bluuebunny/crossref_metadata_2025 huggingface dataset:
Effects of the physical state of tropospheric ammonium-sulfate-nitrate particles on global aerosol direct radiative forcing
Authors: Martin S. T. , Hung H.-M. , Park R. J. , Jacob D. J. , Spurr R. J. D. , Chance K. V. , Chin M.
Published: April 2010

Abstract. The effect of aqueous versus crystalline sulfate-nitrate-ammonium tropospheric particles on global aerosol direct radiative forcing is assessed. A global three-dimensional chemical transport model predicts sulfate, nitrate, and ammonium aerosol mass. An aerosol thermodynamics model is called twice, once for the upper side (US) and once for lower side (LS) of the hysteresis loop of particle phase. On the LS, the sulfate mass budget is 40% solid ammonium sulfate, 12% letovicite, 11% ammonium bisulfate, and 37% aqueous. The LS nitrate mass budget is 26% solid ammonium nitrate, 7% aqueous, and 67% gas-phase nitric acid release due to increased volatility upon crystallization. The LS ammonium budget is 45% solid ammonium sulfate, 10% letovicite, 6% ammonium bisulfate, 4% ammonium nitrate, 7% ammonia release due to increased volatility, and 28% aqueous. LS aerosol water mass partitions as 22% effloresced to the gas-phase and 78% remaining as aerosol mass. The predicted US/LS global fields of aerosol mass are employed in a Mie scattering model to generate global US/LS aerosol optical properties, including scattering efficiency, single scattering albedo, and asymmetry parameter. Global annual average LS optical depth and mass scattering efficiency are, respectively, 0.023 and 10.7 m2 (g SO4-2)-1, which compare to US values of 0.030 and 13.9 m2 (g SO4-2)-1. Radiative transport is computed, first for a base case having no aerosol and then for the two global fields corresponding to the US and LS of the hysteresis loop. Regional, global, seasonal, and annual averages of top-of-the-atmosphere aerosol radiative forcing on the LS and US (FL and FU, respectively, in W m-2) are calculated. Including both anthropogenic and natural emissions, we obtain global annual averages of FL=-0.750, FU=-0.930, and DFU,L=24% for full sky calculations without clouds and FL=-0.485, FU=-0.605, and DFU,L=25% when clouds are included. Regionally, DFU,L=48% over the USA, 55% over Europe, and 34% over East Asia. Seasonally, DFU,L varies from 18% in DJF to 75% in SON over the USA. The global annual average contribution from anthropogenic aerosol is FL=-0.314 and FU=-0.404, which yield normalized direct radiative forcings (G) of GL=-205 W (g SO4-2)-1 and GU=-264 W (g SO4-2)-1.
Highly resolved global distribution of tropospheric NO2 using GOME narrow swath mode data
Authors: Beirle S. , Platt U. , Wenig M. , Wagner T.
Published: April 2010

Abstract. The Global Ozone Monitoring Experiment (GOME) allows the retrieval of tropospheric vertical column densities (VCDs) of NO2 on a global scale. Regions with enhanced industrial activity can clearly be detected, but the standard spatial resolution of the GOME ground pixels (320x40km2) is insufficient to resolve regional trace gas distributions or individual cities. Every 10 days within the nominal GOME operation, measurements are executed in the so called narrow swath mode with a much better spatial resolution (80x40km2). We use this data (1997-2001) to construct a detailed picture of the mean global tropospheric NO2 distribution. Since - due to the narrow swath - the global coverage of the high resolution observations is rather poor, it has proved to be essential to deseasonalize the single narrow swath mode observations to retrieve adequate mean maps. This is done by using the GOME backscan information. The retrieved high resolution map illustrates the shortcomings of the standard size GOME pixels and reveals an unprecedented wealth of details in the global distribution of tropospheric NO2. Localised spots of enhanced NO2 VCD can be directly associated to cities, heavy industry centers and even large power plants. Thus our result helps to check emission inventories. The small spatial extent of NO2 "hot spots" allows us to estimate an upper limit of the mean lifetime of boundary layer NOx of 17h on a global scale. The long time series of GOME data allows a quantitative comparison of the narrow swath mode data to the nominal resolution. Thus we can analyse the dependency of NO2 VCDs on pixel size. This is important for comparing GOME data to results of new satellite instruments like SCIAMACHY (launched March 2002 on ENVISAT), OMI (launched July 2004 on AURA) or GOME II (to be launched 2005) with an improved spatial resolution.
Heterogeneous freezing of single sulfuric acid solution droplets: laboratory experiments utilizing an acoustic levitator
Authors: Ettner M. , Mitra S. K. , Borrmann S.
Published: April 2010

Abstract. The heterogeneous freezing temperatures of single binary sulfuric acid solution droplets were measured in dependency of acid concentration down to temperatures as low as -50°C. In order to avoid influence of supporting substrates on the freezing characteristics, a new technique has been developed to suspend the droplet by means of an acoustic levitator. The droplets contained immersed particles of graphite, kaolin or montmorillonite in order to study the influence of the presence of such contamination on the freezing temperature. The radii of the suspended droplets spanned the range between 0.4 and 1.1mm and the concentration of the sulfuric acid solution varied between 5 and 14 weight percent. The presence of the particles in the solution raises the freezing temperature with respect to homogeneous freezing of these solution droplets. The pure solution droplets can be supercooled up to 40 degrees below the ice-acid solution thermodynamic equilibrium curve. Depending on the concentration of sulfuric acid and the nature of the impurity the polluted droplets froze between -11°C and -35°C. The new experimental set-up, combining a deep freezer with a movable ultrasonic levitator and suitable optics, proved to be a useful approach for such investigations on individual droplets.
Global carbon monoxide as retrieved from SCIAMACHY by WFM-DOAS
Authors: Buchwitz M. , de Beek R. , Bramstedt K. , Noël S. , Bovensmann H. , Burrows J. P.
Published: April 2010

Abstract. First results concerning the retrieval of tropospheric carbon monoxide (CO) from satellite solar backscatter radiance measurements in the near-infrared spectral region (~2.3µm) are presented. The Weighting Function Modified (WFM) DOAS retrieval algorithm has been used to retrieve vertical columns of CO from SCIAMACHY/ENVISAT nadir spectra. We present detailed results for three days from the time periode January to October 2003 selected to have good overlap with the daytime CO measurements of MOPITT onboard EOS Terra. Because the WFM-DOAS Version 0.4 CO columns presented in this paper are scaled by a constant factor of 0.5 to compensate for an obvious overestimation we focus on the variability of the retrieved columns rather than on their absolute values. It is shown that plumes of CO resulting from, e.g. biomass burning in Africa, are detectable with single overpass SCIAMACHY data. Globally, the SCIAMACHY CO columns are in reasonable agreement with the Version 3 CO column data product of MOPITT. For example, for measurements over land, where the quality of the data is typically better than over ocean due to higher surface reflectivity, the standard deviation of the difference with respect to MOPITT is in the range 0.4-0.6x1018 molecules/cm2 and the linear correlation coefficient is between 0.4 and 0.7. The level of agreement between the data of both sensors depends on time and location but is typically within 30% for most latitudes. In the southern hemisphere outside Antarctica SCIAMACHY tends to give systematically higher values than MOPITT. More studies are needed to find out what the reasons for the observed differences with respect to MOPITT are and how the algorithm can be modified to improve the quality of the CO columns as retrieved from SCIAMACHY.
Laboratory evidence for volume-dominated nucleation of ice in supercooled water microdroplets
Authors: Duft D. , Leisner T.
Published: April 2010

Abstract. We report on measurements of the rate of homogeneous ice nucleation in supercooled water microdroplets levitated in an electrodynamic balance. By comparison of the freezing probability for droplets of radius 49µm and 19µm, we are able to conclude that homogeneous freezing is a volume-proportional process and that surface nucleation might only be important, if at all, for much smaller droplets.
Formation of solid particles in synoptic-scale Arctic PSCs in early winter 2002/2003
Authors: Larsen N. , Knudsen B. M. , Svendsen S. H. , Deshler T. , Rosen J. M. , Kivi R. , Weisser C. , Schreiner J. , Mauerberger K. , Cairo F. , Ovarlez J. , Oelhaf H. , Spang R.
Published: April 2010

Abstract. Polar stratospheric clouds (PSC) have been observed in early winter (December 2002) during the SOLVE II/Vintersol campaign, both from balloons carrying comprehensive instrumentation for measurements of chemical composition, size distributions, and optical properties of the particles, as well as from individual backscatter soundings from Esrange and Sodankylä. The observations are unique in the sense that the PSC particles seem to have formed in the early winter under synoptic temperature conditions and not being influenced by mountain lee waves. A sequence of measurements during a 5-days period shows a gradual change between liquid and solid type PSCs with the development of a well-known sandwich structure. It appears that all PSC observations show the presence of a background population of solid particles, occasionally mixed in with more optically dominating liquid particles. The measurements have been compared with results from a detailed microphysical and optical simulation of the formation processes. Calculated extinctions are in good agreement with SAGE-III measurements from the same period. Apparently the solid particles are controlled by the synoptic temperature history while the presence of liquid particles is controlled by the local temperatures at the time of observation. The temperature histories indicate that the solid particles are nucleated above the ice frost point, and a surface freezing mechanism for this is included in the model. Reducing the calculated freezing rates by a factor 10-20, the model is able to simulate the observed particle size distributions and reproduce observed HNO3 gas phase concentrations.
Systematic reduction of complex tropospheric chemical mechanisms, Part I: sensitivity and time-scale analyses
Authors: Whitehouse L. E. , Tomlin A. S. , Pilling M. J.
Published: April 2010

Abstract. Explicit mechanisms describing the complex degradation pathways of atmospheric volatile organic compounds (VOCs) are important, since they allow the study of the contribution of individual VOCS to secondary pollutant formation. They are computationally expensive to solve however, since they contain large numbers of species and a wide range of time-scales causing stiffness in the resulting equation systems. This paper and the following companion paper describe the application of systematic and automated methods for reducing such complex mechanisms, whilst maintaining the accuracy of the model with respect to important species and features. The methods are demonstrated via application to version 2 of the Leeds Master Chemical Mechanism. The methods of Jacobian analysis and overall rate sensitivity analysis proved to be efficient and capable of removing the majority of redundant reactions and species in the scheme across a wide range of conditions relevant to the polluted troposphere. The application of principal component analysis of the rate sensitivity matrix was computationally expensive due to its use of the decomposition of very large matrices, and did not produce significant reduction over and above the other sensitivity methods. The use of the quasi-steady state approximation (QSSA) proved to be an extremely successful method of removing the fast time-scales within the system, as demonstrated by a local perturbation analysis at each stage of reduction. QSSA species were automatically selected via the calculation of instantaneous QSSA errors based on user-selected tolerances. The application of the QSSA led to the removal of a large number of alkoxy radicals and excited Criegee bi-radicals via reaction lumping. The resulting reduced mechanism was shown to reproduce the concentration profiles of the important species selected from the full mechanism over a wide range of conditions, including those outside of which the reduced mechanism was generated. As a result of a reduction in the number of species in the scheme of a factor of 2, and a reduction in stiffness, the computational time required for simulations was reduced by a factor of 4 when compared to the full scheme.
The vertical distribution of aerosols, Saharan dust and cirrus clouds in Rome (Italy) in the year 2001
Authors: Gobbi G. P. , Barnaba F. , Ammannato L.
Published: April 2010

Abstract. A set of 813 lidar profiles of tropospheric aerosol and cirrus clouds extinction and depolarization observed in Rome, Italy, between February 2001 and February 2002 is analyzed and discussed. The yearly record reveals a meaningful contribution of both cirrus clouds (38%) and Saharan dust (12%) to the total optical thickness (OT) of 0.26, at 532nm. Seasonal analysis shows the planetary boundary layer (PBL) aerosols to be confined below 2km in winter and 3.8km in summer, with relevant OT shifting from 0.08 to 0.16, respectively. Cirrus clouds maximise in spring and autumn, in both cases with average OT similar to the PBL aerosols one. With the exception of winter months, Saharan dust is found to represent an important third layer mostly residing between PBL aerosols and cirrus clouds, with yearly average OT0.03. Saharan dust and cirrus clouds were detected in 20% and in 45% of the observational days, respectively. Validation of the lidar OT retrievals against collocated sunphotometer observations show very good agreement. These results represent one of the few yearly records of tropospheric aerosol vertical profiles available in the literature.
Measurements of the sum of HO2NO2 and CH3O2NO2 in the remote troposphere
Authors: Murphy J. G. , Thornton J. A. , Wooldridge P. J. , Day D. A. , Rosen R. S. , Cantrell C. , Shetter R. E. , Lefer B. , Cohen R. C.
Published: April 2010

Abstract. The chemistry of peroxynitric acid (HO2NO2) and methyl peroxynitrate (CH3O2NO2)is predicted to be particularly important in the upper troposphere where temperatures are frequently low enough that these compounds do not rapidly decompose. At temperatures below 240K, we calculate that about 20% of NOy in the mid- and high-latitude upper troposphere is HO2NO2. Under these conditions, the reaction of OH with HO2NO2 is estimated to account for as much as one third of the permanent loss of hydrogen radicals. During the Tropospheric Ozone Production about the Spring Equinox (TOPSE) campaign, we used thermal dissociation laser-induced fluorescence (TD-LIF) to measure the sum of peroxynitrates (PNs HO2NO2+CH3O2NO2+PAN+PPN+...) aboard the NCAR C-130 research aircraft. We infer the sum of HO2NO2 and CH3O2NO2 as the difference between PN measurements and gas chromatographic measurements of the two major peroxy acyl nitrates, peroxy acetyl nitrate (PAN) and peroxy propionyl nitrate (PPN). Comparison with NOy and other nitrogen oxide measurements confirms the importance of HO2NO2 and CH3O2NO2 to the reactive nitrogen budget and shows that current thinking about the chemistry of these species is approximately correct. During the spring high latitude conditions sampled during the TOPSE experiment, the model predictions of the contribution of (HO2NO2+CH3O2NO2) to NOy are highly temperature dependent: on average 30% of NOy at 230K, 15% of NOy at 240K, and 5% of NOy above 250K. The temperature dependence of the inferred concentrations corroborates the contribution of overtone photolysis to the photochemistry of peroxynitric acid. A model that includes IR photolysis (J=1x10-5s-1) agreed with the observed sum of HO2NO2+CH3O2NO2 to better than 35% below 240K where the concentration of these species is largest.
Technical note: an interannual inversion method forcontinuous CO2 data
Authors: Law R. M.
Published: April 2010

Abstract. A sequential synthesis inversion method is described to estimate CO2 sources from continuous atmospheric data. The sequential method makes the problem computationally feasible. The method is assessed using four-hourly synthetic concentration data generated from known sources. Multi-year mean sources and seasonal cycles are estimated with comparable quality as those from a traditional inversion of monthly mean data. Interannual variations in the estimated sources are closer to those of the known sources using the four-hourly data rather than monthly data. The computational cost of the basis function simulations can be reduced by generating responses that are only six months long. This does not significantly degrade the inversion results compared to using responses that are 12 months in length.
Quantification of topographic venting of boundary layer air to the free troposphere
Authors: Henne S. , Furger M. , Nyeki S. , Steinbacher M. , Neininger B. , de Wekker S. F. J. , Dommen J. , Spichtinger N. , Stohl A. , Prévôt A. S. H.
Published: April 2010

Abstract. Net vertical air mass export by thermally driven flows from the atmospheric boundary layer (ABL) to the free troposphere (FT) above deep Alpine valleys was investigated. The vertical export of pollutants above mountainous terrain is presently poorly represented in global chemistry transport models (GCTMs) and needs to be quantified. Air mass budgets were calculated using aircraft observations obtained in deep Alpine valleys. The results show that on average 3 times the valley air mass is exported vertically per day under fair weather conditions. During daytime the type of valleys investigated in this study can act as an efficient "air pump" that transports pollutants upward. The slope wind system within the valley plays an important role in redistributing pollutants. Nitrogen oxide emissions in mountainous regions are efficiently injected into the FT. This could enhance their ozone (O3) production efficiency and thus influences tropospheric pollution budgets. Once lifted to the FT above the Alps pollutants are transported horizontally by the synoptic flow and are subject to European pollution export. Forward trajectory studies show that under fair weather conditions two major pathways for air masses above the Alps dominate. Air masses moving north are mixed throughout the whole tropospheric column and further transported eastward towards Asia. Air masses moving south descend within the subtropical high pressure system above the Mediterranean.
The EISCAT meteor-head method – a review and recent observations
Authors: Pellinen-Wannberg A.
Published: April 2010

Abstract. Since the very first meteor observations at EISCAT in December 1990, the experimental method has improved significantly. This is due to a better understanding of the phenomenon and a recent major upgrade of the EISCAT signal processing and data storage capabilities. Now the simultaneous spatial-time resolution is under 100 m-ms class. To illuminate the meteor target for as long as possible and simultaneously get as good altitude resolution as possible, various coding techniques have been used, such as Barker codes and random codes with extremely low side lobe effects. This paper presents some background and the current view of the meteor head echo process at EISCAT as well as the observations which support this view, such as altitude distributions, dual-frequency target sizes and vector velocities. It also presents some preliminary results from recent very high resolution tristatic observations.
The impact of anthropogenic chlorine emissions, stratospheric ozone change and chemical feedbacks on stratospheric water
Authors: Röckmann T. , Grooß J.-U. , Müller R.
Published: April 2010

Abstract. Mixing ratios of water (H2O) in the stratosphere appear to increase due to increased input of H2O and methane from the troposphere and due to intensified oxidation of CH4 in the stratosphere, but many of the underlying mechanisms are not yet understood. Here we identify and quantify three chemical mechanisms which must have led to more efficient oxidation of CH4 in the stratosphere over the past several decades: 1) The increase in stratospheric chlorine levels due to anthropogenic CFC emissions, 2) the thinning of the stratospheric ozone column and 3) enhanced OH levels in the stratosphere due to increasing H2O levels themselves. In combination with the increase in tropospheric CH4 mixing ratios and with solar cycle related variations of upper stratospheric ozone, these effects can explain about 50% of the additional conversion of CH4 to H2O as observed throughout the stratosphere. The relative contributions from the individual processes have varied over the past decades.
Technical Note: A diagnostic for ozone contributions of various NOx emissions in multi-decadal chemistry-climate model simulations
Authors: Grewe V.
Published: April 2010

Abstract. Nitrogen oxide (NOx=NO+NO2) emissions from various sources contribute to the ozone budget. The identification of these contributions is important, e.g. for the assessment of emissions from traffic. The non-linear character of ozone chemistry complicates the online diagnosis during multi-decadal chemistry-climate simulations. A methodology is suggested, which is efficient enough to be incorporated in multi-decadal simulations. Eight types of NOx emissions are included in the model. For each a NOy (=all N components, except N2 and N2O) tracer and an ozone tracer is included in the model, which experience the same emissions and loss processes like the online chemistry fields. To calculate the ozone changes caused by an individual NOx emission, the assumption is made that the NOx relative contributions from various sources are identical to the NOy relative contributions. To evaluate this method each NOx emission has been increased by 5% and a detailed error analysis is given. In the regions of the main impact of individual sources the potential error of the calculated contribution is significantly smaller than the contribution. Moreover, the changes caused by an increase of the emissions of 5% were detected with a higher accuracy than the potential error of the absolute contribution.
Tracing troposphere-to-stratosphere transport above a mid-latitude deep convective system
Authors: Hegglin M. I. , Brunner D. , Wernli H. , Schwierz C. , Martius O. , Hoor P. , Fischer H. , Parchatka U. , Spelten N. , Schiller C. , Krebsbach M. , Weers U. , Staehelin J. , Peter Th.
Published: April 2010

Abstract. Within the project SPURT (trace gas measurements in the tropopause region) a variety of trace gases have been measured in situ in order to investigate the role of dynamical and chemical processes in the extra-tropical tropopause region. In this paper we report on a flight on 10 November 2001 leading from Hohn, Germany (52ºN) to Faro, Portugal (37ºN) through a strongly developed deep stratospheric intrusion. This streamer was associated with a large convective system over the western Mediterranean with potentially significant troposphere-to-stratosphere transport. Along major parts of the flight we measured unexpectedly high NOy mixing ratios. Also H2O mixing ratios were significantly higher than stratospheric background levels confirming the extraordinary chemical signature of the probed air masses in the interior of the streamer. Backward trajectories encompassing the streamer enable to analyze the origin and physical characteristics of the air masses and to trace troposphere-to-stratosphere transport. Near the western flank of the intrusion features caused by long range transport, such as tropospheric filaments characterized by sudden drops in the O3 and NOy mixing ratios and enhanced CO and H2O can be reconstructed in great detail using the reverse domain filling technique. These filaments indicate a high potential for subsequent mixing with the stratospheric air. At the south-western edge of the streamer a strong gradient in the NOy and the O3 mixing ratios coincides very well with a sharp gradient in potential vorticity in the ECMWF fields. In contrast, in the interior of the streamer the observed highly elevated NOy and H2O mixing ratios up to a potential temperature level of 365 K and potential vorticity values of maximum 10 PVU cannot be explained in terms of resolved troposphere-to-stratosphere transport along the backward trajectories. Also mesoscale simulations with a High Resolution Model reveal no direct evidence for convective H2O injection up to this level. Elevated H2O mixing ratios in the ECMWF and HRM model are seen only up to about tropopause height at 340 hPa and 270hPa, respectively, well below flight altitude of about 200 hPa. However, forward tracing of the convective influence as identified by satellite brightness temperature measurements and counts of lightning strokes shows that during this part of the flight the aircraft was closely following the border of an air mass which was heavily impacted by convective activity over Spain and Algeria. This is evidence that deep convection at mid-latitudes may have a large impact on the tracer distribution of the lowermost stratosphere reaching well above the thunderstorms anvils as claimed by recent studies using cloud-resolving models.
Explicit simulations of aerosol physics in a cloud-resolving model: a sensitivity study based on an observed convective cloud
Authors: Ekman A. M. L. , Wang C. , Wilson J. , Ström J.
Published: April 2010

Abstract. The role of convection in introducing aerosols and promoting the formation of new particles to the upper troposphere has been examined using a cloud-resolving model coupled with an interactive explicit aerosol module. A baseline simulation suggests good agreement in the upper troposphere between modeled and observed results including concentrations of aerosols in different size ranges, mole fractions of key chemical species, and concentrations of ice particles. In addition, a set of 34 sensitivity simulations has been carried out to investigate the sensitivity of modeled results to the treatment of various aerosol physical and chemical processes in the model. The size distribution of aerosols is proved to be an important factor in determining the aerosols' fate within the convective cloud. Nucleation mode aerosols (here defined by 0≤d≤5.84 nm) are quickly transferred to the larger modes as they grow through coagulation of aerosols and condensation of H2SO4. Accumulation mode aerosols (here defined by d≥31.0 nm) are almost completely removed by nucleation (activation of cloud droplets) and impact scavenging. However, a substantial part (up to 10% of the boundary layer concentration) of the Aitken mode aerosol population (here defined by 5.84 nm≤d≤31.0 nm) reaches the top of the cloud and the free troposphere. These particles may continually survive in the upper troposphere, or over time form ice crystals, both that could impact on the atmospheric radiative budget. The sensitivity simulations performed indicate that critical processes in the model causing a substantial change in the upper tropospheric number concentration of Aitken mode aerosols are coagulation of aerosols, condensation of H2SO4, nucleation scavenging, nucleation of aerosols and the transfer of aerosol mass and number between different aerosol bins. In particular, for aerosols in the Aitken mode to grow to CCN size, coagulation of aerosols appears to be more important than condensation of H2SO4. Less important processes are dry deposition, impact scavenging and the initial vertical distribution and concentration of aerosols. It is interesting to note that in order to sustain a vigorous storm cloud, the supply of CCN must be continuous over a considerably long time period of the simulation. Hence, the treatment of the growth of particles is in general much more important than the initial aerosol concentration itself.
Simultaneous lidar observations of temperatures and waves in the polar middle atmosphere on the east and west side of the Scandinavian mountains: a case study on 19/20 January 2003
Authors: Blum U. , Fricke K. H. , Baumgarten G. , Schöch A.
Published: April 2010

Abstract. Atmospheric gravity waves have been the subject of intense research for several decades because of their extensive effects on the atmospheric circulation and the temperature structure. The U. Bonn lidar at the Esrange and the ALOMAR RMR lidar at the Andøya Rocket Range are located in northern Scandinavia 250 km apart on the east and west side of the Scandinavian mountain ridge. During January and February 2003 both lidar systems conducted measurements and retrieved atmospheric temperatures. On 19/20 January 2003 simultaneous measurements for more than 7 h were possible. Although during most of the campaign time the atmosphere was not transparent for the propagation of orographically induced gravity waves, they were nevertheless observed at both lidar stations with considerable amplitudes during these simultaneous measurements. And while the source of the observed waves cannot be determined unambiguously, the observations show many characteristics of orographically excited gravity waves. The wave patterns at ALOMAR show a random distribution with time whereas at the Esrange a persistency in the wave patterns is observable. This persistency can also be found in the distribution of the most powerful vertical wavelengths. The mode values are both at about 5 km vertical wavelength, however the distributions are quite different, narrow at the Esrange with values from λz=2–6 km and broad at ALOMAR, covering λz=1–12 km vertical wavelength. In particular the difference between the observations at ALOMAR and at the Esrange can be understood by different orographic conditions while the propagation conditions were quite similar. At both stations the waves deposit energy in the atmosphere with increasing altitude, which leads to a decrease of the observed gravity wave potential energy density with altitude. The meteorological situation during these measurements was different from common winter situations. The ground winds were mostly northerlies, changed in the upper troposphere and lower stratosphere to westerlies and returned to northerlies in the middle stratosphere.
Simulation of ozone production in a complex circulation region using nested grids
Authors: Taghavi M. , Cautenet S. , Foret G.
Published: April 2010

Abstract. During the ESCOMPTE precampaign (summer 2000, over Southern France), a 3-day period of intensive observation (IOP0), associated with ozone peaks, has been simulated. The comprehensive RAMS model, version 4.3, coupled on-line with a chemical module including 29 species, is used to follow the chemistry of the polluted zone. This efficient but time consuming method can be used because the code is installed on a parallel computer, the SGI 3800. Two runs are performed: run 1 with a single grid and run 2 with two nested grids. The simulated fields of ozone, carbon monoxide, nitrogen oxides and sulfur dioxide are compared with aircraft and surface station measurements. The 2-grid run looks substantially better than the run with one grid because the former takes the outer pollutants into account. This on-line method helps to satisfactorily retrieve the chemical species redistribution and to explain the impact of dynamics on this redistribution.
Radar observations of meteor trails, and their interpretation using Fresnel holography: a new tool in meteor science
Authors: Elford W. G.
Published: April 2010

Abstract. A Fresnel transform technique has been developed at Adelaide to analyse radar meteor echoes detected in the transverse mode. The genesis for this technique was the study of the structure of the scattering ionization immediately behind the head of the trail, in order to deduce the degree of fragmentation of the ablating meteoroid. The technique has been remarkably successful in not only giving insight into the fragmentation of meteoroids, but also revealing other significant features of the trails including diffusion, lateral motion of the trail during formation due to wind drift, and phase of the scattered signal in the vicinity of the head of the trail. A serendipitous outcome of the analysis is the measurement of the speed and deceleration of the meteoroid producing the trail to a precision far exceeding that available from any other method applied to transverse scatter data. Examples of the outcomes of the technique applied to meteor echoes obtained with a 54MHz narrow beam radar are presented.
Rapid meridional transport of tropical airmasses to the Arctic during the major stratospheric warming in January 2003
Authors: Kleinböhl A. , Kuttippurath J. , Sinnhuber M. , Sinnhuber B.-M. , Küllmann H. , Künzi K. , Notholt J.
Published: April 2010

Abstract. We present observations of unusually high values of ozone and N2O in the middle stratosphere that were observed by the airborne submillimeter radiometer ASUR in the Arctic. The observations took place in the meteorological situation of a major stratospheric warming that occurred in mid-January 2003 and was dominated by a wave 2 event. On 23 January 2003 the observed N2O and O3 mixing ratios around 69° N in the middle stratosphere reached maximum values of ~190 ppb and ~10 ppm, respectively. The similarities of these N2O profiles in a potential temperature range between 800 and 1200 K with N2O observations around 20° N on 1 March 2003 by the same instrument suggest that the observed Arctic airmasses were transported from the tropics quasi-isentropically. This is confirmed by 5-day back trajectory calculations which indicate that the airmasses between about 800 and 1000 K had been located around 20° N 3–5 days prior to the measurement in the Arctic. Calculations with a linearized ozone chemistry model along calculated as well as idealized trajectories, initialized with the low-latitude ASUR ozone measurements, give reasonable agreement with the Arctic ozone measurement by ASUR. PV distributions suggest that these airmasses did not stay confined in the Arctic region which makes it unlikely that this dynamical situation lead to the formation of dynamically caused pockets of low ozone.
Pole-to-pole validation of GOME WFDOAS total ozone with groundbased data
Authors: Weber M. , Lamsal L. N. , Coldewey-Egbers M. , Bramstedt K. , Burrows J. P.
Published: April 2010

Abstract. This paper summarises the validation of GOME total ozone retrieved using the Weighting Function Differential Optical Absorption Spectroscopy (WFDOAS) algorithm Version 1.0. This algorithm has been described in detail in a companion paper by Coldewey-Egbers et al. (2005). Compared to the operational GDP (GOME Data Processor) V3, several improvements to the total ozone retrieval have been introduced that account for the varying ozone dependent contribution to rotational Raman scattering, includes a new cloud scheme, and uses the GOME measured effective albedo in the retrieval. In this paper the WFDOAS results have been compared with selected ground-based measurements from the WOUDC (World Ozone and UV Radiation Data Centre) that collects total ozone measurements from a global network of stations covering all seasons. From the global validation excellent agreement between WFDOAS and ground data was observed. The agreement lies within ±1%, and very little seasonal variations in the differences are found. In the polar regions and at high solar zenith angles, however, a positive bias varying between 5 and 8% is found near the polar night period. As a function of solar zenith angle as well as of the retrieved total ozone, the WFDOAS differences to ground polar data, however, show a much weaker dependence as compared to the operational GOME Data Processor Version 3 of GOME that represents a significant improvement. Very few stations carry out simultaneous measurements by Brewer and Dobson spectrometers over an extended period (three years or more). Simultaneous Brewer and Dobson measurements from Hradec Kralove, Czech Republic (50.2N, 15.8E) and Hohenpeissenberg, Germany (47.8N, 11.0E) covering the period 1996-1999 have been compared with our GOME results. Agreement with Brewers are generally better than with the simultaneous Dobson measurements and this may be explained by the neglect of stratospheric (ozone) temperature correction in the standard ozone retrieval from the ground.
Fall vortex ozone as a predictor of springtime total ozone at high northern latitudes
Authors: Kawa S. R. , Newman P. A. , Stolarski R. S. , Bevilacqua R. M.
Published: April 2010

Abstract. Understanding the impact of atmospheric dynamical variability on observed changes in stratospheric O3 is a key to understanding how O3 will change with future climate dynamics and trace gas abundances. In this paper we examine the linkage between interannual variability in total column O3 at northern high latitudes in March and lower-to-mid stratospheric vortex O3 in the prior November. We find that these two quantities are significantly correlated in the years available from TOMS, SBUV, and POAM data (1978-2004). Additionally, we find that the increase in March O3 variability from the 1980s to years post-1990 is also seen in the November vortex O3, i.e., interannual variability in both quantities is much larger in the later years. The cause of this correlation is not clear, however. Interannual variations in March total O3 are known to correspond closely with variations in winter stratospheric wave driving consistent with the effects of varying residual circulation, temperature, and chemical loss. Variation in November vortex O3 may also depend on dynamical wave activity, but the dynamics in fall are less variable than in winter and spring. We do not find significant correlations of dynamic indicators for November such as temperature, heat flux, or polar average total O3 with the November vortex O3, nor with dynamical indicators later in winter and spring that might lead to a connection to March. We discuss several potential hypotheses for the observed correlation but do not find strong evidence for any considered mechanism. We present the observations as a phenomenon whose understanding may improve our ability to predict the dependence of O3 on changing dynamics and chemistry.
Evaluation of the pathways of tropospheric nitrophenol formation from benzene and phenol using a multiphase model
Authors: Harrison M. A. J. , Heal M. R. , Cape J. N.
Published: April 2010

Abstract. Phenols are a major class of volatile organic compounds (VOC) whose reaction within, and partitioning between, the gas and liquid phases affects their lifetime within the atmosphere, the local oxidising capacity, and the extent of production of nitrophenols, which are toxic chemicals. In this work, a zero-dimension box model was constructed to quantify the relative importance of different nitration pathways, and partitioning into the liquid phase, of mono-aromatic compounds in order to help elucidate the formation pathways of 2- and 4-nitrophenol in the troposphere. The liquid phase contributed significantly to the production of nitrophenols for liquid water content (Lc) values exceeding 3x10-9, and for a range of assumed liquid droplet diameter, even though the resultant equilibrium partitioning to the liquid phase was much lower. For example, in a "typical" model scenario, with Lc=3x10-7, 58% of nitrophenol production occurred in the liquid phase but only 2% of nitrophenol remained there, i.e. a significant proportion of nitrophenol observed in the gas phase may actually be produced via the liquid phase. The importance of the liquid phase was enhanced at lower temperatures, by a factor ~1.5-2 at 278K c.f. 298K. The model showed that nitrophenol production was particularly sensitive to the values of the rate coefficients for the liquid phase reactions between phenol and OH or NO3 reactions, but insensitive to the rate coefficient for the reaction between benzene and OH, thus identifying where further experimental data are required.
Validation of SCIAMACHY AMC-DOAS water vapour columns
Authors: Noël S. , Buchwitz M. , Bovensmann H. , Burrows J. P.
Published: April 2010

Abstract. A first validation of water vapour total column amounts derived from measurements of the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) in the visible spectral region has been performed. For this purpose, SCIAMACHY water vapour data have been determined for the year 2003 using an extended version of the Differential Optical Absorption Spectroscopy (DOAS) method, called Air Mass Corrected (AMC-DOAS). The SCIAMACHY results are compared with corresponding water vapour measurements by the Special Sensor Microwave Imager (SSM/I) and with model data from the European Centre for Medium-Range Weather Forecasts (ECMWF). In confirmation of previous results it could be shown that SCIAMACHY derived water vapour columns are typically slightly lower than both SSM/I and ECMWF data, especially over ocean areas. However, these deviations are much smaller than the observed scatter of the data which is caused by the different temporal and spatial sampling and resolution of the data sets. For example, the overall difference with ECMWF data is only -0.05 g/cm2 whereas the typical scatter is in the order of 0.5 g/cm2. Both values show almost no variation over the year. In addition, first monthly means of SCIAMACHY water vapour data have been computed. The quality of these monthly means is currently limited by the availability of calibrated SCIAMACHY spectra. Nevertheless, first comparisons with ECMWF data show that SCIAMACHY (and similar instruments) are able to provide a new independent global water vapour data set.
Naturally driven variability in the global secondary organic aerosol over a decade
Authors: Tsigaridis K. , Lathière J. , Kanakidou M. , Hauglustaine D. A.
Published: April 2010

Abstract. In order to investigate the variability of the secondary organic aerosol (SOA) distributions and budget and provide a measure for the robustness of the conclusions on human induced changes of SOA, a global 3-dimensional chemistry transport model describing both the gas and the particulate phase chemistry of the troposphere has been applied. The response of the global budget of SOA to temperature and moisture changes as well as to biogenic emission changes over a decade (1984-1993) has been evaluated. The considered emissions of biogenic non-methane volatile organic compounds (VOC) are driven by temperature, light and vegetation. They vary between 756 and 810 Tg Cy-1 and are therefore about 5.5 times higher than the anthropogenic VOC emissions. All secondary aerosols (sulphuric, nitrates and organics) are computed on-line together with the aerosol associated water. Over the studied decade, the computed natural variations (8%) in the chemical SOA production from biogenic VOC oxidation equal the chemical SOA production from anthropogenic VOC oxidation. Maximum values are calculated for 1990 (warmer and drier) and minimum values for 1986 (colder and wetter). The SOA computed variability results from a 7% increase in biogenic VOC emissions from 1986 to 1990 combined with 8.5% and 6% increases in the wet and dry deposition of SOA and leads to about 11.5% increase in the SOA burden of biogenic origin. The present study also demonstrates the importance of the hydrological cycle in determining the built up and fate of SOA in the atmosphere. It also reveals the existence of significant positive and negative feedback mechanisms in the atmosphere responsible for the non linear relationship between emissions of biogenic VOC and SOA burden.
Impact of palmitic acid coating on the water uptake and loss of ammonium sulfate particles
Authors: Garland R. M. , Wise M. E. , Beaver M. R. , DeWitt H. L. , Aiken A. C. , Jimenez J. L. , Tolbert M. A.
Published: April 2010

Abstract. While water insoluble organics are prevalent in the atmosphere, it is not clear how the presence of such species alters the chemical and physical properties of atmospheric aerosols. Here we use a combination of FTIR spectroscopy, Transmission Electron Microscopy (TEM) and Aerosol Mass Spectrometry (AMS) to characterize ammonium sulfate particles coated with palmitic acid. Coated aerosols were generated by atomizing pure ammonium sulfate, mixing the particles with a heated flow of nitrogen with palmitic acid vapor, and then flowing the mixture through an in-line oven to create internally mixed particles. The mixing state of the particles was probed using the AMS data and images from the TEM. Both of these probes suggest that the particles were internally mixed. Water uptake by the mixed particles was then probed at 273 K. It was found that for ammonium sulfate containing ~20 wt% palmitic acid the deliquescence relative humidity (DRH) was the same as for pure ammonium sulfate (80±3% RH). For particles with ~50 wt% palmitic acid however, the mixed particles began to take up water at relative humidities as low at 69% and continued to slowly take up water to 85% RH without fully deliquescing. In addition to studies of water uptake, water loss was also investigated. Here coatings of up to 50 wt% had no impact on the efflorescence relative humidity. These studies suggest that even if insoluble substances coat salt particles in the atmosphere, there may be relatively little effect on the resulting water uptake and loss.
Trends of halon gases in polar firn air: implications for their emission distributions
Authors: Reeves C. E. , Sturges W. T. , Sturrock G. A. , Preston K. , Oram D. E. , Schwander J. , Mulvaney R. , Barnola J.-M. , Chappellaz J.
Published: April 2010

Abstract. Four halons (H-1301, H-1211, H-2402 and H-1202) have been measured in air samples collected from polar firn from Dome Concordia (Dome C), Antarctica, from Devon Island, Canada and the North Greenland Ice Core Project (NGRIP) site, Greenland. H-2402 and H-1202 are reported for the first time in firn air. The depth profiles show the concentrations of all four halons to be close to zero (i.e. below the detection limit of 0.001 ppt) at the base of the firn thus demonstrating their entirely anthropogenic origin. This is the first evidence of this for H-2402 and H-1202. A 2-D atmospheric model was run with emissions previously derived using archive air measurements from the southern hemisphere mid-latitudes to produce historical trends in atmospheric concentrations at the firn sites, which were then input into a firn diffusion model to produce concentration depth profiles for comparison with the firn measurements. This comparison provides an evaluation of the model-derived atmospheric concentration histories in both hemispheres and thus an indirect evaluation of the emission rates and distributions used in the atmospheric model. Atmospheric concentration trends produced using global emissions previously determined from measurements at Cape Grim are found to be consistent with the firn data from the southern hemisphere. Further emissions of H-1202 in recent years (late 1980s onwards) are likely to have come from latitudes mostly south of 40° N, but emissions prior to that may have come from further north. Emissions of H-1211 may also have shifted to latitudes south of 40° N during the late 1980s. Following comparison of the atmospheric model output with the firn data, modelled atmospheric trends of total organic bromine in the form of halons were derived for both polar regions.