bluuebunny/crossref_metadata_2025 huggingface dataset:
Evidence for ice particles in the tropical stratosphere from in-situ measurements
Authors: de Reus M. , Borrmann S. , Heymsfield A. J. , Weigel R. , Schiller C. , Mitev V. , Frey W. , Kunkel D. , Kürten A. , Curtius J. , Sitnikov N. M. , Ulanovsky A. , Ravegnani F.
Published: April 2010

Abstract. In-situ ice crystal size distribution measurements are presented within the tropical troposphere and lower stratosphere. The measurements were performed using a combination of a Forward Scattering Spectrometer Probe (FSSP-100) and a Cloud Imaging Probe (CIP) which were installed on the Russian high altitude research aircraft M55 "Geophysica" during the SCOUT-O3 campaign in Darwin, Australia. The objective of the campaign was to characterise the outflow of the Hector convective system, which appears on an almost daily basis during the pre-monsoon season over the Tiwi Islands, north of Darwin. In total 90 encounters with ice clouds, between 10 and 19 km altitude were selected from the dataset and were analysed. Six of these encounters were observed in the lower stratosphere, up to 1.4 km above the local tropopause, and were a result of overshooting convection. The ice crystals observed in the stratosphere comprise sizes up to 400 μm maximum dimension, include an ice water content of 0.1×10−3–1.7×10−3 g m−3 and were observed at ambient relative humidities (with respect to ice) between 75 and 157%. Three modal lognormal size distributions were fitted to the average size distributions for different potential temperature intervals, showing that the shape of the size distribution of the stratospheric ice clouds are similar to those observed in the upper troposphere. In the tropical troposphere the effective radius of the ice cloud particles decreases from 100 μm at about 10 km altitude, to 3 μm at the tropopause, while the ice water content decreases from 0.04 to 10−5 g m−3. No clear trend in the number concentration was observed with altitude, due to the thin and inhomogeneous characteristics of the observed cirrus clouds. The ice water content calculated from the observed ice crystal size distribution is compared to the ice water content derived from two hygrometer instruments. This independent measurement of the ice water content agrees within the combined uncertainty of the instruments for ice water contents exceeding 2×10−4 g m−3. Stratospheric residence times, calculated based on gravitational settling only, show that the ice crystals observed in the stratosphere over the Hector storm system have a high potential for humidifying the stratosphere. Utilizing total aerosol number concentration measurements from a four channel condensation particle counter, it can be shown that the fraction of activated ice particles with respect to the number of available aerosol particles ranges from 1:300 to 1:30 000 for tropical upper tropospheric ice clouds with ambient temperatures below −75°C.
Introduction: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) – integrating aerosol research from nano to global scales
Authors: Kulmala M. , Asmi A. , Lappalainen H. K. , Carslaw K. S. , Pöschl U. , Baltensperger U. , Hov Ø. , Brenquier J.-L. , Pandis S. N. , Facchini M. C. , Hansson H.-C. , Wiedensohler A. , O'Dowd C. D.
Published: April 2010

Abstract. The European Aerosol Cloud Climate and Air Quality Interactions project EUCAARI is an EU Research Framework 6 integrated project focusing on understanding the interactions of climate and air pollution. EUCAARI works in an integrative and multidisciplinary way from nano- to global scale. EUCAARI brings together several leading European research groups, state-of-the-art infrastructure and some key scientists from third countries to investigate the role of aerosol on climate and air quality. Altogether 48 partners from 25 countries are participating in EUCAARI. During the first 16 months EUCAARI has built operational systems e.g. established pan-European measurement network for Lagrangian studies and four stations in developing countries. Also an improved understanding of nanoscale processes (like nucleation) has been implemented in global models. Here we present the research methods, organisation, operations and first results of EUCAARI.
Carbonaceous aerosols at urban influenced sites in Norway
Authors: Yttri K. E. , Dye C. , Braathen O.-A. , Simpson D. , Steinnes E.
Published: April 2010

Abstract. Little is known regarding levels and source strength of carbonaceous aerosols in Scandinavia. In the present study, ambient aerosol (PM10 and PM2.5) concentrations of elemental carbon (EC), organic carbon (OC), water-insoluble organic carbon (WINSOC), and water-soluble organic carbon (WSOC) are reported for a curbside site, an urban background site, and a suburban site in Norway in order to investigate their spatial and seasonal variations. Aerosol filter samples were collected using tandem filter sampling to correct for the positive sampling artefact introduced by semi volatile OC. Analyses were performed using the thermal optical transmission (TOT) instrument from Sunset Lab Inc., which corrects for charring during analysis. Finally, we estimated the relative contribution of OC from wood burning based on the samples content of levoglucosan. Levels of EC varied by more than one order of magnitude between sites, likely due to the higher impact of vehicular traffic at the curbside and the urban background sites. In winter, the level of particulate organic carbon (OCp) at the suburban site was equal to (for PM10) or even higher (for PM2.5) than the levels observed at the curbside and the urban background sites. This finding was attributed to the impact of residential wood burning at the suburban site in winter, which was confirmed by a high mean concentration of levoglucosan (407 ng m−3). This finding indicates that exposure to primary combustion derived OCp could be equally high in residential areas as in a city center. It is demonstrated that OCp from wood burning (OCwood) accounted for almost all OCp at the suburban site in winter, allowing a new estimate of the ratio TCp/levoglucosan for both PM10 and PM2.5. Particulate carbonaceous material (PCM = Organic matter + Elemental matter) accounted for 46–83% of PM10 at the sites studied when considering the positive artefact of semi volatile OC, thus being the major contributor to PM.
Stratospheric BrONO2observed by MIPAS
Authors: Höpfner M. , Orphal J. , von Clarmann T. , Stiller G. , Fischer H.
Published: April 2010

Abstract. The first measurements of stratospheric bromine nitrate (BrONO2) are reported. Bromine nitrate has been clearly identified in atmospheric infrared emission spectra recorded with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) aboard the European Envisat satellite, and stratospheric concentration profiles have been determined for different conditions (day and night, different latitudes). The BrONO2 concentrations show strong day/night variations, with much lower concentrations during the day. Maximum volume mixing ratios observed during night are 20 to 25 pptv. The observed concentration profiles are in agreement with estimations from photochemical models and show that the current understanding of stratospheric bromine chemistry is generally correct.
Methyl chavicol: characterization of its biogenic emission rate, abundance, and oxidation products in the atmosphere
Authors: Bouvier-Brown N. C. , Goldstein A. H. , Worton D. R. , Matross D. M. , Gilman J. B. , Kuster W. C. , Welsh-Bon D. , Warneke C. , de Gouw J. A. , Cahill T. M. , Holzinger R.
Published: April 2010

Abstract. We report measurements of ambient atmospheric mixing ratios for methyl chavicol and determine its biogenic emission rate. Methyl chavicol, a biogenic oxygenated aromatic compound, is abundant within and above Blodgett Forest, a ponderosa pine forest in the Sierra Nevada Mountains of California. Methyl chavicol was detected simultaneously by three in-situ instruments – a gas chromatograph with mass spectrometer detector (GC-MS), a proton transfer reaction mass spectrometer (PTR-MS), and a thermal desorption aerosol GC-MS (TAG) – and found to be abundant within and above Blodgett Forest, a ponderosa pine forest in the Sierra Nevada Mountains of California. Methyl chavicol atmospheric mixing ratios are strongly correlated with 2-methyl-3-buten-2-ol (MBO), a light- and temperature-dependent biogenic emission from the ponderosa pine trees at Blodgett Forest. Scaling from this correlation, methyl chavicol emissions account for 4–68% of the carbon mass emitted as MBO in the daytime, depending on the season. From this relationship, we estimate a daytime basal emission rate of 0.72–10.2 μgCg−1h−1, depending on needle age and seasonality. We also present the first observations of its oxidation products (4-methoxybenzaldehyde and 4-methyoxy benzene acetaldehyde) in the ambient atmosphere. Methyl chavicol is a major essential oil component of many plant species. This work suggests that methyl chavicol plays a significant role in the atmospheric chemistry of Blodgett Forest, and potentially other sites, and should be included explicitly in both biogenic volatile organic carbon emission and atmospheric chemistry models.
Real-time observation of secondary aerosol formation during a fog event in London
Authors: Dall'Osto M. , Harrison R. M. , Coe H. , Williams P.
Published: April 2010

Abstract. A fog event was monitored with state-of-the art real-time aerosol mass spectrometers in an urban background location in London (England) during the REPARTEE-I experiment. Specific particle types rich in hydroxymethanesulphonate (HMS) were found only during the fog event. Formation of inorganic and organic secondary aerosol was observed as soon as fog was detected and two different mechanisms are suggested to be responsible for the production of two different types of aerosol. Humic-like substances (HULIS) appear to be produced in the gas phase and condense into the interstitial aerosol, while nitrate aerosol is produced in the liquid phase within the droplet. Not only are secondary aerosol constituents produced during the fog event, but the primary aerosol is observed to be processed by the fog event, dramatically changing its chemical properties.
Sensitivities of the absorptive partitioning model of secondary organic aerosol formation to the inclusion of water
Authors: Barley M. , Topping D. O. , McFiggans G. , Jenkin M. E.
Published: April 2010

Abstract. Depending on the assumptions about the participation of water in absorptive partitioning, the prediction of the distribution of semi-volatile organic component between the gaseous and condensed phases is shown to be highly sensitive to the ambient relative humidity and the formulation of the partitioning model used. Further sensitivities to the assumed pre-existing particulate loading and to parameterised organic component non-ideality are explored and shown to contribute significantly to the variation in predicted secondary organic particulate loading.
Effects of model resolution on entrainment (inversion heights), cloud-radiation interactions, and cloud radiative forcing
Authors: Guo H. , Liu Y. , Daum P. H. , Zeng X. , Li X. , Tao W.-K.
Published: April 2010

Abstract. We undertook three-dimensional numerical studies of a marine stratus deck under a strong inversion using an interactive shortwave- and longwave-radiation module. A suite of sensitivity tests were conducted to address the effects of model resolution on entrainment (inversion heights), cloud-radiation interactions, and cloud radiative-forcings by varying model horizontal resolution only, varying vertical resolution only, and varying horizontal- and vertical-resolution simultaneously but with a fixed aspect ratio of 2.5. Our results showed that entrainment (inversion height) is more sensitive to vertical- than to horizontal-resolution. A vertical resolution finer than 40 m can simulate spatial- and temporal-variations in the inversion height well. The inversion height decreases with increasing vertical resolution, but tends to increase with increasing horizontal resolution. Cloud liquid water path doubles after refining both the vertical- and horizontal-resolution by a factor of four. This doubling is associated with a positive feedback between cloud water and cloud top radiative cooling, which amplifies small differences initiated by changes in the model resolution. The magnitude of the cloud radiative-forcing tends to increase with increasing model resolution, mainly attributable to the increase in the cloud liquid water path. Shortwave radiative forcing is dominant, and more sensitive to model resolution than the longwave counterpart.
Carbon monoxide distributions from the upper troposphere to the mesosphere inferred from 4.7 μm non-local thermal equilibrium emissions measured by MIPAS on Envisat
Authors: Funke B. , López-Puertas M. , García-Comas M. , Stiller G. P. , von Clarmann T. , Höpfner M. , Glatthor N. , Grabowski U. , Kellmann S. , Linden A.
Published: April 2010

Abstract. We present global distributions of carbon monoxide (CO) from the upper troposphere to the mesosphere observed by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat. Vertically resolved volume mixing ratio profiles have been retrieved from 4.7 μm limb emission spectra under consideration of non-local thermodynamic equilibrium. The precision of individual CO profiles is typically 5–30 ppbv (15–40%). Estimated systematic errors are in the order of 8–15%. Below 60 km, the vertical resolution is 4–7 km. The data set which covers 54 days from September 2003 to March 2004 has been derived with an improved retrieval version including (i) the retrieval of log(vmr), (ii) the consideration of illumination-dependent vibrational population gradients along the instrument's line of sight, and (iii) joint-fitted vmr horizontal gradients in latitudinal and longitudinal directions. A detailed analysis of spatially resolved CO distributions during the 2003/2004 Northern Hemisphere major warming event demonstrate the potential of MIPAS CO observations to obtain new information on transport processes during dynamical active episodes, particularly on those acting in the vertical. From the temporal evolution of zonally averaged CO abundances, we derived extraordinary polar winter descent velocities of 1200 m per day inside the recovered polar vortex in January 2004. Middle stratospheric CO abundances show a well established correlation with the chemical source CH4, particularly in the tropics. In the upper troposphere, a~moderate CO decrease from September 2003 to March 2004 was observed. Upper tropospheric CO observations provide a detailed picture of long-range transport of polluted air masses and uplift events. MIPAS observations taken on 9–11 September 2003 confirm the trapping of convective outflow of polluted CO-rich air from Southeast Asia into the Asian monsoon anticyclone, which has been described in previous studies. Upper tropospheric CO plumes, observed by MIPAS on this day, were predominantly located in the Northern Hemisphere. Most of these plumes could be related to Southeast Asian pollution by means of backward trajectory calculations. During 20–22 October, southern hemispheric biomass burning was the most likely source of the major CO plumes observed over the Southern Atlantic and Indian Ocean.
Towards closing the gap between hygroscopic growth and activation for secondary organic aerosol – Part 2: Theoretical approaches
Authors: Petters M. D. , Wex H. , Carrico C. M. , Hallbauer E. , Massling A. , McMeeking G. R. , Poulain L. , Wu Z. , Kreidenweis S. M. , Stratmann F.
Published: April 2010

Abstract. We examine the hygroscopic properties of secondary organic aerosol particles generated through the reaction of alpha-pinene and ozone using a continuous flow reaction chamber. The water activity versus composition relationship is calculated from measurements of growth factors at relative humidities up to 99.6% and from measurements of cloud condensation nuclei activity. The observed relationships are complex, suggesting highly non-ideal behavior for aerosol water contents at relative humidities less than 98%. We present two models that may explain the observed water activity-composition relationship equally well. The first model assumes that the aerosol is a pseudo binary mixture of infinitely water soluble compounds and sparingly soluble compounds that gradually enter the solution as dilution increases. The second model is used to compute the Gibbs free energy of the aerosol-water mixture and shows that the aerosol behaves similarly to what can be expected for single compounds that contain a certain fraction of oxygenated and non-polar functional groups.
Ice supersaturations and cirrus cloud crystal numbers
Authors: Krämer M. , Schiller C. , Afchine A. , Bauer R. , Gensch I. , Mangold A. , Schlicht S. , Spelten N. , Sitnikov N. , Borrmann S. , de Reus M. , Spichtinger P.
Published: April 2010

Abstract. Upper tropospheric observations outside and inside of cirrus clouds of water vapour mixing ratios sometimes exceeding water saturation, yielding up to more than 200% relative humidities over ice (RHice) have been reported from aircraft and balloon measurements in recent years. From these observations a lively continuous discussion arose on whether there is a lack of understanding of ice cloud microphysics or if the water measurements are tainted with large uncertainties or flaws. Here, RHice in clear air and in ice clouds is investigated: strictly quality checked aircraft in-situ observations of RHice were performed during 28 flights in tropical, mid-latitude and Arctic field experiments in the temperature range 183–250 K. In our field measurements, no supersaturations above water saturation are found. Nevertheless, super- or subsaturations inside of cirrus are frequently observed at low temperatures (<205 K) in our field data set. To explain persistent RHice deviating from saturation, we analysed the number densities of ice crystals recorded during 20 flights. From the combined analysis – using conventional microphysics – of supersaturations and ice crystal numbers, we show that the high, persistent supersaturations observed inside of cirrus are caused by unexpected, frequent very low ice crystal numbers that could hardly be explained by homogeneous ice nucleation. Heterogeneous ice formation or the suppression of freezing might better explain the observed ice crystal numbers. Thus, our lack of understanding of the high supersaturations with implications to the microphysical and radiative properties of cirrus, the vertical redistribution of water and climate, is traced back to the understanding of the freezing process at low temperatures.
Integrated water vapor above Ny Ålesund, Spitsbergen: a multisensor intercomparison
Authors: Palm M. , Melsheimer C. , Noël S. , Notholt J. , Burrows J. , Schrems O.
Published: April 2010

Abstract. Water vapor is an important constituent of the atmosphere. Because of its abundance it plays an important role for the radiation budget of the atmosphere and has major influence on weather and climate. In this work the integrated water vapor (IWV) measurements derived from the measurements of two satellite sensors, SCIAMACHY and AMSU-B, and two ground-based sensors, a Fourier-transform spectrometer (FTIR) and an O3 microwave ozone sensor (RAM), are compared to radio-sonde measurements in Ny Ålesund, 79° N. All four remote sensors exploit different principles and work in different wavelength regions. Combined they deliver a comprehensive picture of the IWV above Ny Ålesund. The ground-based FTIR reproduces the radio-sonde measurements very well and also shows a high correlation and very little scatter of about 10%. The other remote sensing instruments show a good correlation with the coincident radio-sonde measurements but show high scatter of about 20% (standard deviation). The ground-based RAM performs similar to the satellite instruments, which is somewhat surprising, because measuring IWV is only a by-product for this sensor. The RAM sensor records a measurement every hour and is therefore suited to observe the diurnal variation. As measured by the RAM and FTIR the variance within 4 h is often in excess of 50% (minimum – maximum of the measured IWV). This large variance in the integrated water vapor renders the comparison of different sensors a difficult task. The derived variance of the instruments when compared to radio-sonde measurements can be explained by the high natural variability of IWV.
Utilising polyphenylene oxide for high exposure solar UVA dosimetry
Authors: Turnbull D. J. , Schouten P. W.
Published: April 2010

Abstract. Researchers at the University of Southern Queensland have developed a personal UV dosimeter that can quantitatively assess high exposure solar UVA exposures. The chemical polyphenylene oxide has been previously reported on its ability to measure high UVB exposures. This current research has found that polyphenylene oxide, cast in thin film form, is responsive to both the UVA and UVB parts of the solar spectrum. Further to this, the UVB wavelengths were filtered out with the use of mylar. This combined system responded to the UVA wavelengths only and underwent a change in optical absorbance as a result of UVA exposure. Preliminary results indicate that this UVA dosimeter saturates steadily when exposed to sunlight and can measure exposures of more than 20 MJ/m2 of solar UVA radiation with an uncertainty level of no more than ±5%.
Depletion of gaseous polycyclic aromatic hydrocarbons by a forest canopy
Authors: Choi S.-D. , Li H. , Su Y. , Gevao B. , Harner T. , Staebler R. M. , Wania F.
Published: April 2010

Abstract. Rapid uptake of gaseous polycyclic aromatic hydrocarbons (PAHs) by a forest canopy was observed at Borden in Southern Ontario, Canada during bud break in early spring 2003. High volume air samples were taken on 12 individual days at three different heights (44.4, 29.1, and 16.7 m) on a scaffolding tower and on the forest floor below the canopy (1.5 m). Concentrations of PAHs were positively correlated to ambient temperature, resulting from relatively warm and polluted air masses passing over the Eastern United States and Toronto prior to arriving at the sampling site. An analysis of vertical profiles and gas/particle partitioning of the PAHs showed that gaseous PAHs established a concentration gradient with height, whereas levels of particulate PAHs were relatively uniform, implying that only the uptake of gaseous PAHs by the forest canopy was sufficiently rapid to be observed. Specifically, the gaseous concentrations of intermediate PAHs, such as phenanthrene, anthracene, and pyrene, during budburst and leaf emergence were reduced within and above the canopy. When a gradient was observed, the percentage of PAHs on particles increased at the elevations experiencing a decrease in gas phase concentrations. The uptake of intermediate PAHs by the canopy also led to significant differences in gaseous PAH composition with height. These results are the most direct evidence yet of the filter effect of forest canopies for gaseous PAHs in early spring. PAH deposition fluxes and dry gaseous deposition velocities to the forest canopy were estimated from the concentration gradients.
Spectral UV measurements in Austria from 1994 to 2006: investigations of short- and long-term changes
Authors: Simic S. , Weihs P. , Vacek A. , Kromp-Kolb H. , Fitzka M.
Published: April 2010

Abstract. Influences of atmospheric variability on short- and long-term changes of spectral UV irradiance measured at the Sonnblick observatory (47.03 N, 12.57 E, 3106 m) during the period from 1994 to 2006 is studied. Measurements are performed with a Brewer ozone single spectrophotometer and with a Bentham DM150 spectroradiometer (double monochromator). The influence of ozone, albedo and clouds on UV variability is evaluated separately using 10-year climatology. It is found that the effect of total ozone on short-term variability of UV irradiance at 305 nm can be more than 200% and on average more than 50%. Clouds can cause variability of 150% or more and on average 35%. Variability caused by albedo is maximum 32%. Long-term trends are investigated for the time period from 1994 to 2006 using the non-parametric Mann-Kendall trend test. Significant downwards trends (99% confidence level) were found for solar zenith angle 55° at wavelengths from 305 nm to 324 nm and CIE.
Comparison of ground-based Brewer and FTIR total O3 monitoring techniques
Authors: Schneider M. , Redondas A. , Hase F. , Guirado C. , Blumenstock T. , Cuevas E.
Published: April 2010

Abstract. We compare the currently most precise, ground-based total O3 measurement techniques: Brewer and FTIR. We give an overview of the similarities and the differences between the measurements and the retrieval approaches of both experiments. By means of coinciding measurements performed at the Atmospheric Observatory of Izaña from 2005 to 2007 we show that the small differences between both techniques are in excellent agreement with the theoretical predictions. Our empirical study confirms that both FTIR and Brewer measurements are able to continuously monitor total O3 amounts with a precision of better than 0.4%.
Synergetic aerosol retrieval from SCIAMACHY and AATSR onboard ENVISAT
Authors: Holzer-Popp T. , Schroedter-Homscheidt M. , Breitkreuz H. , Martynenko D. , Klüser L.
Published: April 2010

Abstract. The synergetic aerosol retrieval method SYNAER (Holzer-Popp et al., 2002a) has been extended to the use of ENVISAT measurements. It exploits the complementary information of a radiometer and a spectrometer onboard one satellite platform to extract aerosol optical depth (AOD) and speciation (as choice from a representative set of pre-defined mixtures of water-soluble, soot, mineral dust, and sea salt components). SYNAER consists of two retrieval steps. In the first step the radiometer is used to do accurate cloud screening, and subsequently to quantify the aerosol optical depth (AOD) at 550 nm and spectral surface brightness through a dark field technique. In the second step the spectrometer is applied to choose the most plausible aerosol type through a least square fit of the measured spectrum with simulated spectra using the AOD and surface brightness retrieved in the first step. This method was developed and a first case study evaluation against few (15) multi-spectral ground-based AERONET sun photometer observations was conducted with a sensor pair (ATSR-2 and GOME) onboard ERS-2. However, due to instrumental limitations the coverage of SYNAER/ERS-2 and the AERONET network in 1997/98 is very sparse and thus only few coincidences with AERONET were found. Therefore, SYNAER was transferred to similar sensors AATSR and SCIAMACHY onboard ENVISAT. While transferring to the new sensor pair a thorough evaluation of the synergetic methodology and its information content has been conducted, which led to significant improvements in the methodology: an update of the aerosol model, an improved cloud detection, and an enhanced dark field albedo characterization. This paper describes the information content analysis and these improvements in detail and presents first results of applying the SYNAER methodology to AATSR and SCIAMACHY.
Secondary organic aerosol (SOA) formation from reaction of isoprene with nitrate radicals (NO3)
Authors: Ng N. L. , Kwan A. J. , Surratt J. D. , Chan A. W. H. , Chhabra P. S. , Sorooshian A. , Pye H. O. T. , Crounse J. D. , Wennberg P. O. , Flagan R. C. , Seinfeld J. H.
Published: April 2010

Abstract. Secondary organic aerosol (SOA) formation from the reaction of isoprene with nitrate radicals (NO3) is investigated in the Caltech indoor chambers. Experiments are performed in the dark and under dry conditions (RH<10%) using N2O5 as a source of NO3 radicals. For an initial isoprene concentration of 18.4 to 101.6 ppb, the SOA yield (defined as the ratio of the mass of organic aerosol formed to the mass of parent hydrocarbon reacted) ranges from 4.3% to 23.8%. By examining the time evolutions of gas-phase intermediate products and aerosol volume in real time, we are able to constrain the chemistry that leads to the formation of low-volatility products. Although the formation of ROOR from the reaction of two peroxy radicals (RO2) has generally been considered as a minor channel, based on the gas-phase and aerosol-phase data it appears that RO2+RO2 reaction (self reaction or cross-reaction) in the gas phase yielding ROOR products is a dominant SOA formation pathway. A wide array of organic nitrates and peroxides are identified in the aerosol formed and mechanisms for SOA formation are proposed. Using a uniform SOA yield of 10% (corresponding to Mo≅10 μg m−3), it is estimated that ~2 to 3 Tg yr−1 of SOA results from isoprene + NO3. The extent to which the results from this study can be applied to conditions in the atmosphere depends on the fate of peroxy radicals (i.e. the relative importance of RO2+RO2 versus RO2+NO3 reactions) in the nighttime troposphere.
Antarctic network of lamp-calibrated multichannel radiometers for continuous ozone and uv radiation data
Authors: Redondas A. , Torres C. , Meinander O. , Lakkala K. , García R. , Cuevas E. , Ochoa H. , Deferrari G. , Díaz S.
Published: April 2010

Abstract. Three NILU-UV multichannel radiometers have been installed in 1999 at the Argentinian sites of Ushuaia (54S), Marambio (64S) and Belgrano-II (77S) in order to continuously monitor UV radiation, photosynthetically active radiation and total ozone. The measurements were established by INM, Spain in collaboration with FMI, Finland, DNA-IAA, Argentina and CADIC, Argentina to observe and characterize the spatial and temporal evolution of ozone and ultraviolet radiation in the Antarctic region. Special attention has been given to the quality control and quality assurance of the measurements under harsh climatological conditions. The ozone and UV time series of 2000–2006 were calibrated using a polynomial fit for lamp measurements performed every second week all year round. The gaps in these data are minimal, with almost no data missing, and the data products are available from http://www.polarvortex.org in near real time. The data products include the erythemally-weighted UV, UVB and UVA radiation, photosynthetically active radiation (PAR), total ozone (O3) and a cloud parameter (CLT). For UV data, dose rates as well as daily doses are available; from these the maximum measured UV indices (UVI), during 2000–2006, were 12.0, 9.7 and 8.1 at Ushuaia, Marambio and Belgrano-II, respectively.
Analysis of aircraft and satellite measurements from the intercontinental chemical transport experiment (INTEX-B) to quantify long-range transport of East Asian Sulfur to Canada
Authors: van Donkelaar A. , Martin R. V. , Leaitch W. R. , Macdonald A. M. , Walker T. W. , Streets D. G. , Zang Q. , Dunlea E. , Jimenez J. L. , Dibb J. E. , Huley G. , Weber R. , Andreae M. O..
Published: April 2010

Abstract. We interpret a suite of satellite, aircraft, and ground-based measurements over the North Pacific Ocean and western North America during April–May 2006 as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign to understand the implications of long-range transport of East Asian emissions to North America. The Canadian component of INTEX-B included 33 vertical profiles from a Cessna 207 aircraft equipped with an aerosol mass spectrometer. Long-range transport of organic aerosols was insignificant. Measured sulfate plumes in the free troposphere over British Columbia exceeded 1 μg/m3. We update the global anthropogenic emission inventory in a chemical transport model (GEOS-Chem) and use it to interpret the observations. Trends in Aerosol Optical Depth (AOD) retrieved from two satellite instruments (MISR and MODIS) for 2000–2006 are analyzed with GEOS-Chem to estimate an annual growth in Chinese sulfur emissions of 6.2% and 9.6%, respectively. Analysis of aircraft sulfate measurements from the NASA DC-8 over the central Pacific, the NSF C-130 over the east Pacific and the Cessna over British Columbia indicates most Asian sulfate over the ocean is in the lower free troposphere (800–600 hPa), with a decrease in pressure toward land due to orographic effects. We calculate that 63% of the measured sulfate at 600 hPa over British Columbia is due to East Asian sources. Simulation of INTEX-B and May 1985 aircraft measurements off the northwest coast of the United States reveals a 2.4–3.4 fold increase in the relative contribution of East Asian sulfate to the total burden. Campaign-average simulations indicate anthropogenic East Asian sulfur emissions increase mean springtime sulfate in Western Canada at the surface by 0.14–0.19 μg/m3 (~30%) and account for 40% of the overall regional sulfate burden between 1 and 5 km. Mean measured daily surface sulfate concentrations taken in the Vancouver area increase by 0.27 μg/m3 per 10% increase in the simulated fraction of Asian sulfate, suggesting current East Asian emissions degrade local air quality.
Reconstruction of the solar spectral UV irradiance for nowcasting of the middle atmosphere state on the basis of LYRA measurements
Authors: Egorova T. , Rozanov E. , Hochedez J.-F. , Schmutz W.
Published: April 2010

Abstract. The LYRA instrument onboard ESA PROBA2 satellite will provide 6-hourly solar irradiance at the Lyman-alpha (121.6 nm) and the Herzberg continuum (~200–220 nm wavelength range). Because the nowcasting of the neutral and ionic state of the middle atmosphere requires the solar irradiance for the wide spectral area (120–680 nm) we have developed the statistical tool for the reconstruction of the full spectrum from the LYRA measurements. The accuracy of the reconstructed irradiance has been evaluated with 1-D transient radiative-convective model with neutral and ion chemistry using the daily solar spectral irradiance measured with SUSIM and SOLSTICE instruments onboard UARS satellite. We compared the results of transient 1-yr long model simulations for 2000 driven by the observed and reconstructed solar irradiance and showed that the reconstruction of the full spectrum using linear regression equation based on the solar irradiance in two LYRA channels can be successfully used for nowcasting of the middle atmosphere. We have also defined some conditions when the proposed approach does not provide reasonable accuracy.
Radiative forcing from modelled and observed stratospheric ozone changes due to the 11-year solar cycle
Authors: Isaksen I. S. A. , Rognerud B. , Myhre G. , Haigh J. D. , Rumbold S. T. , Shine K. P. , Zerefos C. , Tourpali K. , Randel W.
Published: April 2010

Abstract. Three analyses of satellite observations and two sets of model studies are used to estimate changes in the stratospheric ozone distribution from solar minimum to solar maximum and are presented for three different latitudinal bands: Poleward of 30° north, between 30° north and 30° south and poleward of 30° south. In the model studies the solar cycle impact is limited to changes in UV fluxes. There is a general agreement between satellite observation and model studies, particular at middle and high northern latitudes. Ozone increases at solar maximum with peak values around 40 km. The profiles are used to calculate the radiative forcing (RF) from solar minimum to solar maximum. The ozone RF, calculated with two different radiative transfer schemes is found to be negligible (a magnitude of 0.01 Wm−2 or less), compared to the direct RF due to changes in solar irradiance, since contributions from the longwave and shortwave nearly cancel each other. The largest uncertainties in the estimates come from the lower stratosphere, where there is significant disagreement between the different ozone profiles.
Water vapor release from biofuel combustion
Authors: Parmar R. S. , Welling M. , Andreae M. O. , Helas G.
Published: April 2010

Abstract. We report on the emission of water vapor from biofuel combustion. Concurrent measurements of carbon monoxide and carbon dioxide are used to scale the concentrations of water vapor found, and are compared to carbon in the biofuel. Fuel types included hardwood (oak and African musasa), softwood (pine and spruce, partly with green needles), and African savanna grass. The session-averaged ratio of H2O to the sum of CO and CO2 in the emissions from 16 combustion experiments ranged from 1.2 to 3.7 on average, indicating the presence of water that is not chemically bound. This biofuel moisture content ranged from 33% in the dry African hardwood, musasa, to 220% in fresh pine branches with needles. The moisture content from fresh biofuel contributes distinctly to the water vapor in biomass burning emissions, and its influence on meteorology needs to be evaluated.
Long-term solar UV radiation reconstructed by Artificial Neural Networks (ANN)
Authors: Feister U. , Junk J. , Woldt M.
Published: April 2010

Abstract. Artificial Neural Networks (ANN) are efficient tools to derive solar UV radiation from measured meteorological parameters such as global radiation, aerosol optical depths and atmospheric column ozone. The ANN model has been tested with different combinations of data from the two sites Potsdam and Lindenberg, and used to reconstruct solar UV radiation at eight European sites by more than 100 years into the past. Annual totals of UV radiation derived from reconstructed daily UV values reflect interannual variations and long-term patterns that are compatible with variabilities and changes of measured input data, in particular global dimming by about 1980–1990, subsequent global brightening, volcanic eruption effects such as that of Mt. Pinatubo, and the long-term ozone decline since the 1970s. Patterns of annual erythemal UV radiation are very similar at sites located at latitudes close to each other, but different patterns occur between UV radiation at sites in different latitude regions.
Evaluation of tropospheric and stratospheric ozone trends over Western Europe from ground-based FTIR network observations
Authors: Vigouroux C. , De Mazière M. , Demoulin P. , Servais C. , Hase F. , Blumenstock T. , Kramer I. , Schneider M. , Mellqvist J. , Strandberg A. , Velazco V. , Notholt J. , Sussmann R. , Stremme W. , Rockmann A. , Gardiner T. , Coleman M. , Woods P.
Published: April 2010

Abstract. Within the European project UFTIR (Time series of Upper Free Troposphere observations from an European ground-based FTIR network), six ground-based stations in Western Europe, from 79° N to 28° N, all equipped with Fourier Transform infrared (FTIR) instruments and part of the Network for the Detection of Atmospheric Composition Change (NDACC), have joined their efforts to evaluate the trend of several direct and indirect greenhouse gases over the period 1995–2004. The retrievals of CO, CH4, C2H6, N2O, CHClF2, and O3 have been optimized. Using the optimal estimation method, some vertical information can be obtained in addition to total column amounts. A bootstrap resampling method has been implemented to determine annual partial and total column trends for the target gases. The present work focuses on the ozone results. The retrieved time series of partial and total ozone columns are validated with ground-based correlative data (Brewer, Dobson, UV-Vis, ozonesondes, and Lidar). The observed total column ozone trends are in agreement with previous studies: 1) no total column ozone trend is seen at the lowest latitude station Izaña (28° N); 2) slightly positive total column trends are seen at the two mid-latitude stations Zugspitze and Jungfraujoch (47° N), only one of them being significant; 3) the highest latitude stations Harestua (60° N), Kiruna (68° N) and Ny-Ålesund (79° N) show significant positive total column trends. Following the vertical information contained in the ozone FTIR retrievals, we provide partial columns trends for the layers: ground-10 km, 10–18 km, 18–27 km, and 27–42 km, which helps to distinguish the contributions from dynamical and chemical changes on the total column ozone trends. We obtain no statistically significant trends in the ground–10 km layer for five out of the six ground-based stations. We find significant positive trends for the lowermost stratosphere at the two mid-latitude stations, and at Ny-Ålesund. We find smaller, but significant trends for the 18–27 km layer at Kiruna, Harestua, Jungfraujoch, and Izaña. The results for the upper layer are quite contrasted: we find significant positive trends at Kiruna, Harestua, and Jungfraujoch, and significant negative trends at Zugspitze and Izaña. These ozone partial columns trends are discussed and confronted to previous studies.
Case studies of particle formation events observed in boreal forests: implications for nucleation mechanisms
Authors: Yu F. , Turco R.
Published: April 2010

Abstract. Aerosol nucleation events observed worldwide may have significant climatic and health implications. However, the specific nucleation mechanisms remain ambiguous. Here, we report case studies of six nucleation events observed during an intensive field campaign at a boreal forest site (Hyytiälä, Finland) in spring 2005. The present analysis is based on comprehensive kinetic simulations using an ion-mediated nucleation (IMN) model in which the key physical and chemical parameters are constrained by a variety of recent measurements. Out of roughly 30 nucleation event days sampled during the campaign, four were initially selected on the basis of indications that the observed air masses were relatively homogeneous. It happens that all four of these days exhibited medium to high electrical overcharging of the nucleated nanoparticles. In each of these well-defined cases, reasonable agreement is found between the predictions and field data for a range of variables, including critical nucleation sizes, size-dependent overcharging ratios, and the concentrations of 1.8–3 nm stable clusters and 3–6 nm particles, and their diurnal variations. However, to extend the scope of the study, one case of weak electrical overcharging, and one of clear undercharging, of the nucleated particles were also selected. These electrical states represented less than about 20% of the total event-days recorded, and among this smaller sample there were no days on which the sampled air masses appeared reasonable uniform over the entire nucleation event. Thus, it is perhaps not surprising that the consistency between model simulations and measurements during these more anomalous periods was less satisfying. We tentatively conclude that the outcomes in these cases were influenced by, among other things, the significant variability in the sampled air masses and the possible role of species other than sulfuric acid in the nucleation process. Statistically, roughly 80% of the nucleation events recorded during the Hyytiälä campaign exhibited mean size-dependent overcharging ratios within the range, or exceeding, those predicted by the IMN model, suggesting that ion nucleation processes are significant. The nucleation rates calculated using the IMN modeling approach are contrasted with those predicted by other theories/models, and key differences between the results are discussed.
Odin/OSIRIS observations of stratospheric NO3 through sunrise and sunset
Authors: McLinden C. A. , Haley C. S.
Published: April 2010

Abstract. The nitrate radical (NO3) has been detected in visible limb-scattered spectra measured by the Optical Spectrograph and InfraRed Imager System (OSIRIS) on-board the Odin satellite when observing at large solar zenith angles (91–97°). Apparent slant column densities of NO3 at tangent heights between 10 and 45 km are derived via spectral fitting in the 590–680 nm window. Using observations from multiple scans spanning solar zenith angles of 91–97°, the rapid evolution of NO3 through sunrise and sunset can be traced. Slant column densities are found to be consistent with those simulated using a radiative transfer model with coupled photochemistry. In addition, a strong dependence of NO3 with temperature is observed. These results indicate that OSIRIS possesses signal-to-noise sufficient to make useful measurements of scattered sunlight out to solar zenith angles of 96–97° and suggests the possibility of retrieving profile information for NO3 and other species at large solar zenith angles.
Emulating IPCC AR4 atmosphere-ocean and carbon cycle models for projecting global-mean, hemispheric and land/ocean temperatures: MAGICC 6.0
Authors: Meinshausen M. , Raper S. C. B. , Wigley T. M. L.
Published: April 2010

Abstract. Current scientific knowledge on the future response of the climate system to human-induced perturbations is comprehensively captured by various model intercomparison efforts. In the preparation of the Fourth Assessment Report (AR4) of the Intergovernmental Panel on Climate Change (IPCC), intercomparisons were organized for atmosphere-ocean general circulation models (AOGCMs) and carbon cycle models, named "CMIP3" and "C4MIP", respectively. Despite their tremendous value for the scientific community and policy makers alike, there are some difficulties in interpreting the results. For example, key radiative forcings have not been considered or standardized in the majority of AOGCMs integrations and carbon cycle runs. Furthermore, the AOGCM analysis of plausible emission pathways was restricted to only three SRES scenarios. This study attempts to address these issues. We present an updated version of MAGICC, the simple carbon cycle-climate model used in past IPCC Assessment Reports with enhanced representation of time-varying climate sensitivities, carbon cycle feedbacks, aerosol forcings and ocean heat uptake characteristics. This new version of MAGICC (6.0) is successfully calibrated against the higher complexity AOGCM and carbon cycle models. Parameterizations of MAGICC 6.0 are provided. Previous MAGICC versions and emulations shown in IPCC AR4 (WG1, Fig. 10.26, page 803) yielded, in average, a 10% larger global-mean temperature increase over the 21st century compared to the AOGCMs. The reasons for this difference are discussed. The emulations presented here using MAGICC 6.0 match the mean AOGCM responses to within 2.2% for the SRES scenarios. This enhanced emulation skill is due to: the comparison on a "like-with-like" basis using AOGCM-specific subsets of forcings, a new calibration procedure, as well as the fact that the updated simple climate model can now successfully emulate some of the climate-state dependent effective climate sensitivities of AOGCMs. The mean diagnosed effective climate sensitivities of the AOGCMs is 2.88°C, about 0.33°C cooler than the reported slab ocean climate sensitivities. Finally, we examine the combined climate system and carbon cycle emulations for the complete range of IPCC SRES emission scenarios and some lower mitigation pathways.
Technical Note: Review of methods for linear least-squares fitting of data and application to atmospheric chemistry problems
Authors: Cantrell C. A.
Published: April 2010

Abstract. The representation of data, whether geophysical observations, numerical model output or laboratory results, by a best fit straight line is a routine practice in the geosciences and other fields. While the literature is full of detailed analyses of procedures for fitting straight lines to values with uncertainties, a surprising number of scientists blindly use the standard least squares method, such as found on calculators and in spreadsheet programs, that assumes no uncertainties in the x values. Here, the available procedures for estimating the best fit straight line to data, including those applicable to situations for uncertainties present in both the x and y variables, are reviewed. Representative methods that are presented in the literature for bivariate weighted fits are compared using several sample data sets, and guidance is presented as to when the somewhat more involved iterative methods are required, or when the standard least-squares procedure would be expected to be satisfactory. A spreadsheet-based template is made available that employs one method for bivariate fitting.