bluuebunny/crossref_metadata_2025 huggingface dataset:
Injection in the lower stratosphere of biomass fire emissions followed by long-range transport: a MOZAIC case study
Authors: Cammas J.-P. , Brioude J. , Chaboureau J.-P. , Duron J. , Mari C. , Mascart P. , Nédélec P. , Smit H. , Pätz H.-W. , Volz-Thomas A. , Stohl A. , Fromm M.
Published: April 2010

Abstract. This paper analyses a stratospheric injection by deep convection of biomass fire emissions over North America (Alaska, Yukon and Northwest Territories) on 24 June 2004 and its long-range transport over the eastern coast of the United States and the eastern Atlantic. The case study is done using MOZAIC observations of ozone, carbon monoxide, nitrogen oxides (NOx+PAN) and water vapour during the crossing of the southernmost tip of an upper level trough over the Eastern Atlantic on 30 June 03:00 UTC and 10:00 UTC and in a vertical profile over Washington DC on 30 June 17:00 UTC, and by lidar observations of aerosol backscattering at Madison (University of Wisconsin) on 28 June. Attribution of the plumes to the boreal fires is achieved by backward simulations with a Lagrangian particle dispersion model (FLEXPART). A simulation with the Meso-NH model for the source region shows that a boundary layer tracer, mimicking the boreal forest fire smoke, is lofted into the lowermost stratosphere (2–5 pvu layer) during the diurnal convective cycle. The isentropic levels (above 335 K) correspond to those of the downstream MOZAIC observations. The parameterized convective detrainment flux is intense enough to fill the volume of a model mesh (20 km horizontal, 500 m vertical) above the tropopause with pure boundary layer air in a time period compatible with the convective diurnal cycle, i.e. about 5 h. The maximum instantaneous detrainment fluxes deposited about 15–20% of the initial boundary layer tracer concentration at 335 K, which according to the 275-ppbv carbon monoxide maximum mixing ratio observed by MOZAIC over eastern Atlantic, would be associated with a 1.4–1.8 ppmv carbon monoxide mixing ratio in the boundary layer over the source region.
Measurements of UV radiation on rotating vertical plane at the ALOMAR Observatory (69° N, 16° E), Norway, June 2007
Authors: Sobolewski P. , Krzyścin J. W. , Jarosławski J. , Stebel K.
Published: April 2010

Abstract. Erythemaly weighted UV and total UVA irradiance measured at the ALOMAR (Arctic Lidar Observatory for Middle Atmosphere Research; 69° N, 16° E) in June 2007 by two Kipp & Zonen UV broadband meters type, UV-S-AE-T, are examined. One unit is movable and mounted to rotating vertical plane, and the other is permanently fixed horizontally. The UV broadband meters measure simultaneously to allow the comparison of UV irradiances on vertical and horizontal plane. The entire range of relative exposure variations during clear-sky conditions over ALOMAR is examined using STAR and Radonic1 model (developed at the Meteorological Institute, Munich) for various action spectra (erythema, UVA, and vitamin D3). It seems that multiplication of the daily mean dose from a standard broadband meter placed horizontally by 0.5 gives reasonable estimation of the daily mean exposure on a vertical plane randomly oriented towards Sun. The extreme value and daily variability of relative exposure are the highest for UVA, next for UVB, then for vitamin D3 weighed UV irradiance. The minima of relative exposure (~0.20–0.30) are almost the same for all weighting functions. Specific cloud configuration could lead to significant enhancement of UV relative exposure of rotating plane being the most pronounced when biometer is in shadow. A statistical model is proposed, that it is able to simulate vitamin D3 weighted UV irradiances on vertical surface using explanatory variables: erythemal and total UVA irradiance from standard (horizontal) observations by Kipp & Zonen dual band biometer, the orientation of vertical plane, solar zenith angle, and column amount of total ozone. Statistical model will allow to reconstruct (or monitor) vitamin D3 weighted UV irradiances using available past (or actual) data.
The impact of weather and atmospheric circulation on O3 and PM10 levels at a mid-latitude site
Authors: Demuzere M. , Trigo R. M. , Vila-Guerau de Arellano J. , van Lipzig N. P. M.
Published: April 2010

Abstract. In spite of the strict EU regulations, concentrations of surface ozone and PM10 often exceed the pollution standards for The Netherlands and Europe. Their concentrations are controlled by (precursor) emissions, social and economic developments and a complex combination of meteorological actors. This study tackles the latter, and provides insight in the meteorological processes that play a role in O3 and PM10 levels in Cabauw (The Netherlands). The relations between meteorological actors and air quality are studied on a~local scale based on observations from Cabauw and are determined by a comprehensive correlation analysis and a multiple regression (MLR) analysis in 2 modes, with and without air quality variables as predictors. Furthermore, the objective Lamb Weather Type (WT) approach based on ECMWF (European Center for Medium-range Weather Forecasting) operational data is used to assess the influence of the large-scale circulation on air quality. Keeping in mind its future use in downscaling future climate scenarios for air quality purposes, special emphasis is given to an appropriate selection of the regressor variables readily available from operational meteorological forecasts or OAGCMs (Ocean-Atmosphere coupled General Circulation Models). The regression models perform satisfactory for both O3 and PM10, with an increased performance when including previous days air quality information. The lamb weather types show a seasonal distinct pattern for high (low) episodes of average O3 and PM10 concentrations, and these are clear related with the meteorology-air quality correlation analysis. Although using a circulation type approach can bring some interesting physical relations forward, our analysis reveals the circulation method is limited in terms of short-term air quality forecast for both O3 and PM10. In summary, it is concluded that the use of a regression model is more promising for short-term downscaling from climate scenarios than the use of a weather type classification approach.
Energetic particle precipitation in ECHAM5/MESSy1 – Part 1: Downward transport of upper atmospheric NOx produced by low energy electrons
Authors: Baumgaertner A. J. G. , Jöckel P. , Brühl C.
Published: April 2010

Abstract. The atmospheric chemistry general circulation model ECHAM5/MESSy1 has been extended by processes that parameterize particle precipitation. Several types of particle precipitation that directly affect NOy and HOx concentrations in the middle atmosphere are accounted for and discussed in a series of papers. In the companion paper, the ECHAM5/MESSy1 solar proton event parameterization is discussed, while in the current paper we focus on low energy electrons (LEE) that produce NOx in the upper atmosphere. For the flux of LEE NOx into the top of the model domain a novel technique which can be applied to most atmospheric chemistry general circulation models has been developed and is presented here. The technique is particularly useful for models with an upper boundary between the stratopause and mesopause and therefore cannot directly incorporate upper atmospheric NOx production. The additional NOx source parametrization is based on a measure of geomagnetic activity, the Ap index, which has been shown to be a good proxy for LEE NOx interannual variations. HALOE measurements of LEE NOx that has been transported into the stratosphere are used to develop a scaling function which yields a flux of NOx that is applied to the model top. We describe the implementation of the parameterization as the submodel SPACENOX in ECHAM5/MESSy1 and discuss the results from test simulations. The NOx enhancements and associated effects on ozone are shown to be in good agreement with independent measurements. Ap index data is available for almost one century, thus the parameterization is suitable for simulations of the recent climate.
Global ozone and air quality: a multi-model assessment of risks to human health and crops
Authors: Ellingsen K. , Gauss M. , Van Dingenen R. , Dentener F. J. , Emberson L. , Fiore A. M. , Schultz M. G. , Stevenson D. S. , Ashmore M. R. , Atherton C. S. , Bergmann D. J. , Bey I. , Butler T. , Drevet J. , Eskes H. , Hauglustaine D. A. , Isaksen I. S. A. , Horowitz L. W. , Krol M. , Lamarque J. F. , Lawrence M. G. , van Noije T. , Pyle J. , Rast S. , Rodriguez J. , Savage N. , Strahan S. , Sudo K. , Szopa S. , Wild O.
Published: April 2010

Abstract. Within ACCENT, a European Network of Excellence, eighteen atmospheric models from the U.S., Europe, and Japan calculated present (2000) and future (2030) concentrations of ozone at the Earth's surface with hourly temporal resolution. Comparison of model results with surface ozone measurements in 14 world regions indicates that levels and seasonality of surface ozone in North America and Europe are characterized well by global models, with annual average biases typically within 5–10 nmol/mol. However, comparison with rather sparse observations over some regions suggest that most models overestimate annual ozone by 15–20 nmol/mol in some locations. Two scenarios from the International Institute for Applied Systems Analysis (IIASA) and one from the Intergovernmental Panel on Climate Change Special Report on Emissions Scenarios (IPCC SRES) have been implemented in the models. This study focuses on changes in near-surface ozone and their effects on human health and vegetation. Different indices and air quality standards are used to characterise air quality. We show that often the calculated changes in the different indices are closely inter-related. Indices using lower thresholds are more consistent between the models, and are recommended for global model analysis. Our analysis indicates that currently about two-thirds of the regions considered do not meet health air quality standards, whereas only 2–4 regions remain below the threshold. Calculated air quality exceedances show moderate deterioration by 2030 if current emissions legislation is followed and slight improvements if current emissions reduction technology is used optimally. For the "business as usual" scenario severe air quality problems are predicted. We show that model simulations of air quality indices are particularly sensitive to how well ozone is represented, and improved accuracy is needed for future projections. Additional measurements are needed to allow a more quantitative assessment of the risks to human health and vegetation from changing levels of surface ozone.
Detection of regional scale sea-to-air oxygen emission related to spring bloom near Japan by using in-situ measurements of atmospheric oxygen/nitrogen ratio
Authors: Yamagishi H. , Tohjima Y. , Mukai H. , Sasaoka K.
Published: April 2010

Abstract. We have been carrying out in-situ monitoring of atmospheric O2/N2 ratio at Cape Ochi-ishi (COI; 43°10´ N, 145°30´ E) in the northern part of Japan since March 2005 by using a modified gas chromatography/thermal conductivity detector (GC/TCD). The standard deviation of the O2/N2 ratio is estimated to be about ±14 per meg (≈3 ppm) with intervals of 10 min. Thus, the in-situ measurement system has a 1σ precision of ±6 per meg ((≈1.2 ppm) for one-hour mean O2/N2 ratio. Atmospheric potential oxygen (APO ≈O2+1.1CO2), which is conserved with respect to terrestrial photosynthesis and respiration but reflects changes in air-sea O2 and CO2 fluxes, shows large variabilities from April to early July 2005. Distribution of satellite-derived marine primary production indicates occurrences of strong bloom in the Japan Sea in April and in the Okhotsk Sea and the western North Pacific near Hokkaido Island in June. Back trajectory analysis of air masses indicates that high values of APO, which last for several hours or several days, can be attributed to the oxygen emission associated with the spring bloom of active primary production.
Personal UV exposure on a ski-field at an alpine site
Authors: Siani A. M. , Casale G. R. , Diémoz H. , Agnesod G. , Kimlin M. G. , Lang C. A. , Colosimo A.
Published: April 2010

Abstract. Mountain sites experience enhanced ambient UV radiation levels due to the concurrent effects of shorter radiation path-length, low aerosol load and high reflectivity of the snow surfaces. This study was encouraged by the possibility to collect data of personal UV exposure in the mountainous areas of Italy, for the first time. Personal UV exposure (expressed in terms of Exposure Ratio, ER) of two groups of volunteers (ski instructors and skiers) at the Alpine site of La Thuile (Valle d'Aosta region, Italy) was assessed using polysulphone dosimetry which was tested in a mountainous snow-covered environment. In addition measurements of biological markers of individual response to UV exposure such as skin colorimetric parameters were carried out. It was found that snow and altitude of study site affect calibration curves of polysulphone dosimeters in comparison to a situation without snow. The median ER, taking into account the whole sample, is 0.60 in winter, with a range of 0.29 to 1.46, and 1.02 in spring, ranging from 0.46 to 1.72. There are no differences in exposures across skiers and instructors in spring while in winter skiers experience lower values. UV exposures are not sensitive to the use of sunscreen across instructor/skier group by day or by seasons or by photo-type. With regard to colorimetric parameters, the main result was that both skiers and instructors had on average significantly lower values of L* and b* after exposure i.e. becoming darker but the inappropriate sunscreen use did not reveal any changes in skin colorimetric parameters except in one spring day. In conclusions UV intensities on the ski-fields are often significantly higher than those on horizontal surfaces. Given the high levels of exposure observed in the present study, dedicated public heath messages on the correct sunscreen use should be adopted.
Sea surface wind speed estimation from space-based lidar measurements
Authors: Hu Y. , Stamnes K. , Vaughan M. , Pelon J. , Weimer C. , Wu D. , Cisewski M. , Sun W. , Yang P. , Lin B. , Omar A. , Flittner D. , Hostetler C. , Trepte C. , Winker D. , Gibson G. , Santa-Maria M.
Published: April 2010

Abstract. Global satellite observations of lidar backscatter measurements acquired by the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) mission and collocated sea surface wind speed data from the Advanced Microwave Scanning Radiometer for the Earth Observing System (AMSR-E), are used to investigate the relation between wind driven wave slope variance and sea surface wind speed. The new slope variance – wind speed relation established from this study is similar to the linear relation from Cox-Munk (1954) and the log-linear relation from Wu (1972, 1990) for wind speed larger than 7 m/s and 13.3 m/s, respectively. For wind speed less than 7 m/s, the slope variance is proportional to the square root of the wind speed, assuming a two dimensional isotropic Gaussian wave slope distribution. This slope variance – wind speed relation becomes linear if a one dimensional Gaussian wave slope distribution is assumed. Contributions from whitecaps and subsurface backscattering are effectively removed by using 532 nm lidar depolarization measurements. This new slope variance – wind speed relation is used to derive sea surface wind speed from CALIPSO single shot lidar measurements (70 m spot size), after correcting for atmospheric attenuation. The CALIPSO wind speed result agrees with the collocated AMSR-E wind speed, with 1.2 m/s rms error.
Modelling representation errors of atmospheric CO2 concentrations at a regional scale
Authors: Tolk L. F. , Meesters A. G. C. A. , Dolman A. J. , Peters W.
Published: April 2010

Abstract. Inverse modelling of carbon sources and sinks requires an accurate estimate of the quality of the observations to obtain a realistic estimate of the inferred fluxes and their uncertainties. Representation errors, defined here as the mismatch between point observations and grid cell averages, may add substantial uncertainty to the interpretation of atmospheric CO2 concentration data. We used a high resolution (2 km) mesoscale model (RAMS) to simulate the variations in the CO2 concentration to estimate the representation errors for grid sizes of 10–100 km. Meteorology is the main driver of representation errors in our study causing spatial and temporal variations in the error estimate. Within the nocturnal boundary layer the representation errors are relatively large and mainly determined by unresolved topography at lower model resolutions. During the day, surface CO2 flux variability and mesoscale circulations were found to be the main sources of representation errors. Careful up-scaling of point observations can reduce the importance of the representation error substantially. The remaining representation error is in the order of 0.5–1.5 ppm at 20–100 km resolution.
Carbon monoxide observations from ground stations in France and Europe and long trends in the free troposphere
Authors: Chevalier A. , Gheusi F. , Attié J.-L. , Delmas R. , Zbinden R. , Athier G. , Cousin J.-M.
Published: April 2010

Abstract. Continuous CO measurements performed at 3 high-altitude stations in France are analyzed for the first time. Data are provided by the new PAES (Pollution Atmospherique à l'Echelle Synoptique) network since 2002 for the Puy de Dôme and 2004 for the Pic du Midi and the Donon. CO measurements of 5 another European stations have been analysed to put the PAES stations in an European perspective. The January 2002–April 2005 CO mean levels of surface stations capture the stratification revealed by climatological CO profiles from the airborne observation system MOZAIC (Measurement of OZone and water vapour by Airbus In-service Aircraft). The deviation between the free tropospheric reference MOZAIC and surface data above 2000 m is less than 10% and this deviation can be explained in term of spatial variability, as evidenced by MOPITT CO retrievals at 700 hPa. This suggests that, averaged at a seasonal time scale (4 months), surface data at stations above 2000 m are representative of background CO concentration. This paper focuses then on trends since the 1980s–1990s. The comparison between old (1982–1983) and recent CO mixing ratio (2005) at the Pic du Midi leads to a 10% decrease, consistent with the continuous data series at Zugspitze (ZSP) from 1991 to 2004. This decrease was found to be mainly due to a negative trend of January–April mean levels. The decrease in CO sources over France and Europe appears to be responsible for that trend. The stable values of June–September mean levels suggest that the summertime oxidizing capacity of the atmosphere related to OH radicals is important enough to counterbalance any CO inputs into the troposphere. Our study shows a recent change in CO evolution since 2000 over Western Europe, with a slowed down decrease in CO concentration. Studying specifically the interactions between CO, CH4 and OH turns out to be needed, however, to find definitive explanations to those observations.
Technical Note: Quantification of interferences of wet chemical HONO measurements under simulated polar conditions
Authors: Kleffmann J. , Wiesen P.
Published: April 2010

Abstract. In the present pilot study, an optimized LOPAP instrument for the detection of nitrous acid (HONO) in the atmosphere (DL 0.2 pptV) was tested at the high alpine research station "Jungfraujoch" at 3580 m altitude in the Swiss Alps under conditions comparable to polar regions. HONO concentrations in the range <0.5–50 pptV with an average of 7.5 pptV were observed at the "Jungfraujoch". The diurnal profiles obtained exhibited clear maxima at noon and minima with very low concentration during the night supporting the proposed photochemical production of HONO. In good agreement with recent measurements at the South Pole, it was demonstrated, that interferences of chemical HONO instruments can significantly influence the measurements and lead to considerable overestimations, especially for low pollution level. Accordingly, the correction of interferences is of paramount importance for those instruments, which sample HONO on aqueous or humid surfaces.
Validation of ACE-FTS N2O measurements
Authors: Strong K. , Wolff M. A. , Kerzenmacher T. E. , Walker K. A. , Bernath P. F. , Blumenstock T. , Boone C. , Catoire V. , Coffey M. , De Mazière M. , Demoulin P. , Duchatelet P. , Dupuy E. , Hannigan J. , Höpfner M. , Glatthor N. , Griffith D. W. T. , Jin J. J. , Jones N. , Jucks K. , Kuellmann H. , Kuttippurath J. , Lambert A. , Mahieu E. , McConnell J. C. , Mellqvist J. , Mikuteit S. , Murtagh D. P. , Notholt J. , Piccolo C. , Raspollini P. , Ridolfii M. , Robert C. , Schneider M. , Schrems O. , Semeniuk K. , Senten C. , Stiller G. P. , Strandberg A. , Taylor J. , Tétard C. , Toohey M. , Urban J. , Warneke T. , Wood S.
Published: April 2010

Abstract. The Atmospheric Chemistry Experiment (ACE), also known as SCISAT, was launched on 12 August 2003, carrying two instruments that measure vertical profiles of atmospheric constituents using the solar occultation technique. One of these instruments, the ACE Fourier Transform Spectrometer (ACE-FTS), is measuring volume mixing ratio (VMR) profiles of nitrous oxide (N2O) from the upper troposphere to the lower mesosphere at a vertical resolution of about 3–4 km. In this study, the quality of the ACE-FTS version 2.2 N2O data is assessed through comparisons with coincident measurements made by other satellite, balloon-borne, aircraft, and ground-based instruments. These consist of vertical profile comparisons with the SMR, MLS, and MIPAS satellite instruments, multiple aircraft flights of ASUR, and single balloon flights of SPIRALE and FIRS-2, and partial column comparisons with a network of ground-based Fourier Transform InfraRed spectrometers (FTIRs). Overall, the quality of the ACE-FTS version 2.2 N2O VMR profiles is good over the entire altitude range from 5 to 60 km. Between 6 and 30 km, the mean absolute differences for the satellite comparisons lie between −42 ppbv and +17 ppbv, with most within ±20 ppbv. This corresponds to relative deviations from the mean that are within ±15%, except for comparisons with MIPAS near 30 km, for which they are as large as 22.5%. Between 18 and 30 km, the mean absolute differences are generally within ±10 ppbv, again excluding the aircraft and balloon comparisons. From 30 to 60 km, the mean absolute differences are within ±4 ppbv, and are mostly between −2 and +1 ppbv. Given the small N2O VMR in this region, the relative deviations from the mean are therefore large at these altitudes, with most suggesting a negative bias in the ACE-FTS data between 30 and 50 km. In the comparisons with the FTIRs, the mean relative differences between the ACE-FTS and FTIR partial columns are within ±6.6% for eleven of the twelve contributing stations. This mean relative difference is negative at ten stations, suggesting a small negative bias in the ACE-FTS partial columns over the altitude regions compared. Excellent correlation (R=0.964) is observed between the ACE-FTS and FTIR partial columns, with a slope of 1.01 and an intercept of −0.20 on the line fitted to the data.
Validation of UV-visible aerosol optical thickness retrieved from spectroradiometer measurements
Authors: Brogniez C. , Buchard V. , Auriol F.
Published: April 2010

Abstract. Global and diffuse UV-visible solar irradiances are routinely measured since 2003 with a spectroradiometer operated by the Laboratoire d'Optique Atmosphérique (LOA) located in Villeneuve d'Ascq, France. The analysis of the direct irradiance derived by cloudless conditions enables retrieving the aerosol optical thickness (AOT) spectrum in the 330–450 nm range. The site hosts also sunphotometers from the AERONET/PHOTONS network performing routinely measurements of the AOT at several wavelengths. On one hand, comparisons between the spectroradiometer and the sunphotometer AOT at 440 nm as well as, when available, at 340 and 380 nm, show good agreement. On the other hand, the AOT's spectral variations have been compared using the Angström exponents derived from AOT data at 340 and 440 nm for both instruments. The comparisons show that this parameter is difficult to retrieve accurately due to the small wavelength range and due to the weak AOT values. Thus, AOT derived at wavelengths outside the spectroradiometer range by means of an extrapolation using the Angström parameter would be of poor value, whereas, spectroradiometer's spectral AOT could be used for direct validation of other AOT, such as those provided by satellite instruments.
Lagrangian transport modelling for CO2 using two different biosphere models
Authors: Pieterse G. , Vermeulen A. T. , Baker I. T. , Denning A. S.
Published: April 2010

Abstract. In this work, the performance of the Framework for Atmosphere-Canopy Exchange Modelling (FACEM: Pieterse et al., 2007) coupled to a Lagrangian atmospheric transport model is evaluated for carbon dioxide. Before incorporating FACEM into the Lagrangian COMET model (Vermeulen et al., 2006), its performance for the European domain is compared with the Simple Biosphere model (SiB3: Sellers et al., 1996). Overall, FACEM is well correlated to SiB3 (R2≥0.60), but shows less variability for regions with predominantly bare soil. There is no significant overall bias between the models except for the winter conditions and in general for the Iberian peninsula. When coupled to the COMET transport model, both biosphere models yield similar correlations (R2≥0.60) and bias relative to the 1-hourly concentration measurements for the year 2002, performed at three different sites in Europe; Cabauw (Netherlands), Hegyhatsal (Hungary) and Mace Head (Ireland). The overall results indicate that FACEM is comparable to SiB3 in terms of its applicability for atmospheric modelling studies.
Comparison of OMI ozone and UV irradiance data with ground-based measurements at two French sites
Authors: Buchard V. , Brogniez C. , Auriol F. , Bonnel B. , Lenoble J. , Tanskanen A. , Bojkov B. , Veefkind P.
Published: April 2010

Abstract. Ozone Monitoring Instrument (OMI), launched in July 2004, is dedicated to the monitoring of the Earth's ozone, air quality and climate. OMI provides among other things the total column of ozone (TOC), the surface ultraviolet (UV) irradiance at several wavelengths, the erythemal dose rate and the erythemal daily dose. The main objective of this work is to validate OMI data with ground-based instruments in order to use OMI products (collection 2) for scientific studies. The Laboratoire d'Optique Atmosphérique (LOA) located in Villeneuve d'Ascq in the north of France performs solar UV measurements using a spectroradiometer and a broadband radiometer. The site of Briançon in the French Southern Alps is also equipped with a spectroradiometer operated by Interaction Rayonnement Solaire Atmosphère (IRSA). The instrument belongs to the Centre Européen Médical et Bioclimatologique de Recherche et d'Enseignement Supérieur. The comparison between the TOC retrieved with ground-based measurements and OMI TOC shows good agreement at both sites for all sky conditions. Comparisons of spectral UV on clear sky conditions are also satisfying whereas results of comparisons of the erythemal daily doses and erythemal dose rates for all sky conditions and for clear sky show that OMI overestimates significantly surface UV doses at both sites.
Validation of water vapour profiles from the Atmospheric Chemistry Experiment (ACE)
Authors: Carleer M. R. , Boone C. D. , Walker K. A. , Bernath P. F. , Strong K. , Sica R. J. , Randall C. E. , Vömel H. , Kar J. , Höpfner M. , Milz M. , von Clarmann T. , Kivi R. , Valverde-Canossa J. , Sioris C. E. , Izawa M. R. M. , Dupuy E. , McElroy C. T. , Drummond J. R. , Nowlan C. R. , Zou J. , Nichitiu F. , Lossow S. , Urban J. , Murtagh D. , Dufour D. G.
Published: April 2010

Abstract. The Atmospheric Chemistry Experiment (ACE) mission was launched in August 2003 to sound the atmosphere by solar occultation. Water vapour (H2O), one of the most important molecules for climate and atmospheric chemistry, is one of the key species provided by the two principal instruments, the infrared Fourier Transform Spectrometer (ACE-FTS) and the MAESTRO UV-Visible spectrometer (ACE-MAESTRO). The first instrument performs measurements on several lines in the 1362–2137 cm−1 range, from which vertically resolved H2O concentration profiles are retrieved, from 7 to 90 km altitude. ACE-MAESTRO measures profiles using the water absorption band in the near infrared part of the spectrum at 926.0–969.7 nm. This paper presents a comprehensive validation of the ACE-FTS profiles. We have compared the H2O volume mixing ratio profiles with space-borne (SAGE II, HALOE, POAM III, MIPAS, SMR) observations and measurements from balloon-borne frostpoint hygrometers and a ground based lidar. We show that the ACE-FTS measurements provide H2O profiles with small retrieval uncertainties in the stratosphere (better than 5% from 15 to 70 km, gradually increasing above). The situation is unclear in the upper troposphere, due mainly to the high variability of the water vapour volume mixing ratio in this region. A new water vapour data product from the ACE-MAESTRO (Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation) is also presented and initial comparisons with ACE-FTS are discussed.
Enhancement of N2O during the October–November 2003 solar proton events
Authors: Funke B. , García-Comas M. , López-Puertas M. , Glatthor N. , Stiller G. P. , von Clarmann T. , Semeniuk K. , McConnell J. C.
Published: April 2010

Abstract. In this paper we present evidence of enhanced N2O concentrations in the upper stratosphere/lower mesosphere polar regions after the solar proton events that occurred during October–November 2003. The observations were performed by the MIPAS instrument on the Envisat satellite. Simulations performed using the Canadian Middle Atmospheric Model (CMAM) show that such enhancements are most likely produced by the reaction of N(4S) with NO2, both of which species are largely enhanced just after the solar proton events in the winter polar night.
A combined particle trap/HTDMA hygroscopicity study of mixed inorganic/organic aerosol particles
Authors: Zardini A. A. , Sjogren S. , Marcolli C. , Krieger U. K. , Gysel M. , Weingartner E. , Baltensperger U. , Peter T.
Published: April 2010

Abstract. Atmospheric aerosols are often mixtures of inorganic and organic material. Organics can represent a large fraction of the total aerosol mass and are comprised of water-soluble and insoluble compounds. Increasing attention was paid in the last decade to the capability of mixed inorganic/organic aerosol particles to take up water (hygroscopicity). We performed hygroscopicity measurements of internally mixed particles containing ammonium sulfate and carboxylic acids (citric, glutaric, adipic acid) in parallel with an electrodynamic balance (EDB) and a hygroscopicity tandem differential mobility analyzer (HTDMA). The organic compounds were chosen to represent three distinct physical states. During hygroscopicity cycles covering hydration and dehydration measured by the EDB and the HTDMA, pure citric acid remained always liquid, adipic acid remained always solid, while glutaric acid could be either. We show that the hygroscopicity of mixtures of the above compounds is well described by the Zdanovskii-Stokes-Robinson (ZSR) relationship as long as the two-component particle is completely liquid in the ammonium sulfate/citric acid and in the ammonium sulfate/glutaric acid cases. However, we observe significant discrepancies compared to what is expected from bulk thermodynamics when a solid component is present. We explain this in terms of a complex morphology resulting from the crystallization process leading to veins, pores, and grain boundaries which allow for water sorption in excess of bulk thermodynamic predictions caused by the inverse Kelvin effect on concave surfaces.
Influence of future air pollution mitigation strategies on total aerosol radiative forcing
Authors: Kloster S. , Dentener F. , Feichter J. , Raes F. , van Aardenne J. , Roeckner E. , Lohmann U. , Stier P. , Swart R.
Published: April 2010

Abstract. We apply different aerosol and aerosol precursor emission scenarios reflecting possible future control strategies for air pollution in the ECHAM5-HAM model, and simulate the resulting effect on the Earth's radiation budget. We use two opposing future mitigation strategies for the year 2030: one in which emission reduction legislation decided in countries throughout the world are effectively implemented (current legislation; CLE 2030) and one in which all technical options for emission reductions are being implemented independent of their cost (maximum feasible reduction; MFR 2030). We consider the direct, semi-direct and indirect radiative effects of aerosols. The total anthropogenic aerosol radiative forcing defined as the difference in the top-of-the-atmosphere radiation between 2000 and pre-industrial times amounts to −2.05 W/m2. In the future this negative global annual mean aerosol radiative forcing will only slightly change (+0.02 W/m2) under the "current legislation" scenario. Regionally, the effects are much larger: e.g. over Eastern Europe radiative forcing would increase by +1.50 W/m2 because of successful aerosol reduction policies, whereas over South Asia it would decrease by −1.10 W/m2 because of further growth of emissions. A "maximum feasible reduction" of aerosols and their precursors would lead to an increase of the global annual mean aerosol radiative forcing by +1.13 W/m2. Hence, in the latter case, the present day negative anthropogenic aerosol forcing cloud be more than halved by 2030 because of aerosol reduction policies and climate change thereafter will be to a larger extend be controlled by greenhouse gas emissions. We combined these two opposing future mitigation strategies for a number of experiments focusing on different sectors and regions. In addition, we performed sensitivity studies to estimate the importance of future changes in oxidant concentrations and the importance of the aerosol microphysical coupling within the range of expected future changes. For changes in oxidant concentrations in the future within a realistic range, we do not find a significant effect for the global annual mean radiative aerosol forcing. In the extreme case of only abating SO2 or carbonaceous emissions to a maximum feasible extent, we find deviations from additivity for the radiative forcing over anthropogenic source regions up to 10% compared to an experiment abating both at the same time.
Spatiotemporal variations of ambient PM10 source contributions in Beijing in 2004 using positive matrix factorization
Authors: Xie S. , Liu Z. , Chen T. , Hua L.
Published: April 2010

Abstract. Source contributions to ambient PM10 (particles with an aerodynamic diameter of 10 μm or less) in Beijing, China were determined with positive matrix factorization (PMF) based on ambient PM10 composition data including concentrations of organic carbon (OC), elemental carbon (EC), ions and metal elements, which were simultaneously obtained at six sites through January, April, July and October in 2004. Results from PMF indicated that seven major sources of ambient PM10 were urban fugitive dust, crustal soil, coal combustion, secondary sulfate, secondary nitrate, biomass burning and vehicle emission, respectively. In paticular, urban fugitive dust and crustal soil as two types of dust sources with similar chemical characteristics were differentiated by PMF. Urban fugitive dust contributed the most, accounting for 34.4% of total PM10 mass on an annual basis, with relatively high contributions in all four months, and even covered 50% in April. It also showed higher contributions in southwestern and southeastern areas than in central urban areas. Coal combustion was found to be the primary contributor in January, showing higher contributions in urban areas than in suburban areas with seasonal variation peaking in winter, which accounted for 15.5% of the annual average PM10 concentration. Secondary sulfate and secondary nitrate combined as the largest contributor to PM10 in July and October, with strong seasonal variation peaking in summer, accounting for 38.8% and 31.5% of the total PM10 mass in July and October, respectively. Biomass burning contributions were found in all four months and accounted for 9.8% of the annual average PM10 mass concentration, with obviously higher contribution in October than in other months. Incineration sources were probably located in southwestern Beijing. Contribution from vehicle emission accounted for 5.0% and exhibited no significant seasonal variation. In sum, PM10 source contributions in Beijing showed not only significant seasonal variations but also spatial differences.
Odin stratospheric proxy NOy measurements and climatology
Authors: Brohede S. , McLinden C. A. , Urban J. , Haley C. S. , Jonsson A. I. , Murtagh D.
Published: April 2010

Abstract. Five years of OSIRIS (Optical Spectrograph and InfraRed Imager System) NO2 and SMR (Sub-Millimetre Radiometer) HNO3 observations from the Odin satellite, combined with data from a photochemical box model, have been used to construct a stratospheric proxy NOy data set including the gases: NO, NO2, HNO3, 2×N2O5 and CIONO2. This Odin NOy climatology is based on all daytime measurements and contains monthly mean and standard deviation, expressed as mixing ratio or number density, as function of latitude or equivalent latitude (5° bins) on 17 vertical layers (altitude, pressure or potential temperature) between 14 and 46 km. Comparisons with coincident NOy profiles from the Atmospheric Chemistry Experiment–Fourier Transform Spectrometer (ACE-FTS) instrument were used to evaluate several methods to combine Odin observations with model data. This comparison indicates that the most appropriate merging technique uses OSIRIS measurements of NO2, scaled with model NO/NO2 ratios, to estimate NO. The sum of 2×N2O5 and CIONO2 is estimated from uncertainty-based weighted averages of scaled observations of SMR HNO3 and OSIRIS NO2. Comparisons with ACE-FTS suggest the precision (random error) and accuracy (systematic error) of Odin NOy profiles are about 15% and 20%, respectively. Further comparisons between Odin and the Canadian Middle Atmosphere Model (CMAM) show agreement to within 20% and 2 ppb throughout most of the stratosphere except in the polar vortices. A particularly large disagreement within the Antarctic vortex in the upper stratosphere during spring indicates too strong descent of air in CMAM. The combination of good temporal and spatial coverage, a relatively long data record, and good accuracy and precision make this a valuable NOy product for various atmospheric studies and model assessments.
Typical distribution of the solar erythemal UV radiation over Slovakia
Authors: Pribullová A. , Chmelík M.
Published: April 2010

Abstract. Maps of the solar erythemal ultraviolet (UV) radiation daily doses were created for every month with horizontal resolution of 500 m at geographical domain 47.15 N–49.86 N×16.94 E–22.81 E covering the territory of Slovakia. Cloud modification factor for the UV radiation (cmfUV) was modelled utilizing relation between the cmf of total and UV radiation. The maps of the cmf factor of the UV radiation were created utilizing measurements of total radiation performed at 9 observatories during 1995–2004 period and the model of cmf dependence on altitude. Maps of clear-sky UV radiation daily dose and UV radiation daily dose affected by average cloudiness were constructed for mean monthly total ozone, their upper and lower monthly limits, for two probability levels of snow cover occurrence as criterion for the snow effect incorporation in the model and for 1 day representing typical values of every month. The map-set can be considered as an atlas of the solar erythemal UV radiation over Slovakia.
How small is a small cloud?
Authors: Koren I. , Oreopoulos L. , Feingold G. , Remer L. A. , Altaratz O.
Published: April 2010

Abstract. The interplay between clouds and aerosols and their contribution to the radiation budget is one of the largest uncertainties of climate change. Most work to date has separated cloudy and cloud-free areas in order to evaluate the individual radiative forcing of aerosols, clouds, and aerosol effects on clouds. Here we examine the size distribution and the optical properties of small, sparse cumulus clouds and the associated optical properties of what is considered a cloud-free atmosphere within the cloud field. We show that any separation between clouds and cloud free atmosphere will incur errors in the calculated radiative forcing. The nature of small cumulus cloud size distributions suggests that at any resolution, a significant fraction of the clouds are missed, and their optical properties are relegated to the apparent cloud-free optical properties. At the same time, the cloudy portion incorporates significant contribution from non-cloudy pixels. We show that the largest contribution to the total cloud reflectance comes from the smallest clouds and that the spatial resolution changes the apparent energy flux of a broken cloudy scene. When changing the resolution from 30 m to 1 km (Landsat to MODIS) the average "cloud-free" reflectance at 1.65 μm increases more than 25%, the cloud reflectance decreases by half, and the cloud coverage doubles, resulting in an important impact on climate forcing estimations. The apparent aerosol forcing is on the order of 0.5 to 1 Wm−2 per cloud field.
Combustion particulate emissions in Africa: regional climate modeling and validation
Authors: Konare A. , Liousse C. , Guillaume B. , Solmon F. , Assamoi P. , Rosset R. , Gregoire J. M. , Giorgi F.
Published: April 2010

Abstract. Africa, as a major aerosol source in the world, plays a key role in regional and global geochemical cycles and climate change. Combustion carbonaceous particles, central in this context through their radiative and hygroscopic properties, require ad hoc emission inventories. These inventories must incorporate fossil fuels FF (industries, traffic,...), biofuels BF (charcoal, wood burning,... quite common in Africa for domestic use), and biomass burning BB regularly occurring over vast areas all over the African continent. This latter, subject to rapid massive demographic, migratory, industrial and socio-economic changes, requires continuous emission inventories updating, so as to keep pace with this evolution. Two such different inventories, L96 and L06 with main focus on BB emissions, have been implemented for comparison within the regional climate model RegCM3 endowed with a specialized carbonaceous aerosol module. Resulting modeled black carbon BC and organic carbon OC fields have been compared to past and present composite data set available in Africa. This data set includes measurements from intensive field campaigns (EXPRESSO 1996, SAFARI 2000), from the IDAF/DEBITS surface network and from MODIS, focused on selected west, central and southern African sub-domains. This composite approach has been adopted to take advantage of possible combinations between satellite high-resolution coverage of Africa, regional modeling, use of an established surface network, together with the patchy detailed knowledge issued from past short intensive regional field experiments. Stemming from these particular comparisons, one prominent conclusion is the need for continuous detailed time and spatial updating of combustion emission inventories apt to reflect the rapid transformations of the African continent.
Airborne in-situ measurements of vertical, seasonal and latitudinal distributions of carbon dioxide over Europe
Authors: Gurk C. , Fischer H. , Hoor P. , Lawrence M.G. , Lelieveld J. , Wernli H.
Published: April 2010

Abstract. Airborne in-situ observations of carbon dioxide (CO2) were made during 7 intensive measurement campaigns between November 2001 and April 2003 as part of the SPURT project. Vertical profiles and latitudinal gradients in the upper troposphere/lowermost stratosphere were measured along the western shore of Europe from the subtropics to high northern latitudes during different seasons. In the boundary layer, CO2 exhibits a strong seasonal cycle with the maximum mixing ratios in winter and minimum values in summer, reflecting the strength of CO2 uptake by vegetation. Seasonal variations are strongest in high latitudes and propagate to the free troposphere and lowermost stratosphere, although with reduced amplitude, resulting in increasing CO2 mixing ratios with altitude during the summer. In the lowermost stratosphere, the CO2 seasonal cycle is phase-shifted relative to the free troposphere by approximately 3 months, with highest mixing ratios during the summer.
The travel-related carbon dioxide emissions of atmospheric researchers
Authors: Stohl A.
Published: April 2010

Abstract. Most atmospheric scientists agree that greenhouse gas emissions have already caused significant changes to the global climate system and that these changes will accelerate in the near future. At the same time, atmospheric scientists who – like other scientists – rely on international collaboration and information exchange travel a lot and, thereby, cause substantial emissions of carbon dioxide (CO2). In this paper, the CO2 emissions of the employees working at an atmospheric research institute (the Norwegian Institute for Air Research, NILU) caused by all types of business travel (conference visits, workshops, field campaigns, instrument maintainance, etc.) were calculated for the years 2005–2007. It is estimated that more than 90% of the emissions were caused by air travel, 3% by ground travel and 5% by hotel usage. The travel-related annual emissions were between 1.9 and 2.4 t CO2 per employee or between 3.9 and 5.5 t CO2 per scientist. For comparison, the total annual per capita CO2 emissions are 4.5 t worldwide, 1.2 t for India, 3.8 t for China, 5.9 t for Sweden and 19.1 t for Norway. The travel-related CO2 emissions of a NILU scientist, occurring in 24 days of a year on average, exceed the global average annual per capita emission. Norway's per-capita CO2 emissions are among the highest in the world, mostly because of the emissions from the oil industry. If the emissions per NILU scientist derived in this paper are taken as representative for the average Norwegian researcher, travel by Norwegian scientists would nevertheless account for a substantial 0.2% of Norway's total CO2 emissions. Since most of the travel-related emissions are due to air travel, water vapor emissions, ozone production and contrail formation further increase the relative importance of NILU's travel in terms of radiative forcing.
Amines are likely to enhance neutral and ion-induced sulfuric acid-water nucleation in the atmosphere more effectively than ammonia
Authors: Kurtén T. , Loukonen V. , Vehkamäki H. , Kulmala M.
Published: April 2010

Abstract. We have studied the structure and formation thermodynamics of dimer clusters containing H2SO4 or HSO4− together with ammonia and seven different amines possibly present in the atmosphere, using the high-level ab initio methods RI-MP2 and RI-CC2. As expected from e.g. proton affinity data, the binding of all studied amine – H2SO4 complexes is significantly stronger than that of NH3•H2SO4, while most amine – HSO4− complexes are only somewhat more strongly bound than NH3•HSO4−. Further calculations on larger cluster structures containing dimethylamine or ammonia together with two H2SO4 molecules or one H2SO4 molecule and one HSO4− ion demonstrate that amines, unlike ammonia, significantly assist the growth of not only neutral but also ionic clusters along the H2SO4 co-ordinate. A sensitivity analysis indicates that the difference in complexation free energies for amine- and ammonia-containing clusters is large enough to overcome the mass-balance effect caused by the fact that the concentration of amines in the atmosphere is probably 2 or 3 orders of magnitude lower than that of ammonia. This implies that amines might be more important than ammonia in enhancing neutral and especially ion-induced sulfuric acid-water nucleation in the atmosphere.