bluuebunny/crossref_metadata_2025 huggingface dataset:
Assimilation of stratospheric and mesospheric temperatures from MLS and SABER into a global NWP model
Authors: Hoppel K. W. , Baker N. L. , Coy L. , Eckermann S. D. , McCormack J. P. , Nedoluha G. E. , Siskind D. E.
Published: April 2010

Abstract. The forecast model and three-dimensional variational data assimilation components of the Navy Operational Global Atmospheric Prediction System (NOGAPS) have each been extended into the upper stratosphere and mesosphere to form an Advanced Level Physics High Altitude (ALPHA) version of NOGAPS extending to ~100 km. This NOGAPS-ALPHA NWP prototype is used to assimilate stratospheric and mesospheric temperature data from the Microwave Limb Sounder (MLS) and the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) instruments. A 60-day analysis period in January and February 2006, was chosen that includes a well documented stratospheric sudden warming. SABER and MLS temperatures indicate that the SSW caused the polar winter stratopause at ~40 km to disappear, then reform at ~80 km altitude and slowly descend during February. The NOGAPS-ALPHA analysis reproduces this observed stratospheric and mesospheric temperature structure, as well as realistic evolution of zonal winds, residual velocities, and Eliassen-Palm fluxes that aid interpretation of the vertically deep circulation and eddy flux anomalies that developed in response to this wave-breaking event. The observation minus forecast (O-F) standard deviations for MLS and SABER are ~2 K in the mid-stratosphere and increase monotonically to about 6 K in the upper mesosphere. Increasing O-F standard deviations in the mesosphere are expected due to increasing instrument error and increasing geophysical variance at small spatial scales in the forecast model. In the mid/high latitude winter regions, 10-day forecast skill is improved throughout the upper stratosphere and mesosphere when the model is initialized using the high-altitude analysis based on assimilation of both SABER and MLS data.
Organic composition of carbonaceous aerosols in an aged prescribed fire plume
Authors: Yan B. , Zheng M. , Hu Y. T. , Lee S. , Kim H. K. , Russell A. G.
Published: April 2010

Abstract. Aged smoke from a prescribed fire (dominated by conifers) impacted Atlanta, GA on 28 February 2007 and dramatically increased hourly ambient concentrations of PM2.5 and organic carbon (OC) up to 140 and 72 μg m−3, respectively. It was estimated that over 1 million residents were exposed to the smoky air lasting from the late afternoon to midnight. To better understand the processes impacting the aging of fire plumes, a detailed chemical speciation of carbonaceous aerosols was conducted by gas chromatography/mass spectrometry (GC/MS) analysis. Ambient concentrations of many organic species (levoglucosan, resin acids, retene, n-alkanes and n-alkanoic acids) associated with wood burning emission were significantly elevated on the event day. Levoglucosan increased by a factor of 10, while hopanes, steranes, cholesterol and major polycyclic aromatic hydrocarbons (PAHs) did not show obvious increases. Strong odd over even carbon number predominance was found for n-alkanes versus even over odd predominance for n-alkanoic acids. Alteration of resin acids during transport from burning sites to monitors is suggested by the observations. Our study also suggests that large quantities of biogenic volatile organic compounds (VOCs) and semivolatile organic compounds (SVOCs) were released both as products of combustion and unburned vegetation heated by the fire. Higher leaf temperature can stimulate biogenic VOC and SVOC emissions, which enhanced formation of secondary organic aerosols (SOA) in the atmosphere. This is supported by elevated ambient concentrations of secondary organic tracers (dicarboxylic acids, 2-methyltetrols, pinonic acid and pinic acid). An approximate source profile was built for the aged fire plume to help better understand evolution of wood smoke emission and for use in source impact assessment.
Evaluation of 1,3,5 trimethylbenzene degradation in the detailed tropospheric chemistry mechanism, MCMv3.1, using environmental chamber data
Authors: Metzger A. , Dommen J. , Gaeggeler K. , Duplissy J. , Prevot A. S. H. , Kleffmann J. , Elshorbany Y. , Wisthaler A. , Baltensperger U.
Published: April 2010

Abstract. The degradation mechanism of 1,3,5-trimethyl- benzene (TMB) as implemented in the Master Chemical Mechanism version 3.1 (MCM) was evaluated using data from the environmental chamber at the Paul Scherrer Institute. The results show that the MCM provides a consistent description of the photo-oxidation of TMB/NOx mixtures for a range of conditions. In all cases the agreement between the measurement and the simulation decreases with decreasing VOC-NOx ratio and in addition with increasing precursor concentration. A significant underestimation of the decay rate of TMB and thus underestimation of reactivity in the system, consistent with results from previous appraisals of the MCM, was observed. Much higher nitrous acid (HONO) concentrations compared to simulations and expected from chamber characterization experiments were measured during these smog chamber experiments. A light induced NO2 to HONO conversion at the chamber walls is suggested to occur. This photo-enhanced NO2 to HONO conversion with subsequent HONO photolysis enhances the reactivity of the system. After the implementation of this reaction in the model it describes the decay of TMB properly. Nevertheless, the model still over-predicts ozone at a later stage of the experiment. This can be attributed to a too slow removal of NO2. It is also shown that this photo-enhanced HONO formation is not restricted to TMB photo-oxidation but also occurs in other chemical systems (e.g. α-pinene). However, the influence of HONO as a source of OH radicals is less important in these more reactive systems and therefore the importance of the HONO chemistry is less obvious.
Net effect of the QBO in a chemistry climate model
Authors: Punge H. J. , Giorgetta M. A.
Published: April 2010

Abstract. The quasi-biennial oscillation (QBO) of zonal wind is a prominent mode of variability in the tropical stratosphere. It affects not only the meridional circulation and temperature over a wide latitude range but also the transport and chemistry of trace gases such as ozone. Compared to a QBO less circulation, the long-term climatological means of these quantities are also different. These climatological net effects of the QBO can be studied in general circulation models that extend into the middle atmosphere and have a chemistry and transport component, so-called Chemistry Climate Models (CCMs). In this work we show that the CCM MAECHAM4-CHEM can reproduce the observed QBO variations in temperature and ozone mole fractions when nudged towards observed winds. In particular, it is shown that the QBO signal in transport of nitrogen oxides NOx plays an important role in reproducing the observed ozone QBO, which features a phase reversal slightly below the level of maximum of the ozone mole fraction in the tropics. We then compare two 20-year experiments with the MAECHAM4-CHEM model that differ by including or not including the QBO. The mean wind fields differ between the two model runs, especially during summer and fall seasons in both hemispheres. The differences in the wind field lead to differences in the meridional circulation, by the same mechanism that causes the QBO's secondary meridional circulation, and thereby affect mean temperatures and the mean transport of tracers. In the tropics, the net effect on ozone is mostly due to net differences in upwelling and, higher up, the associated temperature change. We show that a net surplus of up to 15% in NOx in the tropics above 10 hPa in the experiment that includes the QBO does not lead to significantly different volume mixing ratios of ozone. We also note a slight increase in the southern vortex strength as well as earlier vortex formation in northern winter. Polar temperatures differ accordingly. Differences in the strength of the Brewer-Dobson circulation and in further trace gas concentrations are analysed. Our findings underline the importance of a representation of the QBO in CCMs.
Observations of the mesospheric semi-annual oscillation (MSAO) in water vapour by Odin/SMR
Authors: Lossow S. , Urban J. , Gumbel J. , Eriksson P. , Murtagh D.
Published: April 2010

Abstract. Mesospheric water vapour measurements taken by the SMR instrument aboard the Odin satellite between 2002 and 2006 have been analysed with focus on the mesospheric semi-annual circulation in the tropical and subtropical region. This analysis provides the first complete picture of mesospheric SAO in water vapour, covering altitudes above 80 km where previous studies were limited. Our analysis shows a clear semi-annual variation in the water vapour distribution in the entire altitude range between 65 km and 100 km in the equatorial area. Maxima occur near the equinoxes below 75 km and around the solstices above 80 km. The phase reversal occurs in the small layer in-between, consistent with the downward propagation of the mesospheric SAO in the zonal wind in this altitude range. The SAO amplitude exhibits a double peak structure in the equatorial region, with maxima at about 75 km and 81 km. The observed amplitudes show higher values than an earlier analysis based on UARS/HALOE data. The upper peak amplitude remains relatively constant with latitude. The lower peak amplitude decreases towards higher latitudes, but recovers in the Southern Hemisphere subtropics. On the other hand, the annual variation is much more prominent in the Northern Hemisphere subtropics. Furthermore, higher volume mixing ratios during summer and lower values during winter are observed in the Northern Hemisphere subtropics, as compared to the corresponding latitude range in the Southern Hemisphere.
The effect of temperature and water on secondary organic aerosol formation from ozonolysis of limonene, Δ3-carene and α-pinene
Authors: Jonsson Å. M. , Hallquist M. , Ljungström E.
Published: April 2010

Abstract. The effect of reaction temperature and how water vapour influences the formation of secondary organic aerosol (SOA) in ozonolysis of limonene, Δ3-carene and α-pinene, both regarding number and mass of particles, has been investigated by using a laminar flow reactor (G-FROST). Experiments with cyclohexane and 2-butanol as OH scavengers were compared to experiments without any scavenger. The reactions were conducted in the temperature range between 298 and 243 K, and at relative humidities between <10 and 80%. Results showed that there is still a scavenger effect on number and mass concentrations at low temperatures between experiments with and without an addition of an OH scavenger. This shows that the OH chemistry is influencing the SOA formation also at these temperatures. The overall temperature dependence on SOA formation is not as strong as expected from partitioning theory. In some cases there is even a positive temperature dependence that must be related to changes in the chemical mechanism and/or reduced rates of secondary chemistry at low temperatures. The precursor's α-pinene and Δ3-carene exhibit a similar temperature dependence regarding both number and mass of particles formed, whereas limonene shows a different dependence. The water effect at low temperature could be explained by physical uptake and cluster stabilisation. At higher temperatures, only a physical explanation is not sufficient and the observations are in line with water changing the chemical mechanism or reaction rates. The data presented adds to the understanding of SOA contribution to new particle formation and atmospheric degradation mechanisms.
SO2 emissions from Popocatépetl volcano: emission rates and plume imaging using optical remote sensing techniques
Authors: Grutter M. , Basaldud R. , Rivera C. , Harig R. , Junkerman W. , Caetano E. , Delgado-Granados H.
Published: April 2010

Abstract. Sulfur dioxide emissions from the Popocatépetl volcano in central Mexico were measured during the MILAGRO field campaign in March 2006. A stationary scanning DOAS (Differential Optical Absorption Spectrometer) was used to monitor the SO2 emissions from the volcano and the results were compared with traverses done with a COSPEC from the ground and a DOAS instrument on board an ultra-light aircraft. Daytime evolutions as well as day-to-day variation of the SO2 emissions are reported. A value of 2.45±1.39 Gg/day of SO2 is reported from all the daily averages obtained during the month of March 2006, with large variation in maximum and minimum daily averages of 5.97 and 0.56 Gg/day, respectively. The large short-term fluctuations in the SO2 emissions obtained could be confirmed through 2-D visualizations of the SO2 plume measured with a scanning imaging infrared spectrometer. This instrument, based on the passive detection of thermal radiation from the volcanic gas and analysis with FTIR spectrometry, is used for the first time for plume visualization of a specific volcanic gas. A 48-h forward trajectory analysis indicates that the volcanic plume was predominantly directed towards the Puebla/Tlaxcala region (63%), followed by the Mexico City and Cuernavaca/Cuautla regions with 19 and 18% occurrences, respectively. 25% of the modeled trajectories going towards the Puebla region reached altitudes lower than 4000 m a.s.l. but all trajectories remained over this altitude for the other two regions.
Technical Note: Quantitative long-term measurements of VOC concentrations by PTR-MS – measurement, calibration, and volume mixing ratio calculation methods
Authors: Taipale R. , Ruuskanen T. M. , Rinne J. , Kajos M. K. , Hakola H. , Pohja T. , Kulmala M.
Published: April 2010

Abstract. Proton transfer reaction mass spectrometry (PTR-MS) is a technique for online measurements of atmospheric concentrations, or volume mixing ratios, of volatile organic compounds (VOCs). This paper gives a detailed description of our measurement, calibration, and volume mixing ratio calculation methods, which have been designed for long-term stand-alone field measurements by PTR-MS. The PTR-MS instrument has to be calibrated regularly with a gas standard to ensure the accuracy needed in atmospheric VOC measurements. We introduce a novel method for determining an instrument specific relative transmission curve using information obtained from a calibration. This curve enables consistent mixing ratio calculation for VOCs not present in a calibration gas standard. Our method proved to be practical, systematic, and sensitive enough to capture changes in the transmission over time. We also propose a new approach to considering the abundance of H3O+H2O ions in mixing ratio calculation. The approach takes into account the difference in the transmission efficiencies for H3O+ and H3O+H2O ions. To illustrate the functionality of our measurement, calibration, and calculation methods, we present a one-month period of ambient mixing ratio data measured in a boreal forest ecosystem at the SMEAR II station in southern Finland. During the measurement period 27 March–26 April 2007, the hourly averages of the mixing ratios were 0.051–0.57 ppbv for formaldehyde, 0.19–3.1 ppbv for methanol, 0.038–0.39 ppbv for benzene, and 0.020–1.3 ppbv for monoterpenes. The detection limits for the hourly averages were 0.020, 0.060, 0.0036, and 0.0092 ppbv, respectively.
Particle size distributions in the Eastern Mediterranean troposphere
Authors: Kalivitis N. , Birmili W. , Stock M. , Wehner B. , Massling A. , Wiedensohler A. , Gerasopoulos E. , Mihalopoulos N.
Published: April 2010

Abstract. Atmospheric particle size distributions were measured on Crete island, Greece in the Eastern Mediterranean during an intensive field campaign between 28 August and 20 October, 2005. Our instrumentation combined a differential mobility particle sizer (DMPS) and an aerodynamic particle sizer (APS) and measured number size distributions in the size range 0.018 μm–10 μm. Four time periods with distinct aerosol characteristics were discriminated, two corresponding to marine and polluted air masses, respectively. In marine air, the sub-μm size distributions showed two particle modes centered at 67 nm and 195 nm having total number concentrations between 900 and 2000 cm−3. In polluted air masses, the size distributions were mainly unimodal with a mode typically centered at 140 nm, with number concentrations varying between 1800 and 2900 cm−3. Super-μm particles showed number concentrations in the range from 0.01 to 2.5 cm−3 without any clear relation to air mass origin. A small number of short-lived particle nucleation events were recorded, where the calculated particle formation rates ranged between 1.1–1.7 cm−3 s−1. However, no particle nucleation and growth events comparable to those typical for the continental boundary layer were observed. Particles concentrations (Diameter <50 nm) were low compared to continental boundary layer conditions with an average concentration of 300 cm−3. The production of sulfuric acid and its subsequently condensation on preexisting particles was examined with the use of a simplistic box model. These calculations suggested that the day-time evolution of the Aitken particle population was governed mainly by coagulation and that particle formation was absent during most days.
Technical Note: Adapting a fixed-lag Kalman smoother to a geostatistical atmospheric inversion framework
Authors: Michalak A. M.
Published: April 2010

Abstract. Inverse modeling methods are now commonly used for estimating surface fluxes of carbon dioxide, using atmospheric mass fraction measurements combined with a numerical atmospheric transport model. The geostatistical approach to flux estimation takes advantage of the spatial and/or temporal correlation in fluxes and does not require prior flux estimates. In this work, a previously-developed, computationally-efficient, fixed-lag Kalman smoother is adapted for application with a geostatistical approach to atmospheric inversions. This method makes it feasible to perform multi-year geostatistical inversions, at fine resolutions, and with large amounts of data. The new method is applied to the recovery of global gridscale carbon dioxide fluxes for 1997 to 2001 using pseudodata representative of a subset of the NOAA-ESRL Cooperative Air Sampling Network.
Global simulations of aerosol processing in clouds
Authors: Hoose C. , Lohmann U. , Bennartz R. , Croft B. , Lesins G.
Published: April 2010

Abstract. An explicit and detailed representation of in-droplet and in-crystal aerosol particles in stratiform clouds has been introduced in the global aerosol-climate model ECHAM5-HAM. The new scheme allows an evaluation of the cloud cycling of aerosols and an estimation of the relative contributions of nucleation and collision scavenging, as opposed to evaporation of hydrometeors in the global aerosol processing by clouds. On average an aerosol particle is cycled through stratiform clouds 0.5 times. The new scheme leads to important changes in the simulated fraction of aerosol scavenged in clouds, and consequently in the aerosol wet deposition. In general, less aerosol is scavenged into clouds with the new prognostic treatment than what is prescribed in standard ECHAM5-HAM. Aerosol concentrations, size distributions, scavenged fractions and cloud droplet concentrations are evaluated and compared to different observations. While the scavenged fraction and the aerosol number concentrations in the marine boundary layer are well represented in the new model, aerosol optical thickness, cloud droplet number concentrations in the marine boundary layer and the aerosol volume in the accumulation and coarse modes over the oceans are overestimated. Sensitivity studies suggest that a better representation of below-cloud scavenging, higher in-cloud collision coefficients, or a reduced water uptake by seasalt aerosols could reduce these biases.
Comparison of cloud statistics from spaceborne lidar systems
Authors: Berthier S. , Chazette P. , Pelon J. , Baum B.
Published: April 2010

Abstract. The distribution of clouds in a vertical column is assessed on the global scale through analysis of lidar measurements obtained from three spaceborne lidar systems: LITE (Lidar In-space Technology Experiment, NASA), GLAS (Geoscience Laser Altimeter System, NASA), and CALIOP (Cloud-Aerosol LIdar with Orthogonal Polarization). Cloud top height (CTH) is obtained from the LITE profiles based on a simple algorithm that accounts for multilayer cloud structures. The resulting CTH results are compared to those obtained by the operational algorithms of the GLAS and CALIOP instruments. Based on our method, spaceborne lidar data are analyzed to establish statistics on the cloud top height. The resulting columnar results are used to investigate the inter-annual variability in the lidar cloud top heights. Statistical analyses are performed for a range of CTH (high, middle, low) and latitudes (polar, middle latitude and tropical). Probability density functions of CTH are developed. Comparisons of CTH developed from LITE, for 2 weeks of data in 1994, with ISCCP (International Satellite Cloud Climatology Project) cloud products show that the cloud fraction observed from spaceborne lidar is much higher than that from ISCCP. Another key result is that ISCCP products tend to underestimate the CTH of optically thin cirrus clouds. Significant differences are observed between LITE-derived cirrus CTH and both GLAS and CALIOP-derived cirrus CTH. Such a difference is due primarily to the lidar signal-to-noise ratio that is approximately a factor of 3 larger for the LITE system than for the other lidars. A statistical analysis for a full year of data highlights the influence of both the Inter-Tropical Convergence Zone and polar stratospheric clouds.
1-D Air-snowpack modeling of atmospheric nitrous acid at South Pole during ANTCI 2003
Authors: Liao W. , Tan D.
Published: April 2010

Abstract. A 1-D air-snowpack model of HONO has been developed and constrained by observed chemistry and meteorology data. The 1-D model includes molecular diffusion and mechanical dispersion, windpumping in snow, gas phase to quasi-liquid layer phase HONO transfer and quasi-liquid layer nitrate and interstitial air HONO photolysis. Photolysis of nitrate is important as a dominant HONO source inside the snowpack, however, the observed HONO emission from the snowpack was triggered mainly by the equilibrium between quasi liquid layer nitrite and firn air HONO deep down the snow surface (i.e. 30 cm below snow surface). The high concentration of HONO in the firn air is subsequently transported above the snowpack by diffusion and windpumping. The model uncertainties come mainly from lack of measurements and the interpretation of the QLL properties based on the bulk snow measurements. One critical factor is the ionic strength of QLL nitrite, which is estimated here by the bulk snow pH, nitrite concentration, and QLL to bulk snow volume ratio.
Simulation of aerosol optical properties over Europe with a 3-D size-resolved aerosol model: comparisons with AERONET data
Authors: Tombette M. , Chazette P. , Sportisse B. , Roustan Y.
Published: April 2010

Abstract. This paper aims at presenting a model-to-data comparison of the Aerosol Optical Thickness (AOT) and of a few sparse data for Single Scattering Albedo (SSA) over Europe for one year. The main contribution of this paper is the sensitivity study to a large number of parameters, including physical and numerical parameters of the aerosol model itself. The optical parameters are computed from a size-resolved aerosol model embedded in the Polyphemus system. The methodology is first described, showing that several hypothesis can be made for micro-physical aerosol properties. The simulation is made over one year (2001); statistics and monthly time series for the simulation and AERONET data are used to evaluate the ability of the model to reproduce AOT and vertically averaged SSA fields and their variability. The relation with the uncertainties of measurements is discussed. Then a sensitivity study with respect to the mixing state of the particle, the way to take into account water uptake, numerical parameters and physical parameterizations of the model is carried out. The results indicate that the mixing state of particles has an influence on optical parameters, as well as the computation of the wet diameter. But some physical and numerical parameters associated with the aerosol model itself have even more influence under certain conditions, through the uncertainties on the aerosol chemical composition, and their size distribution.
Measurements of size-resolved hygroscopicity in the California coastal zone
Authors: Hegg D. A. , Covert D. S. , Jonsson H. H.
Published: April 2010

Abstract. Aircraft-based measurements of aerosol hygroscopicity, both in the form of size-resolved, diameter growth factors and in the dependence of particle light scattering on relative humidity, are presented for the marine boundary layer of the southern California coastal zone. The chemical composition of the aerosol is collated with the hygroscopicity data, both to examine the mechanism for the increase in aerosol hygroscopicity with altitude and as input for receptor type modeling. The data suggest an increase in aerosol hygroscopicity with altitude, possibly associated with oxidation of organic films. The receptor modeling suggests three distinct aerosol types/sources for this venue: marine, biomass burning and pollution. Model output is used in regression analyses to derive a prognostic mixing rule for the hygroscopicity of aerosol with these three sources. The mixing rule demonstrated substantial prognostic power for submicron hygroscopicity but essentially none for supermicron.
Investigation of the hygroscopic properties of Ca(NO3)2 and internally mixed Ca(NO3)2/CaCO3 particles by micro-Raman spectrometry
Authors: Liu Y. J. , Zhu T. , Zhao D. F. , Zhang Z. F.
Published: April 2010

Abstract. To understand and predict the role of mineral aerosol particles processed by reactive nitrogen species in the atmosphere, the hygroscopic properties of both Ca(NO3)2 and Ca(NO3)2-containing mineral particles must be well understood. Using a micro-Raman system, the hygroscopic behaviors of micro-sized individual Ca(NO3)2 and internally mixed Ca(NO3)2/CaCO3 particles in both dehumidifying and humidifying processes were investigated systematically. In addition to accurate quantification of the dependence of water content on relative humidity (RH), significant new spectroscopic evidence related to chemical structure was also obtained to confirm the occurrence of amorphous solid state and to better understand the phase transition process. The Ca(NO3)2 particles exhibit reversible behavior in the dehumidifying and humidifying processes; they are in the state of solution droplets above 10% RH and amorphous hydrates below 7% RH, and phase transition occurs at 7–10% RH. The hygroscopic behavior of Ca(NO3)2/CaCO3 particles is identical to that of pure Ca(NO3)2 particles, suggesting a negligible effect of the slightly soluble CaCO3 inclusion on the hygroscopic behavior of a(NO3)2/CaCO3 particles.
SO2 oxidation products other than H2SO4 as a trigger of new particle formation. Part 2: Comparison of ambient and laboratory measurements, and atmospheric implications
Authors: Laaksonen A. , Kulmala M. , Berndt T. , Stratmann F. , Mikkonen S. , Ruuskanen A. , Lehtinen K. E. J. , Dal Maso M. , Aalto P. , Petäjä T. , Riipinen I. , Sihto S.-L. , Janson R. , Arnold F. , Hanke M. , Ücker J. , Umann B. , Sellegri K. , O'Dowd C. D. , Viisanen Y.
Published: April 2010

Abstract. Atmospheric new particle formation is generally thought to occur due to homogeneous or ion-induced nucleation of sulphuric acid. We compare ambient nucleation rates with laboratory data from nucleation experiments involving either sulphuric acid or oxidized SO2. Atmospheric nucleation occurs at H2SO4 concentrations 2–4 orders of magnitude lower than binary or ternary nucleation rates of H2SO4 produced from a liquid reservoir, and atmospheric H2SO4 concentrations are very well replicated in the SO2 oxidation experiments. We hypothesize these features to be due to the formation of free HSO5 radicals in pace with H2SO4 during the SO2 oxidation. We suggest that at temperatures above ~250 K these radicals produce nuclei of new aerosols much more efficiently than H2SO4. These nuclei are activated to further growth by H2SO4 and possibly other trace species. However, at lower temperatures the atmospheric relative acidity is high enough for the H2SO4–H2O nucleation to dominate.
Continuous monitoring of the boundary-layer top with lidar
Authors: Baars H. , Ansmann A. , Engelmann R. , Althausen D.
Published: April 2010

Abstract. Continuous lidar observations of the top height of the boundary layer (BL top) have been performed at Leipzig (51.3° N, 12.4° E), Germany, since August 2005. The results of measurements taken with a compact, automated Raman lidar over a one–year period (February 2006 to January 2007) are presented. Main goals of the study are (a) to demonstrate that BL top monitoring with lidar throughout the year is possible, (b) to present the required data analysis method that permits an automated, robust retrieval of BL top at all weather situations, and (c) to use this opportunity to compare the lidar-derived BL top data with respective BL tops hourly predicted by the regional weather forecast model COSMO. Four different lidar methods for the determination of the BL top are discussed. The wavelet covariance algorithm is modified so that an automated retrieval of BL depths from lidar data is possible. Three case studies of simultaneous observations with the Raman lidar, a vertical-wind Doppler lidar, and accompanying radiosonde profiling of temperature and humidity are presented to compare the potential and the limits of the four lidar techniques. The statistical analysis of the one-year data set reveals that the seasonal mean of the daytime (about 08:00–20:00 Local Time, LT) maximum BL top is 1400 m in spring, 1800 m in summer, 1200 m in autumn, and 800 m in winter at the continental, central European site. BL top typically increases by 100–300 m per hour in the morning of convective days. The comparison between the lidar-derived BL top heights and the predictions of COSMO yields a general underestimation of the BL top by about 20% by the model.
Capturing vertical profiles of aerosols and black carbon over the Indian Ocean using autonomous unmanned aerial vehicles
Authors: Corrigan C. E. , Roberts G. C. , Ramana M. V. , Kim D. , Ramanathan V.
Published: April 2010

Abstract. Measurements of the vertical distribution of aerosol properties provide essential information for generating more accurate model estimates of radiative forcing and atmospheric heating rates compared with employing remotely sensed column averaged properties. A month long campaign over the Indian Ocean during March 2006 investigated the interaction of aerosol, clouds, and radiative effects. Routine vertical profiles of aerosol and water vapor were determined using autonomous unmanned aerial vehicles equipped with miniaturized instruments. Comparisons of these airborne instruments with established ground-based instruments and in aircraft-to-aircraft comparisons demonstrated an agreement within 10%. Aerosol absorption optical depths measured directly using the unmanned aircraft differed from columnar AERONET sun-photometer results by only 20%. Measurements of total particle concentration, particle size distributions, aerosol absorption and black carbon concentrations are presented along with the trade wind thermodynamic structure from the surface to 3000 m above sea level. Early March revealed a well-mixed layer up to the cloud base at 500 m above mean sea level (m a.s.l.), followed by a decrease of aerosol concentrations with altitude. The second half of March saw the arrival of a high altitude plume existing above the mixed layer that originated from a continental source and increased aerosol concentrations by more than tenfold, yet the surface air mass showed little change in aerosol concentrations and was still predominantly influenced by marine sources. Black carbon concentrations at 1500 m above sea level increased from 70 ng/m3 to more than 800 ng/m3 with the arrival of this polluted plume. The absorption aerosol optical depth increased from as low as 0.005 to as much as 0.035 over the same period. The spectral dependence of the aerosol absorption revealed an absorption Angstrom exponent of 1.0, which is typical of an aerosol with most of its absorption attributed to black carbon and generally indicates the absorbing component originated from fossil fuel sources and other high-temperature combustion sources. The results indicate that surface measurements do not represent the aerosol properties within the elevated layers, especially if these layers are influenced by long range transport.
Cosmic rays, cloud condensation nuclei and clouds – a reassessment using MODIS data
Authors: Kristjánsson J. E. , Stjern C. W. , Stordal F. , Fjæraa A. M. , Myhre G. , Jónasson K.
Published: April 2010

Abstract. The response of clouds to sudden decreases in the flux of galactic cosmic rays (GCR) – Forbush decrease events – has been investigated using cloud products from the space-borne MODIS instrument, which has been in operation since 2000. By focusing on pristine Southern Hemisphere ocean regions we examine areas where we believe that a cosmic ray signal should be easier to detect than elsewhere. While previous studies have mainly considered cloud cover, the high spatial and spectral resolution of MODIS allows for a more thorough study of microphysical parameters such as cloud droplet size, cloud water content and cloud optical depth, in addition to cloud cover. Averaging the results from the 22 Forbush decrease events that were considered, no statistically significant correlations were found between any of the four cloud parameters and GCR, when autocorrelations were taken into account. Splitting the area of study into six domains, all of them have a negative correlation between GCR and cloud droplet size, in agreement with a cosmic ray – cloud coupling, but in only one of the domains (eastern Atlantic Ocean) was the correlation statistically significant. Conversely, cloud optical depth is mostly negatively correlated with GCR, and in the eastern Atlantic Ocean domain that correlation is statistically significant. For cloud cover and liquid water path, the correlations with GCR are weaker, with large variations between the different domains. When only the six Forbush decrease events with the largest amplitude (more than 10% decrease) were studied, the correlations fit the hypothesis slightly better, with 16 out of 24 correlations having the expected sign, although many of the correlations are quite weak. Introducing a time lag of a few days for clouds to respond to the cosmic ray signal the correlations tend to become weaker and even to change sign.
The role of ice in N2O5 heterogeneous hydrolysis at high latitudes
Authors: Apodaca R. L. , Huff D. M. , Simpson W. R.
Published: April 2010

Abstract. We report evidence for ice catalyzing N2O5 heterogeneous hydrolysis from a study conducted near Fairbanks, Alaska in November 2007. Mixing ratios of N2O5, NO, NO2, and ozone are reported and are used to determine steady state N2O5 lifetimes. When air masses are sub-saturated with respect to ice, the data show longer lifetimes (≈20 min) and elevated N2O5 levels, while ice-saturated air masses show shorter lifetimes (≈6 min) and suppressed N2O5 levels. We also report estimates of aerosol surface area densities that are on the order of 50 μm2/cm3, a surface area density that is insufficient to explain the rapid losses of N2O5 observed in this study, reinforcing the importance of other reactive surfaces such as ice. Consideration of two possible responsible types of ice surfaces, the snowpack and suspended ice particles, indicates that both are reasonable as possible sinks for N2O5. Because ice-saturated conditions are ubiquitous in high latitudes, ice surfaces are likely to be a key loss of N2O5, leading to nitric acid production and loss of NOx in high latitude plumes.
Seasonal variation of nocturnal temperatures between 1 and 105 km altitude at 54° N observed by lidar
Authors: Gerding M. , Höffner J. , Lautenbach J. , Rauthe M. , Lübken F.-J.
Published: April 2010

Abstract. Temperature soundings are performed by lidar at the mid-latitude station of Kühlungsborn (Germany, 54° N, 12° E). The profiles cover the complete range from the lower troposphere (~1 km) to the lower thermosphere (~105 km) by simultaneous and co-located operation of a Rayleigh-Mie-Raman lidar and a potassium resonance lidar. Observations have been done during 266 nights between June 2002 and July 2007, each of 3–15 h length. This large and unique data set provides comprehensive information on the altitudinal and seasonal variation of temperatures from the troposphere to the lower thermosphere. The remaining day-to-day-variability is strongly reduced by harmonic fits at constant altitude levels and a representative data set is achieved. This data set reveals a two-level mesopause structure with an altitude of about 86–87 km (~144 K) in summer and ~102 km (~170 K) during the rest of the year. The average stratopause altitude is ~48 km throughout the whole year, with temperatures varying between 258 and 276 K. From the fit parameters amplitudes and phases of annual, semi-annual, and quarter-annual variations are derived. The amplitude of the annual component is largest with amplitudes of up to 30 K in 85 km, while the quarter-annual variation is smallest and less than 3 K at all altitudes. The lidar data set is compared with ECMWF temperatures below about 70 km altitude and reference data from the NRLMSISE-00 model above. Apart from the temperature soundings the aerosol backscatter ratio is measured between 20 and 35 km. The seasonal variation of these values is presented here for the first time.
Cloud phase identification of Arctic boundary-layer clouds from airborne spectral reflection measurements: test of three approaches
Authors: Ehrlich A. , Bierwirth E. , Wendisch M. , Gayet J.-F. , Mioche G. , Lampert A. , Heintzenberg J.
Published: April 2010

Abstract. Arctic boundary-layer clouds were investigated with remote sensing and in situ instruments during the Arctic Study of Tropospheric Aerosol, Clouds and Radiation (ASTAR) campaign in March and April 2007. The clouds formed in a cold air outbreak over the open Greenland Sea. Beside the predominant mixed-phase clouds pure liquid water and ice clouds were observed. Utilizing measurements of solar radiation reflected by the clouds three methods to retrieve the thermodynamic phase of the cloud are introduced and compared. Two ice indices IS and IP were obtained by analyzing the spectral pattern of the cloud top reflectance in the near infrared (1500–1800 nm wavelength) spectral range which is characterized by ice and water absorption. While IS analyzes the spectral slope of the reflectance in this wavelength range, IS utilizes a principle component analysis (PCA) of the spectral reflectance. A third ice index IA is based on the different side scattering of spherical liquid water particles and nonspherical ice crystals which was recorded in simultaneous measurements of spectral cloud albedo and reflectance. Radiative transfer simulations show that IS, IP and IA range between 5 to 80, 0 to 8 and 1 to 1.25 respectively with lowest values indicating pure liquid water clouds and highest values pure ice clouds. The spectral slope ice index IS and the PCA ice index IP are found to be strongly sensitive to the effective diameter of the ice crystals present in the cloud. Therefore, the identification of mixed-phase clouds requires a priori knowledge of the ice crystal dimension. The reflectance-albedo ice index IA is mainly dominated by the uppermost cloud layer (τ<1.5). Therefore, typical boundary-layer mixed-phase clouds with a liquid cloud top layer will be identified as pure liquid water clouds. All three methods were applied to measurements above a cloud field observed during ASTAR 2007. The comparison with independent in situ microphysical measurements shows the ability of the three approaches to identify the ice phase in Arctic boundary-layer clouds.
Polar organic tracers in PM2.5 aerosols from forests in eastern China
Authors: Wang W. , Wu M. H. , Li L. , Zhang T. , Liu X. D. , Feng J. L. , Li H. J. , Wang Y. J. , Sheng G. Y. , Claeys M. , Fu J. M.
Published: April 2010

Abstract. Photooxidation products of biogenic volatile organic compounds, mainly isoprene and monoterpenes, are significant sources of atmospheric particulate matter in forested regions. The objectives of this study were to examine time series and diel variations of polar organic tracers for the photooxidation of isoprene and α-pinene to investigate whether they are linked with meteorological parameters or trace gases, and to determine their carbon contributions. In addition, the biogenic secondary organic carbon contributions from isoprene were estimated. PM2.5 (particulate matter with an aerodynamic diameter <2.5 μm) aerosol samples were collected from forests in eastern China and compared with data from forested sites in Europe and America. Aerosol sampling was conducted at four sites located along a gradient of ecological succession in four different regions, i.e. Changbai Mountain Nature Reserve (boreal-temperate), Chongming National Forest Park (temperate), Dinghu Mountain Nature Reserve (subtropical) and Jianfengling Nature Reserve in Hainan (tropical) during summer periods when the meteorological conditions are believed to be favorable for photochemical processes. Fifty PM2.5 samples were collected; eighteen organic compounds, organic carbon (OC), elemental carbon and trace gases were measured. Results indicate that the concentration trends of the secondary organic compounds reflected those of the trace gases and meteorological parameters. Very good correlations between the sum concentrations of isoprene oxidation products and atmospheric SO2, O3, NO2, NOx, as well as CO2, at the Changbai site were found. The secondary OC due to isoprene was relatively high in tropical Hainan (0.27 μgC/m3) where isoprene-emitting broadleaf species are dominant, but was comparable in boreal Changbai (0.32 μgC/m3) where coniferous species are prevalent. The contribution of malic acid, which may have both biogenic and anthropogenic sources, to the OC mass was comparable at the four sites.
Chemical isolation in the Asian monsoon anticyclone observed in Atmospheric Chemistry Experiment (ACE-FTS) data
Authors: Park M. , Randel W. J. , Emmons L. K. , Bernath P. F. , Walker K. A. , Boone C. D.
Published: April 2010

Abstract. Evidence of chemical isolation in the Asian monsoon anticyclone is presented using chemical constituents obtained from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer instrument during summer (June–August) of 2004–2006. Carbon monoxide (CO) shows a broad maximum over the monsoon anticyclone region in the upper troposphere and lower stratosphere (UTLS); these enhanced CO values are associated with air pollution transported upward by convection, and confined by the strong anticyclonic circulation. Profiles inside the anticyclone show enhancement of tropospheric tracers CO, HCN, C2H6, and C2H2 between ~12 to 20 km, with maxima near 13–15 km. Strong correlations are observed among constituents, consistent with sources from near-surface pollution and biomass burning. Stratospheric tracers (O3, HNO3 and HCl) exhibit decreased values inside the anticyclone between ~12–20 km. These observations are further evidence of transport of lower tropospheric air into the UTLS region, and isolation of air within the anticyclone. The relative enhancements of tropospheric species inside the anticyclone are closely related to the photochemical lifetime of the species, with strongest enhancement for shorter lived species. Vertical profiles of the ratio of C2H2/CO (used to measure the relative age of air) suggest relatively rapid transport of fresh emissions up to the tropopause level inside the anticyclone.
Aircraft and ground-based measurements of hydroperoxides during the 2006 MILAGRO field campaign
Authors: Nunnermacker L. J. , Weinstein-Lloyd J. B. , Hillery B. , Giebel B. , Kleinman L. I. , Springston S. R. , Daum P. H. , Gaffney J. , Marley N. , Huey G.
Published: April 2010

Abstract. Mixing ratios of hydrogen peroxide and hydroxymethyl hydroperoxide were determined aboard the US Department of Energy G-1 Research Aircraft during the March, 2006 MILAGRO field campaign in Mexico. Ground measurements of total hydroperoxide were made at Tecámac University, about 35 km NW of Mexico City. In the air and on the ground, peroxide mixing ratios near the source region were generally near 1 ppbv. Strong southerly flow resulted in transport of pollutants from Mexico City to two downwind surface sites on several flight days. On these days, it was observed that peroxide concentrations slightly decreased as the G-1 flew progressively downwind. This observation is consistent with low or negative net peroxide production rates calculated for the source region and is due to the very high NOx concentrations in the Mexico City plateau. However, relatively high values of peroxide were observed at takeoff and landing near Veracruz, a site with much higher humidity and lower NOx concentrations.
Improvements of synergetic aerosol retrieval for 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 a 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 for accurate cloud screening, and subsequently to quantify the aerosol optical depth (AOD) at 550 nm and spectral surface brightness through a dark field technique for different pre-defined aerosol mixtures. In the second step the spectrometer is applied to choose the most plausible aerosol mixture through a least square fit of the measured spectrum with simulated spectra using the mixture-dependent values of 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. Due to instrumental limitations the coverage of SYNAER/ERS-2 is very sparse. Therefore, SYNAER was transferred to similar sensors AATSR and SCIAMACHY onboard ENVISAT. While transferring to the new sensor pair significant improvements in the methodology were made based on a thorough evaluation of the methodology: (1) an update of the aerosol model, (2) improved cloud detection in the tropics and sub tropics, and (3) an enhanced dark field albedo characterization. This paper describes these improvements in detail and assesses their combined impact on the results. After a brief assessment of atmospheric noise impact on comparisons of pixel and station measurements a validation against ground-based measurements establishes error bars for the SYNAER/ENVISAT method version 2.0. A theoretical analysis of the information content with regard to aerosol composition (second retrieval step) is presented to quantify the potential and limitations of this new capability provided by the SYNAER method. Building on this analysis, first seasonal and monthly composition results calculated by applying SYNAER version 2.0 to AATSR and SCIAMACHY are shown to demonstrate the potential of the approach. An inter-comparison to earlier results of SYNAER version 1.0 is made for both the validation and the example datasets.