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  • Measurements of the relation between aerosol properties and microphysics and chemistry of low level liquid water clouds in Northern Finland

    Physical and chemical properties of boundary layer clouds, together with relevant aerosol properties, were investigated during the first Pallas Cloud Experiment (First Pace) conducted in northern Finland between 20 October and 9 November 2004. Two stations located 6 km apart from each other at different altitudes were employed in measurements. The low-altitude station was always below the cloud layer, whereas the high-altitude station was inside clouds about 75% of the time during the campaign. Direct measurements of cloud droplet populations showed that our earlier approach of determining cloud droplet residual particle size distributions and corresponding activated fractions using continuous aerosol number size distribution measurements at the two stations is valid, as long as the cloud events are carefully screened to exclude precipitating clouds and to make sure the same air mass has been measured at both stations. We observed that a non-negligible fraction of cloud droplets originated from Aitken mode particles even at moderately-polluted air masses. We found clear evidence on first indirect aerosol effect on clouds but demonstrated also that no simple relation between the cloud droplet number concentration and aerosol particle number concentration exists for this type of clouds. The chemical composition of aerosol particles was dominated by particulate organic matter (POM) and sulphate in continental air masses and POM, sodium and chlorine in marine air masses. The inorganic composition of cloud water behaved similarly to that of the aerosol phase and was not influenced by inorganic trace gases.
  • Increase of the aerosol hygroscopicity by cloud processing in a mesoscale convective system: a case study from the AMMA campaign

    Aerosol properties were measured during an airborne campaign experiment that took place in July 2006 in West Africa within the framework of the African Monsoon Multidisciplinary Analyses (AMMA). The goal of the present study was to determine the main microphysical processes that affect the aerosols during the passage of a mesoscale convective system (MCS) over the region of Niamey in Niger. A significant change in the aerosol profiles measured before and after the passage of the MCS was found in a layer located between 1300 and 3000 m, where the aerosol concentration drastically decreased after the passage of the MCS. Concurrently, a significant increase in the cloud condensation nuclei (CCN) fraction was also observed during the post-MCS period in the same layer. Moreover, the results of the elemental composition analyses of individual particles collected in this layer after the MCS passage have shown higher contributions of sulfate, nitrate and chloride to the total aerosol mass. A mesoscale atmospheric model with on-line dust parameterization and Lagrangian backtrajectories was used to interpret the impact of the MCS on the aerosol properties. The results of the simulation show that the MCS 1) generates dust particles at the surface in the gust front of the system and washout of particles during the system precipitation, 2) modifies the aerosol mixing state (intensive aerosol property) through cloud processing, and 3) enhances CCN activity of particles through coating by soluble material.
  • Evaluation of tropospheric and stratospheric ozone trends over Western Europe from ground-based FTIR network observations

    Within the European project UFTIR (Time series of Upper Free Troposphere observations from an European ground-based FTIR network), six ground-based stations in Western Europe, from 79&deg; N to 28&deg; N, all equipped with Fourier Transform infrared (FTIR) instruments and part of the Network for the Detection of Atmospheric Composition Change (NDACC), have joined their efforts to evaluate the trends of several direct and indirect greenhouse gases over the period 1995–2004. The retrievals of CO, CH<sub>4</sub>, C<sub>2</sub>H<sub>6</sub>, N<sub>2</sub>O, CHClF<sub>2</sub>, and O<sub>3</sub> have been optimized. Using the optimal estimation method, some vertical information can be obtained in addition to total column amounts. A bootstrap resampling method has been implemented to determine annual partial and total column trends for the target gases. The present work focuses on the ozone results. The retrieved time series of partial and total ozone columns are validated with ground-based correlative data (Brewer, Dobson, UV-Vis, ozonesondes, and Lidar). The observed total column ozone trends are in agreement with previous studies: 1) no total column ozone trend is seen at the lowest latitude station Izaña (28&deg; N); 2) slightly positive total column trends are seen at the two mid-latitude stations Zugspitze and Jungfraujoch (47&deg; N), only one of them being significant; 3) the highest latitude stations Harestua (60&deg; N), Kiruna (68&deg; N) and Ny-Ålesund (79&deg; N) show significant positive total column trends. Following the vertical information contained in the ozone FTIR retrievals, we provide partial columns trends for the layers: ground-10 km, 10–18 km, 18–27 km, and 27–42 km, which helps to distinguish the contributions from dynamical and chemical changes on the total column ozone trends. We obtain no statistically significant trends in the ground-10 km layer for five out of the six ground-based stations. We find significant positive trends for the lowermost stratosphere at the two mid-latitude stations, and at Ny-Ålesund. We find smaller, but significant trends for the 18–27 km layer at Kiruna, Harestua, Jungfraujoch, and Izaña. The results for the upper layer are quite contrasted: we find significant positive trends at Kiruna, Harestua, and Jungfraujoch, and significant negative trends at Zugspitze and Izaña. These ozone partial columns trends are discussed and compared with previous studies.
  • Global simulations of aerosol processing in clouds

    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

    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.
  • Observations of mesoscale and boundary-layer scale circulations affecting dust transport and uplift over the Sahara

    Observations of the Saharan boundary layer, made during the GERBILS field campaign, show that mesoscale land surface temperature variations (which were related to albedo variations) induced mesoscale circulations. With weak winds along the aircraft track, land surface temperature anomalies with scales of greater than 10 km are shown to significantly affect boundary-layer temperatures and winds. Such anomalies are expected to affect the vertical mixing of the dusty and weakly stratified Saharan Residual Layer (SRL). Mesoscale variations in winds are also shown to affect dust loadings in the boundary layer. <br><br> Using the aircraft observations and data from the COSMO model, a region of local dust uplift, with strong along-track winds, was identified in one low-level flight. Large eddy model (LEM) simulations based on this location showed linearly organised boundary-layer convection. Calculating dust uplift rates from the LEM wind field showed that the boundary-layer convection increased uplift by approximately 30%, compared with the uplift rate calculated neglecting the convection. The modelled effects of boundary-layer convection on uplift are shown to be larger when the boundary-layer wind is decreased, and most significant when the mean wind is below the threshold for dust uplift and the boundary-layer convection leads to uplift which would not otherwise occur. <br><br> Both the coupling of albedo features to the atmosphere on the mesoscale, and the enhancement of dust uplift by boundary-layer convection are unrepresented in many climate models, but may have significant impacts on the vertical transport and uplift of desert dust. Mesoscale effects in particular tend to be difficult to parametrise.
  • Monthly-averaged anthropogenic aerosol direct radiative forcing over the Mediterranean based on AERONET aerosol properties

    The all-sky direct radiative effect by anthropogenic aerosol (DRE<sub>a</sub>) is calculated in the solar (0.3–4 μm) and infrared (4–200 μm) spectral ranges for six Mediterranean sites. The sites are differently affected by pollution and together reflect typical aerosol impacts that are expected over land and coastal sites of the central Mediterranean basin. Central to the simulations are aerosol optical properties from AERONET sun-/sky-photometer statistics for the year 2003. A discussion on the variability of the overall (natural + anthropogenic) aerosol properties with site location is provided. Supplementary data include MODIS satellite sensor based solar surface albedos, ISCCP products for high- mid- and low cloud cover and estimates for the anthropogenic aerosol fraction from global aerosol models. Since anthropogenic aerosol particles are considered to be smaller than 1 μm in size, mainly the solar radiation transfer is affected with impacts only during sun-light hours. At all sites the (daily average) solar DRE<sub>a</sub> is negative all year round at the top of the atmosphere (ToA). Hence, anthropogenic particles produce over coastal and land sites of the central Mediterranean a significant cooling effect. Monthly DRE<sub>a</sub> values vary from site to site and are seasonally dependent as a consequence of the seasonal dependence of available sun-light and microphysical aerosol properties. At the ToA the monthly average DRE<sub>a</sub> is &minus;(4&plusmn;1) W m<sup>&minus;2</sup> during spring-summer (SS, April–September) and &minus;(2&plusmn;1) W m<sup>&minus;2</sup> during autumn-winter (AW, October–March) at the polluted sites. In contrast, it varies between &minus;(3&plusmn;1) W m<sup>&minus;2</sup> and &minus;(1&plusmn;1) W m<sup>&minus;2</sup> on SS and AW, respectively at the less polluted site. Due to atmospheric absorption the DRE<sub>a</sub> at the surface is larger than at the ToA. At the surface the monthly average DRE<sub>a</sub> varies between the most and the least polluted site between &minus;(7&plusmn;1) W m<sup>&minus;2</sup> and &minus;(4&plusmn;1) W m<sup>&minus;2</sup> during SS, and between &minus;(4&plusmn;3) W m<sup>&minus;2</sup> and &minus;(1&plusmn;1) W m<sup>&minus;2</sup> during AW. The DRE<sub>a</sub> at infrared wavelengths is positive but negligible, especially at the ToA (&lt;0.3 W m<sup>&minus;2</sup>). The average of DRE<sub>a</sub> monthly-means referring to all sites has allowed getting a ToA- and sfc-DRE<sub>a</sub> yearly-mean value of &minus;(3&plusmn;2) and &minus;(5&plusmn;3) W m<sup>&minus;2</sup>, respectively at solar wavelengths. Last data, even if refer to a particular year, indicate that the radiative energy-balance of Central Mediterranean land and coastal sites is quite affected by anthropogenic particles.
  • The Von Kármán constant retrieved from CASES-97 dataset using a variational method

    A variational method is developed to retrieve the von Kármán constant &kappa; from the CASES-97 dataset, collected near Wichita, Kansas, the United States from 6 April to 24 May 1997. In the variational method, a cost function is defined to measure the difference between observed and computed gradients of wind speed, air temperature and specific humidity. An optimal estimated von Kármán constant is obtained by minimizing the cost function through adjusting values of the von Kármán constant. Under neutral stratification, the variational analysis confirms the conventional value of &kappa; (=0.40). For non-neutral stratification, however, &kappa; varies with stability. The computational results show that the &kappa; decreases monotonously from stable to unstable stratification. The variational calculated mean value of the von Kármán constant is 0.383~0.390 when the atmospheric stratification is taken into consideration. Relations between &kappa; and surface momentum and heat flux are also examined.
  • Spectral UV measurements in Austria from 1994 to 2006: investigations of short- and long-term changes

    The influence of variability of atmospheric parameters on short- and long-term changes of spectral UV irradiance measured at the Sonnblick observatory (47.03&deg; N, 12.57&deg; E, 3106 m) during the period from 1994 to 2006 is studied. Measurements were performed with the Brewer #093 single-monochromator spectrophotometer and with a Bentham DM 150 spectroradiometer (double-monochromator). <br> <br> The influence of ozone, albedo, snowline and clouds on UV variability is evaluated for each parameter separately using 10-year climatology. It is found that the effect of total ozone on short-term variability of UV irradiance at 305 nm can be more than 200% and on average more than 50%. Clouds can cause variability of 150% or more and on average 35%. Variability caused by albedo reaches a maximum of 32% in April (6% on average). In summer and autumn, total ozone and clouds strongly influence the variability of UV radiation, whereas in winter and spring ozone has the more pronounced effect. A decrease in snowline height from 3000 m to 800 m a.s.l. enhances the UV irradiance by a factor of 1.24 for clear sky conditions and by a factor of 1.7 for 8/8 cloud cover. <br> <br> Long-term trends are investigated for the time period from 1994 to 2006 based on clear-sky measurements, using the non-parametric Mann-Kendall trend test. Significant downward trends (99% confidence level) are found for solar zenith angle 55&deg; at wavelengths from 305 nm to 324 nm and erythemally weighted irradiance according to CIE, which are caused by an increase in sunshine duration during periods of high total column ozone. Significant trends (90% confidence level) were also found for other combinations of wavelength and SZA.
  • Technical Note: The CCCma third generation AGCM and its extension into the middle atmosphere

    The Canadian Centre for Climate Modelling and Analysis third generation atmospheric general circulation model (AGCM3) is described. The discussion summarizes the details of the complete physics package emphasizing the changes made relative to the second generation version of the model. AGCM3 is the underlying model for applications which include the IPCC fourth assessment, coupled atmosphere-ocean seasonal forecasting, the first generation of the CCCma earth system model (CanESM1), and middle-atmosphere chemistry-climate modelling (CCM). Here we shall focus on issues related to an upwardly extended version of AGCM3, the Canadian Middle-Atmosphere Model (CMAM). The CCM version of CMAM participated in the 2006 WMO/UNEP Scientific Assessment of Ozone Depletion and issues concerning its climate such as the impact of gravity-wave drag, the modelling of a spontaneous QBO, and the seasonality of the breakdown of the Southern Hemisphere polar vortex are discussed here.
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