bluuebunny/crossref_metadata_2025 huggingface dataset:
Temperature climatology and trend estimates in the UTLS region as observed over a southern subtropical site, Durban, South Africa
Authors: Bencherif H. , Diab R. D. , Portafaix T. , Morel B. , Keckhut P. , Moorgawa A.
Published: April 2010

Abstract. Temperature trends in the UTLS region are under-reported, particularly in the Southern Hemisphere, and yet temperature is one of the most important indicators of changes in dynamical and radiative processes in the atmosphere. Here radiosonde data from Durban, South Africa (30.0° S, 30.9° E) over the period 1980 to 2001 (22 years) between 250 and 20 hPa are used to derive a mean temperature climatology and to determine trends. The seasonal cycle at the 250-hPa level is anti-correlated with the seasonal cycles at the 150-hPa and 100-hPa heights. The 100-hPa level (local tropopause) exhibits a minimum temperature in late summer and a maximum in winter, and closely corresponds to previous results for tropical regions. Based on a Fourier analysis, both the annual cycle (AO) and the semi-annual cycle (SAO) are dominant, although the former is about 4 times stronger. The AO is strongest at the 100-hPa height. A trend analysis reveals a cooling trend at almost all heights in the UTLS region, with a maximum cooling rate of 1.09±0.41 K per decade, at 70-hPa. Cooling rates are in good agreement with other studies and are slightly higher in summer than in winter.
The density of humic acids and humic like substances (HULIS) from fresh and aged wood burning and pollution aerosol particles
Authors: Dinar E. , Mentel T. F. , Rudich Y.
Published: April 2010

Abstract. Atmospheric aerosols play significant roles in climatic related phenomena. Size, density and shape of particles affect their fluid-dynamic parameters which in turn dictate their transport and lifecycle. Moreover, density and shape are also related to particles' optical properties, influencing their regional and global radiative effects. In the present study we have measured and compared the effective densities of humic like substances (HULIS) extracted from smoke and pollution aerosol particles to those of molecular weight-fractionated aquatic and terrestrial Humic Substances (HS). The effective density was measured by comparing the electro mobility and vacuum aerodynamic diameter of aerosol particles composed of these compounds. Characterization of chemical parameters such as molecular weight, aromaticity and elemental composition allow us to test how they affect the effective density of these important environmental macromolecules. It is suggested that atmospheric aging processes increase the effective density of HULIS due to oxidation, while packing due to the aromatic moieties plays important role in determining the density of the aquatic HS substances.
A mass spectrometric study of secondary organic aerosols formed from the photooxidation of anthropogenic and biogenic precursors in a reaction chamber
Authors: Alfarra M. R. , Paulsen D. , Gysel M. , Garforth A. A. , Dommen J. , Prévôt A. S. H. , Worsnop D. R. , Baltensperger U. , Coe H.
Published: April 2010

Abstract. An Aerodyne Aerosol Mass Spectrometer (AMS) has been utilised to provide on-line measurements of the mass spectral signatures and mass size distributions of the oxidation products resulting from irradiating 1,3,5-trimethylbenzene (1,3,5-TMB) and α-pinene, separately, in the presence of nitrogen oxide, nitrogen dioxide and propene in a reaction chamber. Mass spectral results indicate that both precursors produce SOA with broadly similar chemical functionality of a highly oxidised nature. However, significant differences occur in the minor mass spectral fragments for the SOA in the two reaction systems, indicating that they have different molecular composition. Nitrogen-containing organic compounds have been observed in the photooxidation products of both precursors, and their formation appeared to be controlled by the temporal variability of NOx. Although the overall fragmentation patterns of the photooxidation products in both systems did not change substantially over the duration of each experiment, the contribution of some individual mass fragments to total mass appeared to be influenced by the irradiation time. The effective densities of the 1,3,5-TMB and α-pinene SOA particles were determined for various particle sizes using the relationship between mobility and vacuum aerodynamic diameters. The effective density for the 1,3,5-TMB SOA ranged from 1.35–1.40 g/cm3, while that for α-pinene SOA ranged from 1.29–1.32 g/cm3. The determined effective densities did not show dependence on irradiation time. Results suggest that further chemical processing of SOA takes place in the real atmosphere, as neither the α-pinene nor the 1,3,5-TMB experimental results reproduce the right relative product distribution between carbonyl-containing and multifunctional carboxylic acid species measured at ambient locations influenced by aged continental organic aerosols.
Radiocarbon analysis in an Alpine ice core: record of anthropogenic and biogenic contributions to carbonaceous aerosols in the past (1650–1940)
Authors: Jenk T. M. , Szidat S. , Schwikowski M. , Gäggeler H. W. , Brütsch S. , Wacker L. , Synal H.-A. , Saurer M.
Published: April 2010

Abstract. Long-term concentration records of carbonaceous particles (CP) are of increasing interest in climate research due to their not yet completely understood effects on climate. Nevertheless, only poor data on their concentrations and sources before the 20th century are available. We present a first long-term record of organic carbon (OC) and elemental carbon (EC) concentrations – the two main fractions of CP – along with the corresponding fraction of modern carbon (fM) derived from radiocarbon (14C) analysis in ice. This allows a distinction and quantification of natural (biogenic) and anthropogenic (fossil) sources in the past. CP were extracted from an ice archive, with resulting carbon quantities in the microgram range. Analysis of 14C by accelerator mass spectrometry (AMS) was therefore highly demanding. We analysed 33 samples of 0.4 to 1 kg ice from a 150.5 m long ice core retrieved at Fiescherhorn glacier in December 2002 (46°33'3.2" N, 08°04'0.4" E; 3900 m a.s.l.). Samples were taken from bedrock up to the firn/ice transition, covering the time period 1650–1940 and thus the transition from the pre-industrial to the industrial era. Before ~1850, OC was approaching a purely biogenic origin with a mean concentration of 24 μg kg−1 and a standard deviation of 7 μg kg−1. In 1940, OC concentration was about a factor of 3 higher than this biogenic background, almost half of it originating from anthropogenic sources, i.e. from combustion of fossil fuels. The biogenic EC concentration was nearly constant over the examined time period with 6 μg kg−1 and a standard deviation of 1 μg kg−1. In 1940, the additional anthropogenic input of atmospheric EC was about 50 μg kg−1.
Technical Note: The MESSy-submodel AIRSEA calculating the air-sea exchange of chemical species
Authors: Pozzer A. , Jöckel P. , Sander R. , Williams J. , Ganzeveld L. , Lelieveld J.
Published: April 2010

Abstract. The new submodel AIRSEA for the Modular Earth Submodel System (MESSy) is presented. It calculates the exchange of chemical species between the ocean and the atmosphere with a focus on organic compounds. The submodel can be easily extended to a large number of tracers, including highly soluble ones. It is demonstrated that the application of explicitly calculated air-sea exchanges with AIRSEA can induce substantial changes in the simulated tracer distributions in the troposphere in comparison to a model setup in which this process is neglected. For example, the simulations of acetone, constrained with measured oceanic concentrations, shows relative changes in the atmospheric surface layer mixing ratios over the Atlantic Ocean of up to 300%.
The ASSET intercomparison of ozone analyses: method and first results
Authors: Geer A. J. , Lahoz W. A. , Bekki S. , Bormann N. , Errera Q. , Eskes H. J. , Fonteyn D. , Jackson D. R. , Juckes M. N. , Massart S. , Peuch V.-H. , Rharmili S. , Segers A.
Published: April 2010

Abstract. This paper aims to summarise the current performance of ozone data assimilation (DA) systems, to show where they can be improved, and to quantify their errors. It examines 11 sets of ozone analyses from 7 different DA systems. Two are numerical weather prediction (NWP) systems based on general circulation models (GCMs); the other five use chemistry transport models (CTMs). The systems examined contain either linearised or detailed ozone chemistry, or no chemistry at all. In most analyses, MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) ozone data are assimilated; two assimilate SCIAMACHY (Scanning Imaging Absorption Spectrometer for Atmospheric Chartography) observations instead. Analyses are compared to independent ozone observations covering the troposphere, stratosphere and lower mesosphere during the period July to November 2003. Biases and standard deviations are largest, and show the largest divergence between systems, in the troposphere, in the upper-troposphere/lower-stratosphere, in the upper-stratosphere and mesosphere, and the Antarctic ozone hole region. However, in any particular area, apart from the troposphere, at least one system can be found that agrees well with independent data. In general, none of the differences can be linked to the assimilation technique (Kalman filter, three or four dimensional variational methods, direct inversion) or the system (CTM or NWP system). Where results diverge, a main explanation is the way ozone is modelled. It is important to correctly model transport at the tropical tropopause, to avoid positive biases and excessive structure in the ozone field. In the southern hemisphere ozone hole, only the analyses which correctly model heterogeneous ozone depletion are able to reproduce the near-complete ozone destruction over the pole. In the upper-stratosphere and mesosphere (above 5 hPa), some ozone photochemistry schemes caused large but easily remedied biases. The diurnal cycle of ozone in the mesosphere is not captured, except by the one system that includes a detailed treatment of mesospheric chemistry. These results indicate that when good observations are available for assimilation, the first priority for improving ozone DA systems is to improve the models. The analyses benefit strongly from the good quality of the MIPAS ozone observations. Using the analyses as a transfer standard, it is seen that MIPAS is ~5% higher than HALOE (Halogen Occultation Experiment) in the mid and upper stratosphere and mesosphere (above 30 hPa), and of order 10% higher than ozonesonde and HALOE in the lower stratosphere (100 hPa to 30 hPa). Analyses based on SCIAMACHY total column are almost as good as the MIPAS analyses; analyses based on SCIAMACHY limb profiles are worse in some areas, due to problems in the SCIAMACHY retrievals.
Regional lightning NOx sources during the TROCCINOX experiment
Authors: Mari C. , Chaboureau J. P. , Pinty J. P. , Duron J. , Mascart P. , Cammas J. P. , Gheusi F. , Fehr T. , Schlager H. , Roiger A. , Lichtenstein M. , Stock P.
Published: April 2010

Abstract. A lightning NOx (LiNOx) source has been implemented in the deep convection scheme of the Meso-NH mesoscale model following a mass-flux formalism coherent with the transport and scavenging of gases inside the convective scheme. In this approach the vertical transport of NO inside clouds is calculated by the parameterization of deep convective transport, thus eliminating the need for a-priori LiNOx profiles. Once produced inside the convective column, NO molecules are redistributed by updrafts and downdrafts and detrained in the environment when the conditions are favorable. The model was applied to three particular flights during the Tropical Convection, Cirrus and Nitrogen Oxides (TROCCINOX) campaign over the tropical area around Bauru on 3–4 March 2004. The convective activity during the three flights was investigated using brightness temperature at 10.7 μm observed from GOES-12 satellite. The use of a model-to-satellite approach reveals that the simulation appears rather realistic compared to the observations. The diurnal cycle of the simulated brightness temperature, CAPE, number of IC flashes, NO entrainment flux are in phase, with a succession of three marked peaks at 18:00 UTC (15:00 LT). These simulated peaks precede the observed afternoon one by about three hours. Comparison of the simulated NOx with observations along the flight tracks show that the model reproduces well the observed NOx levels when the LiNOx source is applied. The budget of entrainment, detrainment and LiNOx convective fluxes shows that the majority of the NO detrained back to the environment comes from lightning source inside the convective columns. Entrainment of NO from the environment and vertical transport from the boundary layer were not significant during the episode. The troposphere is impacted by detrainment fluxes of LiNOx from 4 km altitude to 16 km with maximum values around 14 km altitude. Detrainment fluxes vary between 75 kg(N)/s during nighttime to 400 kg(N)/s at the times of maximun convective activity. Extrapolation of the regional LiNOx source would yield a global LiNOx production around 5.7 Tg(N)/year which is within the current estimates but should not hide the overestimation of the number of flash rates by the model.
Atmospheric HULIS: How humic-like are they? A comprehensive and critical review
Authors: Graber E. R. , Rudich Y.
Published: April 2010

Abstract. A class of organic molecules extracted from atmospheric aerosol particles and isolated from fog and cloud water has been termed HUmic-LIke Substances (HULIS) due to a certain resemblance to terrestrial and aquatic humic and fulvic acids. In light of the interest that this class of atmospheric compounds currently attracts, we comprehensively review HULIS properties, as well as laboratory and field investigations concerning their formation and characterization in atmospheric samples. While sharing some important features such as polyacidic nature, accumulating evidence suggests that atmospheric HULIS differ substantially from terrestrial and aquatic humic substances. Major differences between HULIS and humic substances, including smaller average molecular weight, lower aromatic moiety content, greater surface activity, better droplet activation ability, as well as others, are highlighted. Several alternatives are proposed that may explain such differences: (1) the possibility that mono- and di-carboxylic acids and mineral acids abundant in the atmosphere prevent the formation of large humic "supramolecular associations"; (2) that large humic macromolecules are destroyed in the atmosphere by UV radiation, O3, and OH- radicals; (3) that "HULIS" actually consists of a complex, unresolved mixture of relatively small molecules rather than macromolecular entities; and (4) that HULIS formed via abiotic and short-lived oxidative reaction pathways differ substantially from humic substances formed over long time periods via biologically-mediated reactions. It should also be recalled that the vast majority of studies of HULIS relate to the water soluble fraction, which would include only the fulvic acid fraction of humic substances, and exclude the humic acid (base-soluble) and humin (insoluble) fractions of humic substances. A significant effort towards adopting standard extraction and characterization methods is required to develop a better and meaningful comparison between different HULIS samples.
Observation of unusual chlorine activation by ground-based infrared and microwave spectroscopy in the late Arctic winter 2000/01
Authors: Blumenstock T. , Kopp G. , Hase F. , Hochschild G. , Mikuteit S. , Raffalski U. , Ruhnke R.
Published: April 2010

Abstract. During the Arctic winter of 2000/01, ground-based FTIR and millimetre-wave measurements revealed significant amounts of ClO over Kiruna after the final warming in February 2001. In fact, column amounts of ClO were still increased in March 2001 when temperatures were about 20K above the PSC (Polar Stratospheric Clouds) threshold. At these temperatures, chlorine activation due to heterogeneous processes on PSCs is not possible even in the presence of strong lee wave effects. In order to discuss possible reasons of this feature, time series of other chemical species will be presented and discussed, too. Measurements of HF and COF2 indicated that vortex air was still observed in mid-March 2001. Since the time series of HNO3 column amounts do not give any evidence of a denitrification later than 11 February, chlorine activation persisting for several weeks after the presence of PSCs due to denitrification is rather unlikely. The photolysis of ClONO2-rich air which had been formed at the end of February and beginning of March 2001 as well as chlorine activation due to the presence of an unusual aerosol layer are discussed as possible causes of the increased ClO column amounts after the final warming.
The influence of African air pollution on regional and global tropospheric ozone
Authors: Aghedo A. M. , Schultz M. G. , Rast S.
Published: April 2010

Abstract. We investigate the influence of African biomass burning, biogenic, lightning and anthropogenic emissions on the tropospheric ozone over Africa and globally using a coupled global chemistry climate model. Our model studies indicate that surface ozone concentration may rise by up to 50 ppbv in the burning region during the biomass burning seasons. Biogenic emissions yield between 5–30 ppbv increase in the near surface ozone concentration over tropical Africa. The impact of lightning on surface ozone is negligible, while anthropogenic emissions yield a maximum of 7 ppbv increase in the annual-mean surface ozone concentration over Nigeria, South Africa and Egypt. Our results show that biogenic emissions are the most important African emission source affecting total tropospheric ozone. The influence of each of the African emissions on the global tropospheric ozone burden (TOB) of 384 Tg yields about 9.5 Tg, 19.6 Tg, 9.0 Tg and 4.7 Tg for biomass burning, biogenic, lightning and anthropogenic emissions emitted in Africa respectively. The impact of each of these emission categories on African TOB of 33 Tg is 2.5 Tg, 4.1 Tg, 1.75 Tg and 0.89 Tg respectively, which together represents about 28% of the total TOB calculated over Africa. Our model calculations also suggest that more than 70% of the tropospheric ozone produced by each of the African emissions is found outside the continent, thus exerting a noticeable influence on a large part of the tropical troposphere. Apart from the Atlantic and Indian Ocean, Latin America experiences the largest impact of African emissions, followed by Oceania, the Middle East, Southeast and south-central Asia, northern North America (i.e. the United States and Canada), Europe and north-central Asia, for all the emission categories.
Annual variation of strato-mesospheric carbon monoxide measured by ground-based Fourier transform infrared spectrometry
Authors: Velazco V. , Wood S. W. , Sinnhuber M. , Kramer I. , Jones N. B. , Kasai Y. , Notholt J. , Warneke T. , Blumenstock T. , Hase F. , Murcray F. J. , Schrems O.
Published: April 2010

Abstract. We present long-term time-series of strato-mesospheric CO vertical columns measured from stations located in Antarctica, mid-latitudes and the Arctic, covering the period from 1997–2005. The instrument and the measurement technique allows the separation of tropospheric and strato-mesospheric contributions to the CO column, therefore providing information on the chemistry and dynamics both at low and high altitudes. Data from polar stations show a similar annual variability of strato-mesospheric CO with a strong maximum in late winter and spring. A small enhancement in late summer for some stations, which we call the "summer bulge", can be seen occasionally. Generally, the mid-latitude stations show no significant annual variability of strato-mesospheric CO columns. Measurements were compared with a two-dimensional chemistry-transport model of the middle atmosphere. The annual and latitudinal variations of CO are reproduced well by a model run including thermospheric CO. Comparison with two model scenarios show that the polar winter maximum is due solely to downward transport of thermospheric CO, while CHOx chemistry in the stratosphere could probably contribute to the summer maximum.
High resolution vertical distributions of NO3 and N2O5 through the nocturnal boundary layer
Authors: Brown S. S. , Dubé W. P. , Osthoff H. D. , Wolfe D. E. , Angevine W. M. , Ravishankara A. R.
Published: April 2010

Abstract. The shallow mixing depth and vertical stratification of the lowest levels of the atmosphere at night has implications for the chemistry of nitrogen oxides emitted from the surface. Here we report vertical profiles of NO3, N2O5 and O3 measured from in-situ instruments on a movable carriage on a 300 m tower. The study offers high-resolution (<1 m) vertical distributions of both NO3 and N2O5 and shows that the nocturnal mixing ratios of these compounds vary widely over short vertical distance scales (10 m or less). Furthermore, there are systematic differences in the steady state lifetimes of NO3 and N2O5 and in the partitioning among nitrogen oxides between different near-surface layers. These differences imply that NO3 and N2O5 occupy distinct chemical regimes as a function of altitude, potentially serving as sinks for nitrogen oxides and O3 near the surface but as reservoirs of NOx and O3 aloft.
MIPAS Level 1B algorithms overview: operational processing and characterization
Authors: Kleinert A. , Aubertin G. , Perron G. , Birk M. , Wagner G. , Hase F. , Nett H. , Poulin R.
Published: April 2010

Abstract. This paper gives an overview of the MIPAS Level 1B (L1B) processor whose main objective is to calibrate atmospheric measurements radiometrically, spectrally and geo-located. It presents also the results of instrument characterization done on ground and during the first years in-flight. An accurate calibration is mandatory for high quality atmospheric retrievals. MIPAS has shown very good performance and stability. The noise equivalent spectral radiance ranges from 3 to 50 nW/(cm2 sr cm−1) and is well within the requirements over nearly the whole spetral range. The systematic radiometric error is estimated to be within 1 or 2% in most situations.
Lightning-produced NO2 observed by two ground-based UV-visible spectrometers at Vanscoy, Saskatchewan in August 2004
Authors: Fraser A. , Goutail F. , McLinden C. A. , Melo S. M. L. , Strong K.
Published: April 2010

Abstract. Ground-based measurements of ozone and NO2 differential slant columns by the SAOZ (Système d'Analyse par Observations Zénithales) and UT-GBS (University of Toronto Ground-Based Spectrometer) instruments during the MANTRA 2004 field campaign are presented herein. During the afternoon of 28 August, a thunderstorm passed over the instruments, which were installed at Vanscoy, Saskatchewan (52° N, 107° W). Enhanced differential slant columns of ozone and NO2 were observed by both instruments during the storm, with maximum values of two and 25 times the expected clear sky columns, respectively. The enhanced ozone differential slant columns are primarily due to the longer path traversed by the solar radiation caused by multiple scattering inside the thick cloud layer associated with the thunderstorm. The enhanced NO2 columns are partly attributed to NOx production by lightning. Two new methods are used to separate the NO2 enhancements into contributions from the longer path length and production by lightning. Combining the observed excess NO2 with lightning flash data from the Canadian Lightning Detection Network and Environment Canada Doppler radar measurements, the production of NO2 molecules per lightning flash is determined. Using these two methods, the best estimate of the production rate is found to be (7.88±2.52)×1026 molecules NO2/flash from the UT-GBS and (6.81±2.17)×1026 molecules NO2/flash from SAOZ. These results are consistent with the range of previous estimates reported in the literature.
Evaluation of radar multiple scattering effects in Cloudsat configuration
Authors: Battaglia A. , Ajewole M. O. , Simmer C.
Published: April 2010

Abstract. MonteCarlo simulations have been performed to evaluate the importance of multiple scattering effects in co- and cross-polar radar returns for 94 GHz radars in Cloudsat and airborne configurations. Thousands of vertically structured profiles derived from some different cloud resolving models are used as a test-bed. Mie theory is used to derive the single scattering properties of the atmospheric hydrometeors. Multiple scattering effects in the co-polar channel (reflectivity enhancement) are particularly elusive, especially in airborne configuration. They can be quite consistent in satellite configurations, like CloudSat, especially in regions of high attenuation and in the presence of highly forward scattering layers associated with snow and graupel particles. When the cross polar returns are analysed [but note that CloudSat does not measure any linear depolarization ratio (LDR hereafter)], high LDR values appear both in space and in airborne configurations. The LDR signatures are footprints of multiple scattering effects; although depolarization values as high as −5 dB can be generated including non-spherical particles in single scattering modelling, multiple scattering computations can produce values close to complete depolarization (i.e. LDR=0 dB). Our simulated LDR profiles from an air-borne platform well reproduce, in a simple frame, some experimental observations collected during the Wakasa Bay experiment. Since LDR instrumental uncertainties were not positively accounted for during that experiment, more focused campaigns with air-borne polarimetric radar are recommended. Multiple scattering effects can be important for CloudSat applications like rainfall and snowfall retrievals since single scattering based algorithms will be otherwise burdened by positive biases.
Scavenging of black carbon in mixed phase clouds at the high alpine site Jungfraujoch
Authors: Cozic J. , Verheggen B. , Mertes S. , Connolly P. , Bower K. , Petzold A. , Baltensperger U. , Weingartner E.
Published: April 2010

Abstract. The scavenging of black carbon (BC) in liquid and mixed phase clouds was investigated during intensive experiments in winter 2004, summer 2004 and winter 2005 at the high alpine research station Jungfraujoch (3580 m a.s.l., Switzerland). Aerosol residuals were sampled behind two well characterized inlets; a total inlet which collected cloud particles (droplets and ice particles) as well as interstitial (unactivated) aerosol particles; an interstitial inlet which collected only interstitial aerosol particles. BC concentrations were measured behind each of these inlets along with the submicrometer aerosol number size distribution, from which a volume concentration was derived. These measurements were complemented by in-situ measurements of cloud microphysical parameters. BC was found to be scavenged into the condensed phase to the same extent as the bulk aerosol, which suggests that BC was covered with soluble material through aging processes, rendering it more hygroscopic. The scavenged fraction of BC (FScav,BC), defined as the fraction of BC that is incorporated into cloud droplets and ice crystals, decreases with increasing cloud ice mass fraction (IMF) from FScav,BC=60% in liquid phase clouds to FScav,BC~5–10% in mixed-phase clouds with IMF>0.2. This can be explained by the evaporation of liquid droplets in the presence of ice crystals (Wegener-Bergeron-Findeisen process), releasing BC containing cloud condensation nuclei back into the interstitial phase. In liquid clouds, the scavenged BC fraction is found to decrease with decreasing cloud liquid water content. The scavenged BC fraction is also found to decrease with increasing BC mass concentration since there is an increased competition for the available water vapour.
Stationary planetary wave propagation in Northern Hemisphere winter – climatological analysis of the refractive index
Authors: Li Q. , Graf H.-F. , Giorgetta M. A.
Published: April 2010

Abstract. The probability density on a height-meridional plane of negative refractive index squared f(nk2<0) is introduced as a new analysis tool to investigate the climatology of the propagation conditions of stationary planetary waves based on NCEP/NCAR reanalysis data for 44 Northern Hemisphere boreal winters (1958–2002). This analysis addresses the control of the atmospheric state on planetary wave propagation. It is found that not only the variability of atmospheric stability with altitudes, but also the variability with latitudes has significant influence on planetary wave propagation. Eliassen-Palm flux and divergence are also analyzed to investigate the eddy activities and forcing on zonal mean flow. Only the ultra-long planetary waves with zonal wave number 1, 2 and 3 are investigated. In Northern Hemisphere winter the atmosphere shows a large possibility for stationary planetary waves to propagate from the troposphere to the stratosphere. On the other hand, waves induce eddy momentum flux in the subtropical troposphere and eddy heat flux in the subpolar stratosphere. Waves also exert eddy momentum forcing on the mean flow in the troposphere and stratosphere at middle and high latitudes. A similar analysis is also performed for stratospheric strong and weak polar vortex regimes, respectively. Anomalies of stratospheric circulation affect planetary wave propagation and waves also play an important role in constructing and maintaining of interannual variations of stratospheric circulation.
Definition of "banner clouds" based on time lapse movies
Authors: Schween J. H. , Kuettner J. , Reinert D. , Reuder J. , Wirth V.
Published: April 2010

Abstract. Banner clouds appear on the leeward side of a mountain and resemble a banner or a flag. This article provides a comprehensive definition of "banner clouds". It is based primarily on an extensive collection of time lapse movies, but previous attempts at an explanation of this phenomenon are also taken into account. The following ingredients are considered essential: the cloud must be attached to the mountain but not appear on the windward side; the cloud must originate from condensation of water vapour contained in the air (rather than consist of blowing snow); the cloud must be persistent; and the cloud must not be of convective nature. The definition is illustrated and discussed with the help of still images and time lapse movies taken at Mount Zugspitze in the Bavarian Alps.
Consecutive reactions of aromatic-OH adducts with NO, NO2 and O2: benzene, naphthalene, toluene, m- and p-xylene, hexamethylbenzene, phenol, m-cresol and aniline
Authors: Koch R. , Knispel R. , Elend M. , Siese M. , Zetzsch C.
Published: April 2010

Abstract. Consecutive reactions of adducts, resulting from OH radicals and aromatics, with the tropospheric scavenger molecules O2, NO and NO2 have been studied for benzene, naphthalene, toluene, m- and p-xylene, hexamethylbenzene, phenol, m-cresol and aniline by observing decays of OH at temperatures where the thermal back-decomposition to OH is faster than 3 s−1, typically between 300 and 340 K. The experimental technique was resonance fluorescence with flash photolysis of water as source of OH. Biexponential decays were observed in the presence of either O2 or NO, and triexponential decays were obtained in the presence of NO2. The kinetic analysis was performed by fitting the relevant rate constants of the reaction mechanism to whole sets of decays obtained at various concentrations of aromatic and scavenger. In the case of hexamethylbenzene, the biexponential decays suggest the existence of the ipso-adduct, and the slightly higher necessary temperatures show that it is even more stable. In addition, smog chamber experiments at O2 concentrations from atmospheric composition down to well below 100 ppm have been carried out for benzene, toluene and p-xylene. The drop of the effective rate constant of removal by OH occurs at reasonable O2 levels, given the FP/RF results. Comparison of the adduct reactivities shows for all aromatics of this study that the reaction with O2 predominates over that with NO2 under all tropospheric conditions, and that a reaction with NO may only occur after the reaction with O2.
Investigative modeling of new pathways for secondary organic aerosol formation
Authors: Pun B. K. , Seigneur C.
Published: April 2010

Abstract. Recent advances in secondary organic aerosol (SOA) research are reviewed and the status of current understanding is investigated using a box model of SOA formation. Benzene and isoprene are newly identified precursors that are included in this SOA model; these precursors form SOA via secondary products. The model is also extended to include some representation of aqueous partitioning and the formation of high molecular weight products via oligomerization. Experimental data and empirical relationships are used where possible, because a detailed representation of SOA formation is not supported by the current state of information. Sensitivity studies are conducted with the SOA model and SOA predictions are found to be very sensitive to the treatment of the interactions between particulate water and organic compounds. While uncertainties due to model formulation are significant, influential model parameters include the aerosol partitioning ratios for several small products of isoprene and the partitioning constants for unidentified products (currently, the partitioning constants are derived by fitting experimental data). The pH value used as the reference for the activation of oligomerization is also a critical parameter. Recommendations for future work needed to improve SOA models include the elucidation of the water-organic relationship, the extent of phase separation, and laboratory experiments conducted under conditions more relevant to ambient studies (e.g., lower concentrations, higher relative humidity).
Stable isotopes provide revised global limits of aerobic methane emissions from plants
Authors: Ferretti D. F. , Miller J. B. , White J. W. C. , Lassey K. R. , Lowe D. C. , Etheridge D. M.
Published: April 2010

Abstract. Recently Keppler et al. (2006) discovered a surprising new source of methane – terrestrial plants under aerobic conditions, with an estimated global production of 62–236 Tg yr−1 by an unknown mechanism. This is ~10–40% of the annual total of methane entering the modern atmosphere and ~30–100% of annual methane entering the pre-industrial (0 to 1700 AD) atmosphere. Here we test this reported global production of methane from plants against ice core records of atmospheric methane concentration (CH4) and stable carbon isotope ratios (δ13CH4) over the last 2000 years. Our top-down approach determines that global plant emissions must be much lower than proposed by Keppler et al. (2006) during the last 2000 years and are likely to lie in the range 0–46 Tg yr−1 and 0–176 Tg yr−1 during the pre-industrial and modern eras, respectively.
Development of the adjoint of GEOS-Chem
Authors: Henze D. K. , Hakami A. , Seinfeld J. H.
Published: April 2010

Abstract. We present the adjoint of the global chemical transport model GEOS-Chem, focusing on the chemical and thermodynamic relationships between sulfate – ammonium – nitrate aerosols and their gas-phase precursors. The adjoint model is constructed from a combination of manually and automatically derived discrete adjoint algorithms and numerical solutions to continuous adjoint equations. Explicit inclusion of the processes that govern secondary formation of inorganic aerosol is shown to afford efficient calculation of model sensitivities such as the dependence of sulfate and nitrate aerosol concentrations on emissions of SOx, NOx, and NH3. The accuracy of the adjoint model is extensively verified by comparing adjoint to finite difference sensitivities, which are shown to agree within acceptable tolerances. We explore the robustness of these results, noting how discontinuities in the advection routine hinder, but do not entirely preclude, the use of such comparisons for validation of the adjoint model. The potential for inverse modeling using the adjoint of GEOS-Chem is assessed in a data assimilation framework using simulated observations, demonstrating the feasibility of exploiting gas- and aerosol-phase measurements for optimizing emission inventories of aerosol precursors.
Interannual variability of the stratospheric wave driving during northern winter
Authors: Haklander A. J. , Siegmund P. C. , Kelder H. M.
Published: April 2010

Abstract. The strength of the stratospheric wave driving during northern winter is often quantified by the January–February mean poleward eddy heat flux at 100 hPa, averaged over 40°–80° N (or a similar area and period). Despite the dynamical and chemical relevance of the wave driving, the causes for its variability are still not well understood. In this study, ERA-40 reanalysis data for the period 1979–2002 are used to examine several factors that significantly affect the interannual variability of the wave driving. The total poleward heat flux at 100 hPa is poorly correlated with that in the troposphere, suggesting a decoupling between 100 hPa and the troposphere. However, the individual zonal wave-1 and wave-2 contributions to the wave driving at 100 hPa do exhibit a significant coupling with the troposphere, predominantly their stationary components. The stationary wave-1 contribution to the total wave driving significantly depends on the latitude of the stationary wave-1 source in the troposphere. The results suggest that this dependence is associated with the varying ability of stationary wave-1 activity to enter the tropospheric waveguide at mid-latitudes. The wave driving anomalies are separated into three parts: one part due to anomalies in the zonal correlation coefficient between the eddy temperature and eddy meridional wind, another part due to anomalies in the zonal eddy temperature amplitude, and a third part due to anomalies in the zonal eddy meridional wind amplitude. It is found that year-to-year variability in the zonal correlation coefficient between the eddy temperature and the eddy meridional wind is the most dominant factor in explaining the year-to-year variability of the poleward eddy heat flux.
HDO measurements with MIPAS
Authors: Steinwagner J. , Milz M. , von Clarmann T. , Glatthor N. , Grabowski U. , Höpfner M. , Stiller G. P. , Röckmann T.
Published: April 2010

Abstract. We have used high spectral resolution spectroscopic measurements from the MIPAS instrument on the Envisat satellite to simultaneously retrieve vertical profiles of H2O and HDO in the stratosphere and uppermost troposphere. Variations in the deuterium content of water are expressed in the common δ notation, where δD is the deviation of the Deuterium/Hydrogen ratio in a sample from a standard isotope ratio. A thorough error analysis of the retrievals confirms that reliable δD data can be obtained up to an altitude of ~45 km. Averaging over multiple orbits and thus over longitudes further reduces the random part of the error. The absolute total error of averaged δD is between 36‰ and 111‰. With values lower than 42‰ the total random error is significantly smaller than the natural variability of δD. The data compare well with previous investigations. The MIPAS measurements now provide a unique global data set of high-quality δD data that will provide novel insight into the stratospheric water cycle.
Measurements of O3, NO2 and BrO during the INDOEX campaign using ground based DOAS and GOME satellite data
Authors: Ladstätter-Weißenmayer A. , Altmeyer H. , Bruns M. , Richter A. , Rozanov A. , Rozanov V. , Wittrock F. , Burrows J. P.
Published: April 2010

Abstract. The INDian Ocean EXperiment (INDOEX) was an international, multi-platform field campaign to measure long-range transport of air masses from South and South-East-(SE) Asia towards the Indian Ocean. During the dry monsoon season between January and March 1999, local measurements were carried out from ground based platforms and were compared with satellite based data. The objective of this study was to characterise stratospheric and tropospheric trace gas amounts in the equatorial region, and to investigate the impact of air pollution at this remote site. For the characterisation of the chemical composition of the outflow from the S-SE-Asian region, we performed ground based dual-axis-DOAS (Differential Optical Absorption Spectroscopy) measurements at the KCO (Kaashidhoo Climate Observatory) in the Maldives (5.0° N, 73.5° E). The measurements were conducted using two different observation modes (off-axis and zenith-sky). This technique allows the separation of the tropospheric and stratospheric columns for different trace gases like O3 and NO2. These dual-axis DOAS data were compared with O3-sonde measurements performed at KCO and satellite based GOME (Global Ozone Measuring Experiment) data during the intensive measuring phase of the INDOEX campaign in February and March 1999. From GOME observations, tropospheric and stratospheric columns for O3 and NO2 were retrieved. In addition, the analysis of the O3-sonde measurements allowed the determination of the tropospheric O3 amount. The comparison shows that the results of all three measurement systems agree within their error limits. During the INDOEX campaign, mainly background conditions were observed, but in a single case an increase of tropospheric NO2 during a short pollution event was observed from the ground and the impact on the vertical columns was calculated. GOME measurements showed evidence for small tropospheric contributions to the BrO budget, probably located in the free troposphere and present over long periods of the year. The amounts of BrO have been investigated by the comparison of satellite pixels influenced by high and low cloud conditions based on GOME data which allows the determination of the detection limit of 3.8×1013molecules cm−2 of tropospheric BrO columns.
Arctic smoke – aerosol characteristics during a record smoke event in the European Arctic and its radiative impact
Authors: Treffeisen R. , Tunved P. , Ström J. , Herber A. , Bareiss J. , Helbig A. , Stone R. S. , Hoyningen-Huene W. , Krejci R. , Stohl A. , Neuber R.
Published: April 2010

Abstract. In early May 2006 a record high air pollution event was observed at Ny-Ålesund, Spitsbergen. An atypical weather pattern established a pathway for the rapid transport of biomass burning aerosols from agricultural fires in Eastern Europe to the Arctic. Atmospheric stability was such that the smoke was constrained to low levels, within 2 km of the surface during the transport. A description of this smoke event in terms of transport and main aerosol characteristics can be found in Stohl et al. (2007). This study puts emphasis on the radiative effect of the smoke. The aerosol number size distribution was characterised by lognormal parameters as having an accumulation mode centered around 165–185 nm and almost 1.6 for geometric standard deviation of the mode. Nucleation and small Aitken mode particles were almost completely suppressed within the smoke plume measured at Ny-Ålesund. Chemical and microphysical aerosol information obtained at Mt. Zeppelin (474 m a.s.l) was used to derive input parameters for a one-dimensional radiation transfer model to explore the radiative effects of the smoke. The daily mean heating rate calculated on 2 May 2006 for the average size distribution and measured chemical composition reached 0.55 K day−1 at 0.5 km altitude for the assumed external mixture of the aerosols but showing much higher heating rates for an internal mixture (1.7 K day−1). In comparison a case study for March 2000 showed that the local climatic effects due to Arctic haze, using a regional climate model, HIRHAM, amounts to a maximum of 0.3 K day−1 of heating at 2 km altitude (Treffeisen et al., 2005).
Enhanced tropospheric BrO over Antarctic sea ice in mid winter observed by MAX-DOAS on board the research vessel Polarstern
Authors: Wagner T. , Ibrahim O. , Sinreich R. , Frieß U. , von Glasow R. , Platt U.
Published: April 2010

Abstract. We present Multi AXis-Differential Optical Absorption Spectroscopy (MAX-DOAS) observations of tropospheric BrO carried out on board the German research vessel Polarstern during the Antarctic winter 2006. Polarstern entered the area of first year sea ice around Antarctica on 24 June 2006 and stayed within this area until 15 August 2006. For the period when the ship cruised inside the first year sea ice belt, enhanced BrO concentrations were almost continuously observed. Outside the first year sea ice belt, typically low BrO concentrations were found. Based on back trajectory calculations we find a positive correlation between the observed BrO differential slant column densities (ΔSCDs) and the duration for which the air masses had been in contact with the sea ice surface prior to the measurement. While we can not completely rule out that in several cases the highest BrO concentrations might be located close to the ground, our observations indicate that the maximum BrO concentrations might typically exist in a (possibly extended) layer around the upper edge of the boundary layer. Besides the effect of a decreasing pH of sea salt aerosol with altitude and therefore an increase of BrO with height, this finding might be also related to vertical mixing of air from the free troposphere with the boundary layer, probably caused by convection over the warm ocean surface at polynyas and cracks in the ice. Strong vertical gradients of BrO and O3 could also explain why we found enhanced BrO levels almost continuously for the observations within the sea ice. Based on our estimated BrO profiles we derive BrO mixing ratios of several ten ppt, which is slightly higher than many existing observations. Our observations indicate that enhanced BrO concentrations around Antarctica exist about one month earlier than observed by satellite instruments. From detailed radiative transfer simulations we find that MAX-DOAS observations are up to about one order of magnitude more sensitive to near-surface BrO than satellite observations. In contrast to satellite observations the MAX-DOAS sensitivity hardly decreases for large solar zenith angles and is almost independent from the ground albedo. Thus this technique is very well suited for observations in polar regions close to the solar terminator. For large periods of our measurements the solar elevation was very low or even below the horizon. For such conditions, most reactive Br-compounds might exist as Br2 molecules and ozone destruction and the removal of reactive bromine compounds might be substantially reduced.
Global statistics of liquid water content and effective number concentration of water clouds over ocean derived from combined CALIPSO and MODIS measurements
Authors: Hu Y. , Vaughan M. , McClain C. , Behrenfeld M. , Maring H. , Anderson D. , Sun-Mack S. , Flittner D. , Huang J. , Wielicki B. , Minnis P. , Weimer C. , Trepte C. , Kuehn R.
Published: April 2010

Abstract. This study presents an empirical relation that links the volume extinction coefficients of water clouds, the layer integrated depolarization ratios measured by lidar, and the effective radii of water clouds derived from collocated passive sensor observations. Based on Monte Carlo simulations of CALIPSO lidar observations, this method combines the cloud effective radius reported by MODIS with the lidar depolarization ratios measured by CALIPSO to estimate both the liquid water content and the effective number concentration of water clouds. The method is applied to collocated CALIPSO and MODIS measurements obtained during July and October of 2006, and January 2007. Global statistics of the cloud liquid water content and effective number concentration are presented.