bluuebunny/crossref_metadata_2025 huggingface dataset:
Impact of ship emissions on the microphysical, optical and radiative properties of marine stratus: a case study
Authors: Schreier M. , Kokhanovsky A. A. , Eyring V. , Bugliaro L. , Mannstein H. , Mayer B. , Bovensmann H. , Burrows J. P.
Published: April 2010

Abstract. Modifications of existing clouds by the exhaust of ships are well-known but poorly studied atmospheric effects which could contribute to climate change. The perturbation of a cloud layer by ship-generated aerosol changes the cloud reflectivity and is identified by long curves in satellite images, known as ship tracks. As ship tracks indicate a pollution of a very clean marine environment and also affect the radiation budget below and above the cloud, it is important to investigate their radiative and climatic effects. Satellite-data from MODIS on Terra are used to examine a scene from 10 February 2003 where ship tracks were detected close to the North American West-Coast. The cloud optical and microphysical properties are derived using a semi-analytical retrieval technique combined with a look-up-table approach. Ship-track-pixels are distinguished from the unperturbed cloud pixels and the optical properties of the former are compared to those of the latter. Within the ship tracks a significant change in the droplet number concentration, the effective radius and the optical thickness are found compared to the unaffected cloud. Significant increase of liquid water could not be confirmed. The resulting cloud properties are used to calculate the radiation budget below and above the cloud. Assuming a mean solar zenith angle, the mean surface radiation below the ship track is decreased by 43.25 Wm−2 and the mean reflectance at TOA is increased by 40.73 Wm−2. For the selected scene the ship emission decreases the solar radiation at the surface by 2.10 Wm−2 and increases the backscattered solar radiation at top of the atmosphere (TOA) by 2.00 Wm−2. Increased backscattered radiation is partly compensated by a decrease of the thermal radiation of 0.43 Wm−2. The resulting net-effect at TOA is an increase of 1.57 Wm−2 corresponding to a negative radiative forcing and a cooling.
Performance of Chemical Ionization Reaction Time-of-Flight Mass Spectrometry (CIR-TOF-MS) for the measurement of atmospherically significant oxygenated volatile organic compounds
Authors: Wyche K. P. , Blake R. S. , Ellis A. M. , Monks P. S. , Brauers T. , Koppmann R. , Apel E.
Published: April 2010

Abstract. The performance of a new chemical ionization reaction time-of-flight mass spectrometer (CIR-TOF-MS) utilising the environment chamber SAPHIR (Simulation of Atmospheric Photochemistry In a large Reaction Chamber – Forschungzentrum Jülich, Germany) is described. The work took place as part of the ACCENT (Atmospheric Composition and Change the European NeTwork for excellence) supported oxygenated volatile organic compound (OVOC) measurement intercomparison during January 2005. The experiment entailed the measurement of 14 different atmospherically significant OVOCs at various mixing ratios in the approximate range 10.0–0.6 ppbV. The CIR-TOF-MS operated throughout the exercise with the hydronium ion (H3O+) as the primary chemical ionization (CI) reagent in order to facilitate proton transfer to the analyte OVOCs. The results show the CIR time-of-flight mass spectrometer is capable of detecting a wide range of atmospheric OVOCs down to sub-ppbV mixing ratios with high accuracy and precision. It is demonstrated that the technique has rapid multi-channel response at the required sensitivity, accuracy and precision for atmospheric OVOC measurements.
Characteristics and error estimations of stratospheric ozone and ozone-related species over Poker Flat (65° N, 147° W), Alaska observed by a ground-based FTIR spectrometer from 2001 to 2003
Authors: Kagawa A. , Kasai Y. , Jones N. B. , Yamamori M. , Seki K. , Murcray F. , Murayama Y. , Mizutani K. , Itabe T.
Published: April 2010

Abstract. It is important to obtain the year-to-year trend of stratospheric minor species in the context of global changes. An important example is the trend in global ozone depletion. The purpose of this paper is to report the accuracy and precision of measurements of stratospheric chemical species that are made at our Poker Flat site in Alaska (65° N, 147° W). Since 1999, minor atmospheric molecules have been observed using a Fourier-Transform solar-absorption infrared Spectrometer (FTS) at Poker Flat. Vertical profiles of the abundances of ozone, HNO3, HCl, and HF for the period from 2001 to 2003 were retrieved from the FTS spectra by using Rodgers' formulation of the Optimal Estimation Method (OEM). The accuracy and precision of the retrievals were estimated by formal error analysis. Errors for the total column were estimated to be 5.3%, 3.4%, 5.9%, and 5.3% for ozone, HNO3, HCl, and HF, respectively. The ozone vertical profiles were in good agreement with profiles derived from collocated ozonesonde measurements that were smoothed with averaging kernel functions that had been obtained with the retrieval procedure used in the analysis of spectra from the ground-based FTS (gb-FTS). The O3, HCl, and HF columns that were retrieved from the FTS measurements were consistent with Earth Probe/Total Ozone Mapping Spectrometer (TOMS) and HALogen Occultation Experiment (HALOE) data over Alaska within the error limits of all the respective datasets. This is the first report from the Poker Flat FTS observation site on a number of stratospheric gas profiles including a comprehensive error analysis.
Non-volatile residuals of newly formed atmospheric particles in the boreal forest
Authors: Ehn M. , Petäjä T. , Birmili W. , Junninen H. , Aalto P. , Kulmala M.
Published: April 2010

Abstract. The volatility of sub-micrometer atmospheric aerosol particles was studied in a rural background environment in Finland using a combination of a heating tube and a scanning mobility particle sizer. The analysis focused on nano-particles formed from nucleation bursts which were subsequently observed during their growth in the diameter range between 5 and 60 nm. During the 6 days of new particle formation shown in detail, the concentrations of newly formed particles increased up to 10 000 cm−3. The number of nucleation mode particles measured after volatilization in the heating tube at 280°C was up to 90% of the total number under ambient conditions. Taking into account the absolute accuracy of the size distribution measurements, all ambient particles found in the rural atmosphere could have a non-volatile core after volatilization at 280°C. As the regional new particle formation events developed over time as a result of further vapor condensation, the newly formed particles grew at an average growth rate of 2.4±0.3 nm h−1. Importantly, the non-volatile cores of nucleation mode particles were also observed to grow over time, however, at a lower average growth rate of 0.6±0.3 nm h−1. One implication of the volatility analysis is that the newly formed particles, which have reached ambient diameters of 15 nm, are unlikely to consist of sulfuric acid, ammonium sulfate, and water alone. A relatively constant ratio between the growth rate of the ambient particles as well as their non-volatile cores indicates that non-volatile matter is formed only gradually in the growing particles. The non-volatile fraction of the particles showed some correlation with the ambient temperature. The composition and formation mechanism of this non-volatile material in nucleation mode particles are, to date, not known.
Development of the adjoint of GEOS-Chem
Authors: Henze D. K. , Seinfeld J. H.
Published: April 2010

Abstract. We present the adjoint of the global chemical transport model GEOS-Chem, focusing on the chemical and thermodynamic relationships between sulfate – ammonium – nitrate aerosols and their gas-phase precursors. The adjoint model is constructed from a combination of manually and automatically derived discrete adjoint algorithms and numerical solutions to continuous adjoint equations. Explicit inclusion of the processes that govern secondary formation of inorganic aerosol is shown to afford efficient calculation of model sensitivities such as the dependence of sulfate and nitrate aerosol concentrations on emissions of SOx, NOx, and NH3. The adjoint model is extensively validated by comparing adjoint to finite difference sensitivities, which are shown to agree within acceptable tolerances; most sets of comparisons have a nearly 1:1 correlation and R2>0.9. We explore the robustness of these results, noting how insufficient observations or nonlinearities in the advection routine can degrade the adjoint model performance. The potential for inverse modeling using the adjoint of GEOS-Chem is assessed in a data assimilation framework through a series of tests using simulated observations, demonstrating the feasibility of exploiting gas- and aerosol-phase measurements for optimizing emission inventories of aerosol precursors.
Extinction coefficients retrieved in deep tropical ice clouds from lidar observations using a CALIPSO-like algorithm compared to in-situ measurements from the Cloud Integrated Nephelometer during CRYSTAL-FACE
Authors: Noel V. , Winker D. M. , Garrett T. J. , McGill M.
Published: April 2010

Abstract. This paper presents a comparison of lidar ratios and volume extinction coefficients in tropical ice clouds, retrieved using observations from two instruments: the 532-nm Cloud Physics Lidar (CPL), and the in-situ Cloud Integrating Nephelometer (CIN) probe. Both instruments were mounted on airborne platforms during the CRYSTAL-FACE campaign and took measurements up to 17 km. Coincident observations from two cases of ice clouds located on top of deep convective systems are compared. First, lidar ratios are retrieved from CPL observations of attenuated backscatter, using a retrieval algorithm for opaque cloud similar to one used in the soon-to-be launched CALIPSO mission, and compared to results from the regular CPL algorithm. These lidar ratios are used to retrieve extinction coefficient profiles, which are compared to actual observations from the CIN in-situ probe, putting the emphasis on their vertical variability. When observations coincide, retrievals from both instruments are very similar. Differences are generally variations around the average profiles, and general trends on larger spatial scales are usually well reproduced. The two instruments agree well, with an average difference of less than 11% on optical depth retrievals. Results suggest the CALIPSO Deep Convection algorithm can be trusted to deliver realistic estimates of the lidar ratio, leading to good retrievals of extinction coefficients.
MIPAS Level 1B algorithms overview: operational processing and characterization
Authors: Kleinert A. , Aubertin G. , Perron G. , Birk M. , Wagner G. , Hase F. , Nett H. , Poulin R.
Published: April 2010

Abstract. This paper gives an overview of the MIPAS Level 1B (L1B) processor whose main objective is to calibrate atmospheric measurements radiometrically, spectrally and geo-located. It presents also the results of instrument characterization done during the first years in-flight. MIPAS has shown very good performance and stability.
Modeling iodide – iodate speciation in atmospheric aerosol
Authors: Pechtl S. , Schmitz G. , von Glasow R.
Published: April 2010

Abstract. The speciation of iodine in atmospheric aerosol is currently poorly understood. Models predict negligible iodide concentrations and accumulation of iodate in aerosol, both of which is not confirmed by recent measurements. We present an updated aqueous phase iodine chemistry scheme for use in atmospheric chemistry models and discuss sensitivity studies with the marine boundary layer model MISTRA. These studies show that iodate can be reduced in acidic aerosol by inorganic reactions, i.e., iodate does not necessarily accumulate in particles. Furthermore, the transformation of particulate iodide to volatile iodine species likely has been overestimated in previous model studies due to negligence of collision-induced upper limits for the reaction rates. However, inorganic reaction cycles still do not seem to be sufficient to reproduce the observed range of iodide – iodate speciation in atmospheric aerosol. Therefore, we also investigate the effects of the recently suggested reaction of HOI with dissolved organic matter to produce iodide. If this reaction is fast enough to compete with the inorganic mechanism, it would not only directly lead to enhanced iodide concentrations but, indirectly via speed-up of the inorganic iodate reduction cycles, also to a decrease in iodate concentrations. Hence, according to our model studies, organic iodine chemistry, combined with inorganic reaction cycles, is able to reproduce observations. The presented chemistry cycles are highly dependent on pH and thus offer an explanation for the large observed variability of the iodide – iodate speciation in atmospheric aerosol.
Impact of an improved radiation scheme in the MAECHAM5 General Circulation Model
Authors: Cagnazzo C. , Manzini E. , Giorgetta M. A. , De F. Forster P. M.
Published: April 2010

Abstract. In order to improve the representation of the shortwave radiative transfer in the MAECHAM5 general circulation model, the spectral resolution of the shortwave radiation parameterization used in the model has been increased and extended in the UV-B and UV-C bands. The upgraded shortwave parameterization is first validated offline with a 4 stream discrete-ordinate line-by-line model. Thereafter, two 20-years simulations with the MAECHAM5 middle atmosphere general circulation model are performed to evaluate the temperature changes and the dynamical feedbacks arising from the newly introduced parameterization. The offline clear-sky comparison of the standard and upgraded parameterizations with the discrete ordinate model shows considerable improvement for the upgraded parameterization in terms of shortwave fluxes and heating rates. In the simulation with the upgraded ratiation parameterization, we report a significant warming of almost the entire atmosphere, largest at 1 hPa at the stratopause, and stronger zonal mean zonal winds in the middle atmosphere. The warming at the summer stratopause alleviates the cold bias present in the model when the standard radiation scheme is used. The stronger zonal mean zonal winds induce a dynamical feedback that results in a dynamical warming (cooling) of the polar winter (summer) mesosphere, caused by an increased downward (upward) circulation in the winter (summer) hemisphere. In the troposphere, the changes in the spectral resolution and the associated changes in the cloud optical parameters introduce a relatively small warming and, consistenly, a moisteneing. The warming occurs mostly in the upper troposphere and can contribute to a possible improvement of the model temperature climatology.
Contribution of fungi to primary biogenic aerosols in the atmosphere: active discharge of spores, carbohydrates, and inorganic ions by Asco- and Basidiomycota
Authors: Elbert W. , Taylor P. E. , Andreae M. O. , Pöschl U.
Published: April 2010

Abstract. Spores and related chemical compounds from actively spore-discharging Ascomycota (AAM) and actively spore-discharging Basidiomycota (ABM) are primary biogenic components of air particulate matter (characteristic size range 1–10 μm). Measurement results and budget calculations based on investigations in Amazonia (Balbina, Brazil, July 2001) indicate that the forcible discharge of fungal spores may account for a large proportion of coarse air particulate matter in tropical rainforest regions during the wet season. For the particle diameter range of 1–10 μm, the estimated proportions are ~25% during day-time, ~45% at night, and ~35% on average. For the sugar alcohol, mannitol, the budget calculations indicate that it is suitable for use as a molecular tracer for actively discharged basidiospores (ABS), and that the literature-derived emission ratio of about 5 pg per ABS may be taken as a representative average. ABM emissions may account for most of the atmospheric abundance of mannitol, and can explain the observed diurnal cycle (higher abundance at night). ABM emissions of hexose carbohydrates might also account for a significant proportion of glucose and fructose in air particulate matter, but the literature-derived ratios are not consistent with the observed diurnal cycle (lower abundance at night). AAM emissions appear to account for a large proportion of potassium in air particulate matter over tropical rainforest regions during the wet season, and they can also explain the observed diurnal cycle (higher abundance at night). The results of our investigations and budget calculations for tropical rainforest aerosols are consistent with measurements performed at other locations. Based on the average abundance of mannitol in particulate matter, which is consistent with the above emission ratio and the observed abundance of ABS, we have also calculated a value of ~17 Tg yr−1 as a first estimate for the global average emission rate of ABS over land surfaces. Comparisons with estimated rates of emission and formation of other major types of organic aerosol (~47 Tg yr−1 of anthropogenic primary organic aerosol; 12–70 Tg yr−1 of secondary organic aerosol) indicate that emissions from actively spore-discharging fungi should be taken into account as a significant source of organic aerosol. Their effects might be particularly important in tropical regions, where both physicochemical processes in the atmosphere and biological activity at the Earth's surface are particularly intense, and where the abundance of fungal spores and related chemical compounds are typically higher than in extratropical regions.
SAGE III aerosol extinction validation in the Arctic winter: comparisons with SAGE II and POAM III
Authors: Thomason L. W. , Poole L. R. , Randall C. E.
Published: April 2010

Abstract. The use of SAGE III multiwavelength aerosol extinction coefficient measurements to infer PSC type is contingent on the robustness of both the extinction magnitude and its spectral variation. Past validation with SAGE II and other similar measurements has shown that the SAGE III extinction coefficient measurements are reliable though the comparisons have been greatly weighted toward measurements made at mid-latitudes. Some aerosol comparisons made in the Arctic winter as a part of SOLVE II suggested that SAGE III values, particularly at longer wavelengths, are too small with the implication that both the magnitude and the wavelength dependence are not reliable. Comparisons with POAM III have also suggested a similar discrepancy. Herein, we use SAGE II data as a common standard for comparison of SAGE III and POAM III measurements in the Arctic winters of 2002/2003 through 2004/2005. During the winter, SAGE II measurements are made infrequently at the same latitudes as these instruments. We have mitigated this problem through the use potential vorticity as a spatial coordinate and thus greatly increased the number of coincident events. We find that SAGE II and III extinction coefficient measurements show a high degree of compatibility at both 1020 nm and 450 nm except a 10–20% bias at both wavelengths. In addition, the 452 to 1020 nm extinction ratio shows a consistent bias of ~30% throughout the lower stratosphere. We also find that SAGE II and POAM III are on average consistent though the comparisons show a much higher variability and larger bias than SAGE II/III comparisons. In addition, we find that the two data sets are not well correlated below 18 km. Overall, we find both the extinction values and the spectral dependence from SAGE III are robust and we find no evidence of a significant defect within the Arctic vortex.
Examining aerosol indirect effect under contrasting environments during the ACE-2 experiment
Authors: Guo H. , Penner J. E. , Herzog M. , Pawlowska H.
Published: April 2010

Abstract. The Active Tracer High-resolution Atmospheric Model (ATHAM) has been adopted to examine the aerosol indirect effect in contrasting clean and polluted cloudy boundary layers during the Second Aerosol Characterization Experiment (ACE-2). Model results are in good agreement with available in-situ observations, which provides confidence in the results of ATHAM. Sensitivity tests have been conducted to examine the response of the cloud fraction (CF), cloud liquid water path (LWP), and cloud optical depth (COD) to changes in aerosols in the clean and polluted cases. It is shown for two cases that CF and LWP would decrease or remain nearly constant with an increase in aerosols, a result which shows that the second aerosol indirect effect is positive or negligibly small in these cases. Further investigation indicates that the background meteorological conditions play a critical role in the response of CF and LWP to aerosols. When large-scale subsidence is weak as in the clean case, the dry overlying air above the cloud is more efficiently entrained into the cloud, and in so doing, removes cloud water more efficiently, and results in lower CF and LWP when aerosol burden increases. However, when the large-scale subsidence is strong as in the polluted case, the growth of the cloud top is suppressed and the entrainment drying makes no significant difference when aerosol burden increases. Therefore, the CF and LWP remain nearly constant. In both the clean and polluted cases, the COD tends to increase with aerosols, and the total aerosol indirect effect (AIE) is negative even when the CF and LWP decrease with an increase in aerosols. Therefore, the first AIE dominates the response of the cloud to aerosols.
Source apportionment of submicron organic aerosols at an urban site by linear unmixing of aerosol mass spectra
Authors: Lanz V. A. , Alfarra M. R. , Baltensperger U. , Buchmann B. , Hueglin C. , Prévôt A. S. H.
Published: April 2010

Abstract. Submicron ambient aerosol was characterized in summer 2005 at an urban background site in Zurich, Switzerland, during a three-week measurement campaign. Highly time-resolved samples of non-refractory aerosol components were analyzed with an Aerodyne aerosol mass spectrometer (AMS). Positive matrix factorization (PMF) was used for the first time for AMS data to identify the main components of the total organic aerosol and their sources. The PMF retrieved factors were compared to measured reference mass spectra and were correlated with tracer species of the aerosol and gas phase measurements from collocated instruments. Six factors were found to explain virtually all variance in the data and could be assigned either to sources or to aerosol components such as oxygenated organic aerosol (OOA). Our analysis suggests that at the measurement site only a small (<10%) fraction of organic PM1 originates from freshly emitted fossil fuel combustion. Other primary sources identified to be of similar or even higher importance are charbroiling (10–15%) and wood burning (~10%), along with a minor source interpreted to be influenced by food cooking (6%). The fraction of all identified primary sources is considered as primary organic aerosol (POA). This interpretation is supported by calculated ratios of the modelled POA and measured primary pollutants such as elemental carbon (EC), NOx, and CO, which are in good agreement to literature values. A high fraction (60–69%) of the measured organic aerosol mass is OOA which is interpreted mostly as secondary organic aerosol (SOA). This oxygenated organic aerosol can be separated into a highly aged fraction, OOA I, (40–50%) with low volatility and a mass spectrum similar to fulvic acid, and a more volatile and probably less processed fraction, OOA II (on average 20%). This is the first publication of a multiple component analysis technique to AMS organic spectral data and also the first report of the OOA II component.
Technical Note: Long-term memory effect in the atmospheric CO2 concentration at Mauna Loa
Authors: Varotsos C. , Assimakopoulos M.-N. , Efstathiou M.
Published: April 2010

Abstract. The monthly mean values of the atmospheric carbon dioxide concentration derived from in-situ air samples collected at Mauna Loa Observatory, Hawaii, during 1958–2004 (the longest continuous record available in the world) are analyzed by employing the detrended fluctuation analysis to detect scaling behavior in this time series. The main result is that the fluctuations of carbon dioxide concentrations exhibit long-range power-law correlations (long memory) with lag times ranging from four months to eleven years, which correspond to 1/f noise. This result indicates that random perturbations in the carbon dioxide concentrations give rise to noise, characterized by a frequency spectrum following a power-law with exponent that approaches to one; the latter shows that the correlation times grow strongly. This feature is pointing out that a correctly rescaled subset of the original time series of the carbon dioxide concentrations resembles the original time series. Finally, the power-law relationship derived from the real measurements of the carbon dioxide concentrations could also serve as a tool to improve the confidence of the atmospheric chemistry-transport and global climate models.
Geochemical perspectives from a new Aerosol chemical mass closure
Authors: Guinot B. , Cachier H. , Oikonomou K.
Published: April 2010

Abstract. The aerosol chemical mass closure is revisited and a simple and inexpensive methodology is proposed. This methodology relies on data obtained for aerosol mass, and concentration of the major ions and the two main carbon components, the organic carbon (OC) and the black carbon (BC). Atmospheric particles are separated into coarse (AD>2µm) and fine (AD<2µm) fractions and are treated separately. For the coarse fraction the carbonaceous component is minor and assumption is made for the conversion factor k, of OC-to-POM (Particulate Organic Matter) which is fixed to the value of 1.8 accounting for secondary species. The coarse soluble calcium is shown to display a correlation (regression coefficient f, y axis intercept b) with the missing mass. Conversely, the fine fraction is dominated by organic species and assumption is made for dust which is assumed to have the same f factor as the coarse mode dust. The fine mode mass obtained from chemical analyses is then adjusted to the actual weighed mass by tuning the k conversion factor. The k coefficient is kept different in the two modes due to the expected different origins of the organic particles. Using the f and k coefficients obtained from the data set, the mass closure is reached for each individual sample with an undetermined fraction less than 10%. The procedure has been applied to different urban and peri-urban environments in Europe and in Beijing and its efficiency and uncertainties on f and k values are discussed. The f and k coefficients are shown to offer consistent geochemical indications on aerosol origin and transformations. f allows to retrieve dust mass and its value accounting for Ca abundance in dust at the site of investigation may serve as an indicator of dust origin and aerosol interactions with anthropogenic acids. f values were found to vary in the 0.08–0.12 range in European urban areas, and a broader range in Beijing (0.01–0.16). As expected, k appears to be a relevant proxy for particle origin and ageing and varies in the 1.4–1.8 range. For Beijing, k exhibits high values of about 1.7 in winter and summer. Winter values suggest that fresh coal aerosol might be responsible for such a high k value, which was not taken into account in previous works.
Is aerosol formation in cirrus clouds possible?
Authors: Kazil J. , Lovejoy E. R. , Jensen E. J. , Hanson D. R.
Published: April 2010

Abstract. The recent observation of ultrafine aerosol particles in cirrus clouds has raised the question whether aerosol formation within cirrus clouds is possible, and if so, what mechanisms are involved. We have developed an aerosol parcel model of neutral and charged H2SO4/H2O aerosol processes, including nucleation from the gas phase and loss onto cirrus ice particles. Laboratory thermodynamic data for sulfuric acid uptake and loss by small neutral and charged clusters are used, allowing for a reliable description of both neutral and charged nucleation down to the very low temperatures occurring in the upper troposphere and lower stratosphere. The model implements a first order scheme for resolving the aerosol size distribution within its geometric size sections, which efficiently suppresses numerical diffusion. We operate the model offline on trajectories generated with a detailed 1-D cirrus model which describes ice crystal nucleation, deposition growth, vertical advection of ice crystals and water vapor, and ice crystal sedimentation. In this paper we explore the possibility of aerosol formation within non-convective cirrus clouds and draw conclusions for aerosol formation in anvil cirrus. We find that sulfate aerosol formation within cirrus clouds can proceed even at high ice surface area concentrations, and depends strongly on the size of the cirrus ice crystals and on the surface area concentration of preexisting aerosol particles.
Hygroscopic growth of sub-micrometer and one-micrometer aerosol particles measured during ACE-Asia
Authors: Massling A. , Leinert S. , Wiedensohler A. , Covert D.
Published: April 2010

Abstract. Hygroscopic properties of aerosol particles in the sub-micrometer and one-micrometer size range were measured during the ACE-Asia study (Aerosol Characterization Experiment-Asia) in spring 2001. The measurements took place off the coasts of Japan, Korea, and China. All instruments contributing to this study were deployed in a container on the forward deck of the NOAA Research Vessel Ronald H. Brown. Air masses with primarily marine influence and air masses from the Asian continent affected by both anthropogenic sources and by the transport of desert dust aerosol were encountered during the cruise. Two different systems were used to determine hygroscopic growth of the ambient marine boundary layer aerosol at 90% relative humidity (RH). An H-TDMA-system (Hygroscopicity-Tandem Differential Mobility Analyzer) (Massling et al., 2003) and a newly developed H-DMA-APS-system (Hygroscopicity-Differential Mobility Analyzer-Aerodynamic Particle Sizer) (Leinert and Wiedensohler, 2006) were applied to analyze sub-micrometer and one-micrometer aerosol particles, respectively. Results showed very different hygroscopic behavior in the sub-micrometer size range compared to the one-micrometer size range. In general, for all continentally influenced air masses, the one-micrometer particle population was characterized by two different particle fractions – a nearly hydrophobic fraction with growth factors around 1.0 representative of dust particles and a sea salt fraction with hygroscopic growth factors around 2.0. The number fraction of dust particles was generally about 60% independent of long-range air mass origin. For sub-micrometer particles, a dominant, more hygroscopic particle fraction with growth factors between 1.5 and 1.9 (depending on dry particle size) indicating ammonium sulfate as major component was always found. In marine air masses and for larger sizes within the sub-micrometer range (Dp=250 and 350 nm), a sea salt fraction with growth factors between 2.0 and 2.1 was also observed. For all other air masses, the more hygroscopic particle fraction in the sub-micrometer size range was mostly accompanied by a less hygroscopic particle fraction with growth factors between 1.20 and 1.55 depending on both the continental sources and the dry particle size. Number fractions of this particle group varied between 4 and 39% depending on dry particle size and air mass type. Nearly hydrophobic particles indicating dust particles in the sub-micrometer size regime were only found for particles with Dp=250 and 350 nm during a time period when the aerosol was significantly influenced by transport from Asian desert regions.
Near-real time retrieval of tropospheric NO2 from OMI
Authors: Boersma K. F. , Eskes H. J. , Veefkind J. P. , Brinksma E. J. , van der A R. J. , Sneep M. , van der Oord G. H. J. , Levelt P. F. , Stammes P. , Gleason J. F. , Bucsela E. J.
Published: April 2010

Abstract. We present a new algorithm for the near-real time retrieval – within 3 h of the actual satellite measurement – of tropospheric NO2 columns from the Ozone Monitoring Instrument (OMI). The retrieval system is based on the combined retrieval-assimilation-modelling approach developed at KNMI for off-line tropospheric NO2 from the GOME and SCIAMACHY satellite instruments. We have adapted the off-line system such that the required a priori information ndash; profile shapes and stratospheric background NO2 ndash; is now immediately available upon arrival of the OMI NO2 slant columns and cloud data at KNMI. Slant column NO2 and cloud information arrives at KNMI typically within 80 min of actual OMI observations. Slant columns for NO2 are retrieved using differential optical absorption spectroscopy (DOAS) in the 405–465 nm range. Cloud fraction and cloud pressure are provided by a new cloud retrieval algorithm that uses the absorption of the O2–O2 collision complex near 477 nm. On-line availability of stratospheric slant columns and NO2 profiles is achieved by running the TM4 chemistry transport model (CTM) forward in time based on forecast ECMWF meteo and assimilated NO2 information from all previously observed orbits. OMI NO2 slant columns, after correction for spurious across-track variability, show a random error for individual pixels of approximately 0.7×1015molec.cm–2. As NO2 retrievals are very sensitive to clouds, we evaluated the consistency of cloud fraction and cloud pressure from the new O2–O2 (OMI) algorithm and from the Fast Retrieval Scheme for Cloud Observables (FRESCO). Cloud parameters from the O2–O2 (OMI) algorithm have similar frequency distributions as cloud parameters retrieved from FRESCO (SCIAMACHY) for August 2006. On average, OMI cloud fractions are higher by 0.011, and OMI cloud pressures exceed FRESCO cloud pressures by 60 hPa. As a consistency check, we intercompared OMI near-real time NO2 columns measured at 13:45 h local time to SCIAMACHY off-line NO2 columns measured at 10:00 h local time. In August 2006, both instruments observe very similar spatial patterns of tropospheric NO2 columns, and small differences for most locations on Earth where tropospheric NO2 columns are small. For regions that are strongly polluted, SCIAMACHY observes higher tropospheric NO2 columns than OMI.
Optical properties of absorbing and non-absorbing aerosols retrieved by cavity ring down (CRD) spectroscopy
Authors: Riziq A. A. , Erlick C. , Dinar E. , Rudich Y.
Published: April 2010

Abstract. Application of cavity ring down (CRD) spectrometry for measuring the optical properties of pure and mixed laboratory-generated aerosols is presented. The extinction coefficient (αext), extinction cross section (σext) and extinction efficiency (Qext) were measured for polystyrene spheres (PSS), ammonium sulphate ((NH4)2(SO4)), sodium chloride (NaCl), glutaric acid (GA), and Rhodamine-590 aerosols. The refractive indices of the different aerosols were retrieved by comparing the measured extinction efficiency of each aerosol type to the extinction predicted by Mie theory. Aerosols composed of sodium chloride and glutaric acid in different mixing ratios were used as model for mixed aerosols of two non-absorbing materials, and their extinction and complex refractive index were derived. Aerosols composed of Rhodamine-590 and ammonium sulphate in different mixing ratios were used as model for mixing of absorbing and non-absorbing species, and their optical properties were derived. The refractive indices of the mixed aerosols were also calculated by various optical mixing rules and a core plus shell Mie model. We found that for non-absorbing mixtures, the linear rule, Maxwell-Garnett rule, extended effective medium approximation (EEMA), and core plus shell model give comparable results, with the linear mixing rule giving a slightly better fit than the others. Overall, calculations for the mixed aerosols are not as good as for single component aerosols. For absorbing mixtures, the differences between the refractive indices calculated using the mixing rules and those retrieved by CRD are generally higher.
The global impact of supersaturation in a coupled chemistry-climate model
Authors: Gettelman A. , Kinnison D. E.
Published: April 2010

Abstract. Ice supersaturation is important for understanding condensation in the upper troposphere. Most general circulation models however do not permit supersaturation. In this study, a coupled chemistry climate model, the Whole Atmosphere Community Climate Model (WACCM), is modified to include supersaturation for the ice phase. The study is intended as a sensitivity experiment, to understand the potential impact of supersaturation, and of expected changes to stratospheric water vapor, on climate and chemistry. Results indicate that high clouds decrease and water vapor in the stratosphere increases nearly linearly with supersaturation (20% supersaturation increases water vapor by nearly 20%). The stratospheric Brewer-Dobson circulation slows at high southern latitudes, consistent with slight changes in temperature likely induced by changes to cloud radiative forcing. The cloud changes also cause an increase in the seasonal cycle of near tropopause temperatures, increasing them in boreal summer over boreal winter. There are also impacts on chemistry, with small increases in ozone in the tropical lower stratosphere driven by enhanced production. The radiative impact of changing water vapor is dominated by the reduction in cloud forcing associated with fewer clouds (~+0.6 Wm−2) with a small component likely from radiative effect (greenhouse trapping) of the extra water vapor (~+0.2 Wm−2), consistent with previous work. Representing supersaturation is thus important, and changes to supersaturation resulting from changes in aerosol loading for example, might have a modest impact on global radiative forcing, mostly through changes to clouds. We do not see evidence of a strong impact of water vapor on tropical tropopause temperatures.
Isentropic advection and convective lifting of water vapor in the UT – LS as observed over Brazil (22° S) in February 2004 by in situ high-resolution measurements of H2O, CH4, O3 and temperature
Authors: Durry G. , Huret N. , Hauchecorne A. , Marecal V. , Pommereau J.-P. , Jones R. L. , Held G. , Larsen N. , Renard J.-B.
Published: April 2010

Abstract. The micro-SDLA balloonborne diode laser spectrometer was flown twice from Bauru (22° S, Brazil) in February 2004 during HIBISCUS to yield in situ H2O measurements in the Upper Troposphere (UT) and Lower Stratosphere (LS) and in particular in the Tropical Tropopause Layer (TTL). The overall TTL was found warmer (with a subsaturated cold point near –79°C) and the LS moister compared to former measurements obtained in tropical oceanic conditions. The use of specific balloons with a slow descent, combined with the high-resolution of the laser sensor, allowed us to observe in situ in the UT, the TTL and the LS several thin layers correlated on H2O, CH4, O3, temperature and PV. A component of these layers is associated with the isentropic transport into the UT- LS of extratropical stratospheric air masses. Moreover, the examination of temperature and tracer (CH4, O3) profiles gives insights on the potential contribution of convective transport of H2O in the TTL.
Closure between measured and modelled particle hygroscopic growth during TORCH2 implies ammonium nitrate artefact in the HTDMA measurements
Authors: Gysel M. , Crosier J. , Topping D. O. , Whitehead J. D. , Bower K. N. , Cubison M. J. , Williams P. I. , Flynn M. J. , McFiggans G. B. , Coe H.
Published: April 2010

Abstract. Measurements of aerosol properties were made in aged polluted and clean background air masses encountered at the North Norfolk (UK) coastline during the second field campaign of the Tropospheric ORganic CHemistry project (TORCH2) in May 2004. Hygroscopic growth factor (GF) measurements were performed at 90% relative humidity (RH) for D0=27–217 nm particles using a Hygroscopicity Tandem Differential Mobility Analyser (HTDMA), while the aerosol composition was simultaneously measured with an Aerodyne aerosol mass spectrometer (Q-AMS). During the clean background events the aerosol was characterised by little size dependence of properties with generally large GFs and inorganic sulphate being the dominant compound. In aged polluted air masses the particles were dominated by inorganic sulphate and nitrate at larger sizes, whereas organics were the largest fraction in smaller particles, thus explaining the trend of smaller GFs at smaller sizes. Organics do contribute to the hygroscopic growth, particularly at small sizes, but generally the dominant contribution to growth at 90% RH comes from inorganic salts. The ZSR mixing rule was used to predict GFs based on the chemical composition, theoretical GFs of pure inorganic salts and a "bulk" GF of ~1.20 for the organics. Good quantitative closure with HTDMA measurements as a function of both particle size and time was achieved in the absence of nitrate. However, GFs were clearly overpredicted at times when a significant fraction of nitrate was present. After careful considerations we attribute the overprediction to substantial evaporation losses of ammonium nitrate in the HTDMA instrument. If true, this implies that the ZSR predictions based on composition might be more representative of the actual "bulk" behaviour of undisturbed ambient particles than the HTDMA measurements. The simplified model approach using the ZSR rule and a constant organic growth factor made high size and time resolution possible, which has proven to be essential for a valid closure study. The ZSR mixing rule appears to be sufficiently accurate, as the GF predictions are more sensitive to the exact GFs of the inorganic compounds than to the growth factor of the moderately hygroscopic organics. Therefore a more detailed analysis and modelling of the organic fraction at the expense of time and size resolution is not worth the effort for an aged aerosol and discrepancies in either direction might even be cancelled out by averaging.
Aircraft measurements over Europe of an air pollution plume from Southeast Asia – aerosol and chemical characterization
Authors: Stohl A. , Forster C. , Huntrieser H. , Mannstein H. , McMillan W. W. , Petzold A. , Schlager H. , Weinzierl B.
Published: April 2010

Abstract. An air pollution plume from Southern and Eastern Asia, including regions in India and China, was predicted by the FLEXPART particle dispersion model to arrive in the upper troposphere over Europe on 24–25 March 2006. According to the model, the plume was exported from Southeast Asia only six days earlier, transported into the upper troposphere by a warm conveyor belt, and travelled to Europe in a fast zonal flow. This is confirmed by the retrievals of carbon monoxide (CO) from AIRS satellite measurements, which are in excellent agreement with the model results over the entire transport history. The research aircraft DLR Falcon was sent into this plume west of Spain on 24 March and over Southern Europe on 25 March. On both days, the pollution plume was indeed found close to the predicted locations and, thus, the measurements taken allowed the first detailed characterization of the aerosol content and chemical composition of an anthropogenic pollution plume after a nearly hemispheric transport event. The mixing ratios of CO, reactive nitrogen (NOy) and ozone (O3) measured in the Asian plume were all clearly elevated over a background that was itself likely elevated by Asian emissions: CO by 17–34 ppbv on average (maximum 60 ppbv) and O3 by 2–9 ppbv (maximum 22 ppbv). Positive correlations existed between these species, and a ΔO3/ΔCO slope of 0.25 shows that ozone was formed in this plume, albeit with moderate efficiency. Nucleation mode and Aitken particles were suppressed in the Asian plume, whereas accumulation mode aerosols were strongly elevated and correlated with CO. The suppression of the nucleation mode was likely due to the large pre-existing aerosol surface due to the transported larger particles. Super-micron particles, likely desert dust, were found in part of the Asian pollution plume and also in surrounding cleaner air. The aerosol light absorption coefficient was enhanced in the plume (average values for individual plume encounters 0.25–0.70 Mm−1), as was the fraction of non-volatile Aitken particles. This indicates that black carbon (BC) was an important aerosol component. During the flight on 25 March, which took place on the backside of a trough located over Europe, a mixture of Asian pollution and stratospheric air was found. Asian pollution was mixing into the lower stratosphere, and stratospheric air was mixing into the pollution plume in the troposphere. Turbulence was encountered by the aircraft in the mixing regions, where the thermal stability was low and Richardson numbers were below 0.2. The result of the mixing can clearly be seen in the trace gas data, which are following mixing lines in correlation plots. This mixing with stratospheric air is likely very typical of Asian air pollution, which is often lifted to the upper troposphere and, thus, transported in the vicinity of stratospheric air.
3-D polarised simulations of space-borne passive mm/sub-mm midlatitude cirrus observations: a case study
Authors: Davis C. P. , Evans K. F. , Buehler S. A. , Wu D. L. , Pumphrey H. C.
Published: April 2010

Abstract. Global observations of ice clouds are needed to improve our understanding of their impact on earth's radiation balance and the water-cycle. Passive mm/sub-mm has some advantages compared to other space-borne cloud-ice remote sensing techniques. This paper presents detailed simulated observations for three such instruments, AMSU-B, CIWSIR, and EOS-MLS. The Monte-Carlo radiative transfer code, ARTS-MC, makes proper account of polarisation and uses 3-D spherical geometry. The actual field of view characteristics for each instrument are also accounted for. A 3-D midlatitude cirrus scenario is used, which is derived from Chilbolton cloud radar data and a stochastic method for generating 3-D ice water content fields. Although the main purpose of the work was to demonstrate the capability of accurately simulating observations of this type, the results suggest that cloud inhomogeneity will affect CIWSIR, and EOSMLS low tangent height observations via the beamfilling effect. Also, the results confirm that preferentially oriented ice crystals will produce significant polarisation effects.
The quantitative infrared and NIR spectrum of CH2I2 vapor: vibrational assignments and potential for atmospheric monitoring
Authors: Johnson T. J. , Masiello T. , Sharpe S. W.
Published: April 2010

Abstract. Diiodomethane (CH2I2) photolysis in the presence of ozone is a suggested precursor to new particle aerosol formation, particularly in coastal areas. As part of the PNNL database of gas-phase infrared spectra, the quantitative absorption spectrum of CH2I2 has been acquired at 0.1 cm−1 resolution. Two strong b2 symmetry A-type bands at 584 and 1114 cm−1 are observed, but are not resolved at 760 Torr and appear as B-type. In contrast, the b1 symmetry C-type bands near 5953, 4426 and 3073 cm−1 are resolved with rotational structure, including Q-branches with widths ≤1 cm−1. The quantitative infrared and near-infrared vapor-phase spectra (600–10 000 cm−1) are reported for the first time and discussed in terms of atmospheric monitoring. FT-Raman spectra and ab initio calculations are used to complete vibrational assignments in the C2v point group.