bluuebunny/crossref_metadata_2025 huggingface dataset:
Using neural networks to describe tracer correlations
Authors: Lary D. J. , Müller M. D. , Mussa H. Y.
Published: April 2010

Abstract. Neural networks are ideally suited to describe the spatial and temporal dependence of tracer-tracer correlations. The neural network performs well even in regions where the correlations are less compact and normally a family of correlation curves would be required. For example, the CH4-N2O correlation can be well described using a neural network trained with the latitude, pressure, time of year, and CH4 volume mixing ratio (v.m.r.). In this study a neural network using Quickprop learning and one hidden layer with eight nodes was able to reproduce the CH4-N2O correlation with a correlation coefficient between simulated and training values of 0.9995. Such an accurate representation of tracer-tracer correlations allows more use to be made of long-term datasets to constrain chemical models. Such as the dataset from the Halogen Occultation Experiment (HALOE) which has continuously observed CH4  (but not N2O) from 1991 till the present. The neural network Fortran code used is available for download.
Absolute absorption cross-section and photolysis rate of I2
Authors: Saiz-Lopez A. , Saunders R. W. , Joseph D. M. , Ashworth S. H. , Plane J. M. C.
Published: April 2010

Abstract. Following recent observations of molecular iodine (I2) in the coastal marine boundary layer (MBL) (Saiz-Lopez and Plane, 2004), it has become important to determine the absolute absorption cross-section of I2 at reasonably high resolution, and also to evaluate the rate of photolysis of the molecule in the lower atmosphere. The absolute absorption cross-section (σ) of gaseous I2 at room temperature and pressure (295K, 760Torr) was therefore measured between 182 and 750nm using a Fourier Transform spectrometer at a resolution of 4cm-1 (0.1nm at λ=500nm). The maximum absorption cross-section in the visible region was observed at λ=533.0nm to be σ=(4.24±0.50)x10-18cm2molecule-1. The spectrum is available as supplementary material accompanying this paper. The photo-dissociation rate constant (J) of gaseous I2 was also measured directly in a solar simulator, yielding J(I2)=0.12±0.03s-1 for the lower troposphere. This is in excellent agreement with the value of 0.12±0.015s-1 calculated using the measured absorption cross-section, terrestrial solar flux for clear sky conditions and assuming a photo-dissociation yield of unity. A two-stream radiation transfer model was then used to determine the variation in photolysis rate with solar zenith angle (SZA), from which an analytic expression is derived for use in atmospheric models. Photolysis appears to be the dominant loss process for I2 during daytime, and hence an important source of iodine atoms in the lower atmosphere.
Modelling tracer transport by a cumulus ensemble: lateral boundary conditions and large-scale ascent
Authors: Salzmann M. , Lawrence M. G. , Phillips V. T. J. , Donner L. J.
Published: April 2010

Abstract. The vertical transport of tracers by a cumulus ensemble at the TOGA-COARE site is modelled during a 7 day episode using 2-D and 3-D cloud-resolving setups of the Weather Research and Forecast (WRF) model. Lateral boundary conditions (LBC) for tracers, water vapour, and wind are specified and the horizontal advection of trace gases across the lateral domain boundaries is considered. Furthermore, the vertical advection of trace gases by the large-scale motion (short: vertical large-scale advection of tracers, VLSAT) is considered. It is shown that including VLSAT partially compensates the calculated net downward transport from the middle and upper troposphere (UT) due to the mass balancing mesoscale subsidence induced by deep convection. Depending on whether the VLSAT term is added or not, modelled domain averaged vertical tracer profiles can differ significantly. Differences between a 2-D and a 3-D model run were mainly attributed to an increase in horizontal advection across the lateral domain boundaries due to the meridional wind component not considered in the 2-D setup.
Extrapolating future Arctic ozone losses
Authors: Knudsen B. M. , Harris N. R. P. , Andersen S. B. , Christiansen B. , Larsen N. , Rex M. , Naujokat B.
Published: April 2010

Abstract. Future increases in the concentration of greenhouse gases and water vapour may cool the stratosphere further and increase the amount of polar stratospheric clouds (PSCs). Future Arctic PSC areas have been extrapolated from the highly significant trends 1958-2001. Using a tight correlation between PSC area and the total vortex ozone depletion and taking the decreasing amounts of ozone depleting substances into account we make empirical estimates of future ozone. The result is that Arctic ozone losses increase until 2010-2015 and decrease only slightly afterwards. However, for such a long extrapolation into the future caution is necessary. Tentatively taking the modelled decrease in the ozone trend in the future into account results in almost constant ozone depletions until 2020 and slight decreases afterwards. This approach is a complementary method of prediction to that based on the complex coupled chemistry-climate models (CCMs).
Boreal forest fires in 1997 and 1998: a seasonal comparison using transport model simulations and measurement data
Authors: Spichtinger N. , Damoah R. , Eckhardt S. , Forster C. , James P. , Beirle S. , Marbach T. , Wagner T. , Novelli P. C. , Stohl A.
Published: April 2010

Abstract. Forest fire emissions have a strong impact on the concentrations of trace gases and aerosols in the atmosphere. In order to quantify the influence of boreal forest fire emissions on the atmospheric composition, the fire seasons of 1997 and 1998 are compared in this paper. Fire activity in 1998 was very strong, especially over Canada and Eastern Siberia, whereas it was much weaker in 1997. According to burned area estimates the burning in 1998 was more than six times as intense as in 1997. Based on hot spot locations derived from ATSR (Along Track Scanning Radiometer) data and official burned area data, fire emissions were estimated and their transport was simulated with a Lagrangian tracer transport model. Siberian and Canadian forest fire tracers were distinguished to investigate the transport of both separately. The fire emissions were transported even over intercontinental distances. Due to the El Niño induced meteorological situation, transport from Siberia to Canada was enhanced in 1998. Siberian fire emissions were transported towards Canada and contributed concentrations more than twice as high as those due to Canada's own CO emissions by fires. In 1998 both tracers arrive at higher latitudes over Europe, which is due to a higher North Atlantic Oscillation (NAO) index in 1998. The simulated emission plumes are compared to CMDL (Climate Monitoring and Diagnostics Laboratory) CO2 and CO data, Total Ozone Mapping Spectrometer (TOMS) aerosol index (AI) data and Global Ozone Monitoring Experiment (GOME) tropospheric NO2 and HCHO columns. All the data show clearly enhanced signals during the burning season of 1998 compared to 1997. The results of the model simulation are in good agreement with ground-based as well as satellite-based measurements.
Soot aging time scales in polluted regions during day and night
Authors: Riemer N. , Vogel H. , Vogel B.
Published: April 2010

Abstract. The aging of soot is one of the key uncertainties in the estimation of both the direct and indirect climate effect. While freshly emitted soot is initially hydrophobic and externally mixed, it can be transferred into an internal mixture by coagulation, condensation or photochemical processes. These aging processes affect the hygroscopic qualities and hence the growth behaviour, the optical properties and eventually the lifetime of the soot particles. However, due to computational limits the aging of soot in global climate models is often only parameterised by an estimated turnover rate resulting in a lifetime of soot of several days. Hence, the aging process of soot is one of the key uncertainties governing the burden and effect of black carbon. In this study, we discuss the time scale on which diesel soot is transferred from an external to an internal mixture based on the results of our simulations with a comprehensive mesoscale model. For daytime conditions during summer condensation of sulphuric acid is dominant and the aging process occurs on a time scale of τ =8h close to the sources and τ =2h above the source region. During winter comparable time scales are found but ammonium nitrate becomes more important. During night time condensation is not effective. Then coagulation is the most important aging process and our results show time scales between 10h and 40h.
Enhanced uptake of water by oxidatively processed oleic acid
Authors: Asad A. , Mmereki B. T. , Donaldson D. J.
Published: April 2010

Abstract. A quartz crystal microbalance apparatus has been used to measure the room temperature uptake of water vapour by thin films of oleic acid as a function of relative humidity, both before and following exposure of the films to various partial pressures of gas phase ozone. A rapid increase in the water-sorbing ability of the film is observed as its exposure to ozone is increased, followed by a plateau region in which additional water is taken up more gradually. In this fully-processed region the mass of water taken up by the film is about 4 times that of the unprocessed film. Infrared spectra of the films, measured after variable exposures to ozone, show dramatic increases in both the "free" and hydrogen-bonded O-H stretching regions, and a decrease in the intensity of olefinic features. These results are consistent with the formation of an oxygenated polymeric product or products, as well as the gas phase products previously identified.
Physical properties of the sub-micrometer aerosol over the Amazon rain forest during the wet-to-dry season transition - comparison of modeled and measured CCN concentrations
Authors: Rissler J. , Swietlicki E. , Zhou J. , Roberts G. , Andreae M. O. , Gatti L. V. , Artaxo P.
Published: April 2010

Abstract. Sub-micrometer atmospheric aerosol particles were studied in the Amazon region, 125 km northeast of Manaus, Brazil (-1°55.2'S, 59°28.1'W). The measurements were performed during the wet-to-dry transition period, 4-28 July 2001 as part of the LBA (Large-Scale Biosphere Atmosphere Experiment in Amazonia) CLAIRE-2001 (Cooperative LBA Airborne Regional Experiment) experiment. The number size distribution was measured with two parallel differential mobility analyzers, the hygroscopic growth at 90% RH with a Hygroscopic Tandem Mobility Analyzer (H-TDMA) and the concentrations of cloud condensation nuclei (CCN) with a cloud condensation nuclei counter. A model was developed that uses the H-TDMA data to predict the number of soluble molecules or ions in the individual particles and the corresponding minimum particle diameter for activation into a cloud droplet at a certain supersaturation. Integrating the number size distribution above this diameter, CCN concentrations were predicted with a time resolution of 10 min and compared to the measured concentrations. During the study period, three different air masses were identified and compared: clean background, air influenced by aged biomass burning, and moderately polluted air from recent local biomass burning. For the clean period 2001, similar number size distributions and hygroscopic behavior were observed as during the wet season at the same site in 1998, with mostly internally mixed particles of low diameter growth factor (~1.3 taken from dry to 90% RH). During the periods influenced by biomass burning the hygroscopic growth changed slightly, but the largest difference was seen in the number size distribution. The CCN model was found to be successful in predicting the measured CCN concentrations, typically within 25%. A sensitivity study showed relatively small dependence on the assumption of which model salt that was used to predict CCN concentrations from H-TDMA data. One strength of using H-TDMA data to predict CCN concentrations is that the model can also take into account soluble organic compounds, insofar as they go into solution at 90% RH. Another advantage is the higher time resolution compared to using size-resolved chemical composition data.
Release and dispersion of vegetation and peat fire emissions in the atmosphere over Indonesia 1997/1998
Authors: Langmann B. , Heil A.
Published: April 2010

Abstract. Smoke-haze episodes caused by vegetation and peat fires affect parts of Indonesia every year with significant impacts on human health and climate. Particularly fires in degenerated peat areas release huge amounts of trace gases, e.g. CO2, CO and CH4, and particles into the atmosphere, exceeding by far the emissions per unit area from fires in surface vegetation. However, only limited information is available about the current distribution of pristine and degenerated peat areas in Indonesia, their depth, drainage condition and modification by fire. Particularly during the strong El Niño event in 1997/1998 a huge uncertainty exists about the contribution of Indonesian peat fire emissions to the measured increase of atmospheric CO2, as the published estimates of the peat area burned differ considerably. In this paper we study the contribution of peat fire emissions in Indonesia during the El Niño event 1997/1998. A regional three-dimensional atmosphere-chemistry model is applied over Indonesia using two emission estimates. These vegetation and peat fire emission inventories for Indonesia are set up in 0.5° resolution in weekly intervals and differ only in the size of the fire affected peat areas. We evaluate simulated rainfall and particle concentrations by comparison with observations to draw conclusions on the total carbon emissions released from the vegetation and peat fires in Indonesia in 1997/1998.
Tethered balloon measurements of biogenic volatile organic compounds at a Boreal forest site
Authors: Spirig C. , Guenther A. , Greenberg J. P. , Calanca P. , Tarvainen V.
Published: April 2010

Abstract. Measurements of biogenic volatile organic compounds (VOCs) were performed at Hyytiälä, a Boreal forest site in Southern Finland as part of the OSOA (origin and formation of secondary organic aerosol) project in August 2001. At this site, frequent formation of new particles has been observed and the role of biogenic VOCs in this process is still unclear. Tethered balloons served as platforms to collect VOC samples within the planetary boundary layer at heights up to 1.2 km above ground during daytime. Mean mixed layer concentrations of total monoterpenes varied between 10 and 170 pptv, with a-pinene, limonene and D3-carene as major compounds, isoprene was detected at levels of 2-35 pptv. A mixed layer gradient technique and a budget approach are applied to derive surface fluxes representative for areas of tens to hundreds of square kilometres. Effects of spatial heterogeneity in surface emissions are examined with a footprint analysis. Depending on the source area considered, mean afternoon emissions of the sum of terpenes range between 180 and 300 mg m-2 h-1 for the period of 2-12 August 2001. Surface fluxes close to Hyytiälä were higher than the regional average, and agree well with mean emissions predicted by a biogenic VOC emission model. Total rates of monoterpene oxidation were calculated with a photochemical model. The rates did not correlate with the occurrence of new particle formation, but the ozone pathway was of more importance on days with particle formation. Condensable vapour production from the oxidation of monoterpenes throughout the mixed layer can only account for a fraction of the increase in aerosol mass observed at the surface.
Ozone loss and chlorine activation in the Arctic winters 1991-2003 derived with the tracer-tracer correlations
Authors: Tilmes S. , Müller R. , Grooß J.-U. , Russell III J. M.
Published: April 2010

Abstract. Chemical ozone loss in the Arctic stratosphere was investigated for the twelve years between 1991 and 2003 employing the ozone-tracer correlation method. For this method, the change in the relation between ozone and a long-lived tracer is considered for all twelve years over the lifetime of the polar vortex to calculate chemical ozone loss. Both the accumulated local ozone loss in the lower stratosphere and the column ozone loss were derived consistently, mainly on the basis of HALOE satellite observations. HALOE measurements do not cover the polar region homogeneously over the course of the winter. Thus, to derive an early winter reference function for each of the twelve years, all available measurements were additionally used; for two winters climatological considerations were necessary. Moreover, a detailed quantification of uncertainties was performed. This study further demonstrates the interaction between meteorology and ozone loss. The connection between temperature conditions and chlorine activation, and in turn, the connection between chlorine activation and ozone loss, becomes obvious in the HALOE HCl measurements. Additionally, the degree of homogeneity of ozone loss within the vortex was shown to depend on the meteorological conditions. Results derived here are in general agreement with the results obtained by other methods for deducing polar ozone loss. Differences occur mainly owing to different time periods considered in deriving accumulated ozone loss. However, very strong ozone losses as deduced from SAOZ for January in winters 1993-1994 and 1995-1996 cannot be identified using available HALOE observations in the early winter. In general, strong accumulated ozone loss was found to occur in conjunction with a strong cold vortex containing a large volume of possible PSC existence (VPSC), whereas moderate ozone loss was found if the vortex was less strong and moderately warm. Hardly any ozone loss was calculated for very warm winters with small amounts of VPSC during the entire winter. This study supports the linear relationship between VPSC and the accumulated ozone loss reported by Rex et al. (2004) if VPSC was averaged over the entire winter period. Here, further meteorological factors controlling ozone loss were additionally identified if VPSC was averaged over the same time interval as that for which the accumulated ozone loss was deduced. A significant difference in ozone loss (of ≈36DU) was found due to the different duration of solar illumination of the polar vortex of at maximum 4 hours per day in the observed years. Further, the increased burden of aerosols in the atmosphere after the Pinatubo volcanic eruption in 1991 significantly increased the extent of chemical ozone loss.
Actinic flux and photolysis in water droplets: Mie calculations and geometrical optics limit
Authors: Mayer B. , Madronich S.
Published: April 2010

Abstract. Photolysis of water-soluble components inside cloud droplets by ultraviolet/visible radiation may play an important role in atmospheric chemistry. Two earlier studies have suggested that the actinic flux and hence the photolysis frequency within spherical droplets is enhanced relative to that in the surrounding air, but have given different values for this enhancement. Here, we reconcile these discrepancies by noting slight errors in both studies that, when corrected, lead to consistent results. Madronich (1987) examined the geometric (large droplet) limit and concluded that refraction leads to an enhancement factor, averaged over all incident directions, of 1.56. However, the physically relevant quantity is the enhancement of the average actinic flux (rather than the average enhancement factor) which we show here to be 1.26 in the geometric limit. Ruggaber et al. (1997) used Mie theory to derive energy density enhancements slightly larger than 2 for typical droplet sizes, and applied these directly to the calculation of photolysis rates. However, the physically relevant quantity is the actinic flux (rather than the energy density) which is obtained by dividing the energy density by the refractive index of water, 1.33. Thus, the Mie-predicted enhancement for typical cloud droplet sizes is in the range 1.5, only coincidentally in agreement with the value originally given by Madronich. We also investigated the influence of resonances in the actinic flux enhancement. These narrow spikes which are resolved only by very high resolution calculations are orders of magnitude higher than the intermediate values but contribute only little to the actinic flux enhancement when averaged over droplet size distributions. Finally, a table is provided which may be used to obtain the actinic flux enhancement for the photolysis of any dissolved species.
Multi axis differential optical absorption spectroscopy (MAX-DOAS)
Authors: Hönninger G. , von Friedeburg C. , Platt U.
Published: April 2010

Abstract. Multi Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) in the atmosphere is a novel measurement technique that represents a significant advance on the well-established zenith scattered sunlight DOAS instruments which are mainly sensitive to stratospheric absorbers. MAX-DOAS utilizes scattered sunlight received from multiple viewing directions. The spatial distribution of various trace gases close to the instrument can be derived by combining several viewing directions. Ground based MAX-DOAS is highly sensitive to absorbers in the lowest few kilometres of the atmosphere and vertical profile information can be retrieved by combining the measurements with Radiative Transfer Model (RTM) calculations. The potential of the technique for a wide variety of studies of tropospheric trace species and its (few) limitations are discussed. A Monte Carlo RTM is applied to calculate Airmass Factors (AMF) for the various viewing geometries of MAX-DOAS. Airmass Factors can be used to quantify the light path length within the absorber layers. The airmass factor dependencies on the viewing direction and the influence of several parameters (trace gas profile, ground albedo, aerosol profile and type, solar zenith and azimuth angles) are investigated. In addition we give a brief description of the instrumental MAX-DOAS systems realised and deployed so far. The results of the RTM studies are compared to several examples of recent MAX-DOAS field experiments and an outlook for future possible applications is given.
Non-coincident inter-instrument comparisons of ozone measurements using quasi-conservative coordinates
Authors: Lait L. R. , Newman P. A. , Schoeberl M. R. , McGee T. , Twigg L. , Browell E. V. , Fenn M. A. , Grant W. B. , Butler C. F. , Bevilacqua R. , Davies J. , DeBacker H. , Andersen S. B. , Kyrö E. , Kivi E. , von der Gathen P. , Claude H. , Benesova A. , Skrivankova P. , Dorokhov V. , Zaitcev I. , Braathen G. , Gil M. , Litynska Z. , Moore D. , Gerding M.
Published: April 2010

Abstract. Ozone measurements from ozonesondes, AROTAL, DIAL, and POAM III instruments during the SOLVE-2/VINTERSOL period are composited in a time-varying, flow-following quasi-conservative (PV-θ) coordinate space; the resulting composites from each instrument are mapped onto the other instruments' locations and times. The mapped data are then used to intercompare data from the different instruments. Overall, the four ozone data sets are found to be in good agreement. AROTAL shows somewhat lower values below 16 km, and DIAL has a positive bias at the upper limits of its altitude range. These intercomparisons are consistent with those obtained from more conventional near-coincident profiles, where available. Although the PV-θ mapping technique entails larger uncertainties of individual profile differences compared to direct near-coincident comparisons, the ability to include much larger numbers of comparisons can make this technique advantageous.
Aerosol seasonal variability over the Mediterranean region and relative impact of maritime, continental and Saharan dust particles over the basin from MODIS data in the year 2001
Authors: Barnaba F. , Gobbi G. P.
Published: April 2010

Abstract. The one-year (2001) record of aerosol data from the space borne Moderate Resolution Imaging Spectroradiometer (MODIS) is analyzed focusing on the Mediterranean region. The MODIS aerosol optical thickness standard product (AOT at 550nm) provided over both land and ocean is employed to evaluate the seasonal and spatial variability of the atmospheric particulate over the region. Expected accuracy of the MODIS AOT is (±0.05±0.2xAOT) over land and (±0.03±0.05xAOT) over ocean. The seasonal analysis reveals a significant AOT variability all over the region, with minimum values in Winter (AOT<0.15) and maximum in Summer (AOT>0.2). The spatial variability is also found to be considerable, particularly over land. The impact of some major urban sites and industrialized areas is detectable. For the sole Mediterranean basin, a method (aerosol mask) was implemented to separate the contribution of maritime, continental and desert dust aerosol to the total AOT. Input of both continental and desert dust particles is well captured, showing North-to-South and South-to-North AOT gradients, respectively. A quantitative summary of the AOT seasonal and regional variability is given for different sectors of the Mediterranean basin. Results of this summary were also used to test the aerosol mask assumptions and indicate the method adopted to be suitable for the aerosol type selection. Estimates of the atmospheric aerosol mass load were performed employing specifically-derived mass-to-extinction efficiencies (α). For each aerosol type, a reliable mean α value was determined on the basis of both lidar measurements of extinction and aerosol models. These estimates indicate a total of 43Mtons of desert dust suspended over the basin during 2001. A comparable value is derived for maritime aerosol. Opposite to the dust case, a minor seasonal variability (within 15%) of maritime aerosol mass is found. This latter result is considered a further check of the suitability of the methodology adopted to separate, on the basis of MODIS data, the three aerosol types which dominate the Mediterranean region.
Hemispheric average Cl atom concentration from 13C/12C ratios in atmospheric methane
Authors: Platt U. , Allan W. , Lowe D.
Published: April 2010

Abstract. Methane is a significant atmospheric trace gas in the context of greenhouse warming and climate change. The dominant sink of atmospheric methane is the hydroxyl radical (OH). Recently, a mechanism for production of chlorine radicals (Cl) in the marine boundary layer (MBL) via bromine autocatalysis has been proposed. The importance of this mechanism in producing a methane sink is not clear at present because of the difficulty of in-situ direct measurement of Cl. However, the large kinetic isotope effect of Cl compared with OH produces a large fractionation of 13C compared with 12C in atmospheric methane. This property can be used to estimate the likely minimum size of the methane sink attributable to MBL Cl. By taking account of the mixing of MBL air into the free troposphere, we estimate that the global methane sink due to reaction with Cl atoms in the MBL could be as large as 19Tgyr-1, or about 3.3% of the total CH4 sink. However, its impact on the methane stable carbon isotope budget is large and warrants further attention.
NOGAPS-ALPHA model simulations of stratospheric ozone during the SOLVE2 campaign
Authors: McCormack J. P. , Eckermann S. D. , Coy L. , Allen D. R. , Kim Y.-J. , Hogan T. , Lawrence B. , Stephens A. , Browell E. V. , Burris J. , McGee T. , Trepte C. R.
Published: April 2010

Abstract. This paper presents three-dimensional prognostic O3 simulations with parameterized gas-phase photochemistry from the new NOGAPS-ALPHA middle atmosphere forecast model. We compare 5-day NOGAPS-ALPHA hindcasts of stratospheric O3 with satellite and DC-8 aircraft measurements for two cases during the SOLVE II campaign: (1) the cold, isolated vortex during 11-16 January 2003; and (2) the rapidly developing stratospheric warming of 17-22 January 2003. In the first case we test three different photochemistry parameterizations. NOGAPS-ALPHA O3 simulations using the NRL-CHEM2D parameterization give the best agreement with SAGE III and POAM III profile measurements. 5-day NOGAPS-ALPHA hindcasts of polar O3 initialized with the NASA GEOS4 analyses produce better agreement with observations than do the operational ECMWF O3 forecasts of case 1. For case 2, both NOGAPS-ALPHA and ECMWF 114-h forecasts of the split vortex structure in lower stratospheric O3 on 21 January 2003 show comparable skill. Updated ECMWF O3 forecasts of this event at hour 42 display marked improvement from the 114-h forecast; corresponding updated 42-hour NOGAPS-ALPHA prognostic O3 fields initialized with the GEOS4 analyses do not improve significantly. When NOGAPS-ALPHA prognostic O3 is initialized with the higher resolution ECMWF O3 analyses, the NOGAPS-ALPHA 42-hour lower stratospheric O3 fields closely match the operational 42-hour ECMWF O3 forecast of the 21 January event. We find that stratospheric O3 forecasts at high latitudes in winter can depend on both model initial conditions and the treatment of photochemistry over periods of 1-5 days. Overall, these results show that the new O3 initialization, photochemistry parameterization, and spectral transport in the NOGAPS-ALPHA NWP model can provide reliable short-range stratospheric O3 forecasts during Arctic winter.
Stratospheric aerosol measurements by dual polarisation lidar
Authors: Vaughan G. , Wareing D. P.
Published: April 2010

Abstract. We present measurements of stratospheric aerosol made at Aberystwyth, UK (52.4° N, 4.06° W) during periods of background aerosol conditions. The measurements were made with a lidar system based on a 532nm laser and two polarisation channels in the receiver. When stratospheric aerosol amounts are very small, as at present, this method is, potentially, free of a number of systematic errors that bedevil more commonly-used methods. The method rests on the assumption that the aerosol consists of spherical droplets which do not depolarise the lidar signal, which is valid under most conditions. Maximum lidar ratios in background aerosol of 1.03-1.06 were measured during the period 2001-2004, with integrated backscatter in the range 2-7x10-5sr-1. In January 2003, depolarising aerosol was measured, which invalidated the dual-polarisation measurements. On 10-11 January, the depolarising aerosol was clearly a polar stratospheric cloud (the first lidar observations of such clouds in the British Isles) but the aerosol observed on 7-8 January was too low in altitude and too warm to be a PSC.
Noctilucent clouds and the mesospheric water vapour: the past decade
Authors: von Zahn U. , Baumgarten G. , Berger U. , Fiedler J. , Hartogh P.
Published: April 2010

Abstract. The topic of this paper is the sensitivity of the brightness of noctilucent clouds (NLC) on the ambient water vapour mixing ratio f(H2O). Firstly, we use state-of-the-art models of NLC layer formation to predict NLC brightness changes in response to changes in the 80km mixing ratio f(H2O) for the two cases of ground-based 532nm lidar observations at 69° N and for hemispheric satellite SBUV observations at 252nm wavelength. In this study, we include a re-evaluation of the sensitivity of NLC brightness to changes in solar Lyman α flux. Secondly, we review observations of episodic changes in f(H2O) and those in NLC brightness, the former being available since 1992, the latter since 1979. To this review, we add a new series of observations of f(H2O), performed in the Arctic summer at the ALOMAR observatory. The episodic change exhibited by the Arctic summer means of f(H2O) turns out to be quite different from all those derived from annual means of f(H2O). The latter indicate that since 1996 a significant reduction of annually averaged upper mesospheric water vapour has occurred at low, mid, and high latitudes. These decreases of f(H2O) have been observed over the same time period in which a slow increase of SBUV NLC albedo has occurred. From this scenario and additional arguments we conclude that the cause for the observed long-term increase in NLC albedo remains to be identified. We close with comments on the very different character of decadal variations in NLC brightness and occurrence rate.
Simulating the global atmospheric black carbon cycle: a revisit to the contribution of aircraft emissions
Authors: Hendricks J. , Kärcher B. , Döpelheuer A. , Feichter J. , Lohmann U. , Baumgardner D.
Published: April 2010

Abstract. The black carbon (BC) burden of the upper troposphere and lowermost stratosphere (UTLS) is investigated with the general circulation model (GCM) ECHAM4. The special focus is the contribution of aircraft emissions to the UTLS BC loading. Previous studies on the role of aircraft emissions in the global BC cycle either neglect BC sources located at the Earth's surface or simplify the BC cycle by assuming pre-defined BC residence times. Here, the global BC cycle including emissions, transport, and removal is explicitly simulated. The BC emissions considered include surface sources as well as BC from aviation. This enables a consistent calculation of the relative contribution of aviation to the global atmospheric BC cycle. As a further extension to the previous studies, the aviation-induced perturbation of the UTLS BC particle number concentration is investigated. The uncertainties associated with the model predictions are evaluated by means of several sensitivity studies. Especially, the sensitivity of the results to different assumptions on the BC hygroscopic properties is analysed. The simulated UTLS BC concentrations are compared to in-situ observations. The simulations suggest that the large-scale contribution of aviation to the UTLS BC mass budget typically amounts to only a few percent, even in the most frequented flight regions. The aviation impact far away from these regions is negligible. The simulated aircraft contributions to the UTLS BC particle number concentration are much larger compared to the corresponding mass perturbations. The simulations suggest that aviation can cause large-scale increases in the UTLS BC particle number concentration of more than 30% in regions highly frequented by aircraft. The relative effect shows a pronounced annual variation with the largest relative aviation impact occurring during winter.
Optimizing CO2 observing networks in the presence of model error: results from TransCom 3
Authors: Rayner R. J
Published: April 2010

Abstract. We use a genetic algorithm to construct optimal observing networks of atmospheric concentration for inverse determination of net sources. Optimal networks are those that produce a minimum in average posterior uncertainty plus a term representing the divergence among source estimates for different transport models. The addition of this last term modifies the choice of observing sites, leading to larger networks than would be chosen under the traditional estimated variance metric. Model-model differences behave like sub-grid heterogeneity and optimal networks try to average over some of this. The optimization does not, however, necessarily reject apparently difficult sites to model. Although the results are so conditioned on the experimental set-up that the specific networks chosen are unlikely to be the best choices in the real world, the counter-intuitive behaviour of the optimization suggests the model error contribution should be taken into account when designing observing networks. Finally we compare the flux and total uncertainty estimates from the optimal network with those from the 3 control case. The  3 control case performs well under the chosen uncertainty metric and the flux estimates are close to those from the optimal case. Thus the 3 findings would have been similar if minimizing the total uncertainty guided their network choice.
Linking horizontal and vertical transports of biomass fire emissionsto the tropical Atlantic ozone paradox during the Northern Hemisphere winter season: climatology
Authors: Jenkins G. S. , Ryu J.-H.
Published: April 2010

Abstract. During the Northern hemisphere winter season, biomass burning is widespread in West Africa, yet the total tropospheric column ozone values (<30DU) over much of the Tropical Atlantic Ocean (15°N-5°S) are relatively low. At the same time, the tropospheric column ozone values in the Southern Tropical Atlantic are higher than those in the Northern Hemisphere (ozone paradox). We examine the causes for low tropospheric column ozone values by considering the horizontal and vertical transport of biomass fire emissions in West Africa during November through March, using observed data which characterizes fires, aerosols, horizontal winds, precipitation, lightning and outgoing longwave radiation. We have found that easterly winds prevail in the lower troposphere but transition to westerly winds at pressure levels lower than 500hPa. A persistent anticyclone over West Africa at 700hPa is responsible for strong easterly winds, which causes a net outflow of ozone/ozone precursors from biomass burning in West Africa across the Atlantic Ocean towards South America. The lowest outgoing longwave radiation (OLR) and highest precipitation rates are generally found over the central Atlantic, some distance downstream of fires in West Africa making the vertical transport of ozone and ozone precursors less likely and ozone destruction more likely. However, lightning over land areas in Central Africa and South America can lead to enhanced ozone levels in the upper troposphere especially over the Southern tropical Atlantic during the Northern Hemisphere winter season.
The velocity of meteoroids: a historical review
Authors: Williams I. P.
Published: April 2010

Abstract. Determining the velocity of meteoroids as they enter the Earth's atmosphere is very important since the value is fundamental in calculating the orbit of the meteoroid and hence eventually its origin. We describe early attempts at this determination and highlight problems that exist today.
Assessment of possible airborne impact from risk sites: methodology for probabilistic atmospheric studies
Authors: Baklanov A. A. , Mahura A. G.
Published: April 2010

Abstract. The main purpose of this study is to develop a methodology for a multidisciplinary nuclear risk and vulnerability assessment, and to test this methodology through estimation of a nuclear risk to population in the Northern European countries in case of a severe accident at the nuclear risk sites. For assessment of the probabilistic risk and vulnerability, a combination of social-geophysical factors and probabilities are considered. The main focus of this paper is the description of methodology for evaluation of the atmospheric transport of radioactive releases from the risk site regions based on the long-term trajectory modeling. The suggested methodology is given from the probabilistic point of view. The main questions stated are: What are probabilities and times for radionuclide atmospheric transport to different neighbouring countries and territories in case of the hypothetical accidental release at the nuclear risk site? Which geographical territories or countries are at the highest risk from the hypothetical accidental releases? To answer these questions we suggest applying the following research tools for probabilistic atmospheric studies. First tool is atmospheric modelling to calculate multiyear forward trajectories originated over the sites. Second tool is statistical analyses to explore temporal and spatial structure of calculated trajectories and evaluate different probabilistic impact indicators: atmospheric transport pathways, airflow, fast transport, typical transport time, maximum possible impact zone, maximum reaching distance, etc. These indicators are applicable for further GIS-analysis and integration to estimate regional risk and vulnerability in case of accidental releases at the risk sites and for planning the emergency response and preparedness systems.
Measuring atmospheric naphthalene with laser-induced fluorescence
Authors: Martinez M. , Harder H. , Ren X. , Lesher R. L. , Brune W. H.
Published: April 2010

Abstract. A new method for measuring gas-phase naphthalene in the atmosphere is based on laser-induced fluorescence at low pressure. The fluorescence spectrum of naphthalene near 308 nm was identified. Naphthalene fluorescence quenching by N, O and HO was investigated in the laboratory. No significant quenching was found for HO with mixing ratio up to 2.5%. The quenching rate of naphthalene fluorescence is (1.980.18) 10cmmolecules for N, and (2.480.08)10cmmolecules for O at 297 K. Instrument calibrations were performed with a range of naphthalene mixing ratios between 5 and 80 parts per billion by volume (ppbv, 10. In the current instrument configuration, the detection limit is estimated to be about 20 parts per trillion by volume (pptv, 10 with 2 confidence and a 1-min integration time. Measurements of atmospheric naphthalene in three cities, Nashville, TN, Houston, TX, and New York City, NY, are presented. Good correlation between naphthalene and major anthropogenic pollutants is found.
Commentary on "Improving the seasonal cycle and interannual variations of biomass burning aerosol sources" by Generoso et al.
Authors: Giglio L. , Kendall J. D.
Published: April 2010

Abstract. In a recent published paper, Generoso et al. (2003) describe a method for improving the spatial and temporal distribution of pyrogenic aerosol emission inventories. In the course of their analysis, the authors note several significant discrepancies in the seasonality of burning as observed by the Visible and Infrared Scanner (VIRS) and four other biomass burning data sets derived from satellite observations. In this commentary we explain the source of these discrepancies and clarify the origin of the VIRS observations that were used by Generoso et al.
Model study of multiphase DMS oxidation with a focus on halogens
Authors: von Glasow R. , Crutzen P. J.
Published: April 2010

Abstract. We studied the oxidation of dimethylsulfide (DMS) in the marine boundary layer (MBL) with a one-dimensional numerical model and focused on the influence of halogens. Our model runs show that there is still significant uncertainty about the end products of the DMS addition pathway, which is especially caused by uncertainty in the product yield of the reaction of the intermediate product methyl sulfinic acid (MSIA) with OH. BrO strongly increases the importance of the addition branch in the oxidation of DMS even when present at mixing ratios smaller than 0.5pmol mol-1. The inclusion of halogen chemistry leads to higher DMS oxidation rates and smaller DMS to SO2 conversion efficiencies. The DMS to SO2 conversion efficiency is also drastically reduced under cloudy conditions. In cloud-free model runs between 5 and 15% of the oxidized DMS reacts further to particulate sulfur, in cloudy runs this fraction is almost 100%. Sulfate production by HOClaq and HOBraq is important in cloud droplets even for small Br- deficits and related small gas phase halogen concentrations. In general, more particulate sulfur is formed when halogen chemistry is included. A possible enrichment of HCO3- in fresh sea salt aerosol would increase pH values enough to make the reaction of S(IV)* (=SO2,aq+HSO3-+SO32-) with O3 dominant for sulfate production. It leads to a shift from methyl sulfonic acid (MSA) to non-sea salt sulfate (nss-SO42-) production but increases the total nss-SO42- only somewhat because almost all available sulfur is already oxidized to particulate sulfur in the base scenario. We discuss how realistic this is for the MBL. We found the reaction MSAaq+OH to contribute about 10% to the production of nss-SO42- in clouds. It is unimportant for cloud-free model runs. Overall we find that the presence of halogens leads to processes that decrease the albedo of stratiform clouds in the MBL.
Effect of organic compounds on nanoparticle formation in diluted diesel exhaust
Authors: Mathis U. , Mohr M. , Zenobi R.
Published: April 2010

Abstract. The nucleation of nanoparticles in the exhaust of a modern light-duty diesel vehicle was investigated on a chassis dynamometer. This laboratory study is focused on the influence of volatile organic compounds (VOCs) on nucleation of volatile nanoparticles. Different organic compounds were added to the dilution air of the particle sampling under different sampling conditions. Sample temperature and relative sample humidity were varied in a wide range. The number size distribution of the particles was measured with a scanning mobility particle sizer (SMPS) and showed significant differences in response to the added organic compounds. While the nucleation mode particles showed a large variation in concentration, the accumulation mode particles remained unchanged for all compounds. Depending on the functional group, organic compounds were capable of initiating and increasing (alcohols and toluene) or decreasing (acetone, aniline, and methyl tert-butyl ether (MTBE)) nucleation mode particles. Short volatile aliphatic hydrocarbons (hexane and cyclohexane) turned out to be without effect on nucleation of nanoparticles. Possible reasons for the differences are discussed.
On the distribution of relative humidity in cirrus clouds
Authors: Spichtinger P. , Gierens K. , Smit H. G. J. , Ovarlez J. , Gayet J.-F.
Published: April 2010

Abstract. We have analysed relative humidity statistics from measurements in cirrus clouds taken unintentionally during the Measurement of OZone by Airbus In-service airCraft project (MOZAIC). The shapes of the in-cloud humidity distributions change from nearly symmetric in relatively warm cirrus (warmer than −40°C) to considerably positively skew (i.e. towards high humidities) in colder clouds. These results are in agreement to findings obtained recently from the INterhemispheric differences in Cirrus properties from Anthropogenic emissions (INCA) campaign (Ovarlez et al., 2002). We interprete the temperature dependence of the shapes of the humidity distributions as an effect of the length of time a cirrus cloud needs from formation to a mature equilibrium stage, where the humidity is close to saturation. The duration of this transitional period increases with decreasing temperature. Hence cold cirrus clouds are more often met in the transitional stage than warm clouds.
Meteor velocity determination with plasma physics
Authors: Dyrud L. P. , Denney K. , Close S. , Oppenheim M. , Chau J. , Ray L.
Published: April 2010

Abstract. Understanding the global meteor flux at Earth requires the measurement of meteor velocities. While several radar methods exist for measuring meteor velocity, they may be biased by plasma reflection mechanisms. This paper presents a new method for deriving meteoroid velocity from the altitudinal extent of non-specular trails. This method employs our recent discoveries on meteor trail plasma instability. Dyrud et al. (2002) demonstrated that meteor trails are unstable over a limited altitude range, and that the precise altitudes of instability are dependent on the meteoroid that generated the trail. Since meteor trail instability results in field aligned irregularities (FAI) that allow for radar reflection, non-specular trail observations may be used to derive velocity. We use ALTAIR radar data of combined head echos and non-specular trails to test non-specular trail derived velocity against head echo velocities. Meteor velocities derived from non-specular trail altitudinal width match to within 5 km/s when compared with head echo range rates from the same meteor. We apply this technique to Piura radar observations of hundreds of non-specular trails to produce histograms of occurrence of meteor velocity based solely on this non-specular trails width criterion. The results from this study show that the most probable velocity of meteors seen by the Piura radar is near 50 km/s, which is comparable with modern head echo studies.