bluuebunny/crossref_metadata_2025 huggingface dataset:
Atmospheric effects and societal consequences of regional scale nuclear conflicts and acts of individual nuclear terrorism
Authors: Toon O. B. , Turco R. P. , Robock A. , Bardeen C. , Oman L. , Stenchikov G. L.
Published: April 2010

Abstract. We assess the potential damage and smoke production associated with the detonation of small nuclear weapons in modern megacities. While the number of nuclear warheads in the world has fallen by about a factor of three since its peak in 1986, the number of nuclear weapons states is increasing and the potential exists for numerous regional nuclear arms races. Eight countries are known to have nuclear weapons, 2 are constructing them, and an additional 32 nations already have the fissile material needed to build substantial arsenals of low-yield (Hiroshima-sized) explosives. Population and economic activity worldwide are congregated to an increasing extent in megacities, which might be targeted in a nuclear conflict. Our analysis shows that, per kiloton of yield, low yield weapons can produce 100 times as many fatalities and 100 times as much smoke from fires as high-yield weapons, if they are targeted at city centers. A single "small'' nuclear detonation in an urban center could lead to more fatalities, in some cases by orders of magnitude, than have occurred in the major historical conflicts of many countries. We analyze the likely outcome of a regional nuclear exchange involving 100 15-kt explosions (less than 0.1% of the explosive yield of the current global nuclear arsenal). We find that such an exchange could produce direct fatalities comparable to all of those worldwide in World War II, or to those once estimated for a "counterforce'' nuclear war between the superpowers. Megacities exposed to atmospheric fallout of long-lived radionuclides would likely be abandoned indefinitely, with severe national and international implications. Our analysis shows that smoke from urban firestorms in a regional war would rise into the upper troposphere due to pyro-convection. Robock et al. (2006) show that the smoke would subsequently rise deep into the stratosphere due to atmospheric heating, and then might induce significant climatic anomalies on global scales.We also anticipate substantial perturbations of global ozone. While there are many uncertainties in the predictions we make here, the principal unknowns are the type and scale of conflict that might occur. The scope and severity of the hazards identified pose a significant threat to the global community. They deserve careful analysis by governments worldwide advised by a broad section of the world scientific community, as well as widespread public debate.
Climatic consequences of regional nuclear conflicts
Authors: Robock A. , Oman L. , Stenchikov G. L. , Toon O. B. , Bardeen C. , Turco R. P.
Published: April 2010

Abstract. We use a modern climate model and new estimates of smoke generated by fires in contemporary cities to calculate the response of the climate system to a regional nuclear war between emerging third world nuclear powers using 100 Hiroshima-size bombs (less than 0.03% of the explosive yield of the current global nuclear arsenal) on cities in the subtropics. We find significant cooling and reductions of precipitation lasting years, which would impact the global food supply. The climate changes are large and long-lasting because the fuel loadings in modern cities are quite high and the subtropical solar insolation heats the resulting smoke cloud and lofts it into the high stratosphere, where removal mechanisms are slow. While the climate changes are less dramatic than found in previous "nuclear winter'' simulations of a massive nuclear exchange between the superpowers, because less smoke is emitted, the changes are more long-lasting because the older models did not adequately represent the stratospheric plume rise.
SAWA experiment – properties of mineral dust aerosol as seen by synergic lidar and sun-photometer measurements
Authors: Kardas A. E. , Markowicz K. M. , Malinowski S. P. , Karasiński G. , Stacewicz T. , Stelmaszczyk K. , Hochhertz C. , Woeste L.
Published: April 2010

Abstract. We propose a method of retrieving basic information on mineral dust aerosol particles from synergic sun-photometer and multi-wavelength lidar measurements as well as from the observations of lidar light depolarisation. We use this method in a case study of mineral dust episode in Central Europe. Lidar signals are inversed with a modified Klett-Fernald algorithm. Aerosol optical depth measured with the sun-photometer allows to reduce uncertainties in the inversion procedure through which we estimate vertical profile of aerosol extinction. Next we assume that aerosol particles may be represented by ensemble of randomly oriented, identical spheroids. Having calculated vertical profiles of aerosol extinction coefficients for lidar wavelengths, we compute the profiles of local Angstrom exponent. We use laser beam depolarisation together with the calculated Angstrom exponents to estimate the shapes (aspect ratios) and sizes of the spheroids. Numerical calculations are performed with the transition matrix (T-matrix) algorithm by M. Mishchenko. The proposed method was first used during SAWA measurement campaign in Warsaw, spring 2005, to characterise the particles of desert dust, drifting over Poland with a southern-eastern wind (13–14 April). Observations and T-matrix calculations show that mode radii of spheroids representative for desert aerosols' particles are in the range of 0.15–0.3 μm, while their aspect ratios are lower than 0.7 or larger than 1.7.
The latitude dependence and probability distribution of polar mesospheric turbulence
Authors: Rapp M. , Becker E. , Strelnikov B. , Lübken F.-J.
Published: April 2010

Abstract. We consider in-situ observations and results from a global circulation model to study the latitude dependence and probability distribution of polar mesospheric turbulence. A comparison of summer observations at 69° N and 79° N shows that mesospheric turbulence weakens towards the summer pole. Furthermore, these data suggest that at both latitudes in about ~70% of all samples there are non-turbulent altitude bins in the considered altitude range between 70 and 95 km. The remaining 30% with detectable turbulence show an approximately log-normal distribution of dissipation rates. A low-resolution model version with a gravity wave (GW) parameterization explains the observed latitude dependence as a consequence of a downshift of the breaking levels towards the summer pole and an accompanying decay of turbulent heating per unit mass. When we do not use a GW parameterization but employ a high spatial resolution instead to simulate GW effects explicitly, the model predicts a similar latitudinal dependence with weakening turbulence towards the summer pole. In addition, the model also produces a log-normal distribution of dissipation rates. The simulated probability distribution is more narrow than in the observations since the model resolves at most mid-frequency GWs, whereas real turbulence is also excited by smaller-scale disturbances. The GW resolving simulation suggests a weaker tropospheric GW source at polar latitudes as the dominating mechanism for the latitudinal dependence.
The T1-T2 study: evolution of aerosol properties downwind of Mexico City
Authors: Doran J. C. , Arnott W. P. , Barnard J. C. , Cary R. , Coulter R. , Fast J. D. , Kassianov E. I. , Kleinman L. , Laulainen N. S. , Martin T. , Paredes-Miranda G. , Pekour M. S. , Shaw W. J. , Smith D. F. , Springston S. R. , Yu X.-Y.
Published: April 2010

Abstract. As part of a major atmospheric chemistry and aerosol field program carried out in March of 2006, a study was conducted in the area to the north and northeast of Mexico City to investigate the evolution of aerosols and their associated optical properties in the first few hours after their emission. The focus of the T1-T2 aerosol study was to investigate changes in the specific absorption αABS (absorption per unit mass, with unit of m2 g−1) of black carbon as it aged and became coated with compounds such as sulfate and organic carbon, evolving from an external to an internal mixture. Such evolution has been reported in previous studies. The T1 site was located just to the north of the Mexico City metropolitan area; the T2 site was situated approximately 35 km farther to the northeast. Nephelometers, particle soot absorption photometers, photoacoustic absorption photometers, and organic and elemental carbon analyzers were used to measure the optical properties of the aerosols and the carbon concentrations at each of the sites. Radar wind profilers and radiosonde systems helped to characterize the meteorology and to identify periods when transport from Mexico City over T1 and T2 occurred. Organic and elemental carbon concentrations at T1 showed diurnal cycles reflecting the nocturnal and early morning buildup from nearby sources, while concentrations at T2 appeared to be more affected by transport from Mexico City. Specific absorption during transport periods was lower than during other times, consistent with the likelihood of fresher emissions being found when the winds blew from Mexico City over T1 and T2. The specific absorption at T2 was larger than at T1, which is also consistent with the expectation of more aged particles with encapsulated black carbon being found at the more distant location. In situ measurements of single scattering albedo with an aircraft and a ground station showed general agreement with column-averaged values derived from rotating shadowband radiometer data, although some differences were found that may be related to boundary-layer evolution.
Daytime tropospheric loss of hexanal and trans-2-hexenal: OH kinetics and UV photolysis
Authors: Jiménez E. , Lanza B. , Martínez E. , Albaladejo J.
Published: April 2010

Abstract. The ultraviolet (λ=250–370 nm) photolysis and the OH-initiated oxidation of hexanal and trans-2-hexenal, which are relevant atmospheric processes, have been investigated at room temperature and as a function of temperature (T=263–353 K), respectively. This kinetic study as a function of temperature is reported here for the first time. Absolute absorption cross sections (σλ) were obtained using a recently built system operating in the UV region. This work represents the first reported σλ for trans-2-hexenal. The obtained σλ allowed the estimation of the photolysis rates (J) of hexanal and trans-2-hexenal across the troposphere. Kinetic measurements of the gas-phase reaction of hydroxyl radicals (OH) with hexanal and trans-2-hexenal were performed by using the laser pulsed photolysis/laser-induced fluorescence technique. Rate coefficients kOH for both aldehydes were determined at temperatures between 263 and 353 K at 50 Torr in helium or argon bath gases. The temperature dependence of kOH for both aldehydes was found to be slightly negative. The tropospheric lifetime of hexanal and trans-2-hexenal due to the chemical removal by OH radicals has been estimated across the troposphere. The loss rate due to the OH chemical removal was compared with the estimated photolysis rates. Our results show that OH-reaction and UV photolysis are the main loss processes for these aldehydes in the troposphere. For hexanal, both processes compete across the troposphere, however, UV photolysis can contribute up to 70% to the overall loss of trans-2-hexenal.
An inverse modeling procedure to determine particle growth and nucleation rates from measured aerosol size distributions
Authors: Verheggen B. , Mozurkewich M.
Published: April 2010

Abstract. Classical nucleation theory is unable to explain the ubiquity of nucleation events observed in the atmosphere. This shows a need for an empirical determination of the nucleation rate. Here we present a novel inverse modeling procedure to determine particle nucleation and growth rates based on consecutive measurements of the aerosol size distribution. The particle growth rate is determined by regression analysis of the measured change in the aerosol size distribution over time, taking into account the effects of processes such as coagulation, deposition and/or dilution. This allows the growth rate to be determined with a higher time-resolution than can be deduced from inspecting contour plots (''banana-plots''). Knowing the growth rate as a function of time enables the evaluation of the time of nucleation of measured particles of a certain size. The nucleation rate is then obtained by integrating the particle losses from time of measurement to time of nucleation. The regression analysis can also be used to determine or verify the optimum value of other parameters of interest, such as the wall loss or coagulation rate constants. As an example, the method is applied to smog chamber measurements. This program offers a powerful interpretive tool to study empirical aerosol population dynamics in general, and nucleation and growth in particular.
The influence of polar vortex ozone depletion on NH mid-latitude ozone trends in spring
Authors: Andersen S. B. , Knudsen B. M.
Published: April 2010

Abstract. Reverse domain-filling trajectory calculations have been performed for the years 1993, 1995, 1996, 1997, and 2000 to calculate the spreading of ozone depleted air from the polar vortex to midlatitudes in spring. We find that for these years with massive Arctic ozone depletion the zonal mean total ozone column at midlatitudes is reduced with between 7 and 12 DU in the April-May period. The polar vortex and remnants have preferred locations which leads to longitudinal differences in the midlatitude ozone trends. Together with decadal variations in circulation the dilution of ozone depleted air may explain the major fraction of longitudinal differences in midlatitude ozone trends. The dilution also has a significant impact on the zonal mean ozone trends. With a multiple linear regression model we find that the dilution may explain 39% of the trend in the period 1979–1997 and 54% of the trend in the period 1979–2002. By calculting the effect of simply removing the dilutions we get the possibly more reliable estimates that that dilution may explain 29% of the trend in the period 1979–1997 and 33% of the trend in the period 1979–2002.
Strong spectral dependence of light absorption by organic carbon particles formed by propane combustion
Authors: Schnaiter M. , Gimmler M. , Llamas I. , Linke C. , Jäger C. , Mutschke H.
Published: April 2010

Abstract. We have measured the extinction and absorption cross sections of carbon particles emitted by a propane diffusion flame both in an aerosol chamber and on size-segregated samples deposited on optical windows. The absorption cross section, the single scattering albedo and the Ångström exponent show drastic dependencies both on the C/O ratio and on the particle size. This is interpretated as being due to the appearance of nucleation modes of smaller organic particles at higher C/O ratios, which were detected by SMPS measurements and partially by TEM analysis. The spectral range of the validity of the absorption power-law (Ångström exponent) model is investigated by vacuum ultraviolet extinction measurements. These measurements give also indications for a preferentially aromatic nature of the OC component of the flame products.
Imaging gravity waves in lower stratospheric AMSU-A radiances, Part 2: validation case study
Authors: Eckermann S. D. , Wu D. L. , Doyle J. D. , Burris J. F. , McGee T. J. , Hostetler C. A. , Coy L. , Lawrence B. N. , Stephens A. , McCormack J. P. , Hogan T. F.
Published: April 2010

Abstract. Two-dimensional radiance maps from Channel 9 (~60–90 hPa) of the Advanced Microwave Sounding Unit (AMSU-A), acquired over southern Scandinavia on 14 January 2003, show plane-wave-like oscillations with a wavelength λh of ~400–500 km and peak brightness temperature amplitudes of up to 0.9 K. The wave-like pattern is observed in AMSU-A radiances from 8 overpasses of this region by 4 different satellites, revealing a growth in the disturbance amplitude from 00:00 UTC to 12:00 UTC and a change in its horizontal structure between 12:00 UTC and 20:00 UTC. Forecast and hindcast runs for 14 January 2003 using high-resolution global and regional numerical weather prediction (NWP) models generate a lower stratospheric mountain wave over southern Scandinavia with peak 90 hPa temperature amplitudes of ~5–7 K at 12:00 UTC and a similar horizontal wavelength, packet width, phase structure and time evolution to the disturbance observed in AMSU-A radiances. The wave's vertical wavelength is ~12 km. These NWP fields are validated against radiosonde wind and temperature profiles and airborne lidar profiles of temperature and aerosol backscatter ratios acquired from the NASA DC-8 during the second SAGE III Ozone Loss and Validation Experiment (SOLVE II). Both the amplitude and phase of the stratospheric mountain wave in the various NWP fields agree well with localized perturbation features in these suborbital measurements. In particular, we show that this wave formed the type II polar stratospheric clouds measured by the DC-8 lidar. To compare directly with the AMSU-A data, we convert these validated NWP temperature fields into swath-scanned brightness temperatures using three-dimensional Channel 9 weighting functions and the actual AMSU-A scan patterns from each of the 8 overpasses of this region. These NWP-based brightness temperatures contain two-dimensional oscillations due to this resolved stratospheric mountain wave that have an amplitude, wavelength, horizontal structure and time evolution that closely match those observed in the AMSU-A data. These comparisons not only verify gravity wave detection and horizontal imaging capabilities for AMSU-A Channel 9, but provide an absolute validation of the anticipated radiance signals for a given three-dimensional gravity wave, based on the modeling of Eckermann and Wu (2006).
Homogeneous nucleation rates of nitric acid dihydrate (NAD) at simulated stratospheric conditions – Part I: Experimental results
Authors: Stetzer O. , Möhler O. , Wagner R. , Benz S. , Saathoff H. , Bunz H. , Indris O.
Published: April 2010

Abstract. The low temperature aerosol chamber AIDA was used to study the nucleation of nitric acid dihydrate (NAD) in super-cooled nitric acid aerosols under simulated stratospheric conditions in the temperature range 192 K–197 K. The nucleating solution droplets had median diameters between 225 and 290 nm and molar fractions of nitric acid between 0.26 and 0.28. Nucleation of solid particles was unambiguously observed in two out of three experiments during time periods of up to five hours. The newly formed crystals could be clearly distinguished from the remaining liquid droplets by their increasing size with an optical particle spectrometer. The solid particles could be unequivocally identified as strongly aspherical nitric acid dihydrate crystals (α-NAD) by in-situ FTIR-spectroscopy. From our experimental data set there is no indication of direct nucleation of NAT or a conversion of NAD into NAT while having saturation ratios with resprect to NAT of about 20–26. The temporal evolutions of the NAD particle concentrations were used to derive individual nucleation rates for NAD. The measured volume nucleation rates ranged from 3.9·105 cm-3s-1 at 195.8 K and XNA=0.27 to 1.9·107 cm-3s-1 at 192.1 K and XNA=0.28. The corresponding hypothetical surface nucleation rates of 2·100 to 1·102 cm-2s-1 are smaller than the parameterisation of Tabazadeh et al. (2002) by factors between 25 and >103.
Emissions of primary aerosol and precursor gases in the years 2000 and 1750, prescribed data-sets for AeroCom
Authors: Dentener F. , Kinne S. , Bond T. , Boucher O. , Cofala J. , Generoso S. , Ginoux P. , Gong S. , Hoelzemann J. J. , Ito A. , Marelli L. , Penner J. E. , Putaud J.-P. , Textor C. , Schulz M. , van der Werf G. R. , Wilson J.
Published: April 2010

Abstract. Inventories for global aerosol and aerosol precursor emissions, and auxiliary information, have been collected, assessed and prepared for the year 2000 (present-day conditions) and for the year 1750 (pre-industrial conditions). These global datasets establish a reference for input in global modeling, when simulating the aerosol impact on climate with state-of-the-art aerosol component modules. These modules stratify aerosol by type, distinguishing among dust, seasalt, sulfate, organic matter and soot. The datasets are also intented to serve as systematic constraints in sensitivity studies of the AeroCom initiative, which aims to evaluate uncertainties in aerosol global modeling. The datasets comprise daily size-resolved emissions of sea-salt and dust and monthly-to-yearly emissions for all other currently known emissions of natural and anthropogenic aerosol (precursors). The emissions are a reference dataset for aerosol modeling in the coming years and benchmark the emissions according to our knowledge in the year 2004.
Application of thermal dissociation-laser induced fluorescence (TD-LIF) to measurement of HNO3, Σalkyl nitrates, Σperoxy nitrates, and NO2 fluxes using eddy covariance
Authors: Farmer D. K. , Wooldridge P. J. , Cohen R. C.
Published: April 2010

Abstract. Nitrogen exchange between the atmosphere and biosphere directly influences atmospheric composition. While much is known about mechanisms of NO and N2O emissions, instrumentation for the study of mechanisms contributing to exchange of other major nitrogen species is quite limited. Here we describe the application of a new technique, thermal dissociation-laser induced fluorescence (TD-LIF), to eddy covariance measurements of the fluxes of NO2, total peroxy acyl and peroxy nitrates, total alkyl and multifunctional alkyl nitrates, and nitric acid. The technique offers the potential for investigating mechanisms of exchange of these species at the canopy scale over timescales from days to years. Examples of flux measurements at a ponderosa pine plantation in the mid-elevation Sierra Nevada Mountains in California are reported and used to evaluate instrument performance.
Interannual variability of global biomass burning emissions from 1997 to 2004
Authors: van der Werf G. R. , Randerson J. T. , Giglio L. , Collatz G. J. , Kasibhatla P. S. , Arellano A. F.
Published: April 2010

Abstract. Biomass burning represents an important source of atmospheric aerosols and greenhouse gases, yet little is known about its interannual variability or the underlying mechanisms regulating this variability at continental to global scales. Here we investigated fire emissions during the 8 year period from 1997 to 2004 using satellite data and the CASA biogeochemical model. Burned area from 2001–2004 was derived using newly available active fire and 500 m burned area datasets from MODIS following the approach described by Giglio et al. (2005). ATSR and VIRS satellite data were used to extend the burned area time series back in time through 1997. In our analysis we estimated fuel loads, including peatland fuels, and the net flux from terrestrial ecosystems as the balance between net primary production (NPP), heterotrophic respiration (Rh), and biomass burning, using time varying inputs of precipitation (PPT), temperature, solar radiation, and satellite-derived fractional absorbed photosynthetically active radiation (fAPAR). For the 1997–2004 period, we found that on average approximately 58 Pg C year−1 was fixed by plants, and approximately 95% of this was returned back to the atmosphere via Rh. Another 4%, or 2.5 Pg C year−1 was emitted by biomass burning; the remainder consisted of losses from fuel wood collection and subsequent burning. At a global scale, burned area and total fire emissions were largely decoupled from year to year. Total carbon emissions tracked burning in forested areas (including deforestation fires in the tropics), whereas burned area was largely controlled by savanna fires that responded to different environmental and human factors. Biomass burning emissions showed large interannual variability with a range of more than 1 Pg C year−1, with a maximum in 1998 (3.2 Pg C year−1) and a minimum in 2000 (2.0 Pg C year−1).
The sensitivity of aerosol in Europe to two different emission inventories and temporal distribution of emissions
Authors: de Meij A. , Krol M. , Dentener F. , Vignati E. , Cuvelier C. , Thunis P.
Published: April 2010

Abstract. The sensitivity to two different emission inventories, injection altitude and temporal variations of anthropogenic emissions in aerosol modelling is studied, using the two way nested global transport chemistry model TM5 focussing on Europe in June and December 2000. The simulations of gas and aerosol concentrations and aerosol optical depth (AOD) with the EMEP and AEROCOM emission inventories are compared with EMEP gas and aerosol surface based measurements, AERONET sun photometers retrievals and MODIS satellite data. For the aerosol precursor gases SO2 and NOx in both months the model results calculated with the EMEP inventory agree better (overestimated by a factor 1.3 for both SO2 and NOx) with the EMEP measurements than the simulation with the AEROCOM inventory (overestimated by a factor 2.4 and 1.9, respectively). Besides the differences in total emissions between the two inventories, an important role is also played by the vertical distribution of SO2 and NOx emissions in understanding the differences between the EMEP and AEROCOM inventories. In December NOx and SO2 from both simulations agree within 50% with observations. In June SO4= evaluated with the EMEP emission inventory agrees slightly better with surface observations than the AEROCOM simulation, whereas in December the use of both inventories results in an underestimate of SO4 with a factor 2. Nitrate aerosol measured in summer is not reliable, however in December nitrate aerosol calculations with the EMEP and AEROCOM emissions agree with 30%, and 60%, respectively with the filter measurements. Differences are caused by the total emissions and the temporal distribution of the aerosol precursor gases NOx and NH3. Despite these differences, we show that the column integrated AOD is less sensitive to the underlying emission inventories. Calculated AOD values with both emission inventories underestimate the observed AERONET AOD values by 20–30%, whereas a case study using MODIS data shows a high spatial agreement. Our evaluation of the role of temporal distribution of anthropogenic emissions on aerosol calculations shows that the daily and weekly temporal distributions of the emissions are only important for NOx, NH3 and aerosol nitrate. However, for all aerosol species SO4=, NH4+, POM, BC, as well as for AOD, the seasonal temporal variations used in the emission inventory are important. Our study shows the value of including at least seasonal information on anthropogenic emissions, although from a comparison with a range of measurements it is often difficult to firmly identify the superiority of specific emission inventories, since other modelling uncertainties, e.g. related to transport, aerosol removal, water uptake, and model resolution, play a dominant role.
Persistence and photochemical decay of springtime total ozone anomalies in the Canadian Middle Atmosphere Model
Authors: Tegtmeier S. , Shepherd T. G.
Published: April 2010

Abstract. The persistence and decay of springtime total ozone anomalies over the entire extratropics (midlatitudes plus polar regions) is analysed using results from the Canadian Middle Atmosphere Model (CMAM), a comprehensive chemistry-climate model. As in the observations, interannual anomalies established through winter and spring persist with very high correlation coefficients (above 0.8) through summer until early autumn, while decaying in amplitude as a result of photochemical relaxation in the quiescent summertime stratosphere. The persistence and decay of the ozone anomalies in CMAM agrees extremely well with observations, even in the southern hemisphere when the model is run without heterogeneous chemistry (in which case there is no ozone hole and the seasonal cycle of ozone is quite different from observations), and even in the northern hemisphere where this version of CMAM (run with fixed external forcing) strongly underestimates the observed interannual variability. This shows that ozone anomaly persistence and decay does not depend on how the springtime anomalies are created or on their magnitude, but reflects the transport and photochemical decay in the model. It is thus a robust diagnostic of model performance.
MALTE – Model to predict new aerosol formation in the lower troposphere
Authors: Boy M. , Hellmuth O. , Korhonen H. , Nilsson E. D. , ReVelle D. , Turnipseed A. , Arnold F. , Kulmala M.
Published: April 2010

Abstract. The manuscript presents a detailed description of the meteorological and chemical code of Malte – a model to predict new aerosol formation in the lower troposphere. The aerosol dynamics are achieved by the new developed UHMA (University of Helsinki Multicomponent Aerosol Model) code with kinetic limited nucleation as responsible mechanism to form new clusters. First results indicate that the model is able to predict the on- and offset of new particle formation as well as the total aerosol number concentrations that were in good agreement with the observations. Further, comparison of predicted and measured H2SO4 concentrations showed a satisfactory agreement. The simulation results indicated that at a certain transitional particle diameter (2–9 nm), organic molecules can begin to contribute significantly to the growth rate compared to sulphuric acid. At even larger particle sizes, organic molecules can dominate the growth rate on days with significant monoterpene concentrations. The intraday vertical evolution of newly formed clusters and particles in two different size ranges resulted in two maxima at the ground and the top of the mixed layer with higher concentrations for the detectable particles above 3 nm below in contrast to the predicted cluster concentrations.
First spectral measurement of the Earth's upwelling emission using an uncooled wideband Fourier transform spectrometer
Authors: Palchetti L. , Belotti C. , Bianchini G. , Castagnoli F. , Carli B. , Cortesi U. , Pellegrini M. , Camy-Peyret C. , Jeseck P. , Té Y.
Published: April 2010

Abstract. The first spectral measurement of Earth's emitted radiation to space in the wideband range from 100 to 1400 cm−1 with 0.5 cm−1 spectral resolution is presented. The measurement was performed from a stratospheric balloon in tropical region using a Fourier transform spectrometer, during a field campaign held in Brazil in June 2005. The instrument, which has uncooled components including the detector module, is a prototype developed as part of the study for the REFIR (Radiation Explorer in the Far InfraRed) space mission. This paper shows the results of the field campaign with particular attention to the measurement capabilities of the prototype. The results are compared with measurements taken by IASI-balloon (Infrared Atmospheric Sounding Interferometer – Balloon version), aboard the same platform, and with forward model estimations. The infrared signature of clouds is observed in the measurements.
Impact of cloud-borne aerosol representation on aerosol direct and indirect effects
Authors: Ghan S. J. , Easter R. C.
Published: April 2010

Abstract. Aerosol particles attached to cloud droplets are much more likely to be removed from the atmosphere and are much less efficient at scattering sunlight than if unattached. Models used to estimate direct and indirect effects of aerosols employ a variety of representations of such cloud-borne particles. Here we use a global aerosol model with a relatively complete treatment of cloud-borne particles to estimate the sensitivity of simulated aerosol, cloud and radiation fields to various approximations to the representation of cloud-borne particles. We find that neglecting transport of cloud-borne particles introduces little error, but that diagnosing cloud-borne particles produces global mean biases of 20% and local errors of up to 40% for many variables of interest. A treatment that predicts the total mass concentration of cloud-borne particles for each mode yields smaller errors and runs 20% faster than the complete treatment.
Chemical composition of boundary layer aerosol over the Atlantic Ocean and at an Antarctic site
Authors: Virkkula A. , Teinilä K. , Hillamo R. , Kerminen V.-M. , Saarikoski S. , Aurela M. , Viidanoja J. , Paatero J. , Koponen I. K. , Kulmala M.
Published: April 2010

Abstract. Aerosol chemical composition was measured over the Atlantic Ocean in November–December 1999 and at the Finnish Antarctic research station Aboa in January 2000. The concentrations of all anthropogenic aerosol compounds decreased clearly from north to south. An anthropogenic influence was still evident in the middle of the tropical South Atlantic, background values were reached south of Cape Town. Chemical mass balance was calculated for high volume filter samples (Dp<3 μm). North of the equator 70–80% of the aerosol consisted of non-sea-salt species. The contribution of sea salt was ~25% in the polluted latitudes, >80% in the Southern Ocean, and <10% at Aboa. The contribution of organic carbon was >10% in most samples, also at Aboa. The correlation of biomass-burning-related aerosol components with 210Pb was very high compared with that between nss calcium and 210Pb which suggests that 210Pb is a better tracer for biomass burning than for Saharan dust. The ratio of the two clear tracers for biomass burning, nss potassium and oxalate, was different in European and in African samples, suggesting that this ratio could be used as an indicator of biomass burning type. The concentrations of continent-related particles decreased exponentially with the distance from Africa. The shortest half-value distance, ~100 km, was for nss calcium. The half-value distance of particles that are mainly in the submicron particles was ~700±200 km. The MSA to nss sulfate ratio, R, increased faster than MSA concentration with decreasing anthropogenic influence, indicating that the R increase could largely be explained by the decrease of anthropogenic sulfate.
Technical note: A method for measuring size-resolved CCN in the atmosphere
Authors: Frank G. P. , Dusek U. , Andreae M. O.
Published: April 2010

Abstract. We present a method to investigate cloud condensation nuclei (CCN) concentrations and activation efficiencies as a function of two independent variables, aerosol particle size and water vapor supersaturation. To date, most ambient CCN measurements have been made as the integral (total) CCN concentration as a function of water vapor supersaturation only. However, since CCN properties of aerosol particles are strongly dependent on particle size, as well as on chemical composition, which commonly varies with particle size, more detailed measurements can provide additional important information about the CCN activation. With size-resolved measurements, the effect of particle size on CCN activity can be kept constant, which makes it possible to directly assess the influence of particle chemistry. The instrumental set-up consists of a differential mobility analyzer (DMA) to select particles of a known size, within a narrow size range. A condensation nuclei (CN) counter (condensation particle counter, CPC) is used to count the total number of particles in that size range, and a CCN counter is used to count the number of CCN as a function of supersaturation, in that same size range. The activation efficiency, expressed as CCN/CN ratios, can thus directly be calculated as a function of particle size and supersaturation. We present examples of the application of this technique, using salt and smoke aerosols produced in the laboratory as well as ambient aerosols.
NO2 Profile Retrieval using airborne multi axis UV-visible skylight absorption measurements over central Europe
Authors: Bruns M. , Buehler S. A. , Burrows J. P. , Richter A. , Rozanov A. , Wang P. , Heue K.-P. , Platt U. , Pundt I. , Wagner T.
Published: April 2010

Abstract. A recent development in ground-based remote sensing of atmospheric constituents by UV/visible absorption measurements of scattered light is the simultaneous use of several directions with small elevation angles in addition to the traditional zenith-sky pointing. The different light paths through the atmosphere enable the vertical distribution of some atmospheric absorbers such as NO2, BrO or O3 to be retrieved. In this study, the amount of profile information that can be retrieved from such measurements on aircraft is investigated for the trace gas NO2. A Sensitivity study on synthetic data is performed for a combination of four lines of sight (LOS) (0° (nadir), 88°, 92°, and 180° (zenith)) and three wavelength regions [center wavelengths: 362.5 nm, 437.5 nm, and 485.0 nm]. This investigation demonstrates the potential of this LOS/wavelengths setup to retrieve a significant amount of profile information from airborne multiaxis differential optical absorption spectrometer (AMAXDOAS) measurements with a vertical resolution of 3.0 to 4.5 km in the lower troposphere and 2.0 to 3.5 km near flight altitude. Above 13 km the profile information content of AMAXDOAS measurements is sparse. Further, retrieved profiles with a significant amount (up to 3.2 ppbv) of NO2 in the boundary layer over the Po-valley (Italy) are presented. Airborne multiaxis measurements are thus a promising tool for atmospheric studies in the troposphere.
Potential impacts of CF3I on ozone as a replacement for CF3Br in aircraft applications
Authors: Li Y. , Patten K. O. , Wuebbles D. J. , Youn D.
Published: April 2010

Abstract. Iodotrifluoromethane (CF3I) has been considered to be a candidate replacement for bromotrifluoromethane (CF3Br), which is used in aircraft for fuel inerting and for fire fighting. In this study, the chemical effects of aircraft-released CF3I on atmospheric ozone were examined with the University of Illinois at Urbana-Champaign two-dimensional chemical-radiative-transport (UIUC 2-D CRT) model. Using an earlier estimate of the aircraft emission profile for tank inerting in military aircraft, the resulting equivalent Ozone Depletion Potentials (ODPs) for CF3I were in the range of 0.07 to 0.25. As a sensitivity study, we also analyzed CF3I emissions associated with fuel inerting if it were to occur at lower altitudes using an alternative estimate. The model calculations of resulting effects on ozone for this case gave ODPs≤0.05. Furthermore, through interactions with the National Institute of Standards and Technology (NIST), we analyzed the potential effects on ozone resulting from using CF3I in fire fighting connected with engine nacelle and auxiliary power unit applications. The scenarios evaluated using the NIST estimate suggested that the ODPs obtained by assuming aircraft flights occurring in several different latitude regions of the Northern Hemisphere are extremely low. According to the model calculation, the altitude where CF3I is released from aircraft is a dominant factor in its ozone depletion effects. On the assumption that the CF3I emission profile is representative of actual release characteristics, aircraft-released CF3I has much lower impacts on the ozone layer and can be a qualified substitute of CF3Br in engine nacelles.
Change in global aerosol composition since preindustrial times
Authors: Tsigaridis K. , Krol M. , Dentener F. J. , Balkanski Y. , Lathière J. , Metzger S. , Hauglustaine D. A. , Kanakidou M.
Published: April 2010

Abstract. To elucidate human induced changes of aerosol load and composition in the atmosphere, a coupled aerosol and gas-phase chemistry transport model of the troposphere and lower stratosphere has been used. This is the first 3-d modeling study that focuses on aerosol chemical composition change since preindustrial times considering the secondary organic aerosol formation together with all other main aerosol components including nitrate. In particular, we evaluate non-sea-salt sulfate (nss-SO4=), ammonium (NH4+), nitrate (NO3-), black carbon (BC), sea-salt, dust, primary and secondary organics (POA and SOA) with a focus on the importance of secondary organic aerosols. Our calculations show that the aerosol optical depth (AOD) has increased by about 21% since preindustrial times. This enhancement of AOD is attributed to a rise in the atmospheric load of BC, nss-SO4=, NO3-, POA and SOA by factors of 3.3, 2.6, 2.7, 2.3 and 1.2, respectively, whereas we assumed that the natural dust and sea-salt sources remained constant. The nowadays increase in carbonaceous aerosol loading is dampened by a 34–42% faster conversion of hydrophobic to hydrophilic carbonaceous aerosol leading to higher removal rates. These changes between the various aerosol components resulted in significant modifications of the aerosol chemical composition. The relative importance of the various aerosol components is critical for the aerosol climatic effect, since atmospheric aerosols behave differently when their chemical composition changes. According to this study, the aerosol composition changed significantly over the different continents and with height since preindustrial times. The presence of anthropogenically emitted primary particles in the atmosphere facilitates the condensation of the semi-volatile species that form SOA onto the aerosol phase, particularly in the boundary layer. The SOA burden that is dominated by the natural component has increased by 24% while its contribution to the AOD has increased by 11%. The increase in oxidant levels and preexisting aerosol mass since preindustrial times is the reason of the burden change, since emissions have not changed significantly. The computed aerosol composition changes translate into about 2.5 times more water associated with non sea-salt aerosol. Additionally, aerosols contain 2.7 times more inorganic components nowadays than during the preindustrial times. We find that the increase in emissions of inorganic aerosol precursors is much larger than the corresponding aerosol increase, reflecting a non-linear atmospheric response.
Probing ice clouds by broadband mid-infrared extinction spectroscopy: case studies from ice nucleation experiments in the AIDA aerosol and cloud chamber
Authors: Wagner R. , Benz S. , Möhler O. , Saathoff H. , Schurath U.
Published: April 2010

Abstract. Series of infrared extinction spectra of ice crystals were recorded in the 6000–800 cm-1 wavenumber regime during expansion cooling experiments in the large aerosol and cloud chamber AIDA of Forschungszentrum Karlsruhe. Either supercooled sulphuric acid solution droplets or dry mineral dust particles were added as seed aerosols to initiate ice formation after having established ice supersaturated conditions inside the chamber. The various ice nucleation runs were conducted at temperatures between 237 and 195 K, leading to median sizes of the nucleated ice particles of 1–15 µm. The measured infrared spectra were fitted with reference spectra from T-matrix calculations to retrieve the number concentration as well as the number size distribution of the generated ice clouds. The ice particles were modelled as finite circular cylinders with aspect ratios ranging from 0.5 to 3.0. Benefiting from the comprehensive diagnostic tools for the characterisation of ice clouds which are available at the AIDA facility, the infrared retrieval results with regard to the ice particle number concentration could be compared to independent measurements with various optical particle counters. This provided a unique chance to quantitatively assess potential errors or solution ambiguities in the retrieval procedure which mainly originate from the difficulty to find an appropriate shape representation for the aspherical particle habits of the ice crystals. Based on these inter-comparisons, we demonstrate that there is no standard retrieval approach which can be routinely applied to all different experimental scenarios. In particular, the concept to account for the asphericity of the ice crystals, the a priori constraints which might be imposed on the unknown number size distribution of the ice crystals (like employing an analytical distribution function), and the wavenumber range which is included in the fitting algorithm should be carefully adjusted to each single retrieval problem.
The influence of African air pollution on regional and global tropospheric chemistry
Authors: Aghedo A. M. , Schultz M. G. , Rast S.
Published: April 2010

Abstract. We investigate the relative importance of African biomass burning, biogenic volatile organic compounds (VOC), lightning and anthropogenic emissions to the tropospheric ozone budget over Africa and globally using a coupled global chemistry climate model. Our model studies indicate that the photochemical surface ozone concentration may rise by up to 50 ppbv in the burning region during the biomass burning seasons. Biogenic VOCs contribute between 5–20 ppbv to the near surface ozone concentration over the tropical African region. The impact of lightning on surface ozone is negligible, while anthropogenic emissions contribute a maximum of 10 ppbv to the surface ozone over Nigeria, South-Africa and Egypt. The annual average of the surface and column ozone over Africa shows that biomass burning is the single most important emission source affecting the African region, while biogenic emissions have the highest contribution during the rainy seasons. The contributions of African emissions to global tropospheric ozone burden (TOB) are about 9 Tg, 13 Tg, 8 Tg and 4 Tg for African biomass burning, biogenic VOC, lightning and anthropogenic emissions respectively. These correspond to 2.4%, 3.4%, 2.1% and 1% of the global tropospheric ozone budget respectively. Over Africa itself, the contribution of each of these emission types is only 2.4 Tg, 2.2 Tg, 1.4 Tg and 0.8 Tg respectively. Outside the continent, African biogenic VOC emissions yield the highest contribution to the TOB. Our model calculations suggest that about 70% of the tropospheric ozone produced from emissions in Africa is found outside the continent, thus exerting a noticeable influence on a large part of the tropical troposphere. Latin America experiences the highest impact of African emissions, followed by southeast and south-central Asia, Oceania, and the Middle East for all the emission categories; while Canada, the United States, Russia, Mongolia, China and Europe experience the least impact of African emissions.
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. While the convection is very sensitive to the heat flux from the fire, the emissions of water vapor play a less significant role. 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.