bluuebunny/crossref_metadata_2025_split huggingface dataset:
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.
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.
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.
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.
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.
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.
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.
Influence of stratospheric airmasses on tropospheric vertical O3 columns based on GOME (Global Ozone Monitoring Experiment) measurements and backtrajectory calculation over the Pacific
Authors: Ladstätter-Weißenmayer A. , Meyer-Arnek J. , Schlemm A. , Burrows J. P. 
Published: April 2010

Abstract. Satellite based GOME (Global Ozone Measuring experiment) data are used to characterize the amount of tropospheric ozone over the tropical Pacific. Tropospheric ozone was determined from GOME data using the Tropospheric Excess Method (TEM). In the tropical Pacific a significant seasonal variation is detected. Tropospheric excess ozone is enhanced during the biomass burning season from September to November due to outflow from the continents. In September 1999 GOME data reveal an episode of increased excess ozone columns over Tahiti (18.0° S; 149.0° W) (Eastern Pacific) compared to Am. Samoa (14.23° S; 170.56° W) and Fiji (18.13° S; 178.40° E), both situated in the Western Pacific. Backtrajectory calculations show that none of the airmasses arriving over the three locations experienced anthropogenic pollution (e. g. biomass burning). Consequently other sources of ozone have to be considered. One possible process leading to an increase of tropospheric ozone is stratosphere-troposphere-exchange. An analysis of the potential vorticity along trajectories arriving above each of the locations reveals that airmasses at Tahiti are subject to enhanced stratospheric influence, compared to Am. Samoa and Fiji. As a result this study shows clear incidents of transport of airmasses from the stratosphere into the troposphere.
Simulation of stratospheric water vapor trends: impact on stratospheric ozone chemistry
Authors: Stenke A. , Grewe V. 
Published: April 2010

Abstract. A transient model simulation of the 40-year time period 1960 to 1999 with the coupled climate-chemistry model (CCM) ECHAM4.L39(DLR)/CHEM shows a stratospheric water vapor increase over the last two decades of 0.7 ppmv and, additionally, a short-term increase after major volcanic eruptions. Furthermore, a long-term decrease in global total ozone as well as a short-term ozone decline in the tropics after volcanic eruptions are modeled. In order to understand the resulting effects of the water vapor changes on lower stratospheric ozone chemistry, different perturbation simulations were performed with the CCM ECHAM4.L39(DLR)/CHEM feeding the water vapor perturbations only to the chemistry part. Two different long-term perturbations of lower stratospheric water vapor, +1 ppmv and +5 ppmv, and a short-term perturbation of +2 ppmv with an e-folding time of two months were applied. An additional stratospheric water vapor amount of 1 ppmv results in a 5–10% OH increase in the tropical lower stratosphere between 100 and 30 hPa. As a direct consequence of the OH increase the ozone destruction by the HOx cycle becomes 6.4% more effective. Coupling processes between the HOx-family and the NOx/ClOx-family also affect the ozone destruction by other catalytic reaction cycles. The NOx cycle becomes 1.6% less effective, whereas the effectiveness of the ClOx cycle is again slightly enhanced. A long-term water vapor increase does not only affect gas-phase chemistry, but also heterogeneous ozone chemistry in polar regions. The model results indicate an enhanced heterogeneous ozone depletion during antarctic spring due to a longer PSC existence period. In contrast, PSC formation in the northern hemisphere polar vortex and therefore heterogeneous ozone depletion during arctic spring are not affected by the water vapor increase, because of the less PSC activity. Finally, this study shows that 10% of the global total ozone decline in the transient model run can be explained by the modeled water vapor increase, but the simulated tropical ozone decrease after volcanic eruptions is caused dynamically rather than chemically.
Aerosol optical depth measurements by airborne sun photometer in SOLVE II: Comparisons to SAGE III, POAM III and airborne spectrometer measurements
Authors: Russell P. , Livingston J. , Schmid B. , Eilers J. , Kolyer R. , Redemann J. , Ramirez S. , Yee J.-H. , Swartz W. , Shetter R. , Trepte C. , Risley A. , Wenny B. , Zawodny J. , Chu W. , Pitts M. , Lumpe J. , Fromm M. , Randall C. , Hoppel K. , Bevilacqua R. 
Published: April 2010

Abstract. The 14-channel NASA Ames Airborne Tracking Sunphotometer (AATS-14) measured solar- beam transmission on the NASA DC-8 during the second SAGE III Ozone Loss and Validation Experiment (SOLVE II). This paper presents AATS-14 results for multiwavelength aerosol optical depth (AOD), including comparisons to results from two satellite sensors and another DC-8 instrument, namely the Stratospheric Aerosol and Gas Experiment III (SAGE III), the Polar Ozone and Aerosol Measurement III (POAM III) and the Direct-beam Irradiance Airborne Spectrometer (DIAS). AATS-14 provides aerosol results at 13 wavelengths λ spanning the range of SAGE III and POAM III aerosol wavelengths. Because most AATS measurements were made at solar zenith angles (SZA) near 90°, retrieved AODs are strongly affected by uncertainties in the relative optical airmass of the aerosols and other constituents along the line of sight (LOS) between instrument and sun. To reduce dependence of the AATS-satellite comparisons on airmass, we perform the comparisons in LOS transmission and LOS optical thickness (OT) as well as in vertical OT (i.e., optical depth, OD). We also use a new airmass algorithm that validates the algorithm we previously used to within 2% for SZA<90°, and in addition provides results for SZA≥90°. For 6 DC-8 flights, 19 January-2 February 2003, AATS and DIAS results for LOS aerosol OT at λ=400nm agree to ≤12% of the AATS value. Mean and root-mean-square (RMS) differences, (DIAS-AATS)/AATS, are -2.3% and 7.7%, respectively. For DC-8 altitudes, AATS-satellite comparisons are possible only for λ>440nm, because of signal depletion for shorter λ on the satellite full-limb LOS. For the 4 AATS-SAGE and 4 AATS-POAM near-coincidences conducted 19-31 January 2003, AATS-satellite AOD differences were ≤0.0041 for all λ>440nm. RMS differences were ≤0.0022 for SAGE-AATS and ≤0.0026 for POAM-AATS. RMS relative differences in AOD ([SAGE-AATS]/AATS) were ≤33% for λ<~755nm, but grew to 59% for 1020nm and 66% at 1545nm. For λ>~755nm, AATS-POAM differences were less than AATS-SAGE differences, and RMS relative differences in AOD ([AATS-POAM]/AATS) were ≤31% for all λ between 440 and 1020nm. Unexplained differences that remain are associated with transmission differences, rather than differences in gas subtraction or conversion from LOS to vertical quantities. The very small stratospheric AOD values that occurred during SOLVE II added to the challenge of the comparisons, but do not explain all the differences.
Nitric Acid Trihydrate (NAT) formation at low NAT supersaturation in Polar Stratospheric Clouds (PSCs)
Authors: Voigt C. , Schlager H. , Luo B. P. , Dörnbrack A. , Roiger A. , Stock P. , Curtius J. , Vössing H. , Borrmann S. , Davies S. , Konopka P. , Schiller C. , Shur G. , Peter T. 
Published: April 2010

Abstract. A PSC was detected on 6 February 2003 in the Arctic stratosphere by in-situ measurements onboard the high-altitude research aircraft Geophysica. Low number densities (~10-4cm-3) of small nitric acid (HNO3) containing particles (d<6µm) were observed at altitudes between 18 and 20km. Provided the temperatures remain below the NAT equilibrium temperature TNAT, these NAT particles have the potential to grow further and to remove HNO3 from the stratosphere, thereby enhancing polar ozone loss. Interestingly, the NAT particles formed in less than a day at temperatures just slightly below TNAT (T>TNAT-3.1K). This unique measurement of PSC formation at extremely low NAT saturation ratios (SNAT≤10) constrains current NAT nucleation theories. We suggest, that the NAT particles have formed heterogeneously, but for certain not on ice. Conversely, meteoritic particles may be favorable candidates for triggering NAT nucleation at the observed low number densities.
Evolution of stratospheric ozone during winter 2002/2003 as observed by a ground-based millimetre wave radiometer at Kiruna, Sweden
Authors: Raffalski U. , Hochschild G. , Kopp G. , Urban J. 
Published: April 2010

Abstract. We present ozone measurements from the millimetre wave radiometer installed at the Swedish Institute of Space Physics (Institutet för rymdfysik, IRF) in Kiruna (67.8° N, 20.4° E, 420 m asl). Nearly continuous operation in the winter of 2002/2003 allows us to give an overview of ozone evolution in the stratosphere between 15 and 55 km. In this study we present a detailed analysis of the Arctic winter 2002/2003. By means of a methodology using equivalent latitudes we investigate the meteorological processes in the stratosphere during the entire winter/spring period. During the course of the winter strong mixing into the vortex took place in the middle and upper stratosphere as a result of three minor and one major warming event, but no evidence was found for significant mixing in the lower stratosphere. Ozone depletion in the lower stratosphere during this winter was estimated by measurements on those days when Kiruna was well inside the Arctic polar vortex. The days were carefully chosen using a definition of the vortex edge based on equivalent latitudes. At the 475 K isentropic level a cumulative ozone loss of about 0.5 ppmv was found starting in January and lasting until mid-March. The early ozone loss is probably a result of the very cold temperatures in the lower stratosphere in December and the geographical extension of the vortex to lower latitudes where solar irradiation started photochemical ozone loss in the pre-processed air. In order to correct for dynamic effects of the ozone variation due to diabatic subsidence of air masses inside the vortex, we used N2O measurements from the Odin satellite for the same time period. The derived ozone loss in the lower stratosphere between mid-December and mid-March varies between 1.1±0.1 ppmv on the 150 ppbv N2O isopleth and 1.7±0.1 ppmv on the 50 ppbv N2O isopleth.
Parametric sensitivity and uncertainty analysis of dimethylsulfide oxidation in the clear-sky remote marine boundary layer
Authors: Lucas D. D. , Prinn R. G. 
Published: April 2010

Abstract. Local and global sensitivity and uncertainty methods are applied to a box model of the dimethylsulfide (DMS) oxidation cycle in the remote marine boundary layer in order to determine the key physical and chemical parameters and sources of uncertainty. The model considers 58 uncertain parameters, and simulates the diurnal gas-phase cycles of DMS, SO2, methanesulfonic acid (MSA), and H2SO4 for clear-sky summertime conditions observed over the Southern Ocean. The results of this study depend on many underlying assumptions, including the DMS mechanism, simulation conditions, and probability distribution functions of the uncertain parameters. A local direct integration method is used to calculate first-order local sensitivity coefficients for infinitesimal perturbations about the parameter means. Key parameters identified by this analysis are related to DMS emissions, vertical mixing, heterogeneous removal, and the DMS+OH abstraction and addition reactions. MSA and H2SO4 are also sensitive to numerous rate constants, which limits the ability of using parameterized mechanisms to predict their concentrations. Of the chemistry, H2SO4 is highly sensitive to the rate constants for a set of nighttime reactions that lead to its production through a non-SO2 path initiated by the oxidation of DMS by NO3. For the global analysis, the probabilistic collocation method is used to propagate the uncertain parameters through the model. The concentrations of DMS and SO2 are uncertain (1-σ) by factors of 3.5 and 2.5, respectively, while MSA and H2SO4 have uncertainty factors that range between 4.1 and 8.6. The main sources of uncertainty in the four species are from DMS emissions and heterogeneous scavenging, but the uncertain rate constants collectively account for up to 59% of the total uncertainty in MSA and 43% in H2SO4. Of the uncertain DMS chemistry, reactions that form and destroy CH3S(O)OO and CH3SO3 are identified as important targets for reducing the uncertainties.