bluuebunny/crossref_metadata_2025 huggingface dataset:
Study of suitability of AvaSpec array spectrometer for solar UV field measurements
Authors: Ansko I. , Eerme K. , Lätt S. , Noorma M. , Veismann U.
Published: April 2010

Abstract. A system to record the ultraviolet (UV) spectra of atmospheric global irradiance with the miniature fiber optic spectrometer AvaSpec-256 was developed for continuous computer-aided spectrometry at Tartu Observatory in 2005. As a result, the database of spectra recorded with 15-min-interval round 24 h over 300–400 nm, has been developed. The quantities retrieved from the spectra have been compared with those measured by the Scintec erythemal UV-SET sensor and the Kipp & Zonen narrowband 306 nm sensor. Almost clear and overcast days were selected for comparison. Reliable results on the spectral distribution of the UV global irradiance as well as the integrated daily spectral doses could be obtained at least during the bright half-year. The results were compared with the calculations performed by means of the LibRadtran package. The biases in irradiance were significant at SZA above 70–75°. At dominating larger SZA the recorded values need sophisticated corrections and remain less reliable. At lower latitudes than that of the study site (58.3°), the reliability of the spectrometer is expected to increase due to a smaller contribution of data measured at large SZA. The variations of the ratio of UV-A/UV-B irradiance, retrieved from the spectra, were investigated. Also the covariation of the narrowband 306 nm irradiance and the irradiance integrated over the whole UV-B range was studied. The biases between the UV-A/UV-B irradiances calculated by means of the LibRadtran package and measured with the AvaSpec were small at SZA below 70°. At larger SZA the values of the ratio as well as the biases increased, significantly depending on total ozone.
GEM-AQ, an on-line global multiscale chemical weather modelling system: model description and evaluation of gas phase chemistry processes
Authors: Kaminski J. W. , Neary L. , Struzewska J. , McConnell J. C. , Lupu A. , Jarosz J. , Toyota K. , Gong S. L. , Côté J. , Liu X. , Chance K. , Richter A.
Published: April 2010

Abstract. Tropospheric chemistry and air quality processes were implemented on-line in the Global Environmental Multiscale weather prediction model. The integrated model, GEM-AQ, was developed as a platform to investigate chemical weather at scales from global to urban. The current chemical mechanism is comprised of 50 gas-phase species, 116 chemical and 19 photolysis reactions, and is complemented by a sectional aerosol module with 5 aerosols types. All tracers are advected using the semi-Lagrangian scheme native to GEM. The vertical transport includes parameterized subgrid-scale turbulence and large scale deep convection. Dry deposition is included as a flux boundary condition in the vertical diffusion equation. Wet deposition of gas-phase species is treated in a simplified way, and only below-cloud scavenging is considered. The emissions used include yearly-averaged anthropogenic, and monthly-averaged biogenic, ocean, soil, and biomass burning emission fluxes, as well as NOx from lightning. In order to evaluate the ability to simulate seasonal variations and regional distributions of trace gases such as ozone, nitrogen dioxide and carbon monoxide, the model was run for a period of five years (2001–2005) on a global uniform 1.5°×1.5° horizontal resolution domain and 28 hybrid levels extending up to 10 hPa. Model results were compared with observations from satellites, aircraft measurement campaigns and balloon sondes. We find that GEM-AQ is able to capture the spatial details of the chemical fields in the middle and lower troposphere. The modelled ozone consistently shows good agreement with observations, except over tropical oceans. The comparison of carbon monoxide and nitrogen dioxide with satellite measurements emphasizes the need for more accurate, year-specific emissions fluxes for biomass burning and anthropogenic sources. Other species also compare well with available observations.
Can we reconcile differences in estimates of carbon fluxes from land-use change and forestry for the 1990s?
Authors: Ito A. , Penner J. E. , Prather M. J. , de Campos C. P. , Houghton R. A. , Kato T. , Jain A. K. , Yang X. , Hurtt G. C. , Frolking S. , Fearon M. G. , Chini L. P. , Wang A. , Price D. T.
Published: April 2010

Abstract. The effect of Land Use Change and Forestry (LUCF) on terrestrial carbon fluxes can be regarded as a carbon credit or debit under the UNFCCC, but scientific uncertainty in the estimates for LUCF remains large. Here, we assess the LUCF estimates by examining a variety of models of different types with different land cover change maps in the 1990s. Annual carbon pools and their changes are separated into different components for separate geographical regions, while annual land cover change areas and carbon fluxes are disaggregated into different LUCF activities and the biospheric response due to CO2 fertilization and climate change. We developed a consolidated estimate of the terrestrial carbon fluxes that combines book-keeping models with process-based biogeochemical models and inventory estimates and yields an estimate of the global terrestrial carbon flux that is within the uncertainty range developed in the IPCC 4th Assessment Report. We examined the USA and Brazil as case studies in order to assess the cause of differences from the UNFCCC reported carbon fluxes. Major differences in the litter and soil organic matter components are found for the USA. Differences in Brazil result from assumptions about the LUC for agricultural purposes. The effects of CO2 fertilization and climate change also vary significantly in Brazil. Our consolidated estimate shows that the small sink in Latin America is within the uncertainty range from inverse models, but that the sink in the USA is significantly smaller than the inverse models estimates. Because there are different sources of errors at the country level, there is no easy reconciliation of different estimates of carbon fluxes at the global level. Clearly, further work is required to develop data sets for historical land cover change areas and models of biogeochemical changes for an accurate representation of carbon uptake or emissions due to LUC.
Seven year particulate matter air quality assessment from surface and satellite measurements
Authors: Gupta P. , Christopher S. A.
Published: April 2010

Abstract. Using seven years of the Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical thickness (AOT) data and ground measurements of particulate matter mass over one site in the Southeastern United States (33.55° N, 86.82° W) we present a comprehensive analysis of various aspects of particulate matter air quality. Monthly, seasonal and inter-annual relationships are examined with emphasis on sampling biases, quality indicators in the AOT product and various cloud clearing criteria. Our results indicate that PM2.5 mass concentration over Northern Birmingham has decreased by about 23% in year 2006 when compared to year 2002 and air quality during summer months was poor when compared to winter months. MODIS-Terra AOT data was available only about 50% of the time due to cloud cover and unfavorable surface conditions. However, the mean difference in monthly mean PM2.5 was less than 2.2 μg m−3 derived using all the data and from only those days when satellite AOT was available indicating that satellite data does not have sampling issues. The correlation between PM2.5 and MODIS AOT increased from 0.52 to 0.62 when hourly PM2.5 data were used instead of daily mean PM2.5 data. Changing box size for satellite data around the ground station during comparisons produced less than ±0.03 difference in mean AOT values for 90% of observations. Application of AOT quality flags reduced the sample size but does not affect AOT-PM2.5 relationship significantly. We recommend using AOT quality flags for daily analysis, whereas long time scale analysis can be performed by using all AOT retrievals to obtain better sampling. Our analysis indicates that satellite data is a useful tool for monitoring particulate matter air quality especially in regions where ground measurements are not available. While these results are representative for the region of interest, it is difficult to extrapolate these results to a larger context without detailed analysis using ancillary data sets.
Quality assurance of the Brewer spectral UV measurements in Finland
Authors: Lakkala K. , Arola A. , Heikkilä A. , Kaurola J. , Koskela T. , Kyrö E. , Lindfors A. , Meinander O. , Tanskanen A. , Gröbner J. , Hülsen G.
Published: April 2010

Abstract. The quality assurance of the two Brewer spectrophotometers of the Finnish Meteorological Institute is discussed in this paper. The complete data processing chain from raw signal to high quality spectra is presented. The quality assurance includes daily maintenance, laboratory characterizations, calculation of long-term spectral responsivity, data processing and quality assessment. The cosine correction of the measurements is based on a new method, and is included in the data processing software. The results showed that the actual cosine correction factor of the two Finnish Brewers can vary between 1.08–1.13 and 1.08–1.12, respectively, depending on the sky radiance distribution and wavelength. The temperature characterization showed a linear temperature dependence between the instruments' internal temperature and the photon counts per cycle, and a temperature correction was used for correcting the measurements. The long-term spectral responsivity was calculated using the time series of several lamps using two slightly different methods. The long-term spectral responsivity was scaled to the irradiance scale of the Helsinki University of Technology (HUT) for the whole of the measurement time-periods 1990–2006 and 1995–2006 for Sodankylä and Jokioinen, respectively. Both Brewers have participated in many international spectroradiometer comparisons, and have shown good stability. The differences between the Brewers and the portable reference spectroradiometer QASUME have been within 5% during 2002–2007.
Modelling the optical properties of fresh biomass burning aerosol produced in a smoke chamber: results from the EFEU campaign
Authors: Hungershoefer K. , Zeromskiene K. , Iinuma Y. , Helas G. , Trentmann J. , Trautmann T. , Parmar R. S. , Wiedensohler A. , Andreae M. O. , Schmid O.
Published: April 2010

Abstract. A better characterisation of the optical properties of biomass burning aerosol as a function of the burning conditions is required in order to quantify their effects on climate and atmospheric chemistry. Controlled laboratory combustion experiments with different fuel types were carried out at the combustion facility of the Max Planck Institute for Chemistry (Mainz, Germany) as part of the "Impact of Vegetation Fires on the Composition and Circulation of the Atmosphere" (EFEU) project. The combustion conditions were monitored with concomitant CO2 and CO measurements. The mass scattering efficiencies of 8.9±0.2 m2 g−1 and 9.3±0.3 m2 g−1 obtained for aerosol particles from the combustion of savanna grass and an African hardwood (musasa), respectively, are larger than typically reported mainly due to differences in particle size distribution. The photoacoustically measured mass absorption efficiencies of 0.51±0.02 m2 g−1 and 0.50±0.02 m2 g−1 were at the lower end of the literature values. Using the measured size distributions as well as the mass scattering and absorption efficiencies, Mie calculations provided effective refractive indices of 1.60−0.010i (savanna grass) and 1.56−0.010i (musasa) (λ=0.55 μm). The apparent discrepancy between the low imaginary part of the refractive index and the high apparent elemental carbon (ECa) fractions (8 to 15%) obtained from the thermographic analysis of impactor samples can be explained by a positive bias in the elemental carbon data due to the presence of high molecular weight organic substances. Potential artefacts in optical properties due to instrument bias, non-natural burning conditions and unrealistic dilution history of the laboratory smoke cannot be ruled out and are also discussed in this study.
Mercury in the snow and firn at Summit Station, Central Greenland, and implications for the study of past atmospheric mercury levels
Authors: Faïn X. , Ferrari C. P. , Dommergue A. , Albert M. , Battle M. , Arnaud L. , Barnola J.-M. , Cairns W. , Barbante C. , Boutron C.
Published: April 2010

Abstract. Gaseous Elemental Mercury (Hg° or GEM) was investigated at Summit Station, Greenland, in the interstitial air extracted from the perennial snowpack (firn) at depths ranging from the surface to 30 m, during summer 2005 and spring 2006. Photolytic production and destruction of Hg° were observed close to the snow surface during summer 2005 and spring 2006, and we observed dark oxidation of GEM up to 270 cm depth in June 2006. Photochemical transformation of gaseous elemental mercury resulted in diel variations in the concentrations of this gas in the near-surface interstitial air, but destruction of Hg° was predominant in June, and production was the main process in July. This seasonal evolution of the chemical mechanisms involving gaseous elemental mercury produces a signal that propagates downward through the firn air, but is unobservably small below 15 m in depth. As a consequence, multi-annual averaged records of GEM concentration should be well preserved in deep firn air at depths below 15 m, and available for the reconstruction of the past atmospheric history of GEM over the last decades.
Mesoscale inversion: first results from the CERES campaign with synthetic data
Authors: Lauvaux T. , Uliasz M. , Sarrat C. , Chevallier F. , Bousquet P. , Lac C. , Davis K. J. , Ciais P. , Denning A. S. , Rayner P. J.
Published: April 2010

Abstract. We investigate the ability of a mesoscale model to reconstruct CO2 fluxes at regional scale. Formally, we estimate the reduction of error for a CO2 flux inversion at 8 km resolution in the South West of France, during four days of the CarboEurope Regional Experiment Strategy (CERES) in spring 2005. Measurements from two towers and two airplanes are available for this campaign. The lagrangian particle dispersion model LPDM was coupled to the non-hydrostatic model Meso-NH and integrated in a matrix inversion framework. Impacts of aircraft and tower measurements are quantified separately and together. We find that the configuration with both towers and aircraft is able to significantly reduce uncertainties on the 4-day averaged CO2 fluxes over about half of the 300×300 km2 domain. Most of this reduction comes from the tower measurements, even though the impact of aircraft measurements remains noticeable. Imperfect knowledge of boundary conditions does not significantly impact the error reduction for surface fluxes. We test alternative strategies to improve the impact of aircraft measurements and find that most information comes from measurements inside the boundary layer. We find that there would be a large improvement in error reduction if we could improve our ability to model nocturnal concentrations at tower sites.
Technical Note: New ground-based FTIR measurements at Ile de La Réunion: observations, error analysis, and comparisons with independent data
Authors: Senten C. , De Mazière M. , Dils B. , Hermans C. , Kruglanski M. , Neefs E. , Scolas F. , Vandaele A. C. , Vanhaelewyn G. , Vigouroux C. , Carleer M. , Coheur P. F. , Fally S. , Barret B. , Baray J. L. , Delmas R. , Leveau J. , Metzger J. M. , Mahieu E. , Boone C. , Walker K. A. , Bernath P. F. , Strong K.
Published: April 2010

Abstract. Ground-based high spectral resolution Fourier-transform infrared (FTIR) solar absorption spectroscopy is a powerful remote sensing technique to obtain information on the total column abundances and on the vertical distribution of various constituents in the atmosphere. This work presents results from two FTIR measurement campaigns in 2002 and 2004, held at Ile de La Réunion (21° S, 55° E). These campaigns represent the first FTIR observations carried out at a southern (sub)tropical site. They serve the initiation of regular, long-term FTIR monitoring at this site in the near future. To demonstrate the capabilities of the FTIR measurements at this location for tropospheric and stratospheric monitoring, a detailed report is given on the retrieval strategy, information content and corresponding full error budget evaluation for ozone (O3), methane (CH4), nitrous oxide (N2O), carbon monoxide (CO), ethane (C2H6), hydrogen chloride (HCl), hydrogen fluoride (HF) and nitric acid (HNO3) total and partial column retrievals. Moreover, we have made a thorough comparison of the capabilities at sea level altitude (St.-Denis) and at 2200 m a.s.l. (Maïdo). It is proved that the performances of the technique are such that the atmospheric variability can be observed, at both locations and in distinct altitude layers. Comparisons with literature and with correlative data from ozone sonde and satellite (i.e., ACE-FTS, HALOE and MOPITT) measurements are given to confirm the results. Despite the short time series available at present, we have been able to detect the seasonal variation of CO in the biomass burning season, as well as the impact of particular biomass burning events in Africa and Madagascar on the atmospheric composition above Ile de La Réunion. We also show that differential measurements between St.-Denis and Maïdo provide useful information about the concentrations in the boundary layer.
The tropical forest and fire emissions experiment: laboratory fire measurements and synthesis of campaign data
Authors: Yokelson R. J. , Christian T. J. , Karl T. G. , Guenther A.
Published: April 2010

Abstract. As part of the Tropical Forest and Fire Emissions Experiment (TROFFEE), tropical forest fuels were burned in a large, biomass-fire simulation facility and the smoke was characterized with open-path Fourier transform infrared spectroscopy (FTIR), proton-transfer reaction mass spectrometry (PTR-MS), gas chromatography (GC), GC/PTR-MS, and filter sampling of the particles. In most cases, about one-third of the fuel chlorine ended up in the particles and about one-half remained in the ash. About 50% of the mass of non-methane organic compounds (NMOC) emitted by these fires could be identified with the available instrumentation. The lab fire emission factors (EF, g compound emitted per kg dry fuel burned) were coupled with EF obtained during the TROFFEE airborne and ground-based field campaigns. This revealed several types of EF dependence on parameters such as the ratio of flaming to smoldering combustion and fuel characteristics. The synthesis of data from the different TROFFEE platforms was also used to derive EF for all the measured species for both primary deforestation fires and pasture maintenance fires – the two main types of biomass burning in the Amazon. Many of the EF are larger than those in widely-used earlier work. This is mostly due to the inclusion of newly-available, large EF for the initially-unlofted smoldering emissions from residual logs in pastures and the assumption that these emissions make a significant contribution (~40%) to the total emissions from pasture fires. The TROFFEE EF for particles with aerodynamic diameter <2.5 microns (EFPM2.5) is 14.8 g/kg for primary deforestation fires and 18.7 g/kg for pasture maintenance fires. These EFPM2.5 are significantly larger than a previous recommendation (9.1 g/kg) and lead to an estimated pyrogenic primary PM2.5 source for the Amazon that is 84% larger. New regional budgets for biogenic and pyrogenic emissions were roughly estimated. Coupled with an estimate of secondary aerosol formation in the Amazon and source apportionment studies, the regional budgets suggest that ~5% of the total mass of the regionally generated NMOC end up as secondary organic aerosol within the Amazonian boundary layer within 1–3 days. New global budgets confirm that biogenic emissions and biomass burning are the two largest global sources of NMOC with an estimated production of approximately 1000 (770–1400) and 500 (250–630) Tg/yr, respectively. It follows that plants and fires may also be the two main global sources of secondary organic aerosol. A limited set of emission ratios (ER) is given for sugar cane burning, which may help estimate the air quality impacts of burning this major crop, which is often grown in densely populated areas.
Modelling UV irradiances on arbitrarily oriented surfaces: effects of sky obstructions
Authors: Hess M. , Koepke P.
Published: April 2010

Abstract. A method is presented to calculate UV irradiances on inclined surfaces that additionally takes into account the influence of sky obstructions caused by obstacles such as mountains, houses, trees, or umbrellas. With this method it is thus possible to calculate the impact of UV radiation on biological systems, such as, for instance, the human skin or eye, in any natural or artificial environment. The method, which consists of a combination of radiation models, is explained here and the accuracy of its results is demonstrated. The effect of a natural skyline is shown for an Alpine ski area, where the UV irradiance even on a horizontal surface may increase due to reflection from snow by more than 10 percent. In contrast, in a street canyon the irradiance on a horizontal surface is reduced to 30% in shadow and to about 75% for a position in the sun.
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 (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 and linear slope variance – wind speed relation are 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. Ocean surface with lowest atmospheric loading and moderate wind speed (7–9 m/s) is used as target for lidar calibration correction.
The role of iron and black carbon in aerosol light absorption
Authors: Derimian Y. , Karnieli A. , Kaufman Y. J. , Andreae M. O. , Andreae T. W. , Dubovik O. , Maenhaut W. , Koren I.
Published: April 2010

Abstract. Iron is a major component of atmospheric aerosols, influencing the light absorption ability of mineral dust, and an important micronutrient that affects oceanic biogeochemistry. The regional distribution of the iron concentration in dust is important for climate studies; however, this is difficult to obtain since it requires in-situ aerosol sampling or simulation of complex natural processes. Simultaneous studies of aerosol chemical composition and radiometric measurements of aerosol optical properties, which were performed in the Negev desert of Israel continuously for about eight years, suggest a potential for deriving a relationship between chemical composition and light absorption properties, in particular the spectral single-scattering albedo. The two main data sets of the present study were obtained by a sun/sky radiometer and a stacked filter unit sampler that collects particles in coarse and fine size fractions. Analysis of chemical and optical data showed the presence of mixed dust and pollution aerosol in the study area, although their sources appear to be different. Spectral SSA showed an evident response to increased concentrations of iron, black carbon equivalent matter, and their mixing state. A relationship that relates the spectral SSA, the percentage of iron in total particulate mass, and the pollution components was derived. Results calculated, using this relationship, were compared with measurements from dust episodes in several locations around the globe. The comparison showed reasonable agreement between the calculated and the observed iron concentrations, and supported the validity of the suggested approach for the estimation of iron concentrations in mineral dust.
Contribution of residential wood combustion and other sources to hourly winter aerosol in Northern Sweden determined by positive matrix factorization
Authors: Krecl P. , Hedberg Larsson E. , Ström J. , Johansson C.
Published: April 2010

Abstract. The combined effect of residential wood combustion (RWC) emissions with stable atmospheric conditions, which frequently occurs in Northern Sweden during wintertime, can deteriorate the air quality even in small towns. To estimate the contribution of RWC to the total atmospheric aerosol loading, positive matrix factorization (PMF) was applied to hourly mean particle number size distributions measured in a residential area in Lycksele during winter 2005/2006. The sources were identified based on the particle number size distribution profiles of the PMF factors, the diurnal contributions patterns estimated by PMF for both weekends and weekdays, and correlation of the modeled particle number concentration per factor with measured aerosol mass concentrations (PM10, PM1, and light-absorbing carbon MLAC) Through these analyses, the factors were identified as local traffic (factor 1), local RWC (factor 2), and local RWC plus long-range transport (LRT) of aerosols (factor 3). In some occasions, the PMF model could not separate the contributions of local RWC from background concentrations since their particle number size distributions partially overlapped. As a consequence, we report the contribution of RWC as a range of values, being the minimum determined by factor 2 and the possible maximum as the contributions of both factors 2 and 3. A multiple linear regression (MLR) of observed PM10, PM1, total particle number, and MLAC concentrations is carried out to determine the source contribution to these aerosol variables. The results reveal RWC is an important source of atmospheric particles in the size range 25–606 nm (44–57%), PM10 (36–82%), PM1 (31–83%), and MLAC (40–76%) mass concentrations in the winter season. The contribution from RWC is especially large on weekends between 18:00 LT and midnight whereas local traffic emissions show similar contributions every day.
Envisat MIPAS measurements of CFC-11: retrieval, validation, and climatology
Authors: Hoffmann L. , Kaufmann M. , Spang R. , Müller R. , Remedios J. J. , Moore D. P. , Volk C. M. , von Clarmann T. , Riese M.
Published: April 2010

Abstract. From July 2002 to March 2004 the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) aboard the European Space Agency's Environmental Satellite (Envisat) measured nearly continuously mid infrared limb radiance spectra. These measurements are utilised to retrieve the global distribution of the chlorofluorocarbon CFC-11 by applying a new fast forward model for Envisat MIPAS and an accompanying optimal estimation retrieval processor. A detailed analysis shows that the total retrieval errors of the individual CFC-11 volume mixing ratios are typically below 10% in the altitude range 10 to 25 km and that the systematic components dominate. Contribution of a priori information to the retrieval results are less than 5 to 10% and the vertical resolution of the observations is about 3 to 4 km in the same vertical range. The data are successfully validated by comparison with several other space experiments, an air-borne in-situ instrument, measurements from ground-based networks, and independent Envisat MIPAS analyses. The retrieval results from 425 000 Envisat MIPAS limb scans are compiled to provide a new climatological data set of CFC-11. The climatology shows significantly lower CFC-11 abundances in the lower stratosphere compared with the Reference Atmospheres for MIPAS (RAMstan V3.1) climatology. Depending on the atmospheric conditions the differences between the climatologies are up to 30 to 110 ppt (45 to 150%) at 19 to 27 km altitude. Additionally, time series of CFC-11 mean abundance and variability for five latitudinal bands are presented. The observed CFC-11 distributions can be explained by the residual mean circulation and large-scale eddy-transports in the upper troposphere and lower stratosphere. The new CFC-11 data set is well suited for further scientific studies.
Validation of aerosol and cloud layer structures from the space-borne lidar CALIOP using a ground-based lidar in Seoul, Korea
Authors: Kim S.-W. , Berthier S. , Raut J.-C. , Chazette P. , Dulac F. , Yoon S.-C.
Published: April 2010

Abstract. We present initial validation results of the space-borne lidar CALIOP onboard CALIPSO satellite using coincidental observations from a ground-based lidar in Seoul National University (SNU), Seoul, Korea (37.46° N, 126.95° E). We analyze six selected cases between September 2006 and February 2007, including 3 daytime and 3 night-time observations and covering different types of clear and cloudy atmospheric conditions. Apparent scattering ratios calculated from the two lidar measurements of total attenuated backscatter at 532 nm show similar aerosol and cloud layer structures both under cloud-free conditions and in cases of multiple aerosol layers underlying semi-transparent cirrus clouds. Agreement on top and base heights of cloud and aerosol layers is generally within 0.10 km, particularly during night-time. This result confirms that the CALIPSO science team algorithms for the discrimination of cloud and aerosol as well as for the detection of layer top and base altitude provide reliable information in such atmospheric conditions. This accuracy of the planetary boundary layer top height under cirrus cloud appears, however, limited during daytime. Under thick cloud conditions, however, information on the cloud top (bottom) height only is reliable from CALIOP (ground-based lidar) due to strong signal attenuations. However, simultaneous space-borne CALIOP and ground-based SNU lidar (SNU-L) measurements complement each other and can be combined to provide full information on the vertical distribution of aerosols and clouds. An aerosol backscatter-to-extinction ratio (BER) estimated from lidar and sunphotometer synergy at the SNU site during the CALIOP overpass is assessed to be 0.023±0.004 sr−1 (i.e. a lidar ratio of 43.2±6.2 sr) from CALIOP and 0.027±0.006 sr−1 (37.4±7.2 sr) from SNU-L. For aerosols within the planetary boundary layer under cloud-free conditions, the aerosol extinction profiles from both lidars are in agreement within about 0.02 km−1. Under semi-transparent cirrus clouds, such profiles also show good agreement for the night-time CALIOP flight, but large discrepancies are found for the daytime flights due to a small signal-to-noise ratio of the CALIOP data.
CCN activation experiments with adipic acid: effect of particle phase and adipic acid coatings on soluble and insoluble particles
Authors: Hings S. S. , Wrobel W. C. , Cross E. S. , Worsnop D. R. , Davidovits P. , Onasch T. B.
Published: April 2010

Abstract. Slightly soluble atmospherically relevant organic compounds may influence particle CCN activity and therefore cloud formation. Adipic acid is a frequently employed surrogate for such slightly soluble organic materials. The 11 published experimental studies on the CCN activity of adipic acid particles are not consistent with each other nor do they, in most cases, agree with the Köhler theory. The CCN activity of adipic acid aerosol particles was studied over a significantly wider range of conditions than in any previous single study. The work spans the conditions of the previous studies and also provides alternate methods for producing "wet" (deliquesced solution droplets) and dry adipic acid particles without the need to produce them by atomization of aqueous solutions. The experiments suggest that the scatter in the previously published CCN measurements is most likely due to the difficulty of producing uncontaminated adipic acid particles by atomization of solutions and possibly also due to uncertainties in the calibration of the instruments. The CCN activation of the small (dm<150 nm) initially dry particles is subject to a deliquescence barrier, while for the larger particles the activation follows the Köhler curve. Wet adipic acid particles follow the Köhler curve over the full range of particle diameters studied. In addition, the effect of adipic acid coatings on the CCN activity of both soluble and insoluble particles has also been studied. When a water-soluble core is coated by adipic acid, the CCN-hindering effect of particle phase is eliminated. An adipic acid coating on hydrophobic soot yields a CCN active particle. If the soot particle is relatively small (dcore≤102 nm), the CCN activity of the coated particles approaches the deliquescence line of adipic acid, suggesting that the total size of the particle determines CCN activation and the soot core acts as a scaffold.
Influence of Giant CCN on warm rain processes in the ECHAM5 GCM
Authors: Posselt R. , Lohmann U.
Published: April 2010

Abstract. Increased Cloud Condensation Nuclei (CCN) load due to anthropogenic activity might lead to non-precipitating clouds because the cloud drops become smaller (for a constant liquid water content) and, therefore, less efficient in rain formation (aerosol indirect effect). Adding giant CCN (GCCN) into such a cloud can initiate precipitation (namely, drizzle) and, therefore, might counteract the aerosol indirect effect. The effect of GCCN on global climate on warm clouds and precipitation within the ECHAM5 General Circulation Model (GCM) is investigated. Therefore, the newly introduced prognostic rain scheme (Posselt and Lohmann, 2007) is applied so that GCCN are directly activated into rain drops. The ECHAM5 simulations with incorporated GCCN show that precipitation is affected only locally. On the global scale, the precipitation amount does not change. Cloud properties like total water (liquid + rain water) and cloud drop number show a larger sensitivity to GCCN. Depending on the amount of added GCCN, the reduction of total water and cloud drops account for up to 20% compared to the control run without GCCN. Thus, the incorporation of the GCCN accelerate the hydrological cycle so that clouds precipitate faster (but not more) and less condensed water is accumulated in the atmosphere. An estimate of the anthropogenic aerosol indirect effect on the climate is obtained by comparing simulations for present-day and pre-industrial climate. The introduction of the prognostic rain scheme lowered the anthropogenic aerosol indirect effect significantly compared to the standard ECHAM5 with the diagnostic rain scheme. The incorporation of the GCCN changes the model state, especially the cloud properties like TWP and Nl. The precipitation changes only locally but globally the precipitation is unaffected because it has to equal the global mean evaporation rate. Changing the cloud properties leads to a local reduction of the aerosol indirect effect and, hence, partly compensating for the increased anthropogenic CCN concentrations in that regions. Globally, the aerosol indirect effect is nearly the same for all simulations.
Chemistry of the Antarctic Boundary Layer and the Interface with Snow: an overview of the CHABLIS campaign
Authors: Jones A. E. , Wolff E. W. , Salmon R. A. , Bauguitte S. J.-B. , Roscoe H. K. , Anderson P. S. , Ames D. , Clemitshaw K. C. , Fleming Z. L. , Bloss W. J. , Heard D. E. , Lee J. D. , Read K. A. , Hamer P. , Shallcross D. E. , Jackson A. V. , Walker S. L. , Lewis A. C. , Mills G. P. , Plane J. M. C. , Saiz-Lopez A. , Sturges W. T. , Worton D. R.
Published: April 2010

Abstract. CHABLIS (Chemistry of the Antarctic Boundary Layer and the Interface with Snow) was a collaborative UK research project aimed at probing the detailed chemistry of the Antarctic boundary layer and the exchange of trace gases at the snow surface. The centre-piece to CHABLIS was the measurement campaign, conducted at the British Antarctic Survey station, Halley, in coastal Antarctica, from January 2004 through to February 2005. The campaign measurements covered an extremely wide range of species allowing investigations to be carried out within the broad context of boundary layer chemistry. Here we present an overview of the CHABLIS campaign. We provide details of the measurement location and introduce the Clean Air Sector Laboratory (CASLab) where the majority of the instruments were housed. We describe the meteorological conditions experienced during the campaign and present supporting chemical data, both of which provide a context within which to view the campaign results. Finally we provide a brief summary of highlights from the measurement campaign. Unexpectedly high halogen concentrations profoundly affect the chemistry of many species at Halley throughout the sunlit months, with a secondary role played by emissions from the snowpack. This overarching role for halogens in coastal Antarctic boundary layer chemistry was completely unanticipated, and the results have led to a step-change in our thinking and understanding.
Diagnosing recent CO emissions and ozone evolution in East Asia using coordinated surface observations, adjoint inverse modeling, and MOPITT satellite data
Authors: Tanimoto H. , Sawa Y. , Yonemura S. , Yumimoto K. , Matsueda H. , Uno I. , Hayasaka T. , Mukai H. , Tohjima Y. , Tsuboi K. , Zhang L.
Published: April 2010

Abstract. Simultaneous ground-based measurements of ozone (O3) and carbon monoxide (CO) were conducted in March 2005 as part of the East Asian Regional Experiment (EAREX) 2005 under the umbrella of the Atmospheric Brown Clouds (ABC) project. Multiple air quality monitoring networks were integrated by performing intercomparison of individual calibration standards and measurement techniques to ensure comparability of ambient measurements, along with providing consistently high time-resolution measurements of O3 and CO at the surface sites in East Asia. Ambient data collected from eight surface stations were compared with simulation results obtained by a regional chemistry transport model to infer recent changes in CO emissions from East Asia. Our inverse estimates of the CO emissions from China up to 2005 suggested an increase of 16% since 2001, in good agreement with the recent MOPITT satellite observations and the bottom-up estimates up to 2006. The O3 enhancement relative to CO in continental pollution plumes traversed in the boundary layer were examined as a function of transport time from the Asian continent to the western Pacific Ocean. The observed ΔO3/ΔCO ratios show increasing tendency during eastward transport events due likely to en-route photochemical O3 formation, suggesting that East Asia is an important O3 source region during spring.
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 an OH x residence time of 1.1×1010 molec OH cm−3 s, corresponding to 3 to 16×107 molecules cm−3 OH within the forest canopy for a 420 to 70 s canopy residence time. We show that ΣAN(g+p) fluxes are consistent with this range in OH if the reaction of OH with ΣANs produces either HNO3 or NO2 with a 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 Quasi-biennial Oscillation and annual variations in tropical ozone from SHADOZ and HALOE
Authors: Witte J. C. , Schoeberl M. R. , Douglass A. R. , Thompson A. M.
Published: April 2010

Abstract. We examine the tropical ozone mixing ratio perturbation fields generated from a monthly ozone climatology using 1998 to 2006 ozonesonde data from the Southern Hemisphere Additional Ozonesondes (SHADOZ) network and the 13-year satellite record from 1993 to 2005 obtained from the Halogen Occultation Experiment (HALOE). The long time series and high vertical resolution of the ozone and temperature profiles from the SHADOZ sondes coupled with good tropical coverage north and south of the equator gives a detailed picture of the ozone structure in the lowermost stratosphere down through the tropopause where the picture obtained from HALOE measurements is blurred by coarse vertical resolution. Ozone perturbations respond to annual variations in the Brewer-Dobson Circulation (BDC) in the region just above the cold-point tropopause to around 20 km. Annual cycles in ozone and temperature are well correlated. Above 20 km, ozone and temperature perturbations are dominated by the Quasi-biennial Oscillation (QBO). Both satellite and sonde records show good agreement between positive and negative ozone mixing ratio anomalies and alternating QBO westerly and easterly wind shears from the Singapore rawinsondes with a mean periodicity of 26 months for SHADOZ and 25 months for HALOE. There is a temporal offset of one to three months with the QBO wind shear ahead of the ozone anomaly field. The meridional length scales for the annual cycle and the QBO, obtained using the temperature anomalies and wind shears in the thermal wind equation, compare well with theoretical calculations.
Tracing biomass burning plumes from the Southern Hemisphere during the AMMA 2006 wet season experiment
Authors: Mari C. H. , Cailley G. , Corre L. , Saunois M. , Attié J. L. , Thouret V. , Stohl A.
Published: April 2010

Abstract. The Lagrangian particle dispersion model FLEXPART coupled with daily active fire products provided by the MODIS instrument was used to forecast the intrusions of the southern hemispheric fire plumes in the Northern Hemisphere during the AMMA (African Monsoon Multidisciplinary Analysis) fourth airborne campaign from 25 July to 31 August 2006 (Special Operation Period SOP2_a2). The imprint of the biomass burning plumes over the Gulf of Guinea showed a well marked intraseasonal variability which is controlled by the position and strength of the southern hemispheric African Easterly Jet (AEJ-S). Three different periods were identified which correspond to active and break phases of the AEJ-S: 25 July–2 August (active phase), 3 August–8 August (break phase) and 9 August–31 August (active phase). During the AEJ-S active phases, the advection of the biomass burning plumes out over the Atlantic ocean was efficient in the mid-troposphere. During the AEJ-S break phases, pollutants emitted by fires were trapped over the continent where they accumulated. The continental circulation increased the possibility for the biomass burning plumes to reach the convective regions located further north. As a consequence, biomass burning plumes were found in the upper troposphere over the Gulf of Guinea during the AEJ-S break phase. Observational evidences from the ozonesounding network at Cotonou and the carbon monoxide measured by MOPITT confirmed the alternation of the AEJ-S phases with low ozone and CO in the mid-troposphere over the Gulf of Guinea during the break phase.
A computationally-efficient secondary organic aerosol module for three-dimensional air quality models
Authors: Liu P. , Zhang Y.
Published: April 2010

Abstract. Accurately simulating secondary organic aerosols (SOA) in three-dimensional (3-D) air quality models is challenging due to the complexity of the physics and chemistry involved and the high computational demand required. A computationally-efficient yet accurate SOA module is necessary in 3-D applications for long-term simulations and real-time air quality forecasting. A coupled gas and aerosol box model (i.e., 0-D CMAQ-MADRID 2) is used to optimize relevant processes in order to develop such a SOA module. Solving the partitioning equations for condensable volatile organic compounds (VOCs) and calculating their activity coefficients in the multicomponent mixtures are identified to be the most computationally-expensive processes. The two processes can be speeded up by relaxing the error tolerance levels and reducing the maximum number of iterations of the numerical solver for the partitioning equations for organic species; conditionally activating organic-inorganic interactions; and parameterizing the calculation of activity coefficients for organic mixtures in the hydrophilic module. The optimal speed-up method can reduce the total CPU cost by up to a factor of 31.4 from benchmark under the rural conditions with 2 ppb isoprene and by factors of 10–71 under various test conditions with 2–10 ppb isoprene and >40% relative humidity while maintaining ±15% deviation. These speed-up methods are applicable to other SOA modules that are based on partitioning theories.