bluuebunny/crossref_metadata_2025_split huggingface dataset:
Surface tensions of multi-component mixed inorganic/organic aqueous systems of atmospheric significance: measurements, model predictions and importance for cloud activation predictions
Authors: Topping D. O. , McFiggans G. B. , Kiss G. , Varga Z. , Facchini M. C. , Decesari S. , Mircea M. 
Published: April 2010

Abstract. In order to predict the physical properties of aerosol particles, it is necessary to adequately capture the behaviour of the ubiquitous complex organic components. One of the key properties which may affect this behaviour is the contribution of the organic components to the surface tension of aqueous particles in the moist atmosphere. Whilst the qualitative effect of organic compounds on solution surface tensions has been widely reported, our quantitative understanding on mixed organic and mixed inorganic/organic systems is limited. Furthermore, it is unclear whether models that exist in the literature can reproduce the surface tension variability for binary and higher order multi-component organic and mixed inorganic/organic systems of atmospheric significance. The current study aims to resolve both issues to some extent. Surface tensions of single and multiple solute aqueous solutions were measured and compared with predictions from a number of model treatments. On comparison with binary organic systems, two predictive models found in the literature provided a range of values resulting from sensitivity to calculations of pure component surface tensions. Results indicate that a fitted model can capture the variability of the measured data very well, producing the lowest average percentage deviation for all compounds studied. The performance of the other models varies with compound and choice of model parameters. The behaviour of ternary mixed inorganic/organic systems was unreliably captured by using a predictive scheme and this was composition dependent. For more "realistic" higher order systems, entirely predictive schemes performed poorly. It was found that use of the binary data in a relatively simple mixing rule, or modification of an existing thermodynamic model with parameters derived from binary data, was able to accurately capture the surface tension variation with concentration. Thus, it would appear that in order to model multi-component surface tensions involving compounds used in this study one requires the use of appropriate binary data. The effect of deviations between predicted and measured surface tensions on predicted cloud activation properties was quantified, by incorporating the surface tension models into an existing thermodynamic framework. Critical saturation ratios as a function of dry size for all of the multi-component systems were computed and it was found that deviations between predictions increased with decreasing particle dry size. As expected, use of the surface tension of pure water, rather than calculate the influence of the solutes explicitly, led to a consistently higher value of the critical saturation ratio indicating that neglect of the compositional effects will lead to significant differences in predicted activation behaviour even at large particle dry sizes.
Contribution of mixing to the upward transport across the TTL
Authors: Konopka P. , Günther G. , Müller R. , dos Santos F. H. S. , Schiller C. , Ravegnani F. , Ulanovsky A. , Schlager H. , Volk C. M. , Viciani S. , Pan L. , McKenna D.-S. , Riese M. 
Published: April 2010

Abstract. During the second part of the TROCCINOX campaign that took place in Brazil in early 2005, chemical species were measured on-board of the high altitude research aircraft Geophysica (ozone, water vapor, NO, NOy, CH4 and CO) in the altitude range up to 20 km (or up to 450 K potential temperature), i.e. spanning the TTL region roughly extending between 350 and 420 K. Analysis of transport across TTL is performed using a new version of the Chemical Lagrangian Model of the Stratosphere (CLaMS). In this new version, the stratospheric model has been extended to the earth surface. Above the tropopause, the isentropic and cross-isentropic advection in CLaMS is driven by ECMWF winds and heating/cooling rates derived from a radiation calculation. Below the tropopause the model smoothly transforms from the isentropic to hybrid-pressure coordinate and, in this way, takes into account the effect of large-scale convective transport as implemented in the ECMWF vertical wind. As with other CLaMS simulations, the irreversible transport, i.e. mixing, is controlled by the local horizontal strain and vertical shear rates. Stratospheric and tropospheric signatures in the TTL can be seen both in the observation and in the model. The composition of air above ≈350 K is mainly controlled by mixing on a time scale of weeks or even months. Based on CLaMS transport studies where mixing can be completely switched off, we deduce that vertical mixing, mainly driven by the vertical shear in the outflow regions of the large-scale convection and in the vicinity of the subtropical jets, is necessary to understand the upward transport of the tropospheric air from the main convective outflow around 350 K up to the tropical tropopause around 380 K. This mechanism is most effective if the outflow of the mesoscale convective systems interacts with the subtropical jets.
Efficiency of the deposition mode ice nucleation on mineral dust particles
Authors: Möhler O. , Field P. R. , Connolly P. , Benz S. , Saathoff H. , Schnaiter M. , Wagner R. , Cotton R. , Krämer M. , Mangold A. , Heymsfield A. J. 
Published: April 2010

Abstract. The deposition mode ice nucleation efficiency of various dust aerosols was investigated at cirrus cloud temperatures between 196 K and 223 K using the aerosol chamber facility AIDA (Aerosol Interaction and Dynamics in the Atmosphere). Arizona test dust (ATD) as a reference material and two dust samples from the Takla Makan desert in Asia (AD1) and Sahara (SD2) were used for the experiments at simulated cloud conditions. The dust particle sizes were almost lognormally distributed with mode diameters between 0.3 µm and 0.5 µm and geometric standard deviations between 1.6 and 1.9. Deposition ice nucleation was most efficient on ATD particles with ice-active particle fractions of about 0.6 and 0.8 at an ice saturation ratio Si<1.15 and temperatures of 223 K and 209 K, respectively. No significant change of the ice nucleation efficiency was found in up to three subsequent cycles of ice activation and evaporation with the same ATD aerosol. The desert dust samples SD2 and AD1 showed a significantly lower fraction of active deposition nuclei, about 0.25 at 223 K and Si<1.35. For all samples the ice activated aerosol fraction could be approximated by an exponential equation as function of Si. This formulation of ice activation spectra may be used to calculate the formation rate of ice crystals in models, if the number concentration of dust particles is known. More experimental work is needed to quantify the variability of the ice activation spectra as function of the temperature and dust particle properties.
Imaging gravity waves in lower stratospheric AMSU-A radiances, Part 1: simple forward model
Authors: Eckermann S. D. , Wu D. L. 
Published: April 2010

Abstract. Using a simplified model of in-orbit radiance acquisition by the Advanced Microwave Sounding Unit (AMSU-A), we derive three-dimensional temperature weighting functions for Channel 9 measurements (peaking at ~60–90 hPa) at all 30 cross-track beam positions and use them to investigate the sensitivity of these radiances to gravity waves. The vertical widths of the weighting functions limit detection to waves with vertical wavelengths of ≳10 km, with slightly better vertical wavelength sensitivity at the outermost scan angles due to the limb effect. Fourier Transforms of two-dimensional cross-track weighting functions reveal optimal sensitivity to cross-track wavelengths at the near-nadir scan angles, where horizontal measurement footprints are smallest. This sensitivity is greater for the AMSU-A on the Aqua satellite than for the identical instruments on the NOAA meteorological satellites, due to a lower orbit altitude and thus smaller horizontal footprints from antenna spreading. Small cross-track asymmetries in the radiance response to gravity waves are found that peak at the mid-range scan angles, with more symmetric responses at near-nadir and far off-nadir scan angles. Three-dimensional simulations show gravity wave oscillations imaged in horizontal AMSU-A radiance maps swept out by the scan pattern and satellite motion. A distorting curvature is added to imaged wave phase lines due to vertical variations in weighting function peaks with cross-track scan angle. This wave distortion is analogous to the well-known ''limb darkening'' and ''limb brightening'' of microwave radiances acquired from purely vertical background temperature profiles by cross-track scanners. Waves propagating along track are more visible in these images at the outermost scan angles than those propagating cross track, due to oversampling and narrower widths of the horizontal measurement footprints in the along track direction. Based on nominal noise floors and representative lower stratospheric wave temperature amplitudes, our modeling indicates that Channel 9 AMSU-A radiances can resolve and horizontally image gravity waves with horizontal wavelengths of ≳150 km and vertical wavelengths of ≳10 km.
Measuring atmospheric CO2 from space using Full Spectral Initiation (FSI) WFM-DOAS
Authors: Barkley M. P. , Frieß U. , Monks P. S. 
Published: April 2010

Abstract. Satellite measurements of atmospheric CO2 concentrations are a rapidly evolving area of scientific research which can help reduce the uncertainties in the global carbon cycle fluxes and provide insight into surface sources and sinks. One of the emerging CO2 measurement techniques is a relatively new retrieval algorithm called Weighting Function Modified Differential Optical Absorption Spectroscopy (WFM-DOAS) that has been developed by Buchwitz et al. (2000). This algorithm is designed to measure the total columns of CO2 (and other greenhouse gases) through the application to spectral measurements in the near infrared (NIR), made by the SCIAMACHY instrument on-board ENVISAT. The algorithm itself is based on fitting the logarithm of a model reference spectrum and its derivatives to the logarithm of the ratio of a measured nadir radiance and solar irradiance spectrum. In this work, a detailed error assessment of this technique has been conducted and it has been found necessary to include suitable a priori information within the retrieval in order to minimize the errors on the retrieved CO2 columns. Hence, a new CO2 retrieval algorithm called Full Spectral Initiation (FSI) WFM-DOAS has been developed which generates a reference spectrum for each individual SCIAMACHY observation using the known properties of the atmosphere and surface at the time of the measurement. Initial retrievals over Siberia during the summer of 2003 show that the measured CO2 columns are not biased from the input a priori data and that whilst the monthly averaged CO2 distributions contain a high degree of variability, they also contain significant spatial features.
Methane production from mixed tropical savanna and forest vegetation in Venezuela
Authors: Crutzen P. J. , Sanhueza E. , Brenninkmeijer C. A. M. 
Published: April 2010

Abstract. Measurements of methane concentrations in the boundary layer in the northern part of the Guayana shield, Venezuela, during the wet season (October 1988), showed the presence of substantial methane surface emissions. The measuring site is within the savanna climate region, but is affected by emissions from savanna and forest vegetation. From day versus night concentration measurements, with higher concentrations during night, a methane source strength near the site of 3–7×1011 molecules/cm2/s can be estimated, which includes emissions from small tracts of flooded soils, termites and especially tropical vegetation. Extrapolated to the entire savanna, this may imply a methane source of ~30–60 Tg yr−1 similar to the one calculated for tropical vegetation on the basis of recently published in vitro plant emission experiments by Keppler et al. (2006), which indicate emissions of ~30 Tg yr−1 for tropical savannas and grasslands and ~78 Tg yr−1 for tropical forests.
The composition of nucleation and Aitken modes particles during coastal nucleation events: evidence for marine secondary organic contribution
Authors: Vaattovaara P. , Huttunen P. E. , Yoon Y. J. , Joutsensaari J. , Lehtinen K. E. J. , O’Dowd C. D. , Laaksonen A. 
Published: April 2010

Abstract. Newly-formed nanometer-sized particles have been observed at coastal and marine environments worldwide. Interestingly, organic species have so far not been detected in those newly-formed nucleation mode particles. In this study, we applied the UFO-TDMA (ultrafine organic tandem differential mobility analyzer) method to study the possible existence of an organic fraction in recently formed coastal nucleation mode particles (d<20 nm) at the Mace Head research station. Furthermore, effects of those nucleation events to potential CCN (cloud condensation nuclei) were studied. The coastal events were typical for the Mace Head region and they occurred at low tide conditions during efficient solar radiation and high biological activity (HBA, i.e. a high mass concentration of chlorophyll a of the ocean) in spring 2002. Additionally, a PHA-UCPC (pulse height analyzer ultrafine condensation particle counter) technique was used to study the composition of newly-formed particles formed in low tide conditions during a lower biological activity (LBA, i.e. a lower mass concentration of chlorophyll a of the ocean) in October 2002. The overall results of the UFO-TDMA and the PHA-UCPC measurements indicate that those coastally/marinely formed nucleation mode particles include a remarkable fraction of secondary organic products, beside iodine oxides, which are likely to be responsible for the nucleation. During clean marine air mass conditions, the origin of those secondary organic oxidation compounds can be related to marine/coastal biota and thus a major fraction of the organics may originate from biosynthetic production of alkenes such as isoprene and their oxidation by iodine, hydroxyl radical, and ozone. During modified marine conditions, also anthropogenic secondary organic compounds may contribute to the nucleation mode organic mass, in addition to biogenic secondary organic compounds. Thus, the UFO-TDMA results suggest that the secondary organic compounds may, in addition to being significant contributors to the nucleation mode processes, accelerate the growth of freshly nucleated particles and increase their survival probability to CCN and even larger radiatively active particle sizes. The results give new insights to the coastal/marine particle formation, growth, and properties. The marine biota driven secondary organic contributions to coastal/marine particle formation and composition can be anticipated in other species specific biologically active oceans and fresh-waters areas around the world and thus, they may be significant also to the global radiative bugdet, atmosphere-biosphere feedbacks, and climate change.
Importance of the surface reaction OH+Cl- on sea salt aerosol for the chemistry of the marine boundary layer – a model study
Authors: von Glasow R. 
Published: April 2010

Abstract. The reaction of the hydroxyl radical with chloride on the surface of sea salt aerosol producing gas phase Cl2 and particulate OH- and its implications for the chemistry of the marine boundary layer under coastal, remote, and very remote conditions have been investigated with a numerical model. This reaction had been suggested by Laskin et al. (2003) to play a major role in the sulfur cycle in the marine boundary layer by increasing the sulfate production in sea salt by O3 oxidation due to the additional production of alkalinity in the particle. Based on literature data a new &amp;quotbest estimate'' for the rate coefficient of the reaction was deduced and applied, showing that the additional initial sulfate production by this reaction is less than 1%, therefore having only a minor impact on sulfate production. Even though the gas phase concentration of Cl2 increased strongly in the model the concentration of Cl radicals increased by less than 5% for the &amp;quotbest guess'' case. Additional feedbacks between the cycles of chlorine and sulfur in the marine boundary layer are discussed as well as a two-stage acidification of large fresh sea salt aerosol.
First space-borne measurements of methanol inside aged tropical biomass burning plumes using the ACE-FTS instrument
Authors: Dufour G. , Boone C. D. , Rinsland C. P. , Bernath P. F. 
Published: April 2010

Abstract. First measurements from space of upper tropospheric and lower stratospheric methanol profiles within aged fire plumes are reported. Elevated levels of methanol at 0–45° S from 30 September to 3 November 2004 have been measured by the high resolution infrared spectrometer ACE-FTS onboard the SCISAT satellite. Methanol volume mixing ratios higher than 4000 pptv are detected and are strongly correlated with other fire products such as CO, C2H6, and HCN. A sensitivity study of the methanol retrieval, accounting for random and systematic contributions, shows that the retrieved methanol profile is reliable from 8.5 to 16.5 km, with an accuracy of about 20% for measurements inside polluted air masses. The upper tropospheric enhancement ratio of methanol with respect to CO is estimated from the correlation plot between methanol and CO for aged tropical biomass burning plumes. This ratio is in good agreement with the ratio measured in the free troposphere (up to 12 km) by recent aircraft studies and does not suggest any secondary production of methanol by oxidation in aged biomass burning plumes.
Correlation between traffic density and particle size distribution in a street canyon and the dependence on wind direction
Authors: Voigtländer J. , Tuch T. , Birmili W. , Wiedensohler A. 
Published: April 2010

Abstract. Combustion of fossil fuel in gasoline and diesel powered vehicles is a major source of aerosol particles in a city. In a street canyon, the number concentration of particles smaller than 300 nm in diameter, which can be inhaled and cause serious health effects, is dominated by particles originating from this source. In this study we measured both, particle number size distribution and traffic density continuously in a characteristic street canyon in Germany for a time period of 6 months. The street canyon with multistory buildings and 4 traffic lanes is very typical for larger cities. Thus, the measurements are also representative for many other street canyons. In contrast to previous studies, we measured and analyzed the particle number size distribution with high size resolution using a Twin Differential Mobility Analyzer (TDMPS). The measured size range was from 3 to 800 nm, separated into 40 size channels. Correlation coefficients between particle number concentration for integrated size ranges and traffic up to 0.5 counts were determined. Correlations were also calculated for each of the 40 size channels of the DMPS system, respectively. We found two maxima of the correlation coefficient for particles about 10 nm and in the size range 60–80 nm in diameter. Furthermore, correlations between traffic and particles in dependence of meteorological data were calculated. Relevant parameters were identified by a multiple regression method. In our experiment only wind parameters have influenced the particle number concentration significantly. Very high correlation coefficients (up to 0.85) could be observed in the lee side of the street canyon as well as particles in the range between 60 and 80 nm in diameter. These values are significantly higher than correlation coefficients for other wind directions and other particle sizes. A minimum was found in the luff side of the street. These findings are in good agreement with theory of fluid dynamics in street canyons.
Key aspects of stratospheric tracer modeling
Authors: Bregman B. , Meijer E. , Scheele R. 
Published: April 2010

Abstract. This study describes key aspects of global chemistry-transport models and the impact on stratospheric tracer transport. We concentrate on global models that use assimilated winds from numerical weather predictions, but the results also apply to tracer transport in general circulation models. We examined grid resolution, numerical diffusion and dispersion of the winds fields, the meteorology update time intervals, update frequency, and time interpolation. For this study we applied the three-dimensional chemistry-transport Tracer Model version 5 (TM5) and a trajectory model and performed several diagnoses focusing on different transport regimes. Covering different time and spatial scales, we examined (1) polar vortex dynamics during the Arctic winter, (2) the large-scale stratospheric meridional circulation, and (3) air parcel dispersion in the tropical lower stratosphere. Tracer distributions inside the Arctic polar vortex show considerably worse agreement with observations when the model grid resolution in the polar region is reduced to avoid numerical instability. Using time interpolated winds improve the tracer distributions only marginally. Considerable improvement is found when the update frequency of the assimilated winds is increased from 6 to 3h, both in the large-scale tracer distribution and the polar regions. It further reduces in particular the vertical dispersion of air parcels in the tropical lower stratosphere. The results in this study demonstrates significant progress in the use of assimilated meteorology in chemistry-transport models, which is important for both short- and long-term integrations.