bluuebunny/crossref_metadata_2025 huggingface dataset:
Validation of ACE-FTS satellite data in the upper troposphere/lower stratosphere (UTLS) using non-coincident measurements
Authors: Hegglin M. I. , Boone C. D. , Manney G. L. , Shepherd T. G. , Walker K. A. , Bernath P. F. , Daffer W. H. , Hoor P. , Schiller C.
Published: April 2010

Abstract. CO, O3, and H2O data in the upper troposphere/lower stratosphere (UTLS) measured by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on Canada's SCISAT-1 satellite are validated using aircraft and ozonesonde measurements. In the UTLS, validation of chemical trace gas measurements is a challenging task due to small-scale variability in the tracer fields, strong gradients of the tracers across the tropopause, and scarcity of measurements suitable for validation purposes. Validation based on coincidences therefore suffers from geophysical noise. Two alternative methods for the validation of satellite data are introduced, which avoid the usual need for coincident measurements: tracer-tracer correlations, and vertical tracer profiles relative to tropopause height. Both are increasingly being used for model validation as they strongly suppress geophysical variability and thereby provide an "instantaneous climatology". This allows comparison of measurements between non-coincident data sets which yields information about the precision and a statistically meaningful error-assessment of the ACE-FTS satellite data in the UTLS. By defining a trade-off factor, we show that the measurement errors can be reduced by including more measurements obtained over a wider longitude range into the comparison, despite the increased geophysical variability. Applying the methods then yields the following upper bounds to the relative differences in the mean found between the ACE-FTS and SPURT aircraft measurements in the upper troposphere (UT) and lower stratosphere (LS), respectively: for CO ±9% and ±12%, for H2O ±30% and ±18%, and for O3 ±25% and ±19%. The relative differences for O3 can be narrowed down by using a larger dataset obtained from ozonesondes, yielding a high bias in the ACE-FTS measurements of 18% in the UT and relative differences of ±8% for measurements in the LS. When taking into account the smearing effect of the vertically limited spacing between measurements of the ACE-FTS instrument, the relative differences decrease by 5–15% around the tropopause, suggesting a vertical resolution of the ACE-FTS in the UTLS of around 1 km. The ACE-FTS hence offers unprecedented precision and vertical resolution for a satellite instrument, which will allow a new global perspective on UTLS tracer distributions.
Tropical thin cirrus and relative humidity observed by the Atmospheric Infrared Sounder
Authors: Kahn B. H. , Liang C. K. , Eldering A. , Gettelman A. , Yue Q. , Liou K. N.
Published: April 2010

Abstract. Global observations of cloud and humidity distributions in the upper troposphere within all geophysical conditions are critically important in order to monitor the present climate and to provide necessary data for validation of climate models to project future climate change. Towards this end, tropical oceanic distributions of thin cirrus optical depth (τ), effective diameter (De), and relative humidity with respect to ice (RHi) within cirrus (RHic) are simultaneously derived from the Atmospheric Infrared Sounder (AIRS). Corresponding increases in De and cloud temperature are shown for cirrus with τ>0.25 that demonstrate quantitative consistency to other surface-based, in situ and satellite retrievals. However, inferred cirrus properties are shown to be less certain for increasingly tenuous cirrus. In-cloud supersaturation is observed for 8–12% of thin cirrus and is several factors higher than all-sky conditions; even higher frequencies are shown for the coldest and thinnest cirrus. Spatial and temporal variations in RHic correspond to cloud frequency while regional variability in RHic is observed to be most prominent over the N. Indian Ocean basin. The largest cloud/clear sky RHi anomalies tend to occur in dry regions associated with vertical descent in the sub-tropics, while the smallest occur in moist ascending regions in the tropics. The characteristics of RHic frequency distributions depend on τ and a peak frequency is located between 60–80% that illustrates RHic is on average biased dry. The geometrical thickness of cirrus is typically less than the vertical resolution of AIRS temperature and specific humidity profiles and thus leads to the observed dry bias, shown with coincident cloud vertical structure obtained from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO). The joint distributions of thin cirrus microphysics and humidity derived from AIRS provide unique and important regional and global-scale insights on upper tropospheric processes not available from surface, in situ, and other contemporary satellite observing platforms.
Preliminary results of GOME-2 water vapour retrievals and first applications in polar regions
Authors: Noël S. , Mieruch S. , Bovensmann H. , Burrows J. P.
Published: April 2010

Abstract. Global total water vapour columns have been derived from measurements of the Global Ozone Monitoring Experiment 2 (GOME-2) on MetOp. For this purpose, the Air Mass Corrected Differential Optical Absorption Spectroscopy (AMC-DOAS) method has been adapted, having previously been applied successfully to GOME (on ERS-2) and SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY, on ENVISAT) data. Comparisons between the derived GOME-2 and SCIAMACHY water vapour columns show a good overall agreement. This gives confidence that the temporal series of water vapour columns from GOME-type instruments (GOME/ERS-2, SCIAMACHY/ENVISAT), which began in 1995, is successfully continued by the MetOp instrumentation until at least 2020. The enhanced temporal and spatial resolution of GOME-2 enables the analysis of diurnal variations in the polar regions. This is especially important because atmospheric data sources in the polar regions are generally sparse. As an exemplary application, daily water vapour total columns over the polar research station Ny Ålesund (78°55'19" N/11°56'33" E) are investigated. At this latitude GOME-2 yields about six data points during daylight hours at varying local times. From these data diurnal variations of water vapour have been successfully retrieved.
The time evolution of aerosol composition over the Mexico City plateau
Authors: Kleinman L. I. , Springston S. R. , Daum P. H. , Lee Y.-N. , Nunnermacker L. J. , Senum G. I. , Wang J. , Weinstein-Lloyd J. , Alexander M. L. , Hubbe J. , Ortega J. , Canagaratna M. R. , Jayne J.
Published: April 2010

Abstract. The time evolution of aerosol concentration and chemical composition in a megacity urban plume was determined based on 8 flights of the DOE G-1 aircraft in and downwind of Mexico City during the March 2006 MILAGRO field campaign. A series of selection criteria are imposed to eliminate data points with non-urban emission influences. Biomass burning has urban and non-urban sources that are distinguished on the basis of CH3CN and CO. In order to account for dilution in the urban plume, aerosol concentrations are normalized to CO which is taken as an inert tracer of urban emission, proportional to the emissions of aerosol precursors. Time evolution is determined with respect to photochemical age defined as −Log10 (NOx/NOy). The geographic distribution of photochemical age and CO is examined, confirming the picture that Mexico City is a source region and that pollutants become more dilute and aged as they are advected towards T1 and T2, surface sites that are located at the fringe of the City and 35 km to the NE, respectively. Organic aerosol (OA) per ppm CO is found to increase 7 fold over the range of photochemical ages studied, corresponding to a change in NOx/NOy from nearly 100% to 10%. In the older samples the nitrate/CO ratio has leveled off suggesting that evaporation and formation of aerosol nitrate are in balance. In contrast, OA/CO increases with age in older samples, indicating that OA is still being formed. The amount of carbon equivalent to the deduced change in OA/CO with age is 56 ppbC per ppm CO. At an aerosol yield of 5% and 8% for low and high yield aromatic compounds, it is estimated from surface hydrocarbon observations that only ~9% of the OA formation can be accounted for. A comparison of OA/CO in Mexico City and the eastern U.S. gives no evidence that aerosol yields are higher in a more polluted environment.
Aerosol distribution over Europe: a model evaluation study with detailed aerosol microphysics
Authors: Langmann B. , Varghese S. , Marmer E. , Vignati E. , Wilson J. , Stier P. , O'Dowd C.
Published: April 2010

Abstract. This paper summarizes an evaluation of model simulations with a regional scale atmospheric climate-chemistry/aerosol model called REMOTE, which has been extended by a microphysical aerosol module. Model results over Europe are presented and compared with available measurements in surface air focusing on the European distribution and variability of primary and secondary aerosols. Additionally, model results obtained with detailed aerosol microphysics are compared to those based on an aerosol bulk mass approach revealing the impact of dry deposition fluxes on atmospheric burden concentration. An improved determination of elevated ozone and sulfate concentrations could be achieved by considering a diurnal cycle in the anthropogenic emission fluxes. Deviation between modelled and measured organic carbon concentrations can be mainly explained by missing formation of secondary organic aerosols and deficiencies in emission data. Changing residential heating practices in Europe, where the use of wood is no longer restricted to rural areas, need to be considered in emission inventories as well as vegetation fire emissions which present a dominant source of organic carbon.
Operational retrieval of Asian sand and dust storm from FY-2C geostationary meteorological satellite and its application to real time forecast in Asia
Authors: Hu X. Q. , Lu N. M. , Niu T. , Zhang P.
Published: April 2010

Abstract. This paper describes an operational retrieval algorithm for the sand/dust storm (SDS) from FY-2C/S-VISSR (Stretched-Visible and Infrared Spin-Scan Radiometer) developed at the National Satellite Meteorological Center (NSMC) of China. This algorithm, called Dust Retrieval Algorithm based on Geostationary Imager (DRAGI), is based on the optical and radiative physical properties of SDS in mid-infrared and thermal infrared spectral regions as well as the observation of all bands in the geostationary imager, which include the Brightness Temperature Difference (BTD) in split window channels, Infrared Difference Dust Index (IDDI) and the ratio of middle infrared reflectance to visible reflectance. It also combines the visible and water vapor bands observation of the geostationary imager to identify the dust clouds from the surface targets and meteorological clouds. The output product is validated by and related to other dust aerosol observations such as the synoptic weather reports, surface visibility, aerosol optical depth (AOD) and ground-based PM10 observations. Using the SDS-IDD product and a data assimilation scheme, the dust forecast model CUACE/Dust achieved a substantial improvement to the SDS predictions in spring 2006.
Robust relations between CCN and the vertical evolution of cloud drop size distribution in deep convective clouds
Authors: Freud E. , Rosenfeld D. , Andreae M. O. , Costa A. A. , Artaxo P.
Published: April 2010

Abstract. In-situ measurements in convective clouds (up to the freezing level) over the Amazon basin show that smoke from deforestation fires prevents clouds from precipitating until they acquire a vertical development of at least 4 km, compared to only 1–2 km in clean clouds. The average cloud depth required for the onset of warm rain increased by ~350 m for each additional 100 cloud condensation nuclei per cm3 at a super-saturation of 0.5% (CCN0.5%). In polluted clouds, the diameter of modal liquid water content grows much slower with cloud depth (at least by a factor of ~2), due to the large number of droplets that compete for available water and to the suppressed coalescence processes. Contrary to what other studies have suggested, we did not observe this effect to reach saturation at 3000 or more accumulation mode particles per cm3. The CCN0.5% concentration was found to be a very good predictor for the cloud depth required for the onset of warm precipitation and other microphysical factors, leaving only a secondary role for the updraft velocities in determining the cloud drop size distributions. The effective radius of the cloud droplets (re) was found to be a quite robust parameter for a given environment and cloud depth, showing only a small effect of partial droplet evaporation from the cloud's mixing with its drier environment. This supports one of the basic assumptions of satellite analysis of cloud microphysical processes: the ability to look at different cloud top heights in the same region and regard their re as if they had been measured inside one well developed cloud. The dependence of re on the adiabatic fraction decreased higher in the clouds, especially for cleaner conditions, and disappeared at re≥~10 μm. We propose that droplet coalescence, which is at its peak when warm rain is formed in the cloud at re=~10 μm, continues to be significant during the cloud's mixing with the entrained air, cancelling out the decrease in re due to evaporation.
Technical Note: Coupling of chemical processes with the Modular Earth Submodel System (MESSy) submodel TRACER
Authors: Jöckel P. , Kerkweg A. , Buchholz-Dietsch J. , Tost H. , Sander R. , Pozzer A.
Published: April 2010

Abstract. The implementation of processes related to chemistry into Earth System Models and their coupling within such systems requires the consistent description of the chemical species involved. We provide a tool (written in Fortran95) to structure and manage information about constituents, hereinafter referred to as tracers, namely the Modular Earth Submodel System (MESSy) generic (i.e., infrastructure) submodel TRACER. With TRACER it is possible to define a multitude of tracer sets, depending on the spatio-temporal representation (i.e., the grid structure) of the model. The required information about a specific chemical species is split into the static meta-information about the characteristics of the species, and its (generally in time and space variable) abundance in the corresponding representation. TRACER moreover includes two submodels. One is TRACER_FAMILY, an implementation of the tracer family concept. It distinguishes between two types: type-1 families are usually applied to handle strongly related tracers (e.g., fast equilibrating species) for a specific process (e.g., advection). In contrast to this, type-2 families are applied for tagging techniques. Tagging means the artificial decomposition of one or more species into parts, which are additionally labelled (e.g., by the region of their primary emission) and then processed as the species itself. The type-2 family concept is designed to conserve the linear relationship between the family and its members. The second submodel is TRACER_PDEF, which corrects and budgets numerical negative overshoots that arise in many process implementations due to the numerical limitations (e.g., rounding errors). The submodel therefore guarantees the positive definiteness of the tracers and stabilises the integration scheme. As a by-product, it further provides a global tracer mass diagnostic. Last but not least, we present the submodel PTRAC, which allows the definition of tracers via a Fortran95 namelist, as a complement to the standard tracer definition by application of the TRACER interface routines in the code. TRACER with its submodels and PTRAC can readily be applied to a variety of models without further requirements. The code and a documentation are included in the electronic supplement.
Cirrus, contrails, and ice supersaturated regions in high pressure systems at northern mid latitudes
Authors: Immler F. , Treffeisen R. , Engelbart D. , Krüger K. , Schrems O.
Published: April 2010

Abstract. During the European heat wave summer 2003 with predominant high pressure conditions we performed a detailed study of upper tropospheric humidity and ice particles which yielded striking results concerning the occurrence of ice supersaturated regions (ISSR), cirrus, and contrails. Our study is based on lidar observations and meteorological data obtained at Lindenberg/Germany (52.2° N, 14.1° E) as well as the analysis of the European centre for medium range weather forecast (ECMWF). Cirrus clouds were detected in 55% of the lidar profiles and a large fraction of them were subvisible (optical depth <0.03). Thin ice clouds were particularly ubiquitous in high pressure systems. The radiosonde data showed that the upper troposphere was very often supersaturated with respect to ice. Relating the radiosonde profiles to concurrent lidar observations reveals that the ISSRs almost always contained ice particles. Persistent contrails observed with a camera were frequently embedded in these thin or subvisible cirrus clouds. The ECMWF cloud parametrisation reproduces the observed cirrus clouds consistently and a close correlation between the ice water path in the model and the measured optical depth of cirrus is demonstrated.
Short-lived pollutants in the Arctic: their climate impact and possible mitigation strategies
Authors: Quinn P. K. , Bates T. S. , Baum E. , Doubleday N. , Fiore A. M. , Flanner M. , Fridlind A. , Garrett T. J. , Koch D. , Menon S. , Shindell D. , Stohl A. , Warren S. G.
Published: April 2010

Abstract. Several short-lived pollutants known to impact Arctic climate may be contributing to the accelerated rates of warming observed in this region relative to the global annually averaged temperature increase. Here, we present a summary of the short-lived pollutants that impact Arctic climate including methane, tropospheric ozone, and tropospheric aerosols. For each pollutant, we provide a description of the major sources and the mechanism of forcing. We also provide the first seasonally averaged forcing and corresponding temperature response estimates focused specifically on the Arctic. The calculations indicate that the forcings due to black carbon, methane, and tropospheric ozone lead to a positive surface temperature response indicating the need to reduce emissions of these species within and outside the Arctic. Additional aerosol species may also lead to surface warming if the aerosol is coincident with thin, low lying clouds. We suggest strategies for reducing the warming based on current knowledge and discuss directions for future research to address the large remaining uncertainties.
Volatile organic compound ratios as probes of halogen atom chemistry in the Arctic
Authors: Cavender A. E. , Biesenthal T. A. , Bottenheim J. W. , Shepson P. B.
Published: April 2010

Abstract. Volatile organic compound concentration ratios can be used as indicators of halogen chemistry that occurs during ozone depletion events in the Arctic during spring. Here we use a combination of modeling and measurements of [acetone]/[propanal] as an indicator of bromine chemistry, and [isobutane]/[n-butane] and [methyl ethyl ketone]/[n-butane] are used to study the extent of chlorine chemistry during four ozone depletion events during the Polar Sunrise Experiment of 1995. Using a 0-D photochemistry model in which the input of halogen atoms is controlled and varied, the approximate ratio of [Br]/[Cl] can be estimated for each ozone depletion event. It is concluded that there must be an additional source of propanal (likely from the snowpack) to correctly simulate the VOC chemistry of the Arctic, and further evidence that the ratio of Br atoms to Cl atoms can vary greatly during ozone depletion events is presented.
Evaluation of model-simulated source contributions to tropospheric ozone with aircraft observations in the factor-projected space
Authors: Shim C. , Wang Y. , Yoshida Y.
Published: April 2010

Abstract. Trace gas measurements of TOPSE and TRACE-P experiments and corresponding global GEOS-Chem model simulations are analyzed with the Positive Matrix Factorization (PMF) method for model evaluation purposes. Specially, we evaluate the model simulated contributions to O3 variability from stratospheric transport, intercontinental transport, and production from urban/industry and biomass burning/biogenic sources. We select a suite of relatively long-lived tracers, including 7 chemicals (O3, NOy, PAN, CO, C3H8, CH3Cl, and 7Be) and 1 dynamic tracer (potential temperature). The largest discrepancy is found in the stratospheric contribution to 7Be. The model underestimates this contribution by a factor of 2–3, corresponding well to a reduction of 7Be source by the same magnitude in the default setup of the standard GEOS-Chem model. In contrast, we find that the simulated O3 contributions from stratospheric transport are in reasonable agreement with those derived from the measurements. However, the springtime increasing trend over North America derived from the measurements are largely underestimated in the model, indicating that the magnitude of simulated stratospheric O3 source is reasonable but the temporal distribution needs improvement. The simulated O3 contributions from long-range transport and production from urban/industry and biomass burning/biogenic emissions are also in reasonable agreement with those derived from the measurements, although significant discrepancies are found for some regions.
Comparison of UV-RSS spectral measurements and TUV model runs for clear skies for the May 2003 ARM aerosol intensive observation period
Authors: Michalsky J. J. , Kiedron P. W.
Published: April 2010

Abstract. The first successful deployment of the fully-operational ultraviolet rotating shadow-band spectroradiometer occurred during the May 2003 US Department of Energy's Atmospheric Radiation Measurement program's Aerosol Intensive Observation Period. The aerosol properties in the visible range were characterized using redundant measurements with several instruments to determine the column aerosol optical depth, the single scattering albedo, and the asymmetry parameter needed as input for radiative transfer calculations of the downwelling direct normal and diffuse horizontal solar irradiance in clear-sky conditions. The Tropospheric Ultraviolet and Visible (TUV) radiative transfer model developed by Madronich and his colleagues at the US National Center for Atmospheric Research was used for the calculations of the spectral irradiance between 300–360 nm. Since there are few ultraviolet measurements of aerosol properties, most of the input aerosol data for the radiative transfer model are based on the assumption that UV input parameters can be extrapolated from the visible portion of the spectrum. Disagreements among available extraterrestrial spectra, which are discussed briefly, suggested that instead of comparing irradiances, measured and modeled spectral transmittances between 300–360 nm should be compared for the seven cases studied. Transmittance was calculated by taking the ratios of the measured irradiances to the Langley-derived, top-of-the-atmosphere irradiances. The cases studied included low to moderate aerosol loads and low to high solar-zenith angles. A procedure for retrieving single scattering albedo in the ultraviolet based on the comparisons of direct and diffuse transmittance is outlined.
Extinction efficiencies of coated absorbing aerosols measured by cavity ring down aerosol spectrometry
Authors: Abo Riziq A. , Trainic M. , Erlick C. , Segre E. , Rudich Y.
Published: April 2010

Abstract. In this study, we measure the extinction efficiency at 532 nm of absorbing aerosol particles coated with a non-absorbing solid and liquid organic shell with coating thickness varying between 5 and 100 nm using cavity ring down aerosol spectrometry. For this purpose, we use nigrosin, an organic black dye, as a model absorbing core and two non-absorbing organic substances as shells, glutaric acid (GA) and Di-Ethyl-Hexyl-Sebacate (DEHS). The measured behavior of the coated particles is consistent with Mie calculations of core-shell particles. Errors between measured and calculated values for nigrosin coated with GA and DEHS are between 0.5% and 10.5% and between 0.5% and 9%, respectively. However, it is evident that the calculations are in better agreement with the measured results for thinner coatings. Possible reasons for these discrepancies are discussed.
Investigating the sources and atmospheric processing of fine particles from Asia and the Northwestern United States measured during INTEX B
Authors: Peltier R. E. , Hecobian A. H. , Weber R. J. , Stohl A. , Atlas E. L. , Riemer D. D. , Blake D. R. , Apel E. , Campos T. , Karl T.
Published: April 2010

Abstract. During the National Aeronautics and Space Administration (NASA) Intercontinental Chemical Transport Experiment, Phase B (INTEX-B), in the spring of 2006, airborne measurements were made in the United States Pacific Northwest of the major inorganic ions and the water-soluble organic carbon (WSOC) of submicron (PM1.0) aerosol. An atmospheric trajectory (HYSPLIT) and a Lagrangian particle dispersion model (Flexpart) quantifying source contributions for carbon monoxide (CO) were used to segregate air masses into those of primarily Asian influence (>75% Asian CO) or North American influence (>75% North American CO). Of the measured compounds, fine particle mass mostly consisted of water-soluble organic carbon and sulfate, with median sulfate and WSOC concentrations in two to four times higher, respectively, in North American air masses versus transported Asian air masses. The fraction of WSOC to sulfate in transported Asian air masses was significantly lower than one at altitudes above 3 km due to depleted organic aerosol, opposite to what has been observed closer to Asia and in the northeastern United States, where organic components were at higher concentrations than sulfate in the free troposphere. The observations could be explained by loss of sulfate and organic aerosol by precipitation scavenging, with reformation of mainly sulfate during advection from Asia to North America. In contrast to free tropospheric measurements, for all air masses below approximately 2 km altitude median WSOC-sulfate ratios were consistently between one and two. WSOC sources were investigated by multivariate linear regression analyses of WSOC and volatile organic compounds (VOCs). In Asian air masses, of the WSOC variability that could be explained (49%), most was related to fossil fuel combustion VOCs, compared to North American air masses, where 75% of the WSOC variability was explained through a nearly equal combination of fossil fuel combustion and biogenic VOCs. Distinct WSOC plumes encountered during the experiment were also studied. A plume observed near the California Central Valley at 0.6 km altitude was related to both fossil fuel combustion and biogenic VOCs. Another Central Valley plume observed over Nevada at 3 to 5 km, in a region of cloud detrainment, was mostly related to biogenic VOCs.
Hygroscopic growth and activation of HULIS particles: experimental data and a new iterative parameterization scheme for complex aerosol particles
Authors: Ziese M. , Wex H. , Nilsson E. , Salma I. , Ocskay R. , Hennig T. , Massling A. , Stratmann F.
Published: April 2010

Abstract. The hygroscopic growth and activation of two HULIS (HUmic LIke Substance) and one Aerosol-Water-Extract sample, prepared from urban-type aerosol, were investigated. All samples were extracted from filters, redissolved in water and atomized for the investigations presented here. The hygroscopic growth measurements were done using LACIS (Leipzig Aerosol Cloud Interaction Simulator) together with a HH-TDMA (High Humidity Tandem Differential Mobility Analyzer). Hygroscopic growth was determined for relative humidities (RHs) up to 99.75%. The critical diameters for activation were measured for supersaturations between 0.2 and 1%. All three samples showed a similar hygroscopic growth behavior, and the two HULIS samples also were similar in their activation behavior, while the Aerosol-Water-Extract turned out to be more CCN active than the HULIS samples. The experimental data was used to derive parameterizations for the hygroscopic growth and activation of HULIS particles. The concept of ρion (Wex et al., 2007a) and the Szyszkowski-equation (Szyszkowski, 1908; Facchini, 1999) were used for parameterizing the Raoult and the Kelvin (surface tension) terms of the Köhler equation, respectively. This concept proved to be very successful for the HULIS samples in the saturation range from RHs larger than 98% up to activation. It was also shown to work well with data on HULIS taken from literature. Here, different atmospheric life-times and/or different sources for the different samples showed up in different coefficients for the parameterization. However, the parameterization did not work out well for the Aerosol-Water-Extract.
Comparison between early Odin-SMR, Aura MLS and CloudSat retrievals of cloud ice mass in the upper tropical troposphere
Authors: Eriksson P. , Ekström M. , Rydberg B. , Wu D. L. , Austin R. T. , Murtagh D. P.
Published: April 2010

Abstract. Emerging microwave satellite techniques are expected to provide improved global measurements of cloud ice mass. CloudSat, Aura MLS and Odin-SMR fall into this category and early cloud ice retrievals from these instruments are compared. The comparison follows the SMR retrieval product and is made for partial ice water columns above 12 km. None of the retrievals shows a significant degree of false cloud detections, the ratio between local mean values from the instruments is fairly constant and a consistent view of the geographical distribution of cloud ice is obtained. However, important differences on the absolute levels exist, where the overall mean is 9.6, 4.2 and 3.7 g m−2 for CloudSat, SMR and MLS, respectively. Assumptions about the particle size distribution (PSD) are a consideration for all three instruments and constitute the dominating retrieval uncertainty for CloudSat. The mean for CloudSat when applying the same PSD as for MLS and SMR was estimated to 6.3 g m−2. A second main consideration for MLS and SMR are the effects caused by the poorer spatial resolution: a possible vertical misplacement of retrieved values and an impact of cloud inhomogeneities. The latter effect was found to be the dominating retrieval uncertainty for SMR, giving a possible mean value range of 2.3–8.9 g m−2. The comparison indicates a common retrieval accuracy in the order of 70%. Already this number should suffice for improved validations of cloud ice parametrisation schemes in atmospheric models, but a substantially better consistency between the datasets should be attainable through an increased understanding of main retrieval error sources.
Space-borne measurements of mesospheric magnesium species – a retrieval algorithm and preliminary profiles
Authors: Scharringhausen M. , Aikin A. C. , Burrows J. P. , Sinnhuber M.
Published: April 2010

Abstract. We present a joint retrieval as well as first results for mesospheric air density and mesospheric Magnesium species (Mg and Mg+) using limb data from the SCIAMACHY instrument on board the European ENVISAT satellite.considered. These species feature Metallic species like neutral Mg, ionized Mg+ and others (Fe, Si, Li, etc.) ablate from meteoric dust, enter the gas phase and occur at high altitudes (≥70 km). Emissions from these species are clearly observed in the SCIAMACHY limb measurements. These emissions are used to retrieve total and thermospheric column densities as well as preliminary profiles of metallic species in the altitude range of 70–92 km. In this paper, neutral Magnesium as well as its ionized counterpart Mg+ is considered. These species feature resonance fluorescence in the wavelength range 279 and 285 nm and thus have a rather simple excitation process. A radiative transfer model (RTM) for the mesosphere has been developed and validated. Based on a ray tracing kernel, radiances in a large wavelength range from 240–300 nm covering limb as well as nadir geometry can be calculated. The forward model has been validated and shows good agreement with established models in the given wavelength range and a large altitude range. The RTM has been coupled to a retrieval based on Optimal Estimation. Air density is retrieved from Rayleigh backscattered light. Mesospheric Mg and Mg+ number densities are retrieved from their emission signals observed in the limb scans of SCIAMACHY. Other species like iron, silicon, OH and NO can be investigated in principle with the same algorithm. Based on the retrieval presented here, SCIAMACHY offers the opportunity to investigate mesospheric species on a global scale and with good vertical resolution for the first time.
Technical note: Analytical formulae for the critical supersaturations and droplet diameters of CCN containing insoluble material
Authors: Kokkola H. , Vesterinen M. , Anttila T. , Laaksonen A. , Lehtinen K. E. J.
Published: April 2010

Abstract. In this paper, we consider the cloud drop activation of aerosol particles consisting of water soluble material and an insoluble core. Based on the Köhler theory, we derive analytical equations for the critical diameters and supersaturations of such particles. We demonstrate the use of the equations by comparing the critical supersaturations of particles composed of ammonium sulfate and insoluble substances with those of model organic particles with varying molecular sizes.
Assessment of high (diurnal) to low (seasonal) frequency variations of isoprene emission rates using a neural network approach
Authors: Boissard C. , Chervier F. , Dutot A. L.
Published: April 2010

Abstract. Using a statistical approach based on artificial neural networks, an emission algorithm (ISO-LF) accounting for high to low frequency variations was developed for isoprene emission rates. ISO-LF was optimised using a data base (ISO-DB) specifically designed for this work, which consists of 1321 emission rates collected in the literature and 34 environmental variables, measured or assessed using National Climatic Data Center or National Centers for Environmental Predictions meteorological databases. ISO-DB covers a large variety of emitters (25 species) and environmental conditions (10° S to 60° N). When only instantaneous environmental regressors (instantaneous air temperature T0 and photosynthetic photon flux density L0) were used, a maximum of 60% of the overall isoprene variability was assessed with the highest emissions being strongly underestimated. ISO-LF includes a total of 9 high (instantaneous) to low (up to 3 weeks) frequency regressors and accounts for up to 91% of the isoprene emission variability, whatever the emission range, species or climate investigated. ISO-LF was found to be mainly sensitive to air temperature cumulated over 3 weeks (T21) and to L0 and T0 variations. T21, T0 and L0 only accounts for 76% of the overall variability.
Air pollution during the 2003 European heat wave as seen by MOZAIC airliners
Authors: Tressol M. , Ordonez C. , Zbinden R. , Brioude J. , Thouret V. , Mari C. , Nedelec P. , Cammas J.-P. , Smit H. , Patz H.-W. , Volz-Thomas A.
Published: April 2010

Abstract. This study presents an analysis of both MOZAIC profiles above Frankfurt and Lagrangian dispersion model simulations for the 2003 European heat wave. The comparison of MOZAIC measurements in summer 2003 with the 11-year MOZAIC climatology reflects strong temperature anomalies (exceeding 4°C) throughout the lower troposphere. Higher positive anomalies of temperature and negative anomalies of both wind speed and relative humidity are found for the period defined here as the heat wave (2–14 August 2003), compared to the periods before (16–31 July 2003) and after (16–31 August 2003) the heat wave. In addition, Lagrangian model simulations in backward mode indicate the suppressed long-range transport in the mid- to lower troposphere and the enhanced southern origin of air masses for all tropospheric levels during the heat wave. Ozone and carbon monoxide also present strong anomalies (both ~+40 ppbv) during the heat wave, with a maximum vertical extension reaching 6 km altitude around 11 August 2003. Pollution in the planetary boundary layer (PBL) is enhanced during the day, with ozone mixing ratios two times higher than climatological values. This is due to a combination of factors, such as high temperature and radiation, stagnation of air masses and weak dry deposition, which favour the accumulation of ozone precursors and the build-up of ozone. A negligible role of a stratospheric-origin ozone tracer has been found for the lower troposphere in this study. From 29 July to 15 August 2003 forest fires burnt around 0.3×106 ha in Portugal and added to atmospheric pollution in Europe. Layers with enhanced CO and NOy mixing ratios, advected from Portugal, were crossed by the MOZAIC aircraft in the free troposphere over Frankfurt. A series of forward and backward Lagrangian model simulations have been performed to investigate the origin of anomalies during the whole heat wave. European anthropogenic emissions present the strongest contribution to the measured CO levels in the lower troposphere (near 30%). This source is followed by Portuguese forest fires which affect the lower troposphere after 6 August 2003 and even the PBL around 10 August 2003. The averaged biomass burning contribution reaches 35% during the affected period. Anthropogenic CO of North American origin only marginally influences CO levels over Europe during that period.
Technical Note: Intercomparison of formaldehyde measurements at the atmosphere simulation chamber SAPHIR
Authors: Wisthaler A. , Apel E. C. , Bossmeyer J. , Hansel A. , Junkermann W. , Koppmann R. , Meier R. , Müller K. , Solomon S. J. , Steinbrecher R. , Tillmann R. , Brauers T.
Published: April 2010

Abstract. The atmosphere simulation chamber SAPHIR at the Research Centre Jülich was used to test the suitability of state-of-the-art analytical instruments for the measurement of gas-phase formaldehyde (HCHO) in air. Five analyzers based on four different sensing principles were deployed: a differential optical absorption spectrometer (DOAS), cartridges for 2,4-dinitrophenylhydrazine (DNPH) derivatization followed by off-line high pressure liquid chromatography (HPLC) analysis, two different types of commercially available wet chemical sensors based on Hantzsch fluorimetry, and a proton-transfer-reaction mass spectrometer (PTR-MS). A new optimized mode of operation was used for the PTR-MS instrument which significantly enhanced its performance for online HCHO detection at low absolute humidities. The instruments were challenged with typical ambient levels of HCHO ranging from zero to several ppb. Synthetic air of high purity and particulate-filtered ambient air were used as sample matrices in the atmosphere simulation chamber onto which HCHO was spiked under varying levels of humidity and ozone. Measurements were compared to mixing ratios calculated from the chamber volume and the known amount of HCHO injected into the chamber; measurements were also compared between the different instruments. The formal and blind intercomparison exercise was conducted under the control of an independent referee. A number of analytical problems associated with the experimental set-up and with individual instruments were identified, the overall agreement between the methods was fair.
Technical Note: Continuity of MIPAS-ENVISAT operational ozone data quality from full- to reduced-spectral-resolution operation mode
Authors: Ceccherini S. , Cortesi U. , Verronen P. T. , Kyrölä E.
Published: April 2010

Abstract. MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) is operating on the ENVIronmental SATellite (ENVISAT) since March 2002. After two years of nearly continuous limb scanning measurements, at the end of March 2004, the instrument was stopped due to problems with the mirror drive of the interferometer. Operations with reduced maximum path difference, corresponding to both a reduced-spectral-resolution and a shorter measurement time, were resumed on January 2005. In order to exploit the reduction in measurement time, the measurement scenario was changed adopting a finer vertical limb scanning. The change of spectral resolution and of measurement scenario entailed an update of the data processing strategy. The aim of this paper is the assessment of the differences in the quality of the MIPAS ozone data acquired before and after the stop of the operations. Two sets of MIPAS ozone profiles acquired in 2003–2004 (full-resolution measurements) and in 2005–2006 (reduced-resolution measurements) are compared with collocated ozone profiles obtained by GOMOS (Global Ozone Monitoring by Occultation of Stars), itself also onboard ENVISAT. The continuity of the GOMOS data quality allows to assess a possible discontinuity of the MIPAS performances. The relative bias and precision of MIPAS ozone profiles with respect to the GOMOS ones have been compared for the measurements acquired before and after the stop of the MIPAS operations. The results of the comparison show that, in general, the quality of the MIPAS ozone profiles retrieved from reduced-resolution measurements is comparable or better than that obtained from the full-resolution dataset. The only significant change in MIPAS performances is observed at pressures around 2 hPa, where the relative bias of the instruments increases by a factor of 2 from the 2003–2004 to 2005–2006 measurements.
The Comparative Reactivity Method – a new tool to measure total OH Reactivity in ambient air
Authors: Sinha V. , Williams J. , Crowley J. N. , Lelieveld J.
Published: April 2010

Abstract. Hydroxyl (OH) radicals play a vital role in maintaining the oxidizing capacity of the atmosphere. To understand variations in OH radicals both source and sink terms must be understood. Currently the overall sink term, or the total atmospheric reactivity to OH, is poorly constrained. Here, we present a new on-line method to directly measure the total OH reactivity (i.e.~total loss rate of OH radicals) in a sampled air mass. In this method, a reactive molecule (X), not normally present in air, is passed through a glass reactor and its concentration is monitored with a suitable detector. OH radicals are then introduced in the glass reactor at a constant rate to react with X, first in the presence of zero air and then in the presence of ambient air containing VOCs and other OH reactive species. Comparing the amount of X exiting the reactor with and without the ambient air allows the air reactivity to be determined. In our existing set up, X is pyrrole and the detector used is a proton transfer reaction mass spectrometer. The present dynamic range for ambient air reactivity is about 6 to 300 s−1, with an overall maximum uncertainty of 25% above 8 s−1 and up to 50% between 6–8 s−1. The system has been tested and calibrated with different single and mixed hydrocarbon standards showing excellent linearity and accountability with the reactivity of the standards. Potential interferences such as high NO in ambient air, varying relative humidity and photolysis of pyrrole within the setup have also been investigated. While interferences due changing humidity and photolysis of pyrrole are easily overcome by ensuring that humidity in the set up does not change drastically and the photolytic loss of pyrrole is measured and taken into account, respectively, NO>10 ppb in ambient air remains a significant interference for the current configuration of the instrument. Field tests in the tropical rainforest of Suriname (~53 s
The measurement of aerosol optical properties at a rural site in Northern China
Authors: Yan P. , Tang J. , Huang J. , Mao J. T. , Zhou X.J. , Liu Q. , Wang Z. F. , Zhou H. G.
Published: April 2010

Abstract. Atmospheric aerosols constitute one of the largest sources of uncertainty in the estimation of radiative forcing for climate. From April 2003 to January 2005, in situ measurements of aerosol optical properties were conducted at a rural site in Northern China, Shangdianzi Global Atmosphere Watch (GAW) regional station (SDZ), about 150 km from Beijing. Mean values (standard deviation, S.D.) of scattering and absorption coefficients for the entire period are 174.6 Mm−1 (189.1 Mm-1) and 17.5 Mm−1 (13.4 Mm-1), respectively. These values are approximately one third of the reported values for scattering coefficients and one fifth of those for absorption coefficients obtained in the Beijing urban area. The mean single scattering albedo (SSA) for the entire period was estimated as 0.88 (0.05), which is about 0.07 higher than the values reported for the Beijing urban area, and also higher than the values (0.85) used in a reported climate simulation for China and India. Both the absorption and scattering coefficients showed a seasonal cycle with the lowest values in winter, while the highest values occurred in summer for absorption coefficients and in fall for scattering coefficients. The mean SSA values were lowest in spring and highest in winter. The daily variations of aerosol absorption and scattering coefficients were strongly influenced by synoptic changes throughout the observation period. A trajectory cluster analysis was applied to discern the source characteristics of aerosol optical properties for different air masses. The cluster-mean aerosol scattering coefficients, absorption coefficients and SSA were all high when the air masses moved from SW and SE-E directions to the site and aerosols were influenced with heavy pollution from the dense population centers and industrial areas. The cluster-mean SSA for air masses coming from the polluted areas was not only higher than those with trajectories from the "clean" directions, but also higher than the reported values for the regions with high pollution emissions (such as the Beijing urban area). This fact might reflect the substantial secondary aerosol production during transport. The characteristics of aerosol optical properties measured at this rural site suggest significant impacts of human activities on the regional aerosol.
Properties of atmospheric humic-like substances – water system
Authors: Salma I. , Ocskay R. , Láng G. G.
Published: April 2010

Abstract. Urban-type PM2.5-fraction aerosol samples were collected and samples of pure atmospheric humic-like substances (HULIS) were isolated from them. Atmospheric concentrations of organic carbon (OC), water soluble organic carbon (WSOC) and HULIS were determined, and UV/Vis spectroscopic properties, solubility and conductivity of HULIS in aqueous samples were investigated. Atmospheric concentrations of OC and WSOC were 8.5 and 4.6 μg m−3, respectively. Hydrophilic WSOC accounted for 39% of WSOC, carbon in HULIS made up 47% of WSOC, and 14% of WSOC was retained on the separation column by irreversible adsorption. Overall average molecular mass and aromatic carbon abundance of HULIS were estimated from molar absorptivity to be 556 Da and 12%, respectively. Both results are substantially smaller than for standard reference fulvic acids, which imply different mechanisms for the formation processes of atmospheric HULIS and aquatic or terrestrial humic matter. HULIS were found to be water soluble as ionic unimers with a saturation concentration of 2–3 g l−1. Their solubility increased again with total HULIS concentration being above approximately 4 g l−1, which was most likely explained by the formation of HULIS aggregates. Solubility increased linearly from approximately 5 up to 20 g l−1 of dissolved HULIS concentration. The ionic dissolution was confirmed by electrochemical conductivity in the investigated concentration interval. Limiting molar conductivity was extrapolated and this was utilized to determine the apparent dissociation degree of HULIS for different concentrations. The dissociation degree was further applied to derive the concentration dependence of the van't Hoff factor of HULIS. The van't Hoff factor decreased monotonically with HULIS concentration; the decrease was substantial for dilute solutions and the relationship became weak for rather concentrated solutions.