bluuebunny/crossref_metadata_2025 huggingface dataset:
CHEM2D-OPP: A new linearized gas-phase ozone photochemistry parameterization for high-altitude NWP and climate models
Authors: McCormack J. P. , Eckermann S. D. , Siskind D. E. , McGee T. J.
Published: April 2010

Abstract. The new CHEM2D-Ozone Photochemistry Parameterization (CHEM2D-OPP) for high-altitude numerical weather prediction (NWP) systems and climate models specifies the net ozone photochemical tendency and its sensitivity to changes in ozone mixing ratio, temperature and overhead ozone column based on calculations from the CHEM2D interactive middle atmospheric photochemical transport model. We evaluate CHEM2D-OPP performance using both short-term (6-day) and long-term (1-year) stratospheric ozone simulations with the prototype high-altitude NOGAPS-ALPHA forecast model. An inter-comparison of NOGAPS-ALPHA 6-day ozone hindcasts for 7 February 2005 with ozone photochemistry parameterizations currently used in operational NWP systems shows that CHEM2D-OPP yields the best overall agreement with both individual Aura Microwave Limb Sounder ozone profile measurements and independent hemispheric (10°–90° N) ozone analysis fields. A 1-year free-running NOGAPS-ALPHA simulation using CHEM2D-OPP produces a realistic seasonal cycle in zonal mean ozone throughout the stratosphere. We find that the combination of a model cold temperature bias at high latitudes in winter and a warm bias in the CHEM2D-OPP temperature climatology can degrade the performance of the linearized ozone photochemistry parameterization over seasonal time scales despite the fact that the parameterized temperature dependence is weak in these regions.
Discriminating raining from non-raining clouds at mid-latitudes using multispectral satellite data
Authors: Nauss T. , Kokhanovsky A. A.
Published: April 2010

Abstract. We propose a new method for the delineation of precipitation using cloud properties derived from optical satellite data. This approach is not only sufficient for the detection of mainly convective precipitation by means of the commonly used connection between infrared cloud top temperature and rainfall probability but enables the detection of stratiform precipitation (e.g., in connection with mid-latitude frontal systems). The scheme presented is based on the concept model, that precipitating clouds must have both a sufficient vertical extent and large enough droplets. Therefore, we have analysed MODIS scenes during the severe European summer floods in 2002 and retrieved functions for the computation of an auto-adaptive threshold value of the effective cloud droplet radius with respect to the corresponding optical thickness which links these cloud properties with rainfall areas on a pixel basis.
Hemispheric ozone variability indices derived from satellite observations and comparison to a coupled chemistry-climate model
Authors: Erbertseder T. , Eyring V. , Bittner M. , Dameris M. , Grewe V.
Published: April 2010

Abstract. Total column ozone is used to trace the dynamics of the lower and middle stratosphere which is governed by planetary waves. In order to analyse the planetary wave activity a Harmonic Analysis is applied to global multi-year total ozone observations from the Total Ozone Monitoring Spectrometer (TOMS). As diagnostic variables we introduce the hemispheric ozone variability indices one and two. They are defined as the hemispheric means of the amplitudes of the zonal waves number one and two, respectively, as traced by the total ozone field. The application of these indices as a simple diagnostic for the evaluation of coupled chemistry-climate models (CCMs) is demonstrated by comparing results of the CCM ECHAM4.L39(DLR)/CHEM (hereafter: E39/C) against satellite observations. It is quantified to what extent a multi-year model simulation of E39/C (representing "2000" climate conditions) is able to reproduce the zonal and hemispheric planetary wave activity derived from TOMS data (1996–2004, Version 8). Compared to the reference observations the hemispheric ozone variability indices one and two of E39/C are too high in the Northern Hemisphere and too low in the Southern Hemisphere. In the Northern Hemisphere, where the agreement is generally better, E39/C produces too strong a planetary wave one activity in winter and spring and too high an interannual variability. For the Southern Hemisphere we reveal that the indices from observations and model differ significantly during the ozone hole season. The indices are used to give reasons for the late formation of the Antarctic ozone hole, the insufficient vortex elongation and eventually the delayed final warming in E39/C. In general, the hemispheric ozone variability indices can be regarded as a simple and robust diagnostic to quantify model-observation differences concerning planetary wave activity. It allows a first-guess on how the dynamics is represented in a model simulation before applying costly and more specific diagnostics.
Differences between ground Dobson, Brewer and satellite TOMS-8, GOME-WFDOAS total ozone observations at Hradec Kralove, Czech
Authors: Vanicek K.
Published: April 2010

Abstract. This paper presents key results achieved by an analysis of the relation between high-quality simultaneous Dobson, Brewer ground and TOMS-V8, GOME-WFDOAS satellite total ozone observations for Hradec Kralove, Czech Republic. Statistically significant seasonal differences with maxima up to 4% of monthly averages have been found between Dobson and Brewer measurements during the winter/spring months. These differences can influence estimations of ozone trends if combined data series are used after replacing a Dobson instrument by a Brewer spectrophotometer. The differences can be attributed mostly to the influence of temperature on ozone absorption coefficients and to total sulphur dioxide. Similar seasonal differences exist between Dobson, GOME and Brewer, TOMS data sets at Hradec Kralove while Dobson versus TOMS and Brewer versus GOME observations fit well with each other within the instrumental accuracy of spectrophotometers. The above findings are supposed to be relevant to other mid and high latitude stations and they have been confirmed by several independent analyses. The conclusions should be considered by data users because the differences between particular ground and satellite data sets can influence validation of satellite ozone observing systems and analyses of recovery of the ozone layer in mid and high latitudes, among others.
Radiative forcing by aerosols as derived from the AeroCom present-day and pre-industrial simulations
Authors: Schulz M. , Textor C. , Kinne S. , Balkanski Y. , Bauer S. , Berntsen T. , Berglen T. , Boucher O. , Dentener F. , Guibert S. , Isaksen I. S. A. , Iversen T. , Koch D. , Kirkevåg A. , Liu X. , Montanaro V. , Myhre G. , Penner J. E. , Pitari G. , Reddy S. , Seland Ø. , Stier P. , Takemura T.
Published: April 2010

Abstract. Nine different global models with detailed aerosol modules have independently produced instantaneous direct radiative forcing due to anthropogenic aerosols. The anthropogenic impact is derived from the difference of two model simulations with prescribed aerosol emissions, one for present-day and one for pre-industrial conditions. The difference in the solar energy budget at the top of the atmosphere (ToA) yields a new harmonized estimate for the aerosol direct radiative forcing (RF) under all-sky conditions. On a global annual basis RF is −0.22 Wm−2, ranging from +0.04 to −0.41 Wm−2, with a standard deviation of ±0.16 Wm−2. Anthropogenic nitrate and dust are not included in this estimate. No model shows a significant positive all-sky RF. The corresponding clear-sky RF is −0.68 Wm−2. The cloud-sky RF was derived based on all-sky and clear-sky RF and modelled cloud cover. It was significantly different from zero and ranged between −0.16 and +0.34 Wm−2. A sensitivity analysis shows that the total aerosol RF is influenced by considerable diversity in simulated residence times, mass extinction coefficients and most importantly forcing efficiencies (forcing per unit optical depth). The clear-sky forcing efficiency (forcing per unit optical depth) has diversity comparable to that for the all-sky/ clear-sky forcing ratio. While the diversity in clear-sky forcing efficiency is impacted by factors such as aerosol absorption, size, and surface albedo, we can show that the all-sky/clear-sky forcing ratio is important because all-sky forcing estimates require proper representation of cloud fields and the correct relative altitude placement between absorbing aerosol and clouds. The analysis of the sulphate RF shows that long sulphate residence times are compensated by low mass extinction coefficients and vice versa. This is explained by more sulphate particle humidity growth and thus higher extinction in those models where short-lived sulphate is present at lower altitude and vice versa. Solar atmospheric forcing within the atmospheric column is estimated at +0.82±0.17 Wm−2. The local annual average maxima of atmospheric forcing exceed +5 Wm−2 confirming the regional character of aerosol impacts on climate. The annual average surface forcing is −1.02±0.23 Wm−2. With the current uncertainties in the modelling of the radiative forcing due to the direct aerosol effect we show here that an estimate from one model is not sufficient but a combination of several model estimates is necessary to provide a mean and to explore the uncertainty.
Modeling of biomass smoke injection into the lower stratosphere by a large forest fire (Part II): sensitivity studies
Authors: Luderer G. , Trentmann J. , Winterrath T. , Textor C. , Herzog M. , Graf H. F. , Andreae M. O.
Published: April 2010

Abstract. The Chisholm forest fire that burned in Alberta, Canada, in May 2001 resulted in injection of substantial amounts of smoke into the lower stratosphere. We used the cloud-resolving plume model ATHAM (Active Tracer High resolution Atmospheric Model) to investigate the importance of different contributing factors to the severe intensification of the convection induced by the Chisholm fire and the subsequent injection of biomass smoke into the lower stratosphere. The simulations show strong sensitivity of the pyro-convection to background meteorology. This explains the observed coincidence of the convective blow-up of the fire plume and the passage of a synoptic cold front. Furthermore, we performed model sensitivity studies to the rate of release of sensible heat and water vapor from the fire. The release of sensible heat by the fire plays a dominant role for the dynamic development of the pyro-cumulonimbus cloud (pyroCb) and the height to which smoke is transported. The convection is very sensitive to the heat flux from the fire. The emissions of water vapor play a less significant role for the injection height but enhance the amount of smoke transported beyond the tropopause level. The aerosol burden in the plume has a strong impact on the microphysical structure of the resulting convective cloud. The dynamic evolution of the pyroCb, however, is only weakly sensitive to the abundance of cloud condensation nuclei (CCN) from the fire. In contrast to previous findings by other studies of convective clouds, we found that fire CCN have a negative effect on the convection dynamics because they give rise to a delay in the freezing of cloud droplets. Even in a simulation without fire CCN, there is no precipitation formation within the updraft region of the pyroCb. Enhancement of convection by aerosols as reported from studies of other cases of convection is therefore not found in our study.
SCIAMACHY Level 1 data: calibration concept and in-flight calibration
Authors: Lichtenberg G. , Kleipool Q. , Krijger J. M. , van Soest G. , van Hees R. , Tilstra L. G. , Acarreta J. R. , Aben I. , Ahlers B. , Bovensmann H. , Chance K. , Gloudemans A. M. S. , Hoogeveen R. W. M. , Jongma R. T. N. , Noël S. , Piters A. , Schrijver H. , Schrijvers C. , Sioris C. E. , Skupin J. , Slijkhuis S. , Stammes P. , Wuttke M.
Published: April 2010

Abstract. The calibration of SCIAMACHY was thoroughly checked since the instrument was launched on-board ENVISAT in February 2002. While SCIAMACHY's functional performance is excellent since launch, a number of technical difficulties have appeared, that required adjustments to the calibration. The problems can be separated into three types: (1) Those caused by the instrument and/or platform environment. Among these are the high water content in the satellite structure and/or MLI layer. This results in the deposition of ice on the detectors in channels 7 and 8 which seriously affects the retrievals in the IR, mostly because of the continuous change of the slit function caused by scattering of the light through the ice layer. Additionally a light leak in channel 7 severely hampers any retrieval from this channel. (2) Problems due to errors in the on-ground calibration and/or data processing affecting for example the radiometric calibration. A new approach based on a mixture of on-ground and in-flight data is shortly described here. (3) Problems caused by principal limitations of the calibration concept, e.g. the possible appearance of spectral structures after the polarisation correction due to unavoidable errors in the determination of atmospheric polarisation. In this paper we give a complete overview of the calibration and problems that still have to be solved. We will also give an indication of the effect of calibration problems on retrievals where possible. Since the operational processing chain is currently being updated and no newly processed data are available at this point in time, for some calibration issues only a rough estimate of the effect on Level 2 products can be given. However, it is the intention of this paper to serve as a future reference for detailed studies into specific calibration issues.
Stratospheric variability and trends in models used for the IPCC AR4
Authors: Cordero E. C. , Forster P. M. de F.
Published: April 2010

Abstract. Atmosphere and ocean general circulation model (AOGCM) experiments for the Intergovernmental Panel on Climate Change Fourth Assessment Report (AR4) are analyzed to better understand model variability and assess the importance of various forcing mechanisms on stratospheric trends during the 20th century. While models represent the climatology of the stratosphere reasonably well in comparison with NCEP reanalysis, there are biases and large variability among models. In general, AOGCMs are cooler than NCEP throughout the stratosphere, with the largest differences in the tropics. Around half the AOGCMs have a top level beneath ~2 hPa and show a significant cold bias in their upper levels (~10 hPa) compared to NCEP, suggesting that these models may have compromised simulations near 10 hPa due to a low model top or insufficient stratospheric levels. In the lower stratosphere (50 hPa), the temperature variability associated with large volcanic eruptions is absent in about half of the models, and in the models that do include volcanic aerosols, half of those significantly overestimate the observed warming. There is general agreement on the vertical structure of temperature trends over the last few decades, differences between models are explained by the inclusion of different forcing mechanisms, such as stratospheric ozone depletion and volcanic aerosols. However, even when human and natural forcing agents are included in the simulations, significant differences remain between observations and model trends, particularly in the upper tropical troposphere (200 hPa–100 hPa), where, since 1979, models show a warming trend and the observations a cooling trend.
Meteorology applied to urban air pollution problems: concepts from COST 715
Authors: Fisher B. , Kukkonen J. , Piringer M. , Rotach M. W. , Schatzmann M.
Published: April 2010

Abstract. The outcome of COST 715 is reviewed from the viewpoint of a potential user who is required to consider urban meteorology within an air pollution assessment. It is shown that descriptive concepts are helpful for understanding the complex structure of the urban boundary layer, but that they only apply under a limited number of conditions. However such concepts are necessary to gain insight into both simple and complex air pollution models. It is argued that wider considerations are needed when considering routine air quality assessments involving an air quality model's formulation and pedigree. Moreover there appears to be a reluctance from model developers to move away from familiar concepts of the atmospheric boundary layer even if they are not appropriate to urban areas. An example is given from COST 715 as to how routine urban meteorological measurements of wind speed may be used and adapted for air quality assessments. Reference to the full COST 715 study is made which provides further details.
MIPAS level 2 operational analysis
Authors: Raspollini P. , Belotti C. , Burgess A. , Carli B. , Carlotti M. , Ceccherini S. , Dinelli B. M. , Dudhia A. , Flaud J.-M. , Funke B. , Höpfner M. , López-Puertas M. , Payne V. , Piccolo C. , Remedios J. J. , Ridolfi M. , Spang R.
Published: April 2010

Abstract. The MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) instrument has been operating on-board the ENVISAT satellite since March 2002. In the first two years, it acquired in a nearly continuous manner high resolution (0.025 cm−1 unapodized) emission spectra of the Earth's atmosphere at limb in the middle infrared region. This paper describes the level 2 near real-time (NRT) and off-line (OL) ESA processors that have been used to derive level 2 geophysical products from the calibrated and geolocated level 1b spectra. The design of the code and the analysis methodology have been driven by the requirements for NRT processing. This paper reviews the performance of the optimized retrieval strategy that has been implemented to achieve these requirements and provides estimated error budgets for the target products: pressure, temperature, O3, H2O, CH4, HNO3, N2O and NO2, in the altitude measurement range from 6 to 68 km. From application to real MIPAS data, it was found that no change was needed in the developed code although an external algorithm was introduced to identify clouds with high opacity and to exclude affected spectra from the analysis. In addition, a number of updates were made to the set-up parameters and to auxiliary data. In particular, a new version of the MIPAS dedicated spectroscopic database was used and, in the OL analysis, the retrieval range was extended to reduce errors due to uncertainties in extrapolation of the profile outside the retrieval range and more stringent convergence criteria were implemented. A statistical analysis on the χ2 values obtained in one year of measurements shows good agreement with the a priori estimate of the forward model errors. On the basis of the first two years of MIPAS measurements the estimates of the forward model and instrument errors are in general found to be conservative with excellent performance demonstrated for frequency calibration. It is noted that the total retrieval error is limited by forward model errors which make effectless a further reduction of random errors. However, such a reduction is within the capabilities of MIPAS measurements, which contain many more spectral signatures of the target species than what has currently been used. Further work is needed to reduce the amplitude of the forward model errors, so that the random error and the total error budget can be reduced accordingly. The importance of the Averaging kernels for a full characterization of the target products is underlined and the equations are provided for their practical applications.
Water vapour profiles by ground-based FTIR spectroscopy: study for an optimised retrieval and its validation
Authors: Schneider M. , Hase F. , Blumenstock T.
Published: April 2010

Abstract. The sensitivity of ground-based instruments measuring in the infrared with respect to tropospheric water vapour content is generally limited to the lower and middle troposphere. The large vertical gradients and variabilities avoid a better sensitivity for the upper troposphere/lower stratosphere (UT/LS) region. In this work an optimised retrieval is presented and it is demonstrated that compared to a commonly applied method, it improves the performance of the FTIR technique. The reasons for this improvement and the possible deficiencies of the method are discussed. Only by applying the method proposed here and using measurements performed at mountain observatories can water vapour variabilities in the UT/LS be detected in a self-consistent manner. The precision, expressed as noise to signal ratio, is estimated at 45%. In the middle and lower troposphere, precisions of 22% are achieved. These estimations are confirmed by a comparison of retrieval results based on real FTIR measurements with coinciding measurements of synoptical meteorological radiosondes.
The structure of the haze plume over the Indian Ocean during INDOEX: tracer simulations and LIDAR observations
Authors: Forêt G. , Flamant C. , Cautenet S. , Pelon J. , Minvielle F. , Taghavi M. , Chazette P.
Published: April 2010

Abstract. Three-dimensional, nested tracer simulations of a pollution plume originating from the Indian sub-continent over the Indian Ocean, in the framework of the Indian Ocean Experiment (INDOEX), between 5 and 9 March 1999, were performed with the Regional Atmospheric Modeling System (RAMS), to provide insight into the transport patterns of the pollutants, as well as to investigate the dynamical mechanisms controlling the vertical structure of the plume and its evolution in the vicinity of the Maldives Islands. Airborne and ground-based LIDAR observations of the structure of the haze plume made on 7 March 1999 were used to assess the quality of the simulations, as well as the impact of grid resolution on the vertical structure of the simulated plume. It is shown that, over the Arabian Sea, in the vicinity of the Maldives Islands, the pollutants composing the plume observed by the airborne LIDAR essentially originated from the city of Madras and that the vertical structure of the plume was controlled by the diurnal cycle of the continental boundary layer depth. A combination of tracer simulations and remote sensing observations (airborne LIDAR, ship-borne photometer, ground-based LIDAR in Goa) was used to analyse the diurnal evolution of the haze plume over the sea. We find evidence that the sea breeze circulation and orographic lifting taking place in the southern part of the Indian sub-continent during the daytime play a crucial role in the modulation of the continental boundary layer depth, and in turn, the haze plume depth. The eastward shift of the subtropical high from central India to the Bay of Bengal after 6 March lead to an increase in the tracer concentrations simulated over the Arabian Sea, in the region of intensive observations north of the Maldives, as transport pathways form Hyderabad and Madras were modified significantly. The nesting of a high horizontal resolution domain (5 km, with 39 vertical levels below 4000 m above mean seal level) allows for a better representation of local dynamics, the circulation of sea and mountains breezes, and therefore a noticeable improvement in the representation of the pollutants' plume in the simulation.
Intercomparison exercise between different radiative transfer models used for the interpretation of ground-based zenith-sky and multi-axis DOAS observations
Authors: Hendrick F. , Van Roozendael M. , Kylling A. , Petritoli A. , Rozanov A. , Sanghavi S. , Schofield R. , von Friedeburg C. , Wagner T. , Wittrock F. , Fonteyn D. , De Mazière M.
Published: April 2010

Abstract. We present the results of an intercomparison exercise between six different radiative transfer (RT) models carried out in the framework of QUILT, an EU funded project based on the exploitation of the Network for the Detection of Stratospheric Change (NDSC). RT modelling is an important step in the interpretation of Differential Optical Absorption Spectroscopy (DOAS) observations. It allows the conversion of slant column densities (SCDs) into vertical column densities (VCDs) using calculated air mass factors (AMFs). The originality of our study resides in comparing SCD simulations in multi-axis (MAX) geometry (trace gases: NO2 and HCHO) and in taking into account photochemical enhancement for calculating SCDs of rapidly photolysing species (BrO, NO2, and OClO) in zenith-sky geometry. Concerning the zenith-sky simulations, the different models agree generally well, especially below 90° SZA. At higher SZA, larger discrepancies are obtained with relative differences ranging between 2% and 14% in some cases. In MAX geometry, good agreement is found between the models with the calculated NO2 and HCHO SCDs differing by no more than 5% in the elevation and solar zenith angle (SZA) ranges investigated (5°–20° and 35°–85°, respectively). The impacts of aerosol scattering, ground albedo, and relative azimuth on MAX simulations have also been tested. Significant discrepancies appear for the aerosol effect, suggesting differences between models in the treatment of aerosol scattering. A better agreement is found in case of the ground albedo and relative azimuth effects. The complete set of initialization data and results have been made publicly available through the QUILT project web site (http://nadir.nilu.no/quilt/), enabling the testing of other RT codes designed for the calculation of SCDs/AMFs.
Global estimation of burned area using MODIS active fire observations
Authors: Giglio L. , van der Werf G. R. , Randerson J. T. , Collatz G. J. , Kasibhatla P.
Published: April 2010

Abstract. We present a method for estimating monthly burned area globally at 1° spatial resolution using Terra MODIS data and ancillary vegetation cover information. Using regression trees constructed for 14 different global regions, MODIS active fire observations were calibrated to burned area estimates derived from 500-m MODIS imagery based on the assumption that burned area is proportional to counts of fire pixels. Unlike earlier methods, we allow the constant of proportionality to vary as a function of tree and herbaceous vegetation cover, and the mean size of monthly cumulative fire-pixel clusters. In areas undergoing active deforestation, we implemented a subsequent correction based on tree cover information and a simple measure of fire persistence. Regions showing good agreement between predicted and observed burned area included Boreal Asia, Central Asia, Europe, and Temperate North America, where the estimates produced by the regression trees were relatively accurate and precise. Poorest agreement was found for southern-hemisphere South America, where predicted values of burned area are both inaccurate and imprecise; this is most likely a consequence of multiple factors that include extremely persistent cloud cover, and lower quality of the 500-m burned area maps used for calibration. Application of our approach to the nine remaining regions yielded comparatively accurate, but less precise, estimates of monthly burned area. We applied the regional regression trees to the entire archive of Terra MODIS fire data to produce a monthly global burned area data set spanning late 2000 through mid-2005. Annual totals derived from this approach showed good agreement with independent annual estimates available for nine Canadian provinces, the United States, and Russia. With our data set we estimate the global annual burned area for the years 2001-2004 to vary between 2.97 million and 3.74 million km2, with the maximum occurring in 2001. These coarse-resolution burned area estimates may serve as a useful interim product until long-term burned area data sets from multiple sensors and retrieval approaches become available.
In-situ measurement of reactive hydrocarbons at Hohenpeissenberg with comprehensive two-dimensional gas chromatography (GC×GC-FID): use in estimating HO and NO3
Authors: Bartenbach S. , Williams J. , Plass-Dülmer C. , Berresheim H. , Lelieveld J.
Published: April 2010

Abstract. During a field campaign at the Meteorological Observatory Hohenpeissenberg (MOHp) in July 2004, volatile organic compounds (VOCs) were measured using comprehensive two-dimensional gas chromatography (GC×GC). Comparison to routinely made gas chromatography mass spectrometry (GC-MS) measurements showed good agreement for a variety of anthropogenic and biogenic ambient VOCs ranging in concentration from below the detection limit (0.1 pmol mol−1) to 180 pmol mol−1. Pronounced diurnal cycles were found for both the biogenic and anthropogenic compounds, driven for the most part by the daily rise and fall of the boundary layer over the station. For the reactive compounds (lifetimes <2 days), a significant, non-zero dependency of the variability on lifetime was found, indicating that chemistry (as opposed to transport alone) was playing a role in determining the ambient VOC concentrations. The relationship was exploited using a single-variate analysis to derive a daytime mean value of HO (5.3±1.4×106molecules cm−3), which compares well to that measured at the site, 3.2±2.3×106molecules cm−3. The analysis was extended to the night time data to estimate concentrations for NO3 (1.47±0.2×108molecules cm−3), which is not measured at the site. The feasibility of this approach for environments dominated by emissions of short-lived VOCs to estimate ambient levels of radical species is discussed.
The water vapour distribution in the Arctic lowermost stratosphere during the LAUTLOS campaign and related transport processes including stratosphere-troposphere exchange
Authors: Karpechko A. , Lukyanov A. , Kyrö E. , Khaikin S. , Korshunov L. , Kivi R. , Vömel H.
Published: April 2010

Abstract. Balloon-borne water vapour measurements during January and February 2004, which were obtained as part of the LAUTLOS campaign at Sodankylä, Finland, 67° N, were used to analyse the water vapour distribution in the wintertime Arctic lowermost stratosphere. A 2.5 km thick layer (or 30 K in the potential temperature scale) above the tropopause is characterized by a significant water vapour variability on a synoptic timescale with values between stratospheric and tropospheric, which is in good agreement with previously reported measurements. A cross-correlation analysis of ozone and water vapour confirms that this layer contains a mixture of stratospheric and tropospheric air masses. Some of the flights sampled laminae of enhanced water vapour above the tropopause. Meteorological analyses and backward trajectory calculations show that these features were related to filaments that had developed along the flanks of cut-off anticyclones, which had been active at this time over the Northern Atlantic. The role of the filaments was however not to transport water vapour from the troposphere to the stratosphere but rather to transport it within the stratosphere away from regions where intensive two-way stratosphere-troposphere exchange (STE) was identified. Intensive STE occurred around cut-off anticyclones in regions of strong winds, where calculations suggest the presence of clear-air turbulence (CAT). Evidences that CAT contributes to the troposphere-to-stratosphere transport (TST) are presented. However, statistically, relation between TST and CAT during the studied period is weak.
Photochemical modelling in the Po basin with focus on formaldehyde and ozone
Authors: Liu L. , Flatøy F. , Ordóñez C. , Braathen G. O. , Hak C. , Junkermann W. , Andreani-Aksoyoglu S. , Mellqvist J. , Galle B. , Prévôt A. S. H. , Isaksen I. S. A.
Published: April 2010

Abstract. As part of the EU project FORMAT (Formaldehyde as a Tracer of Oxidation in the Troposphere), a field campaign was carried out in the vicinity of Milan during the summer of 2002. Results from a 3-D regional chemical transport model (NILU RCTM) were used to interpret the observations focusing primarily on HCHO and ozone. The performance of the model was assessed by comparing model results with ground based and aircraft measurements. The model results show good agreement with surface measurements, and the model is able to reproduce the photochemical episodes during fair weather days. The comparison indicates that the model can represent well the HCHO concentrations as well as their temporal and spatial variability. The relationship between HCHO and (O3×H2O) was used to validate the model ability to predict the HCHO concentrations. Further analysis revealed the importance of the representativeness of different instruments: in-situ concentrations might be locally enhanced by emissions, while long path measurements over a forest can be influenced by rapid formation of HCHO from isoprene. The model is able to capture the plume from the city of Milan and the modelled levels agree generally well with the aircraft measurements, although the wind fields used in the model can lead to a displacement of the ozone plume. During the campaign period, O3 levels were seldom higher than 80 ppb, the peak surface ozone maxima reached 90 ppb. Those relatively low values can be explained by low emissions during the August vacation and unstable weather conditions in this period. The modelled ΔO3/ΔNOz slope at Alzate of 5.1 agrees well with the measured slope of 4.9.
Stratospheric dryness: model simulations and satellite observations
Authors: Lelieveld J. , Brühl C. , Jöckel P. , Steil B. , Crutzen P. J. , Fischer H. , Giorgetta M. A. , Hoor P. , Lawrence M. G. , Sausen R. , Tost H.
Published: April 2010

Abstract. The mechanisms responsible for the extreme dryness of the stratosphere have been debated for decades. A key difficulty has been the lack of comprehensive models which are able to reproduce the observations. Here we examine results from the coupled lower-middle atmosphere chemistry general circulation model ECHAM5/MESSy1 together with satellite observations. Our model results match observed temperatures in the tropical lower stratosphere and realistically represent the seasonal and inter-annual variability of water vapor. The model reproduces the very low water vapor mixing ratios (below 2 ppmv) periodically observed at the tropical tropopause near 100 hPa, as well as the characteristic tape recorder signal up to about 10 hPa, providing evidence that the dehydration mechanism is well-captured. Our results confirm that the entry of tropospheric air into the tropical stratosphere is forced by large-scale wave dynamics, whereas radiative cooling regionally decelerates upwelling and can even cause downwelling. Thin cirrus forms in the cold air above cumulonimbus clouds, and the associated sedimentation of ice particles between 100 and 200 hPa reduces water mass fluxes by nearly two orders of magnitude compared to air mass fluxes. Transport into the stratosphere is supported by regional net radiative heating, to a large extent in the outer tropics. During summer very deep monsoon convection over Southeast Asia, centered over Tibet, moistens the stratosphere.
Efficiency of cloud condensation nuclei formation from ultrafine particles
Authors: Pierce J. R. , Adams P. J.
Published: April 2010

Abstract. Atmospheric cloud condensation nuclei (CCN) concentrations are a key uncertainty in the assessment of the effect of anthropogenic aerosol on clouds and climate. The ability of new ultrafine particles to grow to become CCN varies throughout the atmosphere and must be understood in order to understand CCN formation. We have developed the Probability of Ultrafine particle Growth (PUG) model to answer questions regarding which growth and sink mechanisms control this growth, how the growth varies between different parts of the atmosphere and how uncertainties with respect to the magnitude and size distribution of ultrafine emissions translates into uncertainty in CCN generation. The inputs to the PUG model are the concentrations of condensable gases, the size distribution of ambient aerosol, particle deposition timescales and physical properties of the particles and condensable gases. It was found in most cases that condensation is the dominant growth mechanism and coagulation with larger particles is the dominant sink mechanism for ultrafine particles. In this work we found that the probability of a new ultrafine particle generating a CCN varies from <0.1% to ~90% in different parts of the atmosphere, though in the boundary layer a large fraction of ultrafine particles have a probability between 1% and 40%. Some regions, such as the tropical free troposphere, are areas with high probabilities; however, variability within regions makes it difficult to predict which regions of the atmosphere are most efficient for generating CCN from ultrafine particles. For a given mass of primary ultrafine aerosol, an uncertainty of a factor of two in the modal diameter can lead to an uncertainty in the number of CCN generated as high as a factor for eight. It was found that no single moment of the primary aerosol size distribution, such as total mass or number, is a robust predictor of the number of CCN ultimately generated. Therefore, a complete description of the emissions size distribution is generally required for global aerosol microphysics models.
Modelling iodide – iodate speciation in atmospheric aerosol: Contributions of inorganic and organic iodine chemistry
Authors: Pechtl S. , Schmitz G. , von Glasow R.
Published: April 2010

Abstract. The speciation of iodine in atmospheric aerosol is currently poorly understood. Models predict negligible iodide concentrations but accumulation of iodate in aerosol, both of which is not confirmed by recent measurements. We present an updated aqueous phase iodine chemistry scheme for use in atmospheric chemistry models and discuss sensitivity studies with the marine boundary layer model MISTRA. These studies show that iodate can be reduced in acidic aerosol by inorganic reactions, i.e., iodate does not necessarily accumulate in particles. Furthermore, the transformation of particulate iodide to volatile iodine species likely has been overestimated in previous model studies due to negligence of collision-induced upper limits for the reaction rates. However, inorganic reaction cycles still do not seem to be sufficient to reproduce the observed range of iodide – iodate speciation in atmospheric aerosol. Therefore, we also investigate the effects of the recently suggested reaction of HOI with dissolved organic matter to produce iodide. If this reaction is fast enough to compete with the inorganic mechanism, it would not only directly lead to enhanced iodide concentrations but, indirectly via speed-up of the inorganic iodate reduction cycles, also to a decrease in iodate concentrations. Hence, according to our model studies, organic iodine chemistry, combined with inorganic reaction cycles, is able to reproduce observations. The presented chemistry cycles are highly dependent on pH and thus offer an explanation for the large observed variability of the iodide – iodate speciation in atmospheric aerosol.
Is aerosol formation in cirrus clouds possible?
Authors: Kazil J. , Lovejoy E. R. , Jensen E. J. , Hanson D. R.
Published: April 2010

Abstract. The recent observation of ultrafine aerosol particles in cirrus clouds has raised the question whether aerosol formation within cirrus clouds is possible, and if so, what mechanisms are involved. We have developed an aerosol parcel model of neutral and charged H2SO4/H2O aerosol processes, including nucleation from the gas phase and loss onto cirrus ice particles. Laboratory thermodynamic data for sulfuric acid uptake and loss by small neutral and charged clusters are used, allowing for a reliable description of both neutral and charged nucleation down to the very low temperatures occurring in the upper troposphere and lower stratosphere. The model implements a first order scheme for resolving the aerosol size distribution within its geometric size sections, which efficiently suppresses numerical diffusion. We operate the model offline on trajectories generated with a detailed 1D cirrus model which describes ice crystal nucleation, deposition growth, vertical advection of ice crystals and water vapor, and ice crystal sedimentation. In this paper we explore the possibility of aerosol formation within non-convective cirrus clouds and draw conclusions for aerosol formation in anvil cirrus. We find that sulfate aerosol formation within cirrus clouds can proceed even at high ice surface area concentrations, and depends strongly on the size of the cirrus ice crystals and on the surface area concentration of preexisting aerosol particles.
Extinction coefficients retrieved in deep tropical ice clouds from lidar observations using a CALIPSO-like algorithm compared to in-situ measurements from the cloud integrating nephelometer during CRYSTAL-FACE
Authors: Noel V. , Winker D. M. , Garrett T. J. , McGill M.
Published: April 2010

Abstract. This paper presents a comparison of lidar ratios and volume extinction coefficients in tropical ice clouds, retrieved using observations from two instruments: the 532-nm Cloud Physics Lidar (CPL), and the in-situ Cloud Integrating Nephelometer (CIN) probe. Both instruments were mounted on airborne platforms during the CRYSTAL-FACE campaign and took measurements up to 17 km. Coincident observations from two cases of ice clouds located on top of deep convective systems are compared. First, lidar ratios are retrieved from CPL observations of attenuated backscatter, using a retrieval algorithm for opaque cloud similar to one used in the recently launched CALIPSO mission, and compared to results from the regular CPL algorithm. These lidar ratios are used to retrieve extinction coefficient profiles, which are compared to actual observations from the CIN in-situ probe, putting the emphasis on their vertical variability. When observations coincide, retrievals from both instruments are very similar, in the limits of colocation. Differences are generally variations around the average profiles, and general trends on larger spatial scales are well reproduced. The two instruments agree well, with an average difference of less than 11% on optical depth retrievals. Results suggest the CALIPSO Deep Convection algorithm can be trusted to deliver realistic estimates of the lidar ratio, leading to good retrievals of extinction coefficients.
SAGE III aerosol extinction validation in the Arctic winter: comparisons with SAGE II and POAM III
Authors: Thomason L. W. , Poole L. R. , Randall C. E.
Published: April 2010

Abstract. The use of SAGE III multiwavelength aerosol extinction coefficient measurements to infer PSC type is contingent on the robustness of both the extinction magnitude and its spectral variation. Past validation with SAGE II and other similar measurements has shown that the SAGE III extinction coefficient measurements are reliable though the comparisons have been greatly weighted toward measurements made at mid-latitudes. Some aerosol comparisons made in the Arctic winter as a part of SOLVE II suggested that SAGE III values, particularly at longer wavelengths, are too small with the implication that both the magnitude and the wavelength dependence are not reliable. Comparisons with POAM III have also suggested a similar discrepancy. Herein, we use SAGE II data as a common standard for comparison of SAGE III and POAM III measurements in the Arctic winters of 2002/2003 through 2004/2005. During the winter, SAGE II measurements are made infrequently at the same latitudes as these instruments. We have mitigated this problem through the use of potential vorticity as a spatial coordinate and thus greatly increased of the number of coincident events. We find that SAGE II and III extinction coefficient measurements show a high degree of compatibility at both 1020 nm and 450 nm except a 10–20% bias at both wavelengths. In addition, the 452 to 1020 nm extinction ratio shows a consistent bias of ~30% throughout the lower stratosphere. We also find that SAGE II and POAM III are on average consistent though the comparisons show a much higher variability and larger bias than SAGE II/III comparisons. In addition, we find that SAGE II and POAM III data sets are not well correlated at and below 18 km. Overall, we find both the extinction values and the spectral dependence from SAGE III are robust and we find no evidence of a significant defect within the Arctic vortex.
Signature of Arctic surface ozone depletion events in the isotope anomaly (Δ17O) of atmospheric nitrate
Authors: Morin S. , Savarino J. , Bekki S. , Gong S. , Bottenheim J. W.
Published: April 2010

Abstract. We report the first measurements of the oxygen isotope anomaly of atmospheric inorganic nitrate from the Arctic. Nitrate samples and complementary data were collected at Alert, Nunavut, Canada (82°30 ' N, 62°19 ' W) in spring 2004. Covering the polar sunrise period, characterized by the occurrence of severe boundary layer ozone depletion events (ODEs), our data show a significant correlation between the variations of atmospheric ozone (O3) mixing ratios and Δ17O of nitrate (Δ17O(NO−3)). This relationship can be expressed as: Δ17O(NO−3)/‰, =(0.15±0.03)×O3/(nmol mol–1)+(29.7±0.7), with R2=0.70(n=12), for Δ17O(NO−3) ranging between 29 and 35 ‰. We derive mass-balance equations from chemical reactions operating in the Arctic boundary layer, that describe the evolution of Δ17O(NO−3) as a function of the concentrations of reactive species and their isotopic characteristics. Changes in the relative importance of O3, RO2 and BrO in the oxidation of NO during ODEs, and the large isotope anomalies of O3 and BrO, are the driving force for the variability in the measured Δ17O(NO−3) . BrONO2 hydrolysis is found to be a dominant source of nitrate in the Arctic boundary layer, in agreement with recent modeling studies.
Improved ozone profile retrievals from GOME data with degradation correction in reflectance
Authors: Liu X. , Chance K. , Kurosu T. P.
Published: April 2010

Abstract. We present a simple method to perform degradation correction to Global Ozone Monitoring Experiment (GOME) reflectance spectra by comparing the average reflectance for 60° N–60° S with that at the beginning of GOME observations (July–December 1995) after removing the dependences on solar zenith angle and seasonal variation. The results indicate positive biases of up to ~15–25% in the wavelength range 289–370 nm during 2000–2002; the degradation also exhibits significant dependence on wavelength and viewing zenith angle. These results are consistent with previous studies using radiative transfer models and ozone observations. The degradation causes retrieval biases of up to ~3% (10 DU, 1 DU=2.69×1016 molecules cm−2), 30% (10 DU), 10%, and 40% in total column ozone, tropospheric column ozone, stratospheric ozone and tropospheric ozone, respectively, from our GOME ozone profile retrieval algorithm. In addition, retrieval biases due to degradation vary significantly with latitude. The application of this degradation correction improves the retrievals relative to Dobson and ozonesonde measurements at Hohenpeißenberg station during 2000–2003 and improves the spatiotemporal consistency of retrieval quality during 1996–2003. However, because this method assumes that the deseasonalized globally-averaged reflectance does not change much with time, retrievals with this correction may be inadequate for trend analysis. In addition, it does not correct for instrument biases that have occurred since launch.