlands, hot deserts, tundra, remote glacial and coastal regions and over oceans will be of particular interest.
Seasonal variation of aliphatic amines in marine sub-micrometer particles at the Cape Verde islands
Authors: Müller C. , Iinuma Y. , Karstensen J. , van Pinxteren D. , Lehmann S. , Gnauk T. , Herrmann H.
Published: April 2010

Abstract. Monomethylamine (MA), dimethylamine (DMA) and diethylamine (DEA) were detected at non-negligible concentrations in sub-micrometer particles at the Cap Verde Atmospheric Observatory (CVAO) located on the island of São Vicente in Cape Verde during algal blooms in 2007. The concentrations of these amines in five stage impactor samples ranged from 0–30 pg m−3 for MA, 130–360 pg m−3 for DMA and 5–110 pg m−3 for DEA during the spring bloom in May 2007 and 2–520 pg m−3 for MA, 100–1400 pg m−3 for DMA and 90–760 pg m−3 for DEA during an unexpected winter algal bloom in December 2007. Anomalously high Saharan dust deposition and intensive ocean layer deepening were found at the Atmospheric Observatory and the associated Ocean Observatory during algal bloom periods. The highest amine concentrations in fine particles (impactor stage 2, 0.14–0.42 μm) indicate that amines are likely taken up from the gas phase into the acidic sub-micrometer particles. The contribution of amines to the organic carbon (OC) content ranged from 0.2–2.5% C in the winter months, indicating the importance of this class of compounds to the carbon cycle in the marine environment. Furthermore, aliphatic amines originating from marine biological sources likely contribute significantly to the nitrogen content in the marine atmosphere. The average contribution of the amines to the detected nitrogen species in sub-micrometer particles can be non-negligible, especially in the winter months (0.1% N–1.5% N in the sum of nitrate, ammonium and amines). This indicates that these smaller aliphatic amines can be important for the carbon and the nitrogen cycles in the remote marine environment.
Hit from both sides: tracking industrial and volcanic plumes in Mexico City with surface measurements and OMI SO2 retrievals during the MILAGRO field campaign
Authors: de Foy B. , Krotkov N. A. , Bei N. , Herndon S. C. , Huey L. G. , Martínez A.-P. , Ruiz-Suárez L. G. , Wood E. C. , Zavala M. , Molina L. T.
Published: April 2010

Abstract. Large sulfur dioxide plumes were measured in the Mexico City Metropolitan Area (MCMA) during the MILAGRO field campaign. This paper seeks to identify the sources of these plumes and the meteorological processes that affect their dispersion in a complex mountain basin. Surface measurements of SO2 and winds are analysed in combination with radar wind profiler data to identify transport directions. Satellite retrievals of vertical SO2 columns from the Ozone Monitoring Instrument (OMI) reveal the dispersion from both the Tula industrial complex and the Popocatepetl volcano. Oversampling the OMI swath data to a fine grid (3 by 3 km) and averaging over the field campaign yielded a high resolution image of the average plume transport. Numerical simulations are used to identify possible transport scenarios. The analysis suggests that both Tula and Popocatepetl contribute to SO2 levels in the MCMA, sometimes on the same day due to strong vertical wind shear. During the field campaign, model estimates suggest that the volcano accounts for about one tenth of the SO2 in the MCMA, with a roughly equal split for the rest between urban sources and the Tula industrial complex. The evaluation of simulations with known sources and pollutants suggests that the combination of observations and meteorological models will be useful in identifying sources and transport processes of other plumes observed during MILAGRO.
Large-scale upper tropospheric pollution observed by MIPAS HCN and C2H6 global distributions
Authors: Glatthor N. , von Clarmann T. , Stiller G. P. , Funke B. , Koukouli M. E. , Fischer H. , Grabowski U. , Höpfner M. , Kellmann S. , Linden A.
Published: April 2010

Abstract. We present global upper tropospheric HCN and C2H6 amounts derived from MIPAS/ENVISAT limb emission spectra. HCN and C2H6 are retrieved in the spectral regions 715.5–782.7 cm−1 and 811.5–835.7 cm−1, respectively. The datasets consist of 54 days between September 2003 and March 2004. This period covers the peak and decline of the southern hemispheric biomass burning period and some months thereafter. HCN is a nearly unambiguous tracer of biomass burning with an assumed tropospheric lifetime of several months. Indeed, the most significant feature in the MIPAS HCN dataset is an upper tropospheric plume of enhanced values caused by southern hemispheric biomass burning, which in September and October 2003 extended from tropical South America over Africa, Australia to the Southern Pacific. The spatial extent of this plume agrees well with the MOPITT CO distribution of September 2003. Further there is good agreement with the shapes and mixing ratios of the southern hemispheric HCN and C2H6 fields measured by the ACE experiment between September and November 2005. The MIPAS HCN plume extended from the lowermost observation height of 8 km up to about 16 km altitude, with maximum values of 500–600 pptv in October 2003. It was still clearly visible in December 2003, but had strongly decreased by March 2004, confirming the assumed tropospheric lifetime. The main sources of C2H6 are production and transmission of fossil fuels, followed by biofuel use and biomass burning. The C2H6 distribution also clearly reflected the southern hemispheric biomass burning plume and its seasonal variation, with maximum amounts of 600–700 pptv. Generally there was good spatial overlap between the southern hemispheric distributions of both pollution tracers, except for the region between Peru and the mid-Pacific. Here C2H6was considerably enhanced, whereas the HCN amounts were low. Backward trajectory calculations suggested that industrial pollution was responsible for the elevated C2H6 concentration in these particular air masses. Except for the Asian monsoon anticyclone in September 2003, there were only comparably small regions of enhanced HCN in the Northern Hemisphere. However, C2H6 showed an equally strong northern hemispheric signal between the equator and low midlatitudes, persisting over the whole observation period. Backward trajectory calculations for air masses from this region also point to industrial sources of this pollution. Generally, C2H6/HCN ratios between 1 and 1.5 indicate biomass burning and ratios larger than 1.5 industrial pollution. However, in March 2004 ratios of up to 2 were also found in some regions of the former southern biomass burning plume.
Tropical cirrus and water vapor: an effective Earth infrared iris feedback?
Authors: Fu Q. , Baker M. , Hartmann D. L.
Published: April 2010

Abstract. We revisit a model of feedback processes proposed by Lindzen et al. (2001), in which an assumed 22% reduction in the area of tropical high clouds per degree of sea surface temperature increase produces negative feedbacks associated with upper tropospheric water vapor and cloud radiative effects. We argue that the water vapor feedback is overestimated in Lindzen et al. (2001) by at least 60%, and that the high cloud feedback should be small. Although not mentioned by Lindzen et al, tropical low clouds make a significant contribution to their negative feedback, which is also overestimated. Using more realistic parameters in the model of Lindzen et al., we obtain a feedback factor in the range of −0.15 to −0.51, compared to their larger negative feedback factor of −0.45 to −1.03.
Nucleation events in the continental boundary layer: Influence of physical and meteorological parameters
Authors: Boy M. , Kulmala M.
Published: April 2010

Abstract. The relationship between nucleation events and numerous physical and meteorological parameters was analysed using data collected at the Station for Measuring Forest Ecosystem-Atmosphere Relations (SMEAR II) in Hyytiälä, Finland. To do this, measurements of solar radiation (ultraviolet [UV], global, photosynthetically active radiation [PAR], net, reflected global radiation and reflected PAR), gas concentrations, temperature, humidity, wind direction, horizontal and vertical wind speed, horizontal and vertical wind variances and particle concentrations were collected over a 4 year period. For the year 1999 a detailed analysis of data were completed by examining parameters in order to determine the physical and meteorological conditions favourable to the formation of new particles. A comparison of different wavelength bands during the bursts of new particles led to the suggestion, that UV-A solar radiation seems to be the most probable radiation band concerning the photochemical reactions involved in the production of condensable vapours. Furthermore a high correlation between the daily curves of UV-A irradiance and the concentration of 3–5 nm particles was found throughout the year and examples will be given for two days. During the whole year the concentration of H2O is very low at times nucleation occurs compared to the average of the corresponding month. Especially in June and July many non-event days with high solar irradiance show high amounts of water molecules. To combine these results a "nucleation parameter" was calculated for the year 1999, by dividing UV-A solar radiation by the concentration of H2O and temperature and for clarity all values of the "nucleation parameter" have been divided by the maximum value of the year. Throughout the year nearly all nucleation event days reach a value of 0.2, which means that at this time the "nucleation parameter" reaches 20% of its yearly maximum and non-event days with high values (> 0.1) are mostly accompanied by high concentrations of existing particles.