bluuebunny/crossref_metadata_2025 huggingface dataset:
DMS and MSA measurements in the Antarctic boundary layer: impact of BrO on MSA production
Authors: Read K. A. , Lewis A. C. , Bauguitte S. , Rankin A. M. , Salmon R. A. , Wolff E. W. , Saiz-Lopez A. , Bloss W. J. , Heard D. E. , Lee J. D. , Plane J. M. C.
Published: April 2010

Abstract. In situ measurements of dimethyl sulphide (DMS) and methane sulphonic acid (MSA) were made at Halley Station, Antarctica (75°35´S, 26°19W) during February 2004–February 2005 as part of the CHABLIS (Chemistry of the Antarctic boundary layer and the interface with snow) project. DMS was present in the atmosphere at Halley all year (average 38.1±43 pptV) with a maximum monthly average value of 113.6±52 pptV in February 2004 coinciding temporally with a minimum in sea extent. Whilst seasonal variability and interannual variability can be attributed to a number of factors, short term variability appeared strongly dependent on air mass origin and trajectory pressure height. The MSA and derived non-sea salt sulphate (nss-SO42−) measurements showed no correlation with those of DMS (regression R2=0.039, and R2=0.001, respectively) in-line with the complexity of DMS fluxes, conflicting oxidation routes, transport of air masses and variable spatial coverage of both sea-ice and phytoplankton. MSA was generally low throughout the year, with an annual average of 42 ng m−3 (9.8±13.2 pptV), however MSA: nss-SO42− ratios were high implying a dominance of the addition oxidation route for DMS. Including BrO measurements into MSA production calculations demonstrated the significance of BrO on DMS oxidation within this region of the atmosphere in austral summer. Assuming an 80% yield of DMSO from the reaction of DMS+BrO, an atmospheric concentration of BrO equal to 3 pptV increased the calculated MSA production from DMS by a factor of 9 above that obtained when considering only reaction with the hydroxyl radical.
Impact of the new HNO3-forming channel of the HO2+NO reaction on tropospheric HNO3, NOx, HOx and ozone
Authors: Cariolle D. , Evans M. J. , Chipperfield M. P. , Butkovskaya N. , Kukui A. , Le Bras G.
Published: April 2010

Abstract. We have studied the impact of the recently established reaction NO+HO2→HNO3 on atmospheric chemistry. A pressure and temperature-dependent parameterisation of this minor channel of the NO+HO2→NO2+OH reaction has been included in both a 2-D stratosphere-troposphere model and a 3-D tropospheric chemical transport model (CTM). Significant effects on the nitrogen species and hydroxyl radical concentrations are found throughout the troposphere, with the largest percentage changes occurring in the tropical upper troposphere (UT). Including the reaction leads to a reduction in NOx everywhere in the troposphere, with the largest decrease of 25% in the tropical and southern hemisphere UT. The tropical UT also has a corresponding large increase in HNO3 of 25%. OH decreases throughout the troposphere with the largest reduction of over 20% in the tropical UT. Mean global decreases in OH are around 13% which leads to a increase in CH4 lifetime of 5%. Due to the impact of decreased NOx on the OH:HO2 partitioning, modelled HO2 actually increases in the tropical UT on including the new reaction. The impact on tropospheric ozone is a decrease in the range 5 to 12%, with the largest impact in the tropics and southern hemisphere. Comparison with observations shows that in the region of largest changes, i.e. the tropical UT, the inclusion of the new reaction tends to degrade the model agreement. Elsewhere the model comparisons are not able to critically assess the impact of including this reaction. Only small changes are calculated in the minor species distributions in the stratosphere.
Nanoparticle formation in the exhaust of vehicles running on ultra-low sulfur fuel
Authors:   Hua Du,   Fangqun Yu
Published: April 2010

Abstract. The concern of adverse health impacts from exposure to vehicle-emitted nanoparticles has been escalating over the past few years. In order to meet more stringent EPA emission standards for particle mass emissions, advanced exhaust after-treatment systems such as continuously regenerating diesel particle filters (CRDPFs) have to be employed on vehicles and fuel with ultra-low sulfur is to be used. Although CRDPFs were found to be effective in reducing particle mass emissions, they were revealed to increase the potential of volatile nanoparticle formation. Significant nanoparticle concentrations have also been detected for vehicles running on ultra-low sulfur fuel but without CRDPFs. The main focus of this paper is the formation and evolution of nanoparticles in exhaust plume under ultra-low sulfur condition. Such study is necessary to project future nanoparticle emissions as fuel compositions and after-treatment systems change. We have carried out a comprehensive quantitative assessment of the effects of enhanced sulfur conversion efficiency, sulfur storage/release, and presence of non-volatile cores on nanoparticle formation using a detailed composition resolved aerosol microphysical model with a recently improved H2SO4-H2O homogeneous nucleation (BHN) module. Two well-controlled case studies show good agreement between model predictions and measurements in terms of particle size distribution and temperature dependence of particle formation rate, which leads us to conclude that BHN is the main source of nanoparticles for vehicles equipped with CRDPFs. We found that the employment of CRDPFs may lead to the higher number concentration of nanoparticles (but smaller size) in the exhaust of vehicles running on ultra-low sulfur fuel compared to those emitted from vehicles running on high sulfur fuel. We have also shown that the sulfate storage and release effect can lead to significant enhancement in nanoparticle production under favorable conditions. For vehicles running on ultra-low sulfur fuel but without CRDPFs, the BHN is negligible; however, the condensation of low volatile organic compounds on nanometer-sized non-volatile cores may explain the observed nucleation mode particles.
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 are poor when compared to winter months. MODIS-Terra AOT data was available only about 50% of the time due to cloud cover and favorable surface conditions. However, the mean difference in monthly mean PM2.5 was less than 2.2 μgm−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 without 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.
The role of climate and emission changes in future air quality over southern Canada and northern Mexico
Authors: Tagaris E. , Liao K.-J. , Manomaiphiboon K. , He S. , Woo J.-H. , Amar P. , Russell A. G.
Published: April 2010

Abstract. Potential impacts of global climate and emissions changes on regional air quality over southern (western and eastern) Canada and northern Mexico are examined by comparing future summers' (i.e., 2049–2051) average regional O3 and PM2.5 concentrations with historic concentrations (i.e., 2000–2002 summers). Air quality modeling was conducted using CMAQ and meteorology downscaled from the GISS-GCM using MM5. Emissions for North America are found using US EPA, Mexican and Canadian inventories and projected emissions following CAIR and IPCC A1B emissions scenario. Higher temperatures for all sub-regions and regional changes in mixing height, insolation and precipitation are forecast in the 2049–2051 period. Future emissions are calculated to be lower over both Canadian sub-regions, but higher over northern Mexico. Global climate change, alone, is predicted to affect PM2.5 concentrations more than O3: M8hO3 concentrations are estimated to be slightly different in all examined sub-regions while PM2.5 concentrations are estimated to be higher over both Canadian sub-regions (8% over western and 3% over eastern) but 11% lower over northern Mexico. Climate change combined with the projected emissions lead to greater change in pollutant concentrations: M8hO3 concentrations are simulated to be 6% lower over western Canada and 8% lower over eastern Canada while PM2.5 concentrations are simulated to be 5% lower over western Canada and 11% lower over eastern Canada. Although future emissions over northern Mexico are projected higher, pollutant concentrations are simulated to be lower due to US emissions reductions. Global climate change combined with the projected emissions will decrease M8hO3 4% and PM2.5 17% over northern Mexico.
Diagnosing recent CO emissions and springtime O3 evolution in East Asia using coordinated ground-based observations of O3 and CO during the East Asian Regional Experiment (EAREX) 2005 campaign
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 chemical 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. Comparison of the observed δO3/Δ CO ratios and their modeled spatial distributions suggests an increase in the Δ O3/Δ CO ratio due likely to en-route photochemical O3 formation during eastward transport, confirming that East Asia is an important O3 source region during spring.
Technical Note: REFIR-PAD level 1 data analysis and performance characterization
Authors: Bianchini G. , Palchetti L.
Published: April 2010

Abstract. The outgoing long-wave radiation from the Earth's atmosphere in the far infrared spectral region is mostly unexplored, while is well recognized that the water vapour contribution to greenhouse trapping is dominant in this region. The Radiation Explorer in the Far InfraRed (REFIR) study has proven the feasibility of a space-borne Fourier transform spectrometer able to perform the measurement in the 100–1100 cm−1 range with a resolution of 0.5 cm−1. Following this work a prototype of the spectrometer named REFIR-PAD (Prototype for Applications and Development) has been developed to observe the atmospheric radiance from both ground-based sites and from stratospheric balloon platforms. In this work we describe the REFIR-PAD level 1 data analysis procedure, that, starting from raw instrumental data produces the calibrated atmospheric spectral radiance. Performances of the procedure are also described.
Measurements of UV irradiance within the area of one satellite pixel
Authors: Weihs P. , Blumthaler M. , Rieder H. E. , Kreuter A. , Simic S. , Laube W. , Schmalwieser A. W. , Wagner J. , Tanskanen A.
Published: April 2010

Abstract. A measurement campaign was performed in the region of Vienna and its surroundings from May to July 2007. Within the scope of this campaign erythemal UV was measured at six ground stations within a radius of 30 km. First, the homogeneity of the UV levels within the area of one satellite pixel was studied. Second, the ground UV was compared to ground UV retrieved by the ozone monitoring instrument (OMI) onboard the NASA EOS Aura Spacecraft. During clear sky conditions the difference in erythemal UV measured by the different stations was within the measurement uncertainty of 8%. For partly cloudy conditions and total overcast conditions the discrepancy of momentary values between the stations is up to 200% or even higher. If averages of the UV index over longer time periods are compared the difference between the stations decreases strongly. The agreement is better than 20% within a distance of 10 km between the stations for 3 h averages. The comparison with OMI UV showed for clear sky conditions higher satellite retrieved UV values by on the average approximately 15%. For partly cloudy and overcast conditions the OMI derived surface UV estimates show larger deviation from the ground-based reference data, and even bigger systematic positive bias.
Evaluation of the MERIS aerosol product over land with AERONET
Authors: Vidot J. , Santer R. , Aznay O.
Published: April 2010

Abstract. The Medium Resolution Imaging Spectrometer (MERIS) launched in February 2002 on-board the ENVISAT spacecraft is making global observations of top-of-atmosphere (TOA) radiances. Aerosol optical properties are retrieved over land using Look-Up Table (LUT) based algorithm and surface reflectances in the blue and the red spectral regions. We compared instantaneous aerosol optical thicknesses retrieved by MERIS in the blue and the red at locations containing sites within the Aerosol Robotic Network (AERONET). Between 2002 and 2005, a set of 500 MERIS images were used in this study. The result shows that, over land, MERIS aerosol optical thicknesses are well retrieved in the blue and poorly retrieved in the red, leading to an underestimation of the Angstrom coefficient. Correlations are improved by applying a simple criterion to avoid scenes probably contaminated by thin clouds. To investigate the weakness of the MERIS algorithm, ground-based radiometer measurements have been used in order to retrieve new aerosol models, based on their Inherent Optical Properties (IOP). These new aerosol models slightly improve the correlation, but the main problem of the MERIS aerosol product over land can be attributed to the surface reflectance model in the red.
Estimation of the vertical profile of sulfur dioxide injection into the atmosphere by a volcanic eruption using satellite column measurements and inverse transport modeling
Authors: Eckhardt S. , Prata A. J. , Seibert P. , Stebel K. , Stohl A.
Published: April 2010

Abstract. An analytical inversion method has been developed to estimate the vertical profile of SO2 emissions from volcanic eruptions. The method uses satellite-observed total SO2 columns and an atmospheric transport model (FLEXPART) to exploit the fact that winds change with altitude – thus, the position and shape of the volcanic plume bear information on its emission altitude. The method finds the vertical emission distribution which minimizes the total difference between simulated and observed SO2 columns while also considering a priori information. We have tested the method with the eruption of Jebel at Tair on 30 September 2007 for which a comprehensive observational data set from various satellite instruments (AIRS, OMI, SEVIRI, CALIPSO) is available. Using satellite data from the first 24 h after the eruption for the inversion, we found an emission maximum near 16 km above sea level (asl), and secondary maxima near 5, 9, 12 and 14 km a.s.l. 60% of the emission occurred above the tropopause. The emission profile obtained in the inversion was then used to simulate the transport of the plume over the following week. The modeled plume agrees very well with SO2 total columns observed by OMI, and its altitude and width agree mostly within 1–2 km with CALIPSO observations of stratospheric aerosol produced from the SO2. The inversion result is robust against various changes in both the a priori and the observations. Even when using only SEVIRI data from the first 15 h after the eruption, the emission profile was reasonably well estimated. The method is computationally very fast. It is therefore suitable for implementation within an operational environment, such as the Volcanic Ash Advisory Centers, to predict the threat posed by volcanic ash for air traffic. It could also be helpful for assessing the sulfur input into the stratosphere, be it in the context of volcanic processes or also for proposed geo-engineering techniques to counteract global warming.
The roles of convection, extratropical mixing, and in-situ freeze-drying in the tropical tropopause layer
Authors: Read W. G. , Schwartz M. J. , Lambert A. , Su H. , Livesey N. J. , Daffer W. H. , Boone C. D.
Published: April 2010

Abstract. Mechanisms for transporting and dehydrating air across the tropical tropopause layer (TTL) are investigated with a conceptual two dimensional (2-D) model. The 2-D TTL model combines the Holton and Gettelman cold trap dehydration mechanism (Holton and Gettelman, 2001) with the two column convection model of Folkins and Martin (2005). We investigate 3 possible transport scenarios through the TTL: 1) slow uniform ascent across the level of zero radiative heating without direct convective mixing, 2) convective mixing of H2O vapor at 100% relative humidity with respect to ice (RHi) with no ice retention, and 3) convective mixing of extremely subsaturated air (convective dehydration) with sufficient ice retention such that total H2O is 100% RHi. The three mechanisms produce similar seasonal cycles for H2O that are in good quantitative agreement with the Aura Microwave Limb Sounder (MLS) measurements. We use Aura MLS measurement of CO and Atmospheric Chemistry Experiment-Fourier Transform Spectrometer measurement of HDO to distinguish among the transport mechanisms. Model comparisons with the observations support the view that H2O is predominantly controlled by the cold trap temperature but the trace species CO and HDO show evidence of extratropical mixing and convective mixing of subsaturated tropospheric air and lofted ice. The model provides some insight into the processes affecting the long term trends observed in stratospheric H2O.
Retrieval of stratospheric aerosol size information from OSIRIS limb scattered sunlight spectra
Authors: Bourassa A. E. , Degenstein D. A. , Llewellyn E. J.
Published: April 2010

Abstract. Recent work has shown that the retrieval of stratospheric aerosol vertical profiles is possible using limb scattered sunlight measurements at optical wavelengths. The aerosol number density profile is retrieved for an assumed particle size distribution and composition. This result can be used to derive the extinction at the measured wavelength. However, large systematic error can result from the uncertainty in the assumed size distribution when the result is used to estimate the extinction at other wavelengths. It is shown in this work that the addition of information obtained from the near infrared limb radiance profile at 1530 nm measured by the imaging module of the OSIRIS instrument yields an indication of the aerosol size distribution profile that can be used to improve the fidelity of the retrievals. A comparison of the estimated extinction profile at 1020 nm with coincident occultation measurements demonstrates agreement to within approximately 15% from 12 to 27 km altitude.
Cloud system resolving model study of the roles of deep convection for photo-chemistry in the TOGA COARE/CEPEX region
Authors: Salzmann M. , Lawrence M. G. , Phillips V. T. J. , Donner L. J.
Published: April 2010

Abstract. A cloud system resolving model including photo-chemistry (CSRMC) has been developed based on a prototype version of the Weather Research and Forecasting (WRF) model and is used to study influences of deep convection on chemistry in the TOGA COARE/CEPEX region. Lateral boundary conditions for trace gases are prescribed from global chemistry-transport simulations, and the vertical advection of trace gases by large scale dynamics, which is not reproduced in a limited area cloud system resolving model, is taken into account. The influences of in situ lightning and other processes on NOx, O3, and HOx(=HO2+OH), in the vicinity of the deep convective systems are investigated in a 7-day 3-D 248×248 km2 horizontal domain simulation and several 2-D sensitivity runs with a 500 km horizontal domain. The fraction of NOx chemically lost within the domain varies between 20 and 24% in the 2-D runs, but is negligible in the 3-D run, in agreement with a lower average NOx concentration in the 3-D run despite a greater number of flashes. In all runs, in situ lightning is found to have only minor impacts on the local O3 budget. Mid-tropospheric entrainment is more important on average for the upward transport of O3 in the 3-D run than in the 2-D runs, but at the same time undiluted O3-poor air from the marine boundary layer reaches the upper troposphere more frequently in the 3-D run than in the 2-D runs, indicating the presence of undiluted convective cores. Near zero O3 volume mixing ratios due to the reaction with lightning-produced NO are only simulated in a 2-D sensitivity run with an extremely high number of NO molecules per flash, which is outside the range of current estimates. Stratosphere to troposphere transport of O3 is simulated to occur episodically in thin filaments, but on average net upward transport of O3 from below ~16 km is simulated in association with mean large scale ascent in the region. Ozone profiles in the TOGA COARE/CEPEX region are suggested to be strongly influenced by the intra-seasonal (Madden-Julian) oscillation.
UV albedo of arctic snow in spring
Authors: Meinander O. , Kontu A. , Lakkala K. , Heikkilä A. , Ylianttila L. , Toikka M.
Published: April 2010

Abstract. The relevance of snow for climate studies is based on its physical properties, such as high surface reflectivity. Surface ultraviolet (UV) albedo is an essential parameter for various applications based on radiative transfer modeling. Here, new continuous measurements of the local UV albedo of natural Arctic snow were made at Sodankylä (67.37° N, 26.63° E, 179 m a.s.l.) during the spring of 2007. The data were logged at 1-min intervals. The accumulation of snow was up to 68 cm. The surface layer thickness varied from 0.5 to 35 cm with the snow grain size between 0.2 and 2.5 mm. The midday erythemally weighted UV albedo ranged from 0.6 to 0.8 in the accumulation period and 0.5–0.7 during melting. During the snow melt period, under cases of an almost clear sky and variable cloudiness, an unexpected diurnal decrease of 0.05 in albedo soon after midday, and recovery thereafter, was detected. This diurnal decrease in albedo was found to be asymmetric with respect to solar midday, thus indicating a change in the properties of the snow. Independent UV albedo results with two different types of instruments confirm these findings. The measured temperature of the snow surface was below 0°C on the following mornings. Hence, the reversible diurnal change, evident for ~1–2 h, could be explained by the daily metamorphosis of the surface of the snowpack, in which the temperature of the surface increases, melting some of the snow to liquid water, after which the surface freezes again.
Study of suitability of cheap 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 degrees), 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 calculated by means of the LibRadtran package and the measured ratio of UV-A/UV-B irradiance 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.
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 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 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. Regional through global budgets for biogenic and pyrogenic emissions were roughly estimated. Coupled with previous measurements of secondary aerosol growth 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. The global budgets confirm that biogenic emissions and biomass burning are the two largest global sources of NMOC with an estimated production of approximately 1000 and 500 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.
Remote sensing of cloud sides of deep convection: towards a three-dimensional retrieval of cloud particle size profiles
Authors: Zinner T. , Marshak A. , Lang S. , Martins J. V. , Mayer B.
Published: April 2010

Abstract. The cloud scanner sensor is a central part of a recently proposed satellite remote sensing concept – the three-dimensional (3-D) cloud and aerosol interaction mission (CLAIM-3D) combining measurements of aerosol characteristics in the vicinity of clouds and profiles of cloud microphysical characteristics. Such a set of collocated measurements will allow new insights in the complex field of cloud-aerosol interactions affecting directly the development of clouds and precipitation, especially in convection. The cloud scanner measures radiance reflected or emitted by cloud sides at several wavelengths to derive a profile of cloud particle size and thermodynamic phase. For the retrieval of effective size a Bayesian approach was adopted and introduced in a preceding paper. In this paper the potential of the approach, which has to account for the complex three-dimensional nature of cloud geometry and radiative transfer, is tested in realistic cloud observing situations. In a fully simulated environment realistic cloud resolving modelling provides complex 3-D structures of ice, water, and mixed phase clouds, from the early stage of convective development to mature deep convection. A three-dimensional Monte Carlo radiative transfer is used to realistically simulate the aspired observations. A large number of cloud data sets and related simulated observations provide the database for an experimental Bayesian retrieval. An independent simulation of an additional cloud field serves as a synthetic test bed for the demonstration of the capabilities of the developed retrieval techniques.
Applicability of condensation particle counters to measure atmospheric clusters
Authors: Sipilä M. , Lehtipalo K. , Kulmala M. , Petäjä T. , Junninen H. , Aalto P. P. , Manninen H. E. , Vartiainen E. , Riipinen I. , Kyrö E.-M. , Curtius J. , Kürten A. , Borrmann S. , O'Dowd C. D.
Published: April 2010

Abstract. The ambient and laboratory molecular and ion clusters were investigated. Here we present data on the ambient concentrations of both charged and uncharged molecular clusters as well as the performance of a pulse height condensation particle counter (PH-CPC) and an expansion condensation particle counter (E-CPC). The ambient molecular cluster concentrations were measured using both instruments, and they were deployed in conjunction with ion spectrometers and other aerosol instruments in Hyytiälä, Finland at the SMEAR II station during 1 March to 30 June 2007. The observed cluster concentrations varied and were from ca. 1000 to 100 000 cm−3. Both instruments showed similar concentrations. The average size of detected clusters was approximately 1.8 nm. As the atmospheric measurements at sub 2-nm particles and molecular clusters are a challenging task, and we were most likely unable to detect the smallest clusters, the reported concentrations are our best estimates for minimum cluster concentrations in boreal forest environment.
Growth-deviation model to understand the perceived variety of falling snow
Authors: Nelson J.
Published: April 2010

Abstract. What is the source of snow-crystal variety? This question is answered using a model of snow-crystal growth in a cloud. In the model, crystals start under various initial cloud-crystal conditions, and then encounter growth perturbations from random air-temperature deviations along simple crystal trajectories. To obtain distributions of these deviations, I analyzed recent high-resolution measurements of cloud updrafts and temperatures. The trajectories and distributions are used to estimate the number of possible snow crystal shapes, to a given viewing resolution, from a range of initial conditions. The logarithm of this number, defined here as the perceived shape variety or "diversity", is dominated not by the range of conditions, but rather by the air-temperature deviations along a trajectory. This qualitative result is independent of the viewing resolution. Thus, temperature deviations are the main source of crystal diversity. When plotted against the crystal's initial temperature (here –11 to –19°C), the curve is mitten-shaped, with a main peak at –15.4°C and a smaller, sharper peak near –14.4°C. The mitten shape arises from temperature trends in the crystal's terminal fallspeed and prism-face growth rate. Specifically, the two diversity peaks are due to maxima in growth-rate sensitivity to temperature near –15.4 and –14.0°C. Applying the results to all snow crystals ever formed, then, to 1-μm resolution, all crystals that began near –15°C would appear unique, but some that began near –11°C would not.
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, such as adipic acid, may influence particle CCN activity and therefore cloud formation. 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 and dry adipic acid particles without the need to produce them by atomization of aqueous solutions. The CCN effect of adipic acid coatings on both soluble and insoluble particles has also been studied. The CCN activation of the small (dm
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% and that the systematic components are dominating. Contribution of a priori information to the retrieval results are less than 5 to 10%. The vertical resolution of the observations is about 3 to 4 km. 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.
Simulation of dust aerosol and its regional feedbacks over East Asia using a regional climate model
Authors: Zhang D. F. , Zakey A. S. , Gao X. J. , Giorgi F.
Published: April 2010

Abstract. The ICTP regional climate model (RegCM3) coupled with a desert dust model is used to simulate the radiative forcing and related climate effects of dust aerosols over East Asia. Two sets of experiments encompassing the main dust producing months, February to May, for 10 years (1997–2006) are conducted and inter-compared, one without (Exp. 1) and one with (Exp. 2) the radiative effects of dust aerosols. The simulation results are evaluated against ground station and satellite data. The model captures the basic observed climatology over the area of interest. The spatial and temporal variations of near surface concentration, mass load, and emission of dust aerosols from the main source regions are reproduced by model, with the main model deficiency being an overestimate of dust amount over the source regions and underestimate downwind of these source areas. Both the top-of-the-atmosphere (TOA) and surface radiative fluxes are decreased by dust and this causes a surface cooling locally up to −1°C. The inclusion of dust radiative forcing leads to a reduction of dust emission in the East Asia source regions, which is mainly caused by an increase in local stability and a corresponding decrease in dust lifting. Our results indicate that dust effects should be included in the assessment of climate change over East Asia.
Spatiotemporal variations of NOy species in the northern latitudes stratosphere measured with the balloon-borne MIPAS instrument
Authors: Wiegele A. , Kleinert A. , Oelhaf H. , Ruhnke R. , Wetzel G. , Friedl-Vallon F. , Lengel A. , Maucher G. , Nordmeyer H. , Fischer H.
Published: April 2010

Abstract. This paper presents the spatiotemporal distribution of NOy species at altitudes between 14 and 31 km as measured with the MIPAS-B instrument on the morning of 21 March 2003 in northern Scandinavia. At lower altitudes, temperature variations and the distribution of ClONO2 and the tracer N2O reveal the dynamics along the cross section through the edge of the late arctic polar vortex. At higher altitudes, continuous measurement before, during, and after sunrise provides information about photochemistry illustrating the evolution of the photochemically active gases NO2 and N2O5 around sunrise. The measured temporal evolution of NO2 and N2O5 is compared to box modelling that is run along backward calculated trajectories. With regard to NO2, there is a good agreement between the model and observations in terms of quantity but the photochemistry in the model is slightly too slow. The comparison of measured and modelled N2O5, however, reveals significant differences of the absolute quantities pointing at a too slow photochemistry in the model.
Variability of the total ozone trend over Europe for the period 1950–2004 derived from reconstructed data
Authors: Krzyścin J. W. , Borkowski J. L.
Published: April 2010

Abstract. Long-term variability of total ozone over Europe is discussed using results of a flexible trend model applied to the reconstructed total ozone data for the period 1950–2004. The data base used was built within the objectives of the COST action 726 "Long-term changes and climatology of UV radiation over Europe". The trend pattern, which comprises both anthropogenic and "natural" component, is not a priori assumed but it is a result of a smooth curve fit to the zonal monthly means and monthly grid values. The trend values in 5-year and 10-year intervals in cold (October-next year April) and warm (May–September) seasons are calculated as the differences between the smooth curve values at the end and beginning of selected time intervals divided by length of the intervals. The confidence intervals for the trend values are calculated by the block bootstrapping. The statistically significant negative trends are found almost over whole Europe only in the period 1985–1994. Negative trends up to −3% per decade appeared over small areas in earlier periods when the anthropogenic forcing on the ozone layer was weak. The statistically positive trends are found only during warm seasons 1995–2004 over Svalbard archipelago. The reduction of ozone level in 2004 relative to that before the satellite era is not dramatic, i.e., up to ~−5% and ~−3.5% in the cold and warm subperiod, respectively. Present ozone level is still depleted over many popular resorts in southern Europe and northern Africa. For high latitude regions the trend overturning could be inferred in last decade (1995–2004) as the ozone depleted areas are not found there in 2004 in spite of substantial ozone depletion in the period 1985–1994.
Gas/particle partitioning of carbonyls in the photooxidation of isoprene and 1,3,5-trimethylbenzene
Authors: Healy R. M. , Wenger J. C. , Metzger A. , Duplissy J. , Kalberer M. , Dommen J.
Published: April 2010

Abstract. A new denuder-filter sampling technique has been used to investigate the gas/particle partitioning behaviour of the carbonyl products from the photooxidation of isoprene and 1,3,5-trimethylbenzene. A series of experiments was performed in two atmospheric simulation chambers at atmospheric pressure and ambient temperature in the presence of NOx and at a relative humidity of approximately 50%. The denuder and filter were both coated with the derivatizing agent O-(2,3,4,5,6-pentafluorobenzyl)-hydroxylamine (PFBHA) to enable the efficient collection of gas- and particle-phase carbonyls respectively. The tubes and filters were extracted and carbonyls identified as their oxime derivatives by GC-MS. The carbonyl products identified in the experiments accounted for around 5% and 10% of the mass of secondary organic aerosol formed from the photooxidation of isoprene and 1,3,5-trimethylbenzene respectively. Experimental gas/particle partitioning coefficients were determined for a wide range of carbonyl products formed from the photooxidation of isoprene and 1,3,5-trimethylbenzene and compared with the theoretical values based on standard absorptive partitioning theory. Photooxidation products with a single carbonyl moiety were not observed in the particle phase, but dicarbonyls, and in particular, glyoxal and methylglyoxal, exhibited gas/particle partitioning coefficients several orders of magnitude higher than expected theoretically. These findings support the importance of heterogeneous chemistry as a pathway for SOA formation and growth during the atmospheric degradation of anthropogenic and biogenic hydrocarbons.
Clouds-Aerosols-Precipitation Satellite Analysis Tool (CAPSAT)
Authors: Lensky I. M. , Rosenfeld D.
Published: April 2010

Abstract. A methodology for representing much of the physical information content of the METEOSAT Second Generation (MSG) geostationary satellite using red-green-blue (RGB) composites of the computed physical values of the picture elements is presented. The physical values are the solar reflectance in the solar channels and brightness temperature in the thermal channels. The main RGB compositions are (1) "Day Natural Colors", presenting vegetation in green, bare surface in brown, sea surface in black, water clouds as white, ice as magenta; (2) "Day Microphysical", presenting cloud microstructure using the solar reflectance component of the 3.9 μm, visible and thermal IR channels; (3) "Night Microphysical", also presenting clouds microstructure using the brightness temperature differences between 10.8 and 3.9 μm; (4) "Day and Night", using only thermal channels for presenting surface and cloud properties, desert dust and volcanic emissions; (5) "Air Mass", presenting mid and upper tropospheric features using thermal water vapor and ozone channels. The scientific basis for these rendering schemes is provided, with examples for the applications. The expanding use of these rendering schemes requires their proper documentation and setting as standards, which is the main objective of this publication.
On the volatility and production mechanisms of newly formed nitrate and water soluble organic aerosol in Mexico City
Authors: Hennigan C. J. , Sullivan A. P. , Fountoukis C. I. , Nenes A. , Hecobian A. , Vargas O. , Case Hanks A. T. , Huey L. G. , Lefer B. L. , Russell A. G. , Weber R. J.
Published: April 2010

Abstract. Measurements of atmospheric gases and fine particle chemistry were made in the Mexico City Metropolitan Area (MCMA) at a site ~30 km down wind of the city center. Ammonium nitrate (NH4NO3) dominated the inorganic aerosol fraction and showed a distinct diurnal signature characterized by rapid morning production and a rapid mid-day concentration decrease. The concentration increase was due to both secondary formation and entrainment from the free troposphere. A majority (approximately two-thirds) of the midday concentration decrease was caused by dilution from boundary layer expansion, however a significant fraction (approximately one-third) of the nitrate loss was due to particle evaporation. The water-soluble organic carbon fraction of fine particles (WSOC) and nitrate were highly correlated (R2=0.80) for the entire three-day analysis period, however the WSOC-nitrate correlation was highest (R2=0.88) between the hours of 08:00–12:45, indicating similar sources and processing during this period. The results show that WSOC also experienced evaporation losses and that a significant fraction of the MCMA secondary organic aerosol (SOA) measured at the surface was semi-volatile.