bluuebunny/crossref_metadata_2025 huggingface dataset:
Heterogeneous oxidation of saturated organic aerosols by hydroxyl radicals: Uptake kinetics and condensed-phase products
Authors: George I. J. , Vlasenko A. , Slowik J. G. , Abbatt J. P. D.
Published: April 2010

Abstract. The kinetics and reaction mechanism for the heterogeneous oxidation of saturated organic aerosols by gas-phase OH radicals were investigated under NOx-free conditions. The reaction of 150 nm diameter Bis(2-ethylhexyl) sebacate (BES) particles with OH was studied as a proxy for chemical aging of atmospheric aerosols containing saturated organic matter. An aerosol reactor flow tube combined with an Aerodyne time-of-flight aerosol mass spectrometer (ToF-AMS) and scanning mobility particle sizer (SMPS) was used to study this system. Hydroxyl radicals were produced by 254 nm photolysis of O3 in the presence of water vapour. The kinetics of the heterogeneous oxidation of the BES particles was studied by monitoring the loss of a mass fragment of BES with the ToF-AMS as a function of OH exposure. We measured an initial OH uptake coefficient of γ0 = 1.26 (±0.04), confirming that this reaction is highly efficient. The density of BES particles increased by up to 20% of the original BES particle density at the highest OH exposure studied, consistent with the particle becoming more oxidized. Electrospray ionization mass spectrometry analysis showed that the major particle-phase reaction products are multifunctional carbonyls and alcohols with higher molecular weights than the starting material. Volatilization of oxidation products accounted for a maximum of 17% decrease of the particle volume at the highest OH exposure studied. Tropospheric organic aerosols will become more oxidized from heterogeneous photochemical oxidation, which may affect not only their physical and chemical properties, but also their hygroscopicity and cloud nucleation activity.
An Asian emission inventory of anthropogenic emission sources for the period 1980–2020
Authors: Ohara T. , Akimoto H. , Kurokawa J. , Horii N. , Yamaji K. , Yan X. , Hayasaka T.
Published: April 2010

Abstract. We developed a new emission inventory for Asia (Regional Emission inventory in ASia (REAS) Version 1.1) for the period 1980–2020. REAS is the first inventory to integrate historical, present, and future emissions in Asia on the basis of a consistent methodology. We present here emissions in 2000, historical emissions for 1980–2003, and projected emissions for 2010 and 2020 of SO2, NOx, CO, NMVOC, black carbon (BC), and organic carbon (OC) from fuel combustion and industrial sources. Total energy consumption in Asia more than doubled between 1980 and 2003, causing a rapid growth in Asian emissions, by 28% for BC, 30% for OC, 64% for CO, 108% for NMVOC, 119% for SO2, and 176% for NOx. In particular, Chinese NOx emissions showed a marked increase of 280% over 1980 levels, and growth in emissions since 2000 has been extremely high. These increases in China were mainly caused by increases in coal combustion in the power plants and industrial sectors. NMVOC emissions also rapidly increased because of growth in the use of automobiles, solvents, and paints. By contrast, BC, OC, and CO emissions in China showed decreasing trends from 1996 to 2000 because of a reduction in the use of biofuels and coal in the domestic and industry sectors. However, since 2000, Chinese emissions of these species have begun to increase. Thus, the emissions of air pollutants in Asian countries (especially China) showed large temporal variations from 1980–2003. Future emissions in 2010 and 2020 in Asian countries were projected by emission scenarios and from emissions in 2000. For China, we developed three emission scenarios: PSC (policy success case), REF (reference case), and PFC (policy failure case). In the 2020 REF scenario, Asian total emissions of SO2, NOx, and NMVOC were projected to increase substantially by 22%, 44%, and 99%, respectively, over 2000 levels. The 2020 REF scenario showed a modest increase in CO (12%), a lesser increase in BC (1%), and a slight decrease in OC (–5%) compared with 2000 levels. However, it should be noted that Asian total emissions are strongly influenced by the emission scenarios for China.
The Tropical Forest and fire emissions experiment: overview and airborne fire emission factor measurements
Authors: Yokelson R. J. , Karl T. , Artaxo P. , Blake D. R. , Christian T. J. , Griffith D. W. T. , Guenther A. , Hao W. M.
Published: April 2010

Abstract. The Tropical Forest and Fire Emissions Experiment (TROFFEE) used laboratory measurements followed by airborne and ground based field campaigns during the 2004 Amazon dry season to quantify the emissions from pristine tropical forest and several plantations as well as the emissions, fuel consumption, and fire ecology of tropical deforestation fires. The airborne campaign used an Embraer 110B aircraft outfitted with whole air sampling in canisters, mass-calibrated nephelometry, ozone by uv absorbance, Fourier transform infrared spectroscopy (FTIR), and proton-transfer mass spectrometry (PTR-MS) to measure PM10, O3, CO2, CO, NO, NO2, HONO, HCN, NH3, OCS, DMS, CH4, and up to 48 non-methane organic compounds (NMOC). The Brazilian smoke/haze layers extended to 2–3 km altitude, which is much lower than the 5–6 km observed at the same latitude, time of year, and local time in Africa in 2000. Emission factors (EF) were computed for the 19 tropical deforestation fires sampled and they largely compare well to previous work. However, the TROFFEE EF are mostly based on a much larger number of samples than previously available and they also include results for significant emissions not previously reported such as: nitrous acid, acrylonitrile, pyrrole, methylvinylketone, methacrolein, crotonaldehyde, methylethylketone, methylpropanal, "acetol plus methylacetate," furaldehydes, dimethylsulfide, and C1-C4 alkyl nitrates. Thus, we recommend these EF for all tropical deforestation fires. The NMOC emissions were ~80% reactive, oxygenated volatile organic compounds (OVOC). Our EF for PM10 (17.8±4 g/kg) is ~25% higher than previously reported for tropical forest fires and may reflect a trend towards, and sampling of, larger fires than in earlier studies. A large fraction of the total burning for 2004 likely occurred during a two-week period of very low humidity. The combined output of these fires created a massive "mega-plume" >500 km across that we sampled on September 8. The mega-plume contained high PM10 and 10–50 ppbv of many reactive species such as O3, NH3, NO2, CH3OH, and organic acids. This is an intense and globally important chemical processing environment that is still poorly understood. The mega-plume or "white ocean" of smoke covered a large area in Brazil, Bolivia, and Paraguay for about one month. The smoke was transported >2000 km to the southeast while remaining concentrated enough to cause a 3-4-fold increase in aerosol loading in the São Paulo area for several days.
SAGE II measurements of stratospheric aerosol properties at non-volcanic levels
Authors: Thomason L. W. , Burton S. P. , Luo B.-P. , Peter T.
Published: April 2010

Abstract. Since 2000, stratospheric aerosol levels have been relatively stable and at the lowest levels observed in the historical record. Given the challenges of making satellite measurements of aerosol properties at these levels, we have performed a study of the sensitivity of the product to the major components of the processing algorithm used in the production of SAGE II aerosol extinction measurements and the retrieval process that produces the operational surface area density (SAD) product. We find that the aerosol extinction measurements, particularly at 1020 nm, remain robust and reliable at the observed aerosol levels. On the other hand, background periods, the SAD operational product has an uncertainty of at least a factor of 2 due to the lack of sensitivity to particles with radii less than 100 nm.
Observations of HNO3, ΣAN, ΣPN and NO2 fluxes: evidence for rapid HOx chemistry within a pine forest canopy
Authors: Farmer D. K. , Cohen R. C.
Published: April 2010

Abstract. Measurements of exchange of reactive nitrogen oxides between the atmosphere and a ponderosa pine forest in the Sierra Nevada Mountains are reported. During winter, we observe upward fluxes of NO2, and downward fluxes of total peroxy and peroxy acyl nitrates (ΣPNs), total gas and particle phase alkyl and multifunctional alkyl nitrates (ΣANs(g+p), and the sum of gaseous HNO3 and semi-volatile NO3− particles (HNO3(g+p). We use calculations of the vertical profile and flux of NO, partially constrained by observations, to show that net midday ΣNOyi fluxes in winter are –4.9 ppt m s−1. The signs and magnitudes of these wintertime individual and ΣNOyi fluxes are in the range of prior measurements. In contrast, during summer, we observe downward fluxes only of ΣANs(g+p), and upward fluxes of HNO3(g+p), ΣPNs and NO2 with signs and magnitudes that are unlike most, if not all, previous observations and analyses of fluxes of individual nitrogen oxides. The results imply that the mechanisms contributing to NOy fluxes, at least at this site, are much more complex than previously recognized. We show that the observations of upward fluxes of HNO3(g+p) and ΣPNs during summer are consistent with oxidation of NO2 and acetaldehyde by OH with the product of concentration and residence time equal to 1.1×1010 molec OH cm−3 s, e.g. 3×107 molecules cm−3 OH for a 400 s canopy residence time. We show that ΣAN(g+p) fluxes are consistent with this same OH if the reaction of OH with ΣANs produces either HNO3 or NO2 in 6–30% yield. Calculations of NO fluxes constrained by the NO2 observations and the inferred OH indicate that NOx fluxes are downward into the canopy because of the substantial conversion of NOx to HNO3 and ΣPNs in the canopy. Even so, we derive that NOx emission fluxes of ~15 ng(N) m−2 s−1 at midday during summer are required to balance the NOx and NOy flux budgets. These fluxes are partly explained by estimates of soil emissions (estimated to be between 3 and 6 ng(N) m−2 s−1). One possibility for the remainder of the NOx source is large HONO emissions. Alternatively, the 15 ng(N) m−2 s−1 emission estimate may be too large, and the budget balanced if the deposition of HNO3 and ΣPNs is slower than we estimate, if there are large errors in either our understanding of peroxy radical chemistry, or our assumptions that the budget is required to balance because the fluxes do not obey similarity theory.
The 1985 southern hemisphere mid-latitude total column ozone anomaly
Authors: Bodeker G. E. , Garny H. , Smale D. , Dameris M. , Deckert R.
Published: April 2010

Abstract. One of the most significant events in the evolution of the ozone layer over southern mid-latitudes since the late 1970s was the large decrease observed in 1985. This event remains unexplained and most state-of-the-art atmospheric chemistry-transport models are unable to reproduce it. In this study, the 1985 southern hemisphere mid-latitude total column ozone anomaly is analyzed in detail based on observed daily total column ozone fields, stratospheric dynamical fields, and calculated diagnostics of stratospheric mixing. The 1985 anomaly appears to result from a combination of (i) an anomaly in the meridional circulation resulting from the westerly phase of the equatorial quasi-biennial oscillation (QBO), (ii) weaker transport of ozone from its tropical mid-stratosphere source across the sub-tropical barrier to mid-latitudes related to the particular phasing of the QBO with respect to the annual cycle, and (iii) a solar cycle induced local reduction in ozone. The results based on observations are compared and contrasted with analyses of ozone and dynamical fields from the ECHAM4.L39(DLR)/CHEM coupled chemistry-climate model (hereafter referred to as E39C). Equatorial winds in the E39C model are nudged towards observed winds between 10° S and 10° N and the ability of this model to produce an ozone anomaly in 1985, similar to that observed, confirms the role of the QBO in the anomaly.
Two adaptive radiative transfer schemes for numerical weather prediction models
Authors: Venema V. , Schomburg A. , Ament F. , Simmer C.
Published: April 2010

Abstract. Radiative transfer calculations in atmospheric models are computationally expensive, even if based on simplifications such as the δ-two-stream approximation. In most weather prediction models these parameterisation schemes are therefore called infrequently, accepting additional model error due to the persistence assumption between calls. This paper presents two so-called adaptive parameterisation schemes for radiative transfer in a limited area model: a perturbation scheme that exploits temporal correlations and a local-search scheme that mainly takes advantage of spatial correlations. Utilising these correlations and with similar computational resources, the schemes are able to predict the surface heating rates more accurately than a scheme based on the persistence assumption. An important property of these adaptive schemes is that their accuracy does not decrease much in case of strong reductions in the number of calls to the δ-two-stream scheme. It is hypothesised that the core idea can also be employed in parameterisation schemes for other processes and in other dynamical models.
The direct effect of aerosols on solar radiation based on satellite observations, reanalysis datasets, and spectral aerosol optical properties from Global Aerosol Data Set (GADS)
Authors: Hatzianastassiou N. , Matsoukas C. , Drakakis E. , Stackhouse P. W. , Koepke P. , Fotiadi A. , Pavlakis K. G. , Vardavas I.
Published: April 2010

Abstract. A global estimate of the seasonal direct radiative effect (DRE) of natural plus anthropogenic aerosols on solar radiation under all-sky conditions is obtained by combining satellite measurements and reanalysis data with a spectral radiative transfer model. The estimates are obtained with detailed spectral model computations separating the ultraviolet (UV), visible and near-infrared wavelengths. The global distribution of spectral aerosol optical properties was taken from the Global Aerosol Data Set (GADS) whereas data for clouds, water vapour, ozone, carbon dioxide, methane and surface albedo were taken from various satellite and reanalysis datasets. Using these aerosol properties and other related variables, we generate climatological (for the 12-year period 1984–1995) monthly mean aerosol DREs. The global annual mean DRE on the outgoing SW radiation at the top of atmosphere (TOA, ΔFTOA) is 1.62 Wm−2 (with a range of –10 to 15 Wm−2, positive values corresponding to planetary cooling), the effect on the atmospheric absorption of SW radiation (ΔFatmab) is 1.6 Wm−2 (values up to 35 Wm−2, corresponding to atmospheric warming), and the effect on the surface downward and absorbed SW radiation (Δ Fsurf, and ΔFsurfnet, respectively) is –3.93 and –3.22 Wm−2 (values up to –45 and –35 Wm−2, respectively, corresponding to surface cooling.) According to our results, aerosols decrease/increase the planetary albedo by –3 to 13% at the local scale, whereas on planetary scale the result is an increase of 1.5%. Aerosols can warm locally the atmosphere by up to 0.98 K day−1, whereas they can cool the Earth's surface by up to –2.9 K day−1. Both these effects, which can significantly modify atmospheric dynamics and the hydrological cycle, can produce significant planetary cooling on a regional scale, although planetary warming can arise over highly reflecting surfaces. The aerosol DRE at the Earth's surface compared to TOA can be up to 15 times larger at the local scale. The largest aerosol DRE takes place in the northern hemisphere both at the surface and the atmosphere, arising mainly at ultraviolet and visible wavelengths.
The role of VOC oxidation products in continental new particle formation
Authors: Laaksonen A. , Kulmala M. , O'Dowd C. D. , Joutsensaari J. , Vaattovaara P. , Mikkonen S. , Lehtinen K. E. J. , Sogacheva L. , Dal Maso M. , Aalto P. , Petäjä T. , Sogachev A. , Jun Yoon Y. , Lihavainen H. , Nilsson D. , Cristina Facchini M. , Cavalli F. , Fuzzi S. , Hoffmann T. , Arnold F. , Hanke M. , Sellegri K. , Umann B. , Junkermann W. , Coe H. , Allan J. D. , Rami Alfarra M. , Worsnop D. R. , Riekkola M.-L. , Hyötyläinen T. , Viisanen Y.
Published: April 2010

Abstract. Aerosol physical and chemical properties and trace gas concentrations were measured during the QUEST field campaign in March–April, 2003, in Hyytiälä, Finland. Our aim was to understand the role of oxidation products of VOC's such as mono- and sesquiterpenes in atmospheric nucleation events. Particle chemical compositions were measured using the Aerodyne Aerosol Mass Spectrometer, and chemical compositions of aerosol samples collected with low-pressure impactors and a high volume sampler were analysed using a number of techniques. The results indicate that during and after new particle formation, all particles larger than 50 nm in diameter contained similar organic substances that are likely to be mono- and sesquiterpene oxidation products. The oxidation products identified in the high volume samples were shown to be mostly aldehydes. In order to study the composition of particles in the 10–50 nm range, we made use of Tandem Differential Mobility Analyzer results. We found that during nucleation events, both 10 and 50 nm particle growth factors due to uptake of ethanol vapour correlate strongly with gas-phase monoterpene oxidation product (MTOP) concentrations, indicating that the organic constituents of particles smaller than 50 nm in diameter are at least partly similar to those of larger particles. We furthermore showed that particle growth rates during the nucleation events are correlated with the gas-phase MTOP concentrations. This indicates that VOC oxidation products may have a key role in determining the spatial and temporal features of the nucleation events. This conclusion was supported by our aircraft measurements of new 3–10 nm particle concentrations, which showed that the nucleation event on 28 March 2003, started at the ground layer, i.e. near the VOC source, and evolved together with the mixed layer. Furthermore, no new particle formation was detected upwind away from the forest, above the frozen Gulf of Bothnia.
ACE-FTS observation of a young biomass burning plume: first reported measurements of C2H4, C3H6O, H2CO and PAN by infrared occultation from space
Authors: Coheur P.-F. , Herbin H. , Clerbaux C. , Hurtmans D. , Wespes C. , Carleer M. , Turquety S. , Rinsland C. P. , Remedios J. , Hauglustaine D. , Boone C. D. , Bernath P. F.
Published: April 2010

Abstract. In the course of our study of the upper tropospheric composition with the infrared Atmospheric Chemistry Experiment – Fourier Transform Spectrometer (ACE–FTS), we found an occultation sequence that on 8 October 2005, sampled a remarkable plume near the east coast of Tanzania. Model simulations of the CO distribution in the Southern hemisphere are performed for this period and they demonstrate that the emissions for this event originated from a nearby forest fire, after which the plume was transported from the source region to the upper troposphere. Taking advantage of the very high signal-to-noise ratio of the ACE–FTS spectra over a wide wavenumber range (750–4400 cm−1), we present in-depth analyses of the chemical composition of this plume in the middle and upper troposphere, focusing on the measurements of weakly absorbing pollutants. For this specific biomass burning event, we report simultaneous observations of an unprecedented number of organic species. Measurements of C2H4 (ethene), C3H4 (propyne), H2CO (formaldehyde), C3H6O (acetone) and CH3COO2NO2 (peroxyacetylnitrate, abbreviated as PAN) are the first reported detections using infrared occultation spectroscopy from satellites. Based on the lifetime of the emitted species, we discuss the photochemical age of the plume and also report, whenever possible, the enhancement ratios relative to CO.
Characterization of Polar Stratospheric Clouds with Space-Borne Lidar: CALIPSO and the 2006 Antarctic Season
Authors: Pitts M. C. , Thomason L. W. , Poole L. R. , Winker D. M.
Published: April 2010

Abstract. The role of polar stratospheric clouds in polar ozone loss has been well documented. The CALIPSO satellite mission offers a new opportunity to characterize PSCs on spatial and temporal scales previously impossible. A PSC detection algorithm based on a single wavelength threshold approach has been developed for CALIPSO. The method appears to accurately detect PSCs of all opacities, including tenuous clouds, with a very low rate of false positives and few missed clouds. We applied the algorithm to CALIOP data acquired during the 2006 Antarctic winter season from 13 June through 31 October. The spatial and temporal distribution of CALIPSO PSC observations is illustrated with weekly maps of PSC occurrence. The evolution of the 2006 PSC season is depicted by time series of daily PSC frequency as a function of altitude. Comparisons with "virtual" solar occultation data indicate that CALIPSO provides a different view of the PSC season than attained with previous solar occultation satellites. Measurement-based time series of PSC areal coverage and vertically-integrated PSC volume are computed from the CALIOP data. The observed area covered with PSCs is significantly smaller than would be inferred from the commonly used temperature-based proxy TNAT but is similar in magnitude to that inferred from TSTS . The potential of CALIOP measurements for investigating PSC composition is illustrated using combinations of lidar backscatter and volume depolarization for two CALIPSO PSC scenes.
Development and evaluation of an operational SDS forecasting system for East Asia: CUACE/DUST
Authors: Zhou C. H. , Gong S. L. , Zhang X. Y. , Wang Y. Q. , Niu T. , Liu H. L. , Zhao T. L. , Yang Y. Q. , Hou Q.
Published: April 2010

Abstract. CUACE/Dust, an operational sand and dust storm (SDS) forecasting system for East Asia, was developed at CMA (China Meteorological Administration) by integrating a meso-scale dust aerosol model with a 3DVar data assimilation system that uses both surface network observation data and dust intensity data retrieved from the Chinese Geostationary Satellite FY-2C. For spring 2006, CUACE/Dust successfully forecasted most of the 31 SDS episodes in East Asia. A detailed comparison of the modeling predictions for the 8–12 March episode with surface network observations and lidar measurements revealed a robust forecasting ability of the system. The time series of the forecasted dust concentrations for a number of representative stations for the whole spring 2006 were also evaluated against surface PM10 monitoring data, showing a very good agreement in terms of the SDS timing and magnitudes near source regions where dust aerosols dominate. For the entire domain forecasts in spring 2006 (1 March–31 May), a TS (thread score) system evaluated the performance of the system against all available observations and rendered an averaged TS value of 0.31 for 24 h forecasts, 0.23 for 48 h and 0.21 for 72 h forecasts.
Cloud-scale model intercomparison of chemical constituent transport in deep convection
Authors: Barth M. C. , Kim S.-W. , Wang C. , Pickering K. E. , Ott L. E. , Stenchikov G. , Leriche M. , Cautenet S. , Pinty J.-P. , Barthe Ch. , Mari C. , Helsdon J. , Farley R. , Fridlind A. M. , Ackerman A. S. , Spiridonov V. , Telenta B.
Published: April 2010

Abstract. Transport and scavenging of chemical constituents in deep convection is important to understanding the composition of the troposphere and therefore chemistry-climate and air quality issues. High resolution cloud chemistry models have been shown to represent convective processing of trace gases quite well. To improve the representation of sub-grid convective transport and wet deposition in large-scale models, general characteristics, such as species mass flux, from the high resolution cloud chemistry models can be used. However, it is important to understand how these models behave when simulating the same storm. The intercomparison described here examines transport of six species. CO and O3, which are primarily transported, show good agreement among models and compare well with observations. Models that included lightning production of NOx reasonably predict NOx mixing ratios in the anvil compared with observations, but the NOx variability is much larger than that seen for CO and O3. Predicted anvil mixing ratios of the soluble species, HNO3, H2O2, and CH2O, exhibit significant differences among models, attributed to different schemes in these models of cloud processing including the role of the ice phase, the impact of cloud-modified photolysis rates on the chemistry, and the representation of the species chemical reactivity. The lack of measurements of these species in the convective outflow region does not allow us to evaluate the model results with observations.
The influence of cloud top variability from radar measurements on 3-D radiative transfer
Authors: Richter F. , Barfus K. , Berger F. H. , Görsdorf U.
Published: April 2010

Abstract. In radiative transfer simulations the simplification of cloud top structure by homogenous assumptions can breed to mistakes in comparison to realistic heterogeneous cloud top structures. This paper examines the influence of cloud top heterogeneity on the radiation at the top of the atmosphere. The use of cloud top measurements with a high temporal resolution allows to analyse small spatial cloud top heterogeneities by using the frozen turbulence assumption for the time – space conversion. Radiative observations are often based on satellite measurements, whereas small spatial structures are not considered in such treatments. A spectral analysis of the cloud top measurements showed slopes of power spectra between –1.8 and –2.0, this values are larger then the spectra of –5/3 which is often applied to generate cloud field variability. The comparison of 3-D radiative transfer results from cloud fields with homogenous and heterogeneous tops have been done for a single wavelength of 0.6 μm. The radiative transfer calculations result in lower albedos for heterogeneous cloud tops. The differences of albedos between heterogeneous and homogeneous cloud top decrease with increasing solar zenith angle. The influence of cloud top variability on radiances is shown. Explicitly in forward direction the reflectances for heterogeneous tops are larger, in backward direction lower. The largest difference of the mean reflectances (mean over cloud field) between homogeneous and heterogeneous cloud top is approximately 0.3, which is 30% of illumination.
The effect of H2O adsorption on cloud-drop activation of insoluble particles: a theoretical framework
Authors: Sorjamaa R. , Laaksonen A.
Published: April 2010

Abstract. Cloud droplet activation of wettable insoluble compounds has been studied theoretically by assuming droplet growth to happen through multilayer adsorption. The idea is to include an adsorption isotherm in Köhler theory instead of the solute term. This makes it possible to describe the equilibrium growth of insoluble particles and to find out their critical saturation ratios. The critical saturation ratios calculated in this way are comparable to those of completely soluble particles at certain ranges of adsorption isotherm parameter values. The results indicate that adsorption could cause wettable insoluble compounds to activate in atmospheric conditions. However, more data on the adsorption parameters for wettable organic substances is needed to confirm this conclusion.
Data assimilation of dust aerosol observations for CUACE/Dust forecasting system
Authors: Niu T. , Gong S. L. , Zhu G. F. , Liu H. L. , Hu X. Q. , Zhou C. H. , Wang Y. Q.
Published: April 2010

Abstract. A data assimilation system (DAS) was developed for the Chinese Unified Atmospheric Chemistry Environment – Dust (CUACE/Dust) forecast system and applied in the operational forecasts of sand and dust storm (SDS) in spring 2006. The system is based on a three dimensional variational method (3D-Var) and uses extensively the measurements of surface visibility and dust loading retrieval from the Chinese geostationary satellite FY-2C. The results show that a major improvement to the capability of CUACE/Dust in forecasting the short-term variability in the spatial distribution and intensity of dust concentrations has been achieved, especially in those areas far from the source regions. The seasonal mean Threat Score (TS) over the East Asia in spring 2006 increased from 0.22 to 0.31 by using the data assimilation system, a 41% enhancement. The assimilation results usually agree with the dust loading retrieved from FY-2C and visibility distribution from surface meteorological stations, which indicates that the 3D-Var method is very powerful for the unification of observation and numerical modeling results.
Long-time global radiation for Central Europe derived from ISCCP Dx data
Authors: Petrenz N. , Sommer M. , Berger F. H.
Published: April 2010

Abstract. The global Dx dataset of the "International Satellite Cloud Climatology Project" (ISCCP) with a spatial resolution of about 30×30 km2 was analysed to produce spatially highly resolved long-time datasets to describe the radiation budget for Central Europe over the period of 1984–2000. The computation of shortwave and longwave radiant flux densities at top of atmosphere and at surface was based on 1-D radiative transfer simulations. The simulations were carried out for all relevant atmospheric and surface conditions and the results were inserted into a look-up table. Thus, long-time calculations for all conditions and time slices of the Dx dataset could be realised. The study is focussed on the global radiation at surface. The first examination was carried out for the ISCCP D1 and the ISCCP D2 dataset. These datasets, including cloud and surface information on a different spatial scale (280×280 km2), were applied to the produced look-up table analogue to the Dx data. The calculated global radiation of the D1 and D2 dataset were compared to the Dx dataset. The differences between these datasets mainly range from 5–15 W m−2 (2–6%) with regional peaks up to 25 W m−2 (10%). The evaluation with the GEWEX "Surface Radiation Budget" (SRB) data emphasises differ-ences between 5–25 W m−2 (6–16%) over land areas. Deviations to an ISCCP provided flux data set vary from 0 W m−2 in the North up to 35 W m−2 (0–13%) in the South of Central Europe. The global radiation datasets provided by the "Global Energy Balance Archive" (GEBA) and the "German Meteorological Service" (DWD) agree well, but they are 5–25 W m−2 (7–10%) lower than the Dx results. Annual analyses of global radiation of various regional climate models complete the study. It is figured out that the used models and methods reveal a couple of discrepancies. Especially in wintertime the results of our analysis differ to the considered models. Principally the uncer-tainties were caused by the determined range of values and simplifications for the computation of the radiative transfer simulation.
A new comprehensive approach to characterizing carbonaceous aerosol with an application to wintertime Fresno, California PM2.5
Authors: Herckes P. , Leenheer J. A. , Collett J. L.
Published: April 2010

Abstract. Fine particulate matter (PM2.5) samples were collected during a three week winter period in Fresno (CA). A composite sample was characterized by isolating several distinct fractions and characterizing them by infrared and nuclear magnetic resonance (NMR) spectroscopy. More than 80% of the organic matter in the aerosol samples was recovered and characterized. Only 35% of the organic matter was water soluble with another third soluble in dichloromethane and the remainder insoluble. Within the isolated water soluble material, hydrophobic acid and hydrophilic acids plus neutrals fractions contained the largest amounts of carbon. The hydrophobic acids fraction appears to contain significant amounts of lignin type structures, spectra of the hydrophilic acids plus neutrals fraction are indicative of carbohydrates and secondary organic material. The dichloromethane soluble fraction contains a variety of organic compound families typical of many previous studies of organic aerosol speciation, including alkanes, alkanols, alkanals and alkanoic acids. Finally the water and solvent insoluble fraction exhibits a strong aromaticity as one would expect from black or elemental carbon like material; however, these spectra also show a substantial amount of aliphaticity consistent with linear side chains on the aromatic structures.
Quality assessment of water cycle parameters in REMO by Radar-Lidar synergy
Authors: Hennemuth B. , Weiss A. , Bösenberg J. , Jacob D. , Linné H. , Peters G. , Pfeifer S.
Published: April 2010

Abstract. A comparison study of water cycle parameters derived from ground-based remote-sensing instruments and from the regional model REMO is presented. Observational data sets were collected during three measuring campaigns in summer/autumn 2003 and 2004 at Richard Aßmann Observatory, Lindenberg, Germany. The remote sensing instruments which were used are differential absorption lidar, Doppler lidar, ceilometer, cloud radar, and micro rain radar for the derivation of humidity profiles, ABL height, water vapour flux profiles, cloud parameters, and rain rate. Additionally, surface latent and sensible heat flux and soil moisture were measured. Error ranges and representativity of the data are discussed. For comparisons the regional model REMO was run for all measuring periods with a horizontal resolution of 18 km and 33 vertical levels. Parameter output was every hour. The measured data were transformed to the vertical model grid and averaged in time in order to better fit with gridbox model values. The comparisons show that the atmospheric boundary layer is not adequately simulated, on most days it is too shallow and too moist. This is found to be caused by a wrong partitioning of energy at the surface, particularly a too large latent heat flux. The reason is obviously an overestimation of soil moisture during drying periods by the one-layer scheme in the model. The profiles of water vapour transport within the ABL appear to be realistically simulated. The comparison of cloud cover reveals an underestimation of low-level and mid-level clouds by the model, whereas the comparison of high-level clouds is hampered by the inability of the cloud radar to see cirrus clouds above 10 km. Simulated ABL clouds apparently have a too low cloud base, and the vertical extent is underestimated. The ice water content of clouds agree in model and observation whereas the liquid water content is unsufficiently derived from cloud radar reflectivity in the present study. Rain rates are similar, but the representativeness of both observations and grid box values is low.
Reformulating atmospheric aerosol thermodynamics and hygroscopic growth into haze and clouds
Authors: Metzger S. , Lelieveld J.
Published: April 2010

Abstract. Modeling atmospheric aerosol and cloud microphysics is rather complex, even if chemical and thermodynamical equilibrium is assumed. We show, however, that the thermodynamics can be considerably simplified by reformulating equilibrium to include water, and transform laboratory-based concepts to atmospheric conditions. We generalize the thermodynamic principles that explain hydration and osmosis – merely based on solute solubilities. In chemical and thermodynamical equilibrium the relative humidity (RH) determines the saturation molality, including solute and solvent activities (and activity coefficients), since the water content is fixed by RH for a given aerosol concentration and type. As a consequence, gas/liquid/solid aerosol equilibrium partitioning can be solved analytically and non-iteratively. Our new concept enables an efficient and accurate calculation of the aerosol water mass and to directly link the aerosol hygroscopic growth to haze and cloud formation. We apply our new concept in the 3rd Equilibrium Simplified Aerosol Model (EQSAM3). Its input is limited to the species' solubilities from which a newly introduced stoichiometric coefficient for water is derived. Analogously, we introduce effective stochiometric coefficients for the solutes to account for complete or incomplete dissociation. We show that these coefficients can be assumed constant over the entire activity range and calculated for various inorganic, organic and non-electrolyte compounds, including alcohols, sugars and dissolved gases. EQSAM3 calculates the aerosol composition and gas/liquid/solid partitioning of mixed inorganic/organic multicomponent solutions and the associated water uptake for almost 100 major compounds. It explicitly accounts for particle hygroscopic growth by computing aerosol properties such as single solute molalities, molal based activities, including activity coefficients for volatile compounds, and deliquescence relative humidities of mixed solutes. Various applications and a model inter-comparison indicate that a) the application is not limited to dilute binary solutions, b) sensitive aerosol properties such as the pH of binary and mixed inorganic/organic salt solutions up to saturation can be computed accurately, and c) aerosol associated water is important for atmospheric chemistry, visibility, weather and climate.
MIPAS: an instrument for atmospheric and climate research
Authors: Fischer H. , Birk M. , Blom C. , Carli B. , Carlotti M. , von Clarmann T. , Delbouille L. , Dudhia A. , Ehhalt D. , Endemann M. , Flaud J. M. , Gessner R. , Kleinert A. , Koopmann R. , Langen J. , López-Puertas M. , Mosner P. , Nett H. , Oelhaf H. , Perron G. , Remedios J. , Ridolfi M. , Stiller G. , Zander R.
Published: April 2010

Abstract. MIPAS, the Michelson Interferometer for Passive Atmospheric Sounding, is a mid-infrared emission spectrometer which is part of the core payload of ENVISAT. It is a limb sounder, i.e. it scans across the horizon detecting atmospheric spectral radiances which are inverted to vertical temperature, trace species and cloud distributions. These data can be used for scientific investigations in various research fields including dynamics and chemistry in the altitude region between upper troposphere and lower thermosphere. The instrument is a well calibrated and characterized Fourier transform spectrometer which is able to detect many trace constituents simultaneously. The different concepts of retrieval methods are described including multi-target and two-dimensional retrievals. Operationally generated data sets consist of temperature, H2O, O3, CH4, N2O, HNO3, and NO2 profiles. Measurement errors are investigated in detail and random and systematic errors are specified. The results are validated by independent instrumentation which has been operated at ground stations or aboard balloon gondolas and aircraft. Intercomparisons of MIPAS measurements with other satellite data have been carried out, too. As a result, it has been proven that the MIPAS data are of good quality. MIPAS can be operated in different measurement modes in order to optimize the scientific output. Due to the wealth of information in the MIPAS spectra, many scientific results have already been published. They include intercomparisons of temperature distributions with ECMWF data, the derivation of the whole NOy family, the study of atmospheric processes during the Antarctic vortex split in September 2002, the determination of properties of Polar Stratospheric Clouds, the downward transport of NOx in the middle atmosphere, the stratosphere-troposphere exchange, the influence of solar variability on the middle atmosphere, and the observation of Non-LTE effects in the mesosphere.
Precision validation of MIPAS-Envisat products
Authors: Piccolo C. , Dudhia A.
Published: April 2010

Abstract. This paper discusses the variation and validation of the precision, or estimated random error, associated with the ESA Level 2 products from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). This quantity represents the propagation of the radiometric noise from the spectra through the retrieval process into the Level 2 profile values. The noise itself varies with time, steadily rising between decontamination events, but the Level 2 precision has a greater variation due to the atmospheric temperature which controls the total radiance received. Hence, for all species, the precision varies latitudinally/seasonally with temperature, with a small superimposed temporal structure determined by the degree of ice contamination on the detectors. The precision validation involves comparing two MIPAS retrievals at the intersections of ascending/descending orbits. For 5 days per month of full resolution MIPAS operation, the standard deviation of the matching profile pairs is computed and compared with the precision given in the MIPAS Level 2 data. Even taking into account the propagation of the pressure-temperature retrieval errors into the VMR retrieval, the standard deviation of the matching pairs is usually a factor 1–2 larger than the precision. This is thought to be due to effects such as horizontal inhomogeneity of the atmosphere and instability of the retrieval.
Surface observation of sand and dust storm in East Asia and its application in CUACE/Dust
Authors: Wang Y. Q. , Zhang X. Y. , Gong S. L. , Zhou C. H. , Hu X. Q. , Liu H. L. , Niu T. , Yang Y. Q.
Published: April 2010

Abstract. The spatial-temporal distributions and sources of sand and dust storm (SDS) in East Asia from 2001 to 2006 were investigated on the basis of visibility and PM10 data from the routine SDS and weather monitoring networks run by CMA (China Meteorological Administration). A power functional relationships between PM10 and visibility was found among various regions generally with a good correlation (r2=0.90), especially in Asian SDS source regions. In addition, three SDS occurrence centers, i.e. western China, Mongolia and northern China, were identified with the Mongolia source contributing more dust to the downwind areas including Korea and Japan than other two sources. Generally, high PM10 concentrations were observed in most areas of northern China. The highest value was obtained in the center of western China with a spring daily mean value of 876 μg m−3, and the value in other source regions exceeds 200 μg m−3. These data sets together with the satellite observations in China form the main observation database for the evaluation and data assimilation of CUACE/Dust system – an operational SDS forecasting system for East Asia.
On the vertical distribution of boundary layer halogens over coastal Antarctica: implications for O3, HOx, NOxand the Hg lifetime
Authors: Saiz-Lopez A. , Plane J. M. C. , Mahajan A. S. , Anderson P. S. , Bauguitte S. J.-B. , Jones A. E. , Roscoe H. K. , Salmon R. A. , Bloss W. J. , Lee J. D. , Heard D. E.
Published: April 2010

Abstract. A one-dimensional chemical transport model has been developed to investigate the vertical gradients of bromine and iodine compounds in the Antarctic coastal boundary layer. The model has been applied to interpret recent year-round observations of iodine and bromine monoxides (IO and BrO) at Halley Station, Antarctica. The model requires an equivalent I atom flux of ~109 molecule cm−2 s−1 from the snowpack in order to account for the measured IO levels, which are up to 20 ppt during spring. Using the current knowledge of gas-phase iodine chemistry, the model predicts significant gradients in the vertical distribution of iodine species. However, recent ground-based and satellite observations of IO imply that the radical is well-mixed in the boundary layer, indicating a longer than expected atmospheric lifetime for the radical. This can be modelled by including photolysis of the higher iodine oxides (I2O2, I2O3, I2O4 and I2O5), and rapid recycling of HOI and INO3 through sea-salt aerosol. The model also predicts significant concentrations (up to 25 ppt) of I2O5 in the lowest 10 m of the boundary layer, which could lead to the formation of ultrafine iodine oxide aerosols. Heterogeneous chemistry involving sea-salt aerosol is also necessary to account for the vertical profile of BrO. Iodine chemistry causes a large increase (typically more than 3-fold) in the rate of O3 depletion in the BL, compared with bromine chemistry alone. Rapid entrainment of O3 from the free troposphere is required to account for the observation that on occasion there is little O3 depletion at the surface in the presence of high concentrations of IO and BrO. The halogens also cause significant changes to the vertical profiles of HO and HO2 and the NO2/NO ratio. The average Hg0 lifetime against oxidation is also predicted to be about 10 h during springtime. Overall, our results show that halogens profoundly influence the oxidizing capacity of the Antarctic troposphere.
Global model simulations of the impact of ocean-going ships on aerosols, clouds, and the radiation budget
Authors: Lauer A. , Eyring V. , Hendricks J. , Jöckel P. , Lohmann U.
Published: April 2010

Abstract. International shipping contributes significantly to the fuel consumption of all transport related activities. Specific emissions of pollutants such as sulfur dioxide (SO2) per kg of fuel emitted are higher than for road transport or aviation. Besides gaseous pollutants, ships also emit various types of particulate matter. The aerosol impacts the Earth's radiation budget directly by scattering and absorbing incoming solar radiation and indirectly by changing cloud properties. Here we use ECHAM5/MESSy1-MADE, a global climate model with detailed aerosol and cloud microphysics, to show that emissions from ships significantly increase the cloud droplet number concentration of low maritime water clouds. Whereas the cloud liquid water content remains nearly unchanged in these simulations, effective radii of cloud droplets decrease, leading to cloud optical thickness increase up to 5–10%. The sensitivity of the results is estimated by using three different emission inventories for present day conditions. The sensitivity analysis reveals that shipping contributes with 2.3% to 3.6% to the total sulfate burden and 0.4% to 1.4% to the total black carbon burden in the year 2000. In addition to changes in aerosol chemical composition, shipping increases the aerosol number concentration, e.g. up to 25% in the size range of the accumulation mode (typically >0.1 μm) over the Atlantic. The total aerosol optical thickness over the Indian Ocean, the Gulf of Mexico and the Northeastern Pacific increases up to 8–10% depending on the emission inventory. Changes in aerosol optical thickness caused by the shipping induced modification of aerosol particle number concentration and chemical composition lead to a change of the net top of the atmosphere (ToA) clear sky radiation of about −0.013 W/m2 to −0.036 W/m2 on global annual average. The estimated all-sky direct aerosol effect calculated from these changes ranges between −0.009 W/m2 and −0.014 W/m2. The indirect aerosol effect of ships on climate is found to be far larger than previously estimated. An indirect radiative effect of −0.19 W/m2 to −0.6 W/m2 (change of the top of the atmosphere shortwave radiative flux) is calculated here, contributing 17% to 39% to the total indirect effect of anthropogenic aerosols. This contribution is high because ship emissions are released in regions with frequent low marine clouds in an otherwise clean environment. In addition, the potential impact of particulate matter on the radiation budget is larger over the dark ocean surface than over polluted regions over land.