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We present regional model simulations of the dust emission events during the Bodélé Dust Experiment (BoDEx) that was carried out in February and March 2005 in Chad. A box model version of the dust emission model is used to test different input parameters for the emission model, and to compare the dust emissions computed with observed wind speeds to those calculated with wind speeds from the regional model simulation. While field observations indicate that dust production occurs via self-abrasion of saltating diatomite flakes in the Bodélé, the emission model based on the assumption of dust production by saltation and using observed surface wind speeds as input parameters reproduces observed dust optical thicknesses well. Although the peak wind speeds in the regional model underestimate the highest wind speeds occurring on 10–12 March 2005, the spatio-temporal evolution of the dust cloud can be reasonably well reproduced by this model. Dust aerosol interacts with solar and thermal radiation in the regional model; it is responsible for a decrease in maximum daytime temperatures by about 5 K at the beginning the dust storm on 10 March 2005. This direct radiative effect of dust aerosol accounts for about half of the measured temperature decrease compared to conditions on 8 March. Results from a global dust model suggest that the dust from the Bodélé is an important contributor to dust crossing the African Savannah region towards the Gulf of Guinea and the equatorial Atlantic, where it can contribute up to 40% to the dust optical thickness.
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After briefly discussing several reasons for the energy balance closure problem in the surface layer, the paper focuses on the influence of the low frequency part of the turbulence spectrum on the residual. Changes in the turbulent fluxes in this part of the turbulence spectrum were found to have a significant influence on the changes of the residual. Using the ogive method, it was found that the eddy-covariance method underestimates turbulent fluxes in the case of ogives converging for measuring times longer than the typical averaging interval of 30 min. Additionally, the eddy-covariance method underestimates turbulent fluxes for maximal ogive functions within the averaging interval, both mainly due to advection and non-steady state conditions. This has a considerable influence on the use of the eddy-covariance method.
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During Spring 2003, field experiments were conducted at the summit of Puy de Dôme (1465 m a.s.l.), in Central France, mainly in the free troposphere and during cloudy conditions. During this experiment, cloud condensation nuclei (CCN) concentrations were measured with a thermal gradient CCN counter at applied supersaturations that ranged between 0.2 and 2%. Aerosol size distributions were obtained with a TSI scanning mobility particle sizer (SMPS) consisting of a DMA and a CPC, and aerosol number (CN) concentrations were derived by integrating the SMPS size spectra between 0.015 and 0.3 µm. The isentropic back trajectories were computed for the altitude of the observation site using the Hybrid Single Particle Lagrangian Integrated Trajectory (HY-SPLIT) code from NOAA. For each air mass type, the aerosol bulk chemical composition used was that previously determined from cascade impactor samples by Sellegri et al. (2003). The methodological approach of this study was, firstly, to determine the relationships between CN and CCN concentrations for various air mass types arriving on the observation site. According to their origin, air masses arriving on the observation site are classified into 4 types: continental, clean marine, modified marine and polar. The CN concentrations appear to clearly depend on the type of air mass with the highest concentrations for the continental event and the lowest ones for the marine events. Moreover, a typical range can be attributed for the CCN/CN ratio to each air mass type. Then, the objective was to observe the hygroscopic behavior of aerosol particles upon heating of the sample in a thermo-desorber. Since the heated sample can be considered as representative of the original state of the aerosol, it appears that the evolution of CN to CCN is much more affected when the air mass is modified by aging and mixing processes with the contact of various atmospheric species all along the transport pathway. This result shows indirectly but clearly the presence of an active chemical layer containing more hygroscopic properties on the aerosol particle surface that can favour the particle growth. However, the role played by organic species is not clear and more work is needed to know if organic compounds may act to increase the CCN concentration.
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A new facility has been developed to investigate the formation of new particles from the oxidation of volatile organic compounds emitted from vegetation. The facility consists of a biogenic emissions enclosure, an aerosol growth chamber, and the associated instrumentation. Using the facility, new particle formation events have been induced through the reaction of ozone with three different precursor gas mixtures: an α-pinene test mixture and the emissions of a Holm oak (<i>Quercus ilex</i>) specimen and a loblolly pine (<i>Pinus taeda</i>) specimen. The results demonstrate the variability between species in their potential to form new aerosol products. The emissions of <i>Q. ilex</i> specimen resulted in fewer particles than did α-pinene, although the concentration of monoterpenes was roughly equal in both experiments before the addition of ozone. Conversely, the oxidation of <i>P. taeda</i> specimen emissions led to the formation of more particles than either of the other two gas mixtures, despite a lower initial terpenoid concentration. These variations can be attributed to differences in the speciation of the vegetative emissions with respect to the α-pinene mixture and to each other. Specifically, the presence of β-pinene and other slower-reacting monoterpenes probably inhibited particle formation in the <i>Q. ilex</i> experiment, while the presence of sesquiterpenes, including β-caryophyllene, in the emissions of the <i>P. taeda</i> specimen were the likely cause of the more intense particle formation events observed during that experiment.
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A quasigeostrophic model for the frequency-dependent response of the zonal-mean flow to planetary-wave forcing at Northern Hemisphere (NH) midlatitudes is applied to 4-D-Var ECMWF analysis data for six extended winter seasons. The theoretical response is a non-linear function of the frequency of the forcing, the thermal damping time α<sup>−1</sup>, and a scaling parameter µ which includes the aspect ratio of the meridional to the vertical length scale of the response. Regression of the calculated response from the analyses onto the theoretical response yields height-dependent estimates for both α<sup>−1</sup> and µ. The thermal damping time estimated from this dynamical model is about 2 days in the troposphere, 7–10 days in the stratosphere, and 2–4 days in the lower mesosphere. For the stratosphere and lower mesosphere, the estimates lie within the range of existing radiative damping time estimates, but for the troposphere they are significantly smaller.
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Information about clouds, in particular the accurate identification of cloud free pixels, is crucial for the retrieval of tropospheric vertical column densities from space. The Heidelberg Iterative Cloud Retrieval Utilities (HICRU) retrieve effective cloud fraction using spectra of two instruments designed for trace gas retrievals from space: The Global Ozone Monitoring Experiment (GOME) on the European Remote Sensing Satellite (ERS-2) and the SCanning Imaging Absorption SpectroMeter for Atmospheric CHartographY (SCIAMACHY) on ENVISAT. <P> HICRU applies the widely used threshold method to the so-called Polarization Monitoring Devices (PMDs) with higher spatial resolution compared to the channels used for trace gas retrievals. Cloud retrieval and in particular the identification of cloud free pixels is improved by HICRU through a sophisticated, iterative retrieval of the thresholds which takes their dependency on different instrumental and geometrical parameters into account. The lower thresholds, which represent the surface albedo and strongly affect the results of the algorithm, are retrieved accurately through a four stage classification scheme using image sequence analysis. <P> The design and the results of the algorithm applied to GOME data are described and compared to several other cloud algorithms for GOME. The differences to other cloud algorithms are discussed with respect to the particular characteristics of the algorithms.
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Atmospheric CO<sub>2</sub> concentrations, retrieved from spectral measurements made in the near infrared (NIR) by the SCIAMACHY instrument, using Full Spectral Initiation Weighting Function Modified Differential Optical Absorption Spectroscopy (FSI WFM-DOAS), are compared to ground based Fourier Transform Infrared (FTIR) data and to the output from a global chemistry-transport model. <P> Analysis of the FSI WFM-DOAS retrievals with respect to the ground based FTIR instrument, located at Egbert, Canada, show good agreement with an average negative bias of approximately −4.0% with a standard deviation of 3.0%. This bias which exhibits an apparent seasonal trend, is of unknown origin, though slight differences between the averaging kernels of the instruments and the limited temporal coverage of the FTIR data may be the cause. The relative scatter of the retrieved vertical column densities is larger than the spread of the FTIR measurements. Normalizing the CO<sub>2</sub> columns using the surface pressure does not affect the magnitude of this bias although it slightly decreases the scatter of the FSI data. <P> Comparisons of the FSI retrievals to the TM3 global chemistry-transport model, performed over four selected Northern Hemisphere scenes show reasonable agreement. The correlation, between the time series of the SCIAMACHY and model monthly scene averages, are 0.7 or greater, demonstrating the ability of SCIAMACHY to detect seasonal changes in the CO<sub>2</sub> distribution. The amplitude of the seasonal cycle, peak to peak, observed by SCIAMACHY however, is larger by a factor of 2–3 with respect to the model, which cannot be explained. The yearly means detected by SCIAMACHY are within 2% of those of the model with the mean difference between the CO<sub>2</sub> distributions also approximately 2.0%. Additionally, analysis of the retrieved CO<sub>2</sub> distributions reveals structure not evident in the model fields which correlates well with land classification type. <P> From these comparisons, it is estimated that the overall bias of the CO<sub>2</sub> columns retrieved by the FSI algorithm is <4.0% with the precision of monthly 1°×1° gridded data close to 1.0%.
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The manuscript presents a detailed description of the meteorological and chemical code of Malte – a model to predict new aerosol formation in the lower troposphere. The aerosol dynamics are achieved by the new developed UHMA (University of Helsinki Multicomponent Aerosol Model) code with kinetic limited nucleation as responsible mechanism to form new clusters. First results indicate that the model is able to predict the on- and offset of new particle formation as well as the total aerosol number concentrations that were in good agreement with the observations. Further, comparison of predicted and measured H<sub>2</sub>SO<sub>4</sub> concentrations showed a satisfactory agreement. The simulation results indicated that at a certain transitional particle diameter (2–7 nm), organic molecules can begin to contribute significantly to the growth rate compared to sulphuric acid. At even larger particle sizes, organic molecules can dominate the growth rate on days with significant monoterpene concentrations. The intraday vertical evolution of newly formed clusters and particles in two different size ranges resulted in two maxima at the ground. These particles grow around noon to the detectable size range and agree well with measured vertical profiles.
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This study describes key aspects of global chemistry-transport models and their impact on stratospheric tracer transport. We concentrate on global models that use assimilated winds from numerical weather predictions, but the results also apply to tracer transport in general circulation models. We examined grid resolution, numerical diffusion, air parcel dispersion, the wind or mass flux update frequency, and time interpolation. The evaluation is performed with assimilated meteorology from the "operational analyses or operational data" (OD) from the European Centre for Medium-Range Weather Forecasts (ECMWF). We also show the effect of the mass flux update frequency using the ECMWF 40-year re-analyses (ERA40). <P> We applied the three-dimensional chemistry-transport Tracer Model version 5 (TM5) and a trajectory model and performed several diagnoses focusing on different transport regimes. Covering different time and spatial scales, we examined (1) polar vortex dynamics during the Arctic winter, (2) the large-scale stratospheric meridional circulation, and (3) air parcel dispersion in the tropical lower stratosphere. <P> Tracer distributions inside the Arctic polar vortex show considerably worse agreement with observations when the model grid resolution in the polar region is reduced to avoid numerical instability. The results are sensitive to the diffusivity of the advection. Nevertheless, the use of a computational cheaper but diffusive advection scheme is feasible for tracer transport when the horizontal grid resolution is equal or smaller than 1 degree. The use of time interpolated winds improves the tracer distributions, particularly in the middle and upper stratosphere. Considerable improvement is found both in the large-scale tracer distribution and in the polar regions when the update frequency of the assimilated winds is increased from 6 to 3 h. It considerably reduces the vertical dispersion of air parcels in the tropical lower stratosphere. <P> Strong horizontal dispersion is not necessarily an indication of poor wind quality, as observations indicate. Moreover, the generally applied air parcel dispersion calculations should be interpreted with care, given the strong sensitivity of dispersion with altitude. <P> The results in this study provide a guideline for stratospheric tracer modeling using assimilated winds. They further demonstrate significant progress in the use of assimilated meteorology in chemistry-transport models, relevant for both short- and long-term integrations.
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A calibration for LACIS (Leipzig Aerosol Cloud Interaction Simulator) for its use as a CCN (cloud condensation nuclei) detector has been developed. For this purpose, sodium chloride and ammonium sulfate particles of known sizes were generated and their grown sizes were detected at the LACIS outlet. From these signals, the effective critical super-saturation was derived as a function of the LACIS wall temperature. With this, LACIS is calibrated for its use as a CCN detector. The applicability of LACIS for measurements of the droplet activation, and also of the hygroscopic growth of atmospheric aerosol particles was tested. The activation of the urban aerosol particles used in the measurements was found to occur at a critical super-saturation of 0.46% for particles with a dry diameter of 75 nm, and at 0.42% for 85 nm, respectively. Hygroscopic growth was measured for atmospheric aerosol particles with dry diameters of 150, 300 and 350 nm at relative humidities of 98 and 99%, and it was found that the larger dry particles contained a larger soluble volume fraction of about 0.85, compared to about 0.6 for the 150 nm particles.
