bluuebunny/crossref_metadata_2025 huggingface dataset:
A new actinic flux 4p-spectroradiometer: instrument design and application to clear sky and broken cloud conditions
Authors: Eckstein E. , Perner D. , Brühl Ch. , Trautmann T.
Published: April 2010

Abstract. A new 4p-spectroradiometer was developed for measuring actinic flux especially under cloudy conditions based on a fixed grating imaging spectrograph and a CCD-detector leading to a simultaneous measurement of the spectrum. The new instrument incorporates a novel optical head with a 4p-field of view independent of angle of incidence. Comparisons with the actinic flux spectroradiometer of the Institute of Atmospheric Chemistry of Forschungszentrum Jülich showed a very good agreement within the limit of the uncertainties of the two instruments. Our spectroradiometer was applied to investigate the effects of broken clouds on the actinic flux and photolysis frequencies on the ground during the BERLIOZ campaign. Reductions as well as enhancements compared to the clear sky case were seen, both effects are larger in the UV-A than the UV-B spectral region. Furthermore the new instrument was used for simultaneous measurements in different altitudes on a tower to study the transmission and attenuation of actinic flux in low clouds. A correlation of attenuation with the simultaneously measured liquid water content of the cloud was found.
Köhler theory for a polydisperse droplet population in the presence of a soluble trace gas, and an application to stratospheric STS droplet growth
Authors: Kokkola H. , Romakkaniemi S. , Laaksonen A.
Published: April 2010

Abstract. We consider the equilibrium behavior of a polydisperse aqueous droplet population as a function of relative humidity (RH) when a soluble trace gas, such as nitric acid, is present in the system. The droplet population experiences a splitting when the RH is increased sufficiently. This splitting is not related to the traditional Köhler activation of cloud droplets, as it may occur at relative humidities below 100%. Remarkably, the splitting always takes place in such a way that the largest size class of the (discretized) droplet population starts taking up the soluble trace gas efficiently, growing steeply as a function of RH, and forcing the smaller droplets to shrink. We consider this behavior in terms of open and closed system Köhler curves (open system referring to one in which the trace gas concentration remains constant and closed system to one in which the gas concentration decreases as a result of uptake of the trace gas). We show how the open and closed system Köhler curves are related, and that the splitting of the population can be explained in terms of closed system curves crossing the Köhler maxima of the open system curves. We then go on to consider time-dependent situations, and show that due to gas-phase mass transfer limitations, the splitting of the size distributions moves toward smaller sizes as the rate of RH increase becomes more rapid. Finally, we consider stratospheric supercooled ternary solution droplet populations, and show that the splitting described using the new theory may lead to formation of bimodal size distributions in the stratosphere.
Lidar and in situ observations of continental and Saharan aerosol: closure analysis of particles optical and physical properties
Authors: Gobbi G. P. , Barnaba F. , Van Dingenen R. , Putaud J. P. , Mircea M. , Facchini M. C.
Published: April 2010

Abstract. Single wavelength polarization lidar observations collected at Mt. Cimone (44.2º N, 10.7º E, 1870 m a.s.l.) during the June 2000 MINATROC campaign are analyzed to derive tropospheric profiles of aerosol extinction, depolarization, surface area and volume. Lidar retrievals for the 2170-2245 m level are compared to the same variables as computed from in situ measurements of particles size distributions, performed at the mountain top Station (2165 m a.s.l.) by a differential mobility analyzer (DMA) and an optical particle counter (OPC). A sensitivity analysis of this closure experiment shows that mean relative differences between the backscatter coefficients obtained by the two techniques undergo a sharp decrease when hygroscopic growth to ambient humidity is considered for the DMA dataset, otherwise representative of dry aerosols. Minimization of differences between lidar and size distribution-derived backscatter coefficients allowed to find values of the "best" refractive index, specific to each measurement. These results show the refractive index to increase for air masses proceeding from Africa and Western Europe. Lidar depolarization was observed to minimize mainly in airmasses proceeding from Western Europe, thus indicating a spherical, i.e. liquid nature for such aerosols. Conversely, African, Mediterranean and East Europe aerosol showed a larger depolarizing fraction, mainly due to coexisting refractory and soluble fractions. The analysis shows average relative differences between lidar and in-situ observations of 5% for backscatter, 36% for extinction 41% for surface area and 37% for volume. These values are well within the expected combined uncertainties of the lidar and in situ retrievals. Average differences further decrease during the Saharan dust transport event, when a lidar signal inversion model considering non-spherical scatterers is employed. The quality of the closure obtained between particle counter and lidar-derived aerosol surface area and volume observations constitutes a validation of the technique adopted to retrieve such aerosol properties on the basis of single-wavelength lidar observations.
The H Lyman-a actinic flux in the middle atmosphere
Authors: Reddmann T. , Uhl R.
Published: April 2010

Abstract. The penetration of solar H Lyman-a radiation into the terrestrial middle atmosphere is studied in detail. The Lyman-a actinic flux is calculated with a Monte Carlo approach including multiple resonance scattering of Lyman-a photons within the terrestrial atmosphere and a temperature dependent absorption cross section of molecular oxygen. The dependence of the actinic flux on the temperature profile is significant for O2 column densities greater than about 1024 m-2. For column densities greater than about 5 · 1024 m-2 resonance scattering becomes important at solar zenith angles > 60°. The O(1D) quantum yield of the O2 dissociation by Lyman-a photons is found to decrease from 0.58 in the lower thermosphere to 0.48 in the lower mesosphere. Parameterisations for Lyman-a actinic flux, mean O2 absorption cross section and O(1D) quantum yield including temperature dependence and resonance scattering are given valid up to a O2 column density of about 1025 m-2.
Global chemical weather forecasts for field campaign planning: predictions and observations of large-scale features during MINOS, CONTRACE, and INDOEX
Authors: Lawrence M. G. , Rasch P. J. , von Kuhlmann R. , Williams J. , Fischer H. , de Reus M. , Lelieveld J. , Crutzen P. J. , Schultz M. , Stier P. , Huntrieser H. , Heland J. , Stohl A. , Forster C. , Elbern H. , Jakobs H. , Dickerson R. R.
Published: April 2010

Abstract. The first global tropospheric forecasts of O3 and its precursors have been used in the daily flight planning of field measurement campaigns. The 3-D chemistry-transport model MATCH-MPIC is driven by meteorological data from a weather center (NCEP) to produce daily 3-day forecasts of the global distributions of O3 and related gases, as well as regional CO tracers. This paper describes the forecast system and its use in three field campaigns, MINOS, CONTRACE and INDOEX. An overview is given of the forecasts by MATCH-MPIC and by three other chemical weather forecast models (EURAD, ECHAM, and FLEXPART), focusing on O3 and CO. Total CO and regional CO tracers were found to be the most valuable gases for flight planning, due to their relatively well-defined anthropogenic source regions and lifetimes of one to a few months. CO was in good agreement with the observations on nearly all the flights (generally  r > 0.7, and the relative RMS differences for the deviations from the means was less than 20%). In every case in which the chemical weather forecasts were primarily responsible for the flight plans, the targeted features were observed. Three forecasted phenomena are discussed in detail: outflow from Asia observed in the Mediterranean upper troposphere during MINOS, outflow from North America observed in the middle troposphere over northern Europe during CONTRACE, and the location of the "chemical ITCZ'' over the Indian Ocean during INDOEX. In particular it is shown that although intercontinental pollution plumes such as those observed during MINOS and CONTRACE occur repeatedly during the months around the campaigns, their frequency is sufficiently low (~10--30% of the time) that global chemical weather forecasts are important for enabling them to be observed during limited-duration field campaigns. The MATCH-MPIC chemical weather forecasts, including an interface for making customized figures from the output, are available for community use via http://www.mpch-mainz.mpg.de/~lawrence/forecasts.html.
A condensed-mass advection based model for the simulation of liquid polar stratospheric clouds
Authors: Lowe D. , MacKenzie A. R. , Nikiforakis N. , Kettleborough J.
Published: April 2010

Abstract. We present a condensed-mass advection based model (MADVEC) designed to simulate the condensation/evaporation of liquid polar stratospheric cloud (PSC) particles. A (Eulerian-in-radius) discretization scheme is used, making the model suitable for use in global or mesoscale chemistry and transport models (CTMs). The mass advection equations are solved using an adaption of the weighted average flux (WAF) scheme. We validate the numerical scheme using an analytical solution for multicomponent aerosols. The physics of the model are tested using a test case designed by Meilinger et al. (1995). The results from this test corroborate the composition gradients across the size distribution under rapid cooling conditions that were reported in earlier studies.
Aerosol sources and their contribution to the chemical composition of aerosols in the Eastern Mediterranean Sea during summertime
Authors: Sciare J. , Bardouki H. , Moulin C. , Mihalopoulos N.
Published: April 2010

Abstract. A detailed study on the temporal variability of compounds important in controlling aerosol chemical composition was performed during a one-month experiment conducted during summer 2000 at a background site on Crete, in the Eastern Mediterranean Sea. Contribution of different aerosol sources in the Eastern Mediterranean Basin could be investigated at this location since the site is influenced by a wide range of air masses originating mainly in Europe and Africa. Chemical apportionment was performed for various air mass origins and showed a strong impact of anthropogenic emissions in the Turkey and Central Europe sectors, with black carbon (BC) and non-sea-salt sulfate (nss-SO4) concentrations higher than observed in the Eastern and Western Europe sectors. High levels of non-sea-salt calcium (nss-Ca) were associated with air masses from Africa but also from Central Turkey. Evidence was found that BC calculation based on light absorbance during dust events was biased. This quality-controlled high temporal resolution dataset allowed to investigate in detail the source-receptor relationships responsible for the levels of BC, nss-SO4 and sulfur dioxide (SO2), observed in Crete. Among the results obtained from this model, the major contribution of Turkey and Central Europe was confirmed in terms of anthropogenic emissions. Comparisons with remote optical properties obtained from Satellite observations (SEAWIFS) north of Crete indicates that our ground based aerosol characterization was suitable for describing aerosol properties in the atmospheric column for most of the time during the campaign.
Fluxes of nitrates between snow surfaces and the atmosphere in the European high Arctic
Authors: Beine H. J. , Dominè F. , Ianniello A. , Nardino M. , Allegrini I. , Teinilä K. , Hillamo R.
Published: April 2010

Abstract. Measurements of atmospheric and snow mixing ratios of nitrates and nitrites and their fluxes above the snow surface were made during two intensive campaigns during spring time 2001 at Ny-Ålesund, Svalbard as part of the EU project  "`The NItrogen Cycle and Effects on the oxidation of atmospheric trace species at high latitudes" (NICE). At this coastal site close to the unseasonably unfrozen fjord, of the measured nitrogen species, only HNO3 showed a significant flux on to the snow surface; a mean deposition of -8.7 nmol h-1 m-2 was observed in late April / early May 2001. These fluxes may be due to the reaction of HNO3 with sea salt, and especially NaCl, or may be simply uptake of HNO3 by ice, which is alkaline because of the sea salt in our marine environment. During snowfall periods dry deposition of HNO3 may contribute up to 10% of the N budget in the snow; however, the main source for N is wet deposition in falling snow. The surface snow at Ny-Ålesund showed very complex stratigraphy; the NO3- mixing ratio in snow varied between 65 and 520 ng g-1, the total NO3- content of the snowpack was on the order of 2700 ng cm-2. In comparison the atmospheric boundary layer column showed a NO3- content of only 8 ng cm-2. The limited exchange, however, between the snow and the atmosphere was attributed to low mobility of NO3- in the observed snow. Contrary to other Arctic sites (i.e. Alert, Nunavut or Summit, Greenland) deposition of sea salt and crustal aerosols in this marine environment made the surface snow alkaline; snow NO3- was associated with heavier cations and was not readily available for physical exchange or photochemical reactions.
Twilight tropospheric and stratospheric photodissociation rates derived from balloon borne radiation measurements
Authors: Kylling A. , Danielsen T. , Blumthaler M. , Schreder J. , Johnsen B.
Published: April 2010

Abstract. A new ligthweight multichannel moderate bandwidth filter instrument designed to be flown on balloons, is described. The instrument measures the radiation field within the short UV (center wavelength at 312 nm) and long UV (center wavelength at 340 nm). The angular and spectral characteristics of the instrument are discussed and the calibration procedure outlined. Measurements made during a stratospheric balloon flight at twilight conditions from Gap-Tallard, France, are presented and compared with state-of-the-art radiative transfer model simulations. The model simulations and the measurements agree within ±10% (±20%) for solar zenith angles smaller than 93° (90°) for the 340 (312) nm channel. Based on the model simulations of the measured radiation, actinic flux spectra are reconstructed. These are used to calculate various photodissociation rates.
The impact of mid-latitude intrusions into the polar vortex on ozone loss estimates
Authors: Grooß J.-U. , Müller R.
Published: April 2010

Abstract. Current stratospheric chemical model simulations underestimate substantially the large ozone loss rates that are derived for the Arctic from ozone sondes for January of some years. Until now, no explanation for this discrepancy has been found. Here, we examine the influence of intrusions of mid-latitude air into the polar vortex on these ozone loss estimates. This study focuses on the winter 1991/92, because during this winter the discrepancy between simulated and experimentally derived ozone loss rates is reported to be the largest. Also during the considered period the vortex was disturbed by a strong warming event with large-scale intrusions of mid-latitude air into the polar vortex, which is quite unusual for this time of the year. The study is based on simulations performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). Two methods for determination the ozone loss are investigated, the so-called vortex average approach and the Match method. The simulations for January 1992 show that the intrusions induce a reduction of vortex average ozone mixing ratio corresponding to a systematic offset of the ozone loss rate of about 12 ppb per day. This should be corrected for in the vortex average method. The simulations further suggest, that these intrusions do not cause a significant bias for the Match method due to effective quality control measures in the Match technique.
Inverse transport for the verification of the Comprehensive Nuclear Test Ban Treaty
Authors: Issartel J.-P. , Baverel J.
Published: April 2010

Abstract. An international monitoring system is being built as a verification tool for the Comprehensive Test Ban Treaty. Forty stations will measure on a worldwide daily basis the concentration of radioactive noble gases. The paper introduces, by handling preliminary real data, a new approach of backtracking for the identification of sources of passive tracers after positive measurements. When several measurements are available the ambiguity about possible sources is reduced significantly. The approach is validated against ETEX data. A distinction is made between adjoint and inverse transport shown to be, indeed, different though equivalent ideas. As an interesting side result it is shown that, in the passive tracer dispersion equation, the diffusion stemming from a time symmetric turbulence is necessarily a self-adjoint operator, a result easily verified for the usual gradient closure, but more general.
An investigation of ozone and planetary boundary layer dynamics over the complex topography of Grenoble combining measurements and modeling
Authors: Couach O. , Balin I. , Jiménez R. , Ristori P. , Perego S. , Kirchner F. , Simeonov V. , Calpini B. , van den Bergh H.
Published: April 2010

Abstract. This paper concerns an evaluation of ozone (O3) and planetary boundary layer (PBL) dynamics over the complex topography of the Grenoble region through a combination of measurements and mesoscale model (METPHOMOD) predictions for three days, during July 1999. The measurements of O3 and PBL structure were obtained with a Differential Absorption Lidar (DIAL) system, situated 20 km south of Grenoble at Vif (310 m ASL). The combined lidar observations and model calculations are in good agreement with atmospheric measurements obtained with an instrumented aircraft (METAIR). Ozone fluxes were calculated using lidar measurements of ozone vertical profiles concentrations and the horizontal wind speeds measured with a Radar Doppler wind profiler (DEGREANE. The ozone flux patterns indicate that the diurnal cycle of ozone production is controlled by local thermal winds. The convective PBL maximum height was some 2700 m above the land surface while the nighttime residual ozone layer was generally found between 1200 and 2200 m. Finally we evaluate the magnitude of the ozone processes at different altitudes in order to estimate the photochemical ozone production due to the primary pollutants emissions of Grenoble city and the regional network of automobile traffic.
Differences across the ITCZ in the chemical characteristics of the Indian Ocean MBL aerosol during INDOEX
Authors: Norman M. , Leck C. , Rodhe H.
Published: April 2010

Abstract. The water soluble inorganic part of the sub-micrometer aerosol was measured from two research vessels over the Indian Ocean during the winter monsoon season (February and March) as part of the INDOEX project in 1998 and 1999. Additional measurements were made of gas phase SO2 from one of the vessels in 1999. All samples collected north of the Inter Tropical Convergence Zone, ITCZ, were clearly affected by continental, anthropogenic sources. A sharp transition occurred across the ITCZ with concentrations of nss-SO42-, NH4+ and nss-K+ being lower by a factor of 7-15, >20 and >40, respectively, on the southern side of the ITCZ. The contribution from DMS to the sub-micrometer nss-SO42- was estimated to be up to 40% in clean air north of the ITCZ but less than 10% in polluted air originating from India. South of the ITCZ virtually all nss-SO42- was likely to be derived from oxidation of DMS. The concentration of SO2 decreased rapidly with distance from the Indian coast, the molar ratio SO2/nss-SO42- reaching values below 5% after 35 h travel time over the ocean. Surprisingly, MSA, which is derived from DMS, also showed higher concentrations in the sub-micrometer aerosol north of the ITCZ than south of it. This could be explained by the larger sub-micrometer surface area available north of the ITCZ for the condensation of MSA. South of the ITCZ a major part of the MSA was found on the super-micrometer particles. An analysis based on the air trajectories showed that systematic variation in the observed concentrations was associated with variations in the transport from source regions. For example, differences in time since air parcels left the Arabian or Indian coasts was shown to be an important factor for explaining the substantial differences in absolute concentrations.
A fast H2O total column density product from GOME – Validation with in-situ aircraft measurements
Authors: Wagner T. , Heland J. , Zöger M. , Platt U.
Published: April 2010

Abstract. Atmospheric water vapour is the most important greenhouse gas which is responsible for about 2/3 of the natural greenhouse effect, therefore changes in atmospheric water vapour in a changing climate (the water vapour feedback) is subject to intense debate. H2O is also involved in many important reaction cycles of atmospheric chemistry, e.g. in the production of the OH radical. Thus, long time series of global H2O data are highly required. Since 1995 the Global Ozone Monitoring Experiment (GOME) continuously observes atmospheric trace gases. In particular it has been demonstrated that GOME as a nadir looking UV/vis-instrument is sensitive to many tropospheric trace gases. Here we present a new, fast H2O algorithm for the retrieval of vertical column densities from GOME measurements. In contrast to existing H2O retrieval algorithms it does not depend on additional information like e.g. the climatic zone, aerosol content or ground albedo. It includes an internal cloud-, aerosol-, and albedo correction which is based on simultaneous observations of the oxygen dimer O4. From sensitivity studies using atmospheric radiative modelling we conclude that our H2O retrieval overestimates the true atmospheric H2O vertical column density (VCD) by about 4% for clear sky observations in the tropics and sub-tropics, while it can lead to an underestimation of up to -18% in polar regions. For measurements over (partly) cloud covered ground pixels, however, the true atmospheric H2O VCD might be in general systematically underestimated. We compared the GOME H2O VCDs to ECMWF model data over one whole GOME orbit (extending from the Arctic to the Antarctic) including also totally cloud covered measurements. The correlation of the GOME observations and the model data yield the following results: a slope of 0.96 (r2 = 0.86) and an average bias of 5%. Even for measurements with large cloud fractions between 50% and 100% an average underestimation of only -18% was found. This high accuracy of our GOME H2O data is also confirmed by the excellent agreement with in-situ aircraft measurements during the MINOS campaign in Greece in summer 2001 (slope of 0.97 (r2 = 0.86), and an average bias of only 0.2%). Our H2O algorithm can be directly adapted to the nadir observations of SCIAMACHY (SCanning Imaging Absorption SpectroMeter for Atmospheric CHartographY) which was launched on ENVISAT in March 2002. Near real time H2O column data from GOME and SCIAMACHY might be of great value for meteorological weather forecast.
Ozone production and trace gas correlations during the June 2000 MINATROC intensive measurement campaign at Mt. Cimone
Authors: Fischer H. , Kormann R. , Klüpfel T. , Gurk Ch. , Königstedt R. , Parchatka U. , Mühle J. , Rhee T. S. , Brenninkmeijer C. A. M. , Bonasoni P. , Stohl A.
Published: April 2010

Abstract. An intensive measurement campaign was performed in June 2000 at the Mt. Cimone station (44°11' N-10°42' E, 2165 m asl, the highest mountain in the northern Italian Apennines) to study photochemical ozone production in the lower free troposphere. In general, average mixing ratios of important trace gases were not very high (121 ± 20 ppbv CO, 0.284 ± 0.220 ppbv NOx, 1.15 ± 0.8 ppbv NOy, 58 ± 9 ppbv O3), which indicates a small contribution by local pollution. Those trace gas levels are representative of continental background air, which is further supported by the analysis of VOCs (e.g.: C2H6 = (905 ± 200) pptv, C3H8 = (268 ±110) pptv, C2H2 = (201 ± 102) pptv, C5H8 = (111 ± 124) pptv, benzene = (65 ± 33) pptv). Furthermore, significant diurnal variations for a number of trace gases (O3, CO, NOx, NOy, HCHO) indicate the presence of free tropospheric airmasses at nighttime as a consequence of local catabatic winds. Average mid-day peroxy radical concentrations at Mt. Cimone are of the order of 30 pptv. At mean NO concentrations of the order of 40 pptv this gives rise to significant in situ net O3 production of 0.1-0.3 ppbv/hr. The importance of O3 production is supported by correlations between O3, CO, NOz, and HCHO, and between HCHO, CO and NOy.
Trends and inter-annual variability of methane emissions derived from 1979-1993 global CTM simulations
Authors: Dentener F. , van Weele M. , Krol M. , Houweling S. , van Velthoven P.
Published: April 2010

Abstract. The trend and interannual variability of methane sources are derived from multi-annual simulations of tropospheric photochemistry using a 3-D global chemistry-transport model. Our semi-inverse analysis uses the fifteen years (1979--1993) re-analysis of ECMWF meteorological data and annually varying emissions including photo-chemistry, in conjunction with observed CH4 concentration distributions and trends derived from the NOAA-CMDL surface stations. Dividing the world in four zonal regions (45--90 N, 0--45 N, 0--45 S, 45--90 S) we find good agreement in each region between (top-down) calculated emission trends from model simulations and (bottom-up) estimated anthropogenic emission trends based on the EDGAR global anthropogenic emission database, which amounts for the period 1979--1993 2.7 Tg CH4 yr-1. Also the top-down determined total global methane emission compares well with the total of the bottom-up estimates. We use the difference between the bottom-up and top-down determined emission trends to calculate residual emissions. These residual emissions represent the inter-annual variability of the methane emissions. Simulations have been performed in which the year-to-year meteorology, the emissions of ozone precursor gases, and the stratospheric ozone column distribution are either varied, or kept constant. In studies of methane trends it is most important to include the trends and variability of the oxidant fields. The analyses reveals that the variability of the emissions is of the order of 8Tg CH4 yr-1, and likely related to wetland emissions and/or biomass burning.
Deep convective injection of boundary layer air into the lowermost stratosphere at midlatitudes
Authors: Fischer H. , de Reus M. , Traub M. , Williams J. , Lelieveld J. , de Gouw J. , Warneke C. , Schlager H. , Minikin A. , Scheele R. , Siegmund P.
Published: April 2010

Abstract. On 22 August 2001 a measurement flight was performed with the German research aircraft FALCON from Sardinia to Crete as part of the Mediterranean Oxidant Study (MINOS). Cruising at 8.2 km, the aircraft was forced to climb to 11.2 km over the southern tip of Italy to stay clear of the anvil of a large cumulonimbus tower. During ascent into the lowermost stratosphere in-situ measurements onboard the FALCON indicated several sharp increases in the concentrations of tropospheric trace gases, e.g. CO, acetone, methanol, benzene and acetonitrile, above the anvil. During one particular event deep in the stratosphere, at O3 concentrations exceeding 200 ppv, CO increased from about 60 to 90 ppv, while the concentration of acetone and methanol increased by more than a factor of 2 (0.7 to 1.8 ppv for acetone; 0.4 to 1.4 ppv for methanol). Enhancements for the short lived species benzene are even higher, increasing from 20 pptv in the stratosphere to approx. 130 pptv. The concentrations during the event were higher than background concentrations in the upper troposphere, indicating that polluted boundary layer air was directly mixed into the lowermost stratosphere.
On extreme atmospheric and marine nitrogen fluxes and chlorophyll-a levels in the Kattegat Strait
Authors: Hasager C. B. , Carstensen J. , Ellermann T. , Gustafson B. G. , Hertel O. , Johnsson M. , Markager S. , Ambelas Skjøth C.
Published: April 2010

Abstract. A retrospective analysis is carried out to investigate the importance of the vertical fluxes of nitrogen to the marine sea surface layer in which high chlorophyll a levels may cause blooms of harmful algae and subsequent turn over and oxygen depletion at the bottom of the sea. Typically nitrogen is the limiting factor for phytoplankton in the Kattegat Strait during summer periods (May to August) and the major nitrogen inputs come from the atmosphere and deep-water entrainment. The extreme reoccurrence values of nitrogen from atmospheric wet and dry deposition and deep-water flux entrainments are calculated by the periodic maximum method and the results are successfully compared to a map of chlorophyll return periods based on in-situ observations. The one-year return of extreme atmospheric wet deposition is around 60 mg N m-2 day-1 and 30 mg N m-2 day-1 for deep-water entrainment. Atmospheric nitrogen dry deposition is insignificant in the context of algal blooms. At longer time-scales e.g. at 10-year return, the nitrogen deep-water entrainment is larger than the extreme of atmospheric wet deposition. This indicates that the pool of nitrogen released from the sea bottom by deep-water entrainment forced by high winds greatly exceeds the atmospheric pool of nitrogen washed out by precipitation. At the frontal zone of the Kattegat Strait and Skagerrak, the nitrogen deep-water entrainment is very high and this explains the high 10-year return chlorophyll level at 8 mg m-3 in the Kattegat Strait. In the southern part, the extreme chlorophyll level is only 4 mg m-3 according to the statistics of a multi-year time-series of water samples. The chlorophyll level varies greatly in time and space as documented by a series of SeaWiFS satellite maps (OC4v4 algorithm) of chlorophyll ScanFish and buoy observations from an experimental period in the Kattegat Strait. It is recommended to sample in-situ chlorophyll observation collocated in time to the satellite overpasses of e.g. SeaWiFS and ENVISAT MERIS to ensure improved mapping of the chlorophyll levels in the Danish waters.
Commentary on "Homogeneous nucleation of NAD and NAT in liquid stratospheric aerosols: insufficient to explain denitrification" by Knopf et al.
Authors: Tabazadeh A.
Published: April 2010

Abstract. In a recent published paper Knopf et a1. (2002) have suggested that the homogeneous freezing behavior of stratospheric aerosols, under polar winter conditions, can be simulated experimentally in large bulk phase-sized droplet samples (0.12-0.27 cm in diameter). Their hypothesis is based on the fact that a nucleus, which freezes the supercooled phase, forms within the bulk volume of a given sample, and therefore, if large bulk volumes don't freeze in the laboratory, then small volumes in particles most certainly remain unfrozen in the stratosphere. The important question to ask here is whether their initial hypothesis, which they have used to analyze their data, is even correct to begin with. For example, does a nucleus, which turns over the phase, forms within the bulk volume or on the surface of the supercooled phase? Some recent studies provide both experimental (Tabazadeh et al., 2002a, b) and theoretical (Djikaev et al., 2002, 2003) support for the formation of the nucleus at the surface of a supercooled droplet. If the homogeneous nucleation process initiates at the droplet surface, then the approach taken by Knopf. et al. to study this crystallization process may not be directly applicable to the stratospheric situation.
The detection of solar proton produced 14CO
Authors: Jöckel P. , Brenninkmeijer C. A. M. , Lawrence M. G. , Siegmund P.
Published: April 2010

Abstract. Major solar eruptions (coronal mass ejections) are accompanied by massive ejections of protons. When these charged particles head for the Earth through the interplanetary magnetic field with high flux and energy, a solar proton event (SPE) is recorded. Strong SPEs, in which energetic protons penetrate the atmosphere in large numbers are rare, but do have chemical effects (Crutzen, 1975; Jackman et al., 1990, 2001).  They also have nucleonic effects by which they can almost instantaneously increase the atmospheric production of radio-nuclides, including 14C (radiocarbon), but this has never been demonstrated. We show, using satellite observations and modeling, that the 2nd most intensive set of SPEs on record, that of August-December 1989, must have caused detectable increases in atmospheric 14CO. This is confirmed by a sequence of peaks in the Baring Head (NZ) time series of 14CO observations (Brenninkmeijer, 1993), probably providing a unique indication of production of 14C by solar protons, thus demonstrating the use of SPE 14CO as an atmospheric tracer.
Gas-particle interactions above a Dutch heathland: II. Concentrations and surface exchange fluxes of atmospheric particles
Authors: Nemitz E. , Sutton M. A. , Wyers G. P. , Otjes R. P. , Mennen M. G. , van Putten E. M. , Gallagher M. W.
Published: April 2010

Abstract. Size-dependent particle number fluxes measured by eddy-covariance (EC) and continuous fluxes of ammonium (NH4+) measured with the aerodynamic gradient method (AGM) are reported for a Dutch heathland. Daytime deposition velocities (Vd) by EC with peak values of 5 to 10 mm s-1 increased with particle diameter (dp) over the range 0.1–0.5 µm, and are faster than predicted by current models. With a mean Vd of 2.0 mm s-1 (daytime: 2.7; night-time 0.8 mm s-1) NH4+ fluxes by AGM are overall in agreement with former measurements and NH4+-N dry deposition amounts to 20% of the dry input of NH3-N over the measurement period. These surface exchange fluxes are analyzed together with simultaneous gas-phase flux measurements for indications of gas-particle interactions. On warm afternoons the apparent fluxes of acids and aerosol above the heathland showed several coinciding anomalies, all of which are consistent with NH4+ evaporation during deposition: (i) canopy resistances for HNO3 and HCl of up to 100 s m-1, (ii) simultaneous particle emission of small particles (Dp<0.18 µm) and deposition of larger particles (Dp>0.18 µm), (iii) NH4+ deposition faster than derived from size-distributions and size-segregated EC particle fluxes. These observations coincide with the observations of (i) surface concentration products of NH3 and HNO3 well below the thermodynamic equilibrium value and (ii) Damköhler numbers that indicate chemical conversion to be sufficiently fast to modify exchange fluxes. The measurements imply a removal rate of volatile NH4+ of 3−30×10-6 s-1 averaged over the 1 km boundary-layer, while NH3 deposition is underestimated by typically 20 ng m-2 s-1 (28%) and flux reversal may occur.
Gas-particle interactions above a Dutch heathland: III. Modelling the influence of the NH3-HNO3-NH4NO3 equilibrium on size-segregated particle fluxes
Authors: Nemitz E. , Sutton M. A.
Published: April 2010

Abstract. Micrometeorological measurements of size-segregated particle number fluxes above Dutch heathlands and forests have repeatedly shown simultaneous apparent emission of particles with a diameter (Dp)<0.18 µm and deposition of larger particles when measured with optical particle counters. In order to assess whether this observation may be explained by the equilibrium reaction of ammonia (NH3), nitric acid (HNO3) and ammonium (NH4+), a new numerical model is developed to predict the vertical concentration and flux profiles of the different species as modified by the interaction of equilibration and surface/atmosphere exchange processes. In addition to former studies, the new approach explicitly models the height-dependence of the NH4+ and total aerosol size-distribution. Using this model, it is demonstrated that both gas-to-particle conversion (gtpc) and aerosol evaporation can significantly alter the apparent surface exchange fluxes, and evoke the observed bi-directional particle fluxes under certain conditions. Thus, in general, the NH3-HNO3-NH4NO3 equilibrium needs to be considered when interpreting eddy-covariance particle fluxes. Applied to an extensive dataset of simultaneous flux measurements of particles and gases at Elspeet, NL, the model reproduces the diurnal pattern of the bi-directional exchange well. In agreement with the observation of fast NH4+ deposition, slow nitric acid deposition (both as measured by the aerodynamic gradient method) and small concentration products of NH3×HNO3 at this site, this study suggests that NH4+ evaporation at this site significantly alters surface exchange fluxes.
First retrieval of global water vapour column amounts from SCIAMACHY measurements
Authors: Noël S. , Buchwitz M. , Burrows J. P.
Published: April 2010

Abstract. Global water vapour column amounts have been derived for the first time from measurements of the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) on the European environmental satellite ENVISAT. For this purpose, two different existing retrieval algorithms have been adapted, namely the Air Mass Corrected Differential Absorption Spectroscopy (AMC-DOAS) which was originally designed for GOME and the Weighting Function Modified Differential Absorption Spectroscopy (WFM-DOAS) which was mainly designed for the retrieval of CH4, CO2 and CO from SCIAMACHY near-infrared spectra. Here, both methods have been applied to SCIAMACHY's nadir measurements in the near-visible spectral region around 700 nm. Taking into account a systematic offset of 10%, the results of these two methods agree within a scatter of about ±0.5 g/cm2 with corresponding SSM/I and ECMWF water vapour data. This deviation includes contributions from the temporal and spatial variability of water vapour. In fact, the mean deviation between the SCIAMACHY and the correlative data sets is much smaller: the SCIAMACHY total water vapour columns are typically about 0.15 g/cm2 lower than the SSM/I values and less than 0.1 g/cm2 lower than corresponding ECMWF data. The SCIAMACHY water vapour results agree well with correlative data not only over ocean but also over land, thus showing the capability of SCIAMACHY to derive water vapour concentrations on the global scale.
Analysis of a jet stream induced gravity wave associated with an observed ice cloud over Greenland
Authors: Buss S. , Hertzog A. , Hostettler C. , Bui T. B. , Lüthi D. , Wernli H.
Published: April 2010

Abstract. A polar stratospheric ice cloud (PSC type II) was observed by airborne lidar above Greenland on 14 January 2000. It was the unique observation of an ice cloud over Greenland during the SOLVE/THESEO 2000 campaign. Mesoscale simulations with the hydrostatic HRM model are presented which, in contrast to global analyses, are capable to produce a vertically propagating gravity wave that induces the low temperatures at the level of the PSC afforded for the ice formation. The simulated minimum temperature is ~8 K below the driving analyses and ~4.5 K below the frost point, exactly coinciding with the location of the observed ice cloud. Despite the high elevations of the Greenland orography the simulated gravity wave is not a mountain wave. Analyses of the horizontal wind divergence, of the background wind profiles, of backward gravity wave ray-tracing trajectories, of HRM experiments with reduced Greenland topography and of several diagnostics near the tropopause level provide evidence that the wave is emitted from an intense, rapidly evolving, anticyclonically curved jet stream. The precise physical process responsible for the wave emission could not be identified definitely, but geostrophic adjustment and shear instability are likely candidates. In order to evaluate the potential frequency of such non-orographic polar stratospheric cloud events, the non-linear balance equation diagnostic is performed for the winter 1999/2000. It indicates that ice-PSCs are only occasionally generated by gravity waves emanating from spontaneous adjustment.
Long-term global distribution of earth's shortwave radiation budget at the top of atmosphere
Authors: Hatzianastassiou N. , Fotiadi A. , Matsoukas Ch. , Pavlakis K. , Drakakis E. , Hatzidimitriou D. , Vardavas I.
Published: April 2010

Abstract. The mean monthly shortwave (SW) radiation budget at the top of atmosphere (TOA) was computed on 2.5° longitude-latitude resolution for the 14-year period from 1984 to 1997, using a radiative transfer model with long-term climatological data from the International Satellite Cloud Climatology Project (ISCCP-D2) supplemented by data from the National Centers for Environmental Prediction – National Center for Atmospheric Research (NCEP-NCAR) Global Reanalysis project, and other global data bases such as TIROS Operational Vertical Sounder (TOVS) and Global Aerosol Data Set (GADS). The model radiative fluxes at TOA were validated against Earth Radiation Budget Experiment (ERBE) S4 scanner satellite data (1985–1989). The model is able to predict the seasonal and geographical variation of SW TOA fluxes. On a mean annual and global basis, the model is in very good agreement with ERBE, overestimating the outgoing SW radiation at TOA (OSR) by 0.93 Wm-2 (or by 0.92%), within the ERBE uncertainties. At pixel level, the OSR differences between model and ERBE are mostly within ±10 Wm-2, with ±5 Wm-2 over extended regions, while there exist some geographic areas with differences of up to 40 Wm-2, associated with uncertainties in cloud properties and surface albedo. The 14-year average model results give a planetary albedo equal to 29.6% and a TOA OSR flux of 101.2 Wm-2. A significant linearly decreasing trend in OSR and planetary albedo was found, equal to 2.3 Wm-2 and 0.6% (in absolute values), respectively, over the 14-year period (from January 1984 to December 1997), indicating an increasing solar planetary warming. This planetary SW radiative heating occurs in the tropical and sub-tropical areas (20° S–20° N), with clouds being the most likely cause. The computed global mean OSR anomaly ranges within ±4 Wm-2, with signals from El Niño and La Niña events or Pinatubo eruption, whereas significant negative OSR anomalies, starting from year 1992, are also detected.
Assessment of the applicability of NO-NO2-O3 photostationary state to long-term measurements at the Hohenpeissenberg GAW Station, Germany
Authors: Mannschreck K. , Gilge S. , Plass-Duelmer C. , Fricke W. , Berresheim H.
Published: April 2010

Abstract. Continuous measurements of concentrations of reactive gases, radiation, and meteorological parameters are carried out at the Meteorological Observatory Hohenpeissenberg (MOHp) as part of the Global Atmosphere Watch (GAW) Program. NO, NO2, O3 and JNO2 data from a four-year period (March 1999-December 2002) are evaluated for consistency with photochemical steady state (PSS, Φ=1) conditions. The extent of deviation from PSS reveals a strong dependence on wind direction at the station. Median values of Φ in the south sector are in the range of 2.5-5.7 and show a high variability. In contrast, values for the other directions show a relatively low variability around a median level of 2. When taking into account peroxy radical concentrations (Φext=1) PSS was reached in 13-32% of all cases for the years 1999-2002. The differences in wind sectors can be explained by local effects. It is shown that the height of the sample inlet line, its distance to the forest and the surrounding topography has a strong impact on both the absolute and relative deviations from PSS. Global irradiance and thus, photolysis of NO2 is reduced within the dense forest. Since the reaction of NO with O3 is still proceeding under these conditions, increased NO2/NO ratios are produced locally in air which is transported through the forest and advected to the MOHp site. Estimates of the peroxy radical concentration (RO2) inferred from PSS are compared with peroxy radical measurements made at the site in June 2000 during a three-week campaign. The PSS derived RO2 levels were higher than corresponding measured levels by at least a factor of 2-3. This analysis was made for a wind sector with minimal local effects on PSS. Thus the corresponding Φ median of 2 can be regarded as an upper limit for a deviation from PSS due to chemical reactions, i.e. by peroxy radicals and possible other oxidants converting additional NO to NO2.
Uptake study of ClONO2 and BrONO2 by Halide containing droplets
Authors: Deiber G. , George Ch. , Le Calvé S. , Schweitzer F. , Mirabel Ph.
Published: April 2010

Abstract. The uptake kinetics of gaseous ClONO2 and BrONO2 on aqueous surfaces were measured, as a function of temperature and liquid composition (pure water and NaCl or NaBr containing solutions) using the droplet train technique coupled to a mass spectrometer. The uptake kinetics are driven by the reactivity of these gases and, for both compounds, the uptake rates on pure water or on NaCl solutions (0.1M) are comparable. The uptake coefficient γ of ClONO2 does not depend on the temperature while that of BrONO2 increases slightly when the temperature is raised from 272 to 280K. For ClONO2 and BrONO2, the uptake rates increase on NaBr-doped droplets, enabling the estimation of the mass accommodation coefficient α. The corresponding values for α are 0.108±0.033 for ClONO2 and 0.063±0.021 for BrONO2 where the statistical errors correspond to ±2σ. The reactions of ClONO2 and BrONO2 on NaCl solutions lead respectively to the formation of Cl2 and BrCl. The uptake of ClONO2 on NaBr solutions generates BrCl as primary product, which in turn can react with NaBr to produce Br2. As expected, the only product of BrONO2 reaction on NaBr solution is Br2.
Seasonality and extent of extratropical TST derived from in-situ CO measurements during SPURT
Authors: Hoor P. , Gurk C. , Brunner D. , Hegglin M. I. , Wernli H. , Fischer H.
Published: April 2010

Abstract. We present airborne in-situ trace gas measurements which were performed on eight campaigns between November 2001 and July 2003 during the SPURT-project (SPURenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region). The measurements on a quasi regular basis allowed an overview of the seasonal variations of the trace gas distribution in the tropopause region over Europe from 35°-75°N to investigate the influence of transport and mixing across the extratropical tropopause on the lowermost stratosphere. From the correlation of CO and O3 irreversible mixing of tropospheric air into the lowermost stratosphere is identified. The CO distribution indicates that transport and subsequent mixing of tropospheric air across the extratropical tropopause predominantly affects a layer, which closely follows the shape of the local tropopause. In addition, the seasonal cycle of CO2 illustrates the strong coupling of that layer to the extratropical troposphere. Both, horizontal gradients of CO on isentropes as well as the CO-O3-distribution in the lowermost stratosphere reveal that the influence of quasi-horizontal transport and subsequent mixing weakens with distance from the local tropopause. The mixing layer extends to about 25 K in potential temperature above the local tropopause exhibiting only a weak seasonality. However, at large distances from the tropopause a significant influence of tropospheric air is still evident. The relation between N2O and CO2 indicates that a significant contribution of air originating from the tropical tropopause contributes to the background air in the extratropical lowermost stratosphere.