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We propose a new method for the delineation of precipitation using cloud properties derived from optical satellite data. This approach is not only sufficient for the detection of mainly convective precipitation by means of the commonly used connection between infrared cloud top temperature and rainfall probability but enables the detection of stratiform precipitation (e.g., in connection with mid-latitude frontal systems). The scheme presented is based on the concept model, that precipitating clouds must have both a sufficient vertical extent and large enough droplets. Therefore, we have analysed MODIS scenes during the severe European summer floods in 2002 and retrieved functions for the computation of an auto-adaptive threshold value of the effective cloud droplet radius with respect to the corresponding optical thickness which links these cloud properties with rainfall areas on a pixel basis.
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Aerosol samples were collected at a rural background site in southern Finland in May 2004 during pollution episode (PM<sub>1</sub>~16 µg m<sup>−3</sup>, backward air mass trajectories from south-east), intermediate period (PM<sub>1</sub>~5 µg m<sup>−3</sup>, backtrajectories from north-east) and clean period (PM<sub>1</sub>~2 µg m<sup>−3</sup>, backtrajectories from north-west/north). The elemental composition, morphology and mixing state of individual aerosol particles in three size fractions were studied using transmission electron microscopy (TEM) coupled with energy dispersive X-ray (EDX) microanalyses. The TEM/EDX results were complemented with the size-segregated bulk chemical measurements of selected ions and organic and elemental carbon. Many of the particles in PM<sub>0.2–1</sub> and PM<sub>1–3.3</sub> size fractions were strongly internally mixed with S, C and/or N. The major particle types in PM<sub>0.2–1</sub> samples were 1) soot and 2) (ammonium)sulphates and their mixtures with variable amounts of C, K, soot and/or other inclusions. Number proportions of those two particle groups in PM<sub>0.2–1</sub> samples were 0–12% and 83–97%, respectively. During the pollution episode, the proportion of Ca-rich particles was very high (26–48%) in the PM<sub>1–3.3</sub> and PM<sub>3.3–11</sub> samples, while the PM<sub>0.2–1</sub> and PM<sub>1–3.3</sub> samples contained elevated proportions of silicates (22–33%), metal oxides/hydroxides (1–9%) and tar balls (1–4%). These aerosols originated mainly from polluted areas of Eastern Europe, and some open biomass burning smoke was also brought by long-range transport. During the clean period, when air masses arrived from the Arctic Ocean, PM<sub>1–3.3</sub> samples contained mainly sea salt particles (67–89%) with a variable rate of Cl substitution (mainly by NO<sub>3</sub><sup>−</sup>). During the intermediate period, the PM<sub>1–3.3</sub> sample contained porous (sponge-like) Na-rich particles (35%) with abundant S, K and O. They might originate from the burning of wood pulp wastes of paper industry. The proportion of biological particles and C-rich fragments (probably also biological origin) were highest in the PM<sub>3.3–11</sub> samples (0–81% and 0–22%, respectively). The origin of different particle types and the effect of aging processes on particle composition and their hygroscopic and optical properties are discussed.
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Using new and accurate experimental results concerning the spectroscopic properties of the HNO<sub>3</sub> molecule as well as improved theoretical methods it has been possible to generate an improved set of line parameters for this molecule in the spectral range covered by the MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) experiment. These line parameters, which have been validated using broadband atmospheric spectra recorded by MIPAS, have been included in the last version of the MIPAS spectroscopic database to be used for future processing of the MIPAS spectra.
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The new Modular Earth Submodel System (MESSy) describes atmospheric chemistry and meteorological processes in a modular framework, following strict coding standards. It has been coupled to the ECHAM5 general circulation model, which has been slightly modified for this purpose. A 90-layer model setup up to 0.01 hPa was used at spectral T42 resolution to simulate the lower and middle atmosphere. With the high vertical resolution the model simulates the Quasi-Biennial Oscillation. The model meteorology has been tested to check the influence of the changes to ECHAM5 and the radiation interactions with the new representation of atmospheric composition. In the simulations presented here a Newtonian relaxation technique was applied in the tropospheric part of the domain to weakly nudge the model towards the analysed meteorology during the period 1998–2005. This allows an efficient and direct evaluation with satellite and in-situ data. It is shown that the tropospheric wave forcing of the stratosphere in the model suffices to reproduce major stratospheric warming events leading e.g. to the vortex split over Antarctica in 2002. Characteristic features such as dehydration and denitrification caused by the sedimentation of polar stratospheric cloud particles and ozone depletion during winter and spring are simulated well, although ozone loss in the lower polar stratosphere is slightly underestimated. The model realistically simulates stratosphere-troposphere exchange processes as indicated by comparisons with satellite and in situ measurements. The evaluation of tropospheric chemistry presented here focuses on the distributions of ozone, hydroxyl radicals, carbon monoxide and reactive nitrogen compounds. In spite of minor shortcomings, mostly related to the relatively coarse T42 resolution and the neglect of inter-annual changes in biomass burning emissions, the main characteristics of the trace gas distributions are generally reproduced well. The MESSy submodels and the ECHAM5/MESSy1 model output are available through the internet on request.
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Total column ozone is used to trace the dynamics of the lower and middle stratosphere which is governed by planetary waves. In order to analyse the planetary wave activity a Harmonic Analysis is applied to global multi-year total ozone observations from the Total Ozone Monitoring Spectrometer (TOMS). As diagnostic variables we introduce the hemispheric ozone variability indices one and two. They are defined as the hemispheric means of the amplitudes of the zonal waves number one and two, respectively, as traced by the total ozone field. <br><br> The application of these indices as a simple diagnostic for the evaluation of coupled chemistry-climate models (CCMs) is demonstrated by comparing results of the CCM ECHAM4.L39(DLR)/CHEM (hereafter: E39/C) against satellite observations. It is quantified to what extent a multi-year model simulation of E39/C (representing "2000" climate conditions) is able to reproduce the zonal and hemispheric planetary wave activity derived from TOMS data (1996–2004, Version 8). <br><br> Compared to the reference observations the hemispheric ozone variability indices one and two of E39/C are too high in the Northern Hemisphere and too low in the Southern Hemisphere. In the Northern Hemisphere, where the agreement is generally better, E39/C produces too strong a planetary wave one activity in winter and spring and too high an interannual variability. For the Southern Hemisphere we reveal that the indices from observations and model differ significantly during the ozone hole season. The indices are used to give reasons for the late formation of the Antarctic ozone hole, the insufficient vortex elongation and eventually the delayed final warming in E39/C. <br><br> In general, the hemispheric ozone variability indices can be regarded as a simple and robust diagnostic to quantify model-observation differences concerning planetary wave activity. It allows a first-guess on how the dynamics is represented in a model simulation before applying costly and more specific diagnostics.
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Temperature trends in the UTLS region are under-reported, particularly in the Southern Hemisphere, and yet temperature is one of the most important indicators of changes in dynamical and radiative processes in the atmosphere. Here radiosonde data from Durban, South Africa (30.0° S, 30.9° E) over the period 1980 to 2001 (22 years) between 250 and 20 hPa are used to derive a mean temperature climatology and to determine trends. The seasonal cycle at the 250-hPa level is anti-correlated with the seasonal cycles at the 150-hPa and 100-hPa heights. The 100-hPa level (local tropopause) exhibits a minimum temperature in late summer and a maximum in winter, and closely corresponds to previous results for tropical regions. Based on a Fourier analysis, both the annual cycle (AO) and the semi-annual cycle (SAO) are dominant, although the former is about 4 times stronger. The AO is strongest at the 100-hPa height. A trend analysis reveals a cooling trend at almost all heights in the UTLS region, with a maximum cooling rate of 1.09±0.41 K per decade, at 70-hPa. Cooling rates are in good agreement with other studies and are slightly higher in summer than in winter.
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To elucidate human induced changes of aerosol load and composition in the atmosphere, a coupled aerosol and gas-phase chemistry transport model of the troposphere and lower stratosphere has been used. The present 3-D modeling study focuses on aerosol chemical composition change since preindustrial times considering the secondary organic aerosol formation together with all other main aerosol components including nitrate. In particular, we evaluate non-sea-salt sulfate (nss-SO<sub>4</sub><sup>=</sup>), ammonium (NH<sub>4</sub><sup>+</sup>), nitrate (NO<sub>3</sub><sup>−</sup>), black carbon (BC), sea-salt, dust, primary and secondary organics (POA and SOA) with a focus on the importance of secondary organic aerosols. Our calculations show that the aerosol optical depth (AOD) has increased by about 21% since preindustrial times. This enhancement of AOD is attributed to a rise in the atmospheric load of BC, nss-SO<sub>4</sub><sup>=</sup>, NO<sub>3</sub><sup−</sup>, POA and SOA by factors of 3.3, 2.6, 2.7, 2.3 and 1.2, respectively, whereas we assumed that the natural dust and sea-salt sources remained constant. The nowadays increase in carbonaceous aerosol loading is dampened by a 34–42% faster conversion of hydrophobic to hydrophilic carbonaceous aerosol leading to higher removal rates. These changes between the various aerosol components resulted in significant modifications of the aerosol chemical composition. The relative importance of the various aerosol components is critical for the aerosol climatic effect, since atmospheric aerosols behave differently when their chemical composition changes. According to this study, the aerosol composition changed significantly over the different continents and with height since preindustrial times. The presence of anthropogenically emitted primary particles in the atmosphere facilitates the condensation of the semi-volatile species that form SOA onto the aerosol phase, particularly in the boundary layer. The SOA burden that is dominated by the natural component has increased by 24% while its contribution to the AOD has increased by 11%. The increase in oxidant levels and preexisting aerosol mass since preindustrial times is the reason of the burden change, since emissions have not changed significantly. The computed aerosol composition changes translate into about 2.5 times more water associated with non sea-salt aerosol. Additionally, aerosols contain 2.7 times more inorganic components nowadays than during the preindustrial times. We find that the increase in emissions of inorganic aerosol precursors is much larger than the corresponding aerosol increase, reflecting a non-linear atmospheric response.
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This paper presents key results achieved by an analysis of the relation between high-quality simultaneous Dobson, Brewer ground and TOMS-V8, GOME-WFDOAS satellite total ozone observations for Hradec Kralove, Czech Republic. Statistically significant seasonal differences with maxima up to 4% of monthly averages have been found between Dobson and Brewer measurements during the winter/spring months. These differences can influence estimations of ozone trends if combined data series are used after replacing a Dobson instrument by a Brewer spectrophotometer. The differences can be attributed mostly to the influence of temperature on ozone absorption coefficients and to total sulphur dioxide. Similar seasonal differences exist between Dobson, GOME and Brewer, TOMS data sets at Hradec Kralove while Dobson versus TOMS and Brewer versus GOME observations fit well with each other within the instrumental accuracy of spectrophotometers. The above findings are supposed to be relevant to other mid and high latitude stations and they have been confirmed by several independent analyses. The conclusions should be considered by data users because the differences between particular ground and satellite data sets can influence validation of satellite ozone observing systems and analyses of recovery of the ozone layer in mid and high latitudes, among others.
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Methane in air and seawater was measured in the Eastern Black Sea during the 10–18 December 1999 BIGBLACK project cruise. The measurements allowed for the calculation of supersaturation ratios and methane fluxes across the air-sea interface. CH<sub>4</sub> mixing ratios in air were generally in the 1.8–2.0 ppmv range, while surface (4 m depth) seawater concentrations varied from 4 to 93 ppmv. Above active seep areas, the water was supersaturated to around 500% with respect to the overlying atmosphere. Accordingly, flux densities varied greatly and were up to 3300 umol m<sup>−2</sup> day<sup>−1</sup>. In the Sevastopol harbour, supersaturations up to around 3000%, similar to those at the Danube Delta, were observed, while in the Istanbul harbour supersaturations could not be determined because the very high values of water concentrations led to detector saturation. Simple modelling shows that the observed fluxes do not have any substantial impact on the methane content of the Black Sea atmosphere, as they would only raise its concentrations by less than 50 ppt. On the other hand, calculations performed as part of the CRIMEA project show that mud volcano eruptions could episodically raise the methane concentrations well above their regional background for several tens of kilometres downwind. These calculations, which also apply to mud volcano eruptions elsewhere on the globe, indicate that the spatial extend and the magnitude of the atmospheric perturbation is such that its observation might lie within the capabilities of existing satellite instrumentation such as SCIAMACHY on ENVISAT.
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The upwelling planetary wave activity (PW) from the troposphere controls the intensity of the equator to pole transport of stratospheric ozone by the Brewer-Dobson circulation and thereby modulates the total ozone content at mid- and high-latitudes. Rayleigh lidar temperature data obtained from 1981 to 2001 at mid-latitude were used to study the interannual variability of PW activity in winter (October to April). The spectrum of stratospheric temperature fluctuations exhibits 2 peaks corresponding to 2 dominant modes of free travelling Rossby waves known as 16 day- and 12 day-waves. The 12 day-wave activity is shown to be anticorrelated with the equatorial QBO wind at 40 hPa. During the period 1981–2000 the global PW activity shows a negative trend for months October to January and a positive trend in March and April.
