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This paper presents the spatio-temporal distribution of NO<sub>y</sub> species at altitudes between 14 and 31 km as measured with the MIPAS-B instrument on the morning of 21 March 2003 in northern Scandinavia. At lower altitudes (below about 22 km), temperature variations, the distribution of ClONO<sub>2</sub>, and the tracer N<sub>2</sub>O reveal the dynamics through the edge of the late arctic polar vortex. At higher altitudes, continuous measurement before, during, and after sunrise provides information about photochemistry illustrating the evolution of the photochemically active gases NO<sub>2</sub> and N<sub>2</sub>O<sub>5</sub> around sunrise. The measured temporal evolution of NO<sub>2</sub> and N<sub>2</sub>O<sub>5</sub> is compared to box modelling that is run along backward calculated trajectories. While the comparison of measured and modelled N<sub>2</sub>O<sub>5</sub> reveals significant differences, there is a good agreement between the model and observations for NO<sub>2</sub> in terms of volume mixing ratios but the simulated decrease shortly after sunrise is underestimated compared to the measurements. The differences are attributed to the photolysis rates used in the box model calculations.
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The ICTP regional climate model (RegCM3) coupled with a desert dust aerosol model is used to simulate the net radiative forcing (short-wave and long-wave) and related climate effects of dust aerosols over East Asia. Two sets of experiments are completed and intercompared, one without (Exp. 1) and one with (Exp. 2) the radiative effects of dust aerosols. The experiments encompass the main dust producing months, February through May, for 10 years (1997–2006), and the simulation results are evaluated against ground station and satellite data. The model captures the basic observed climatology over the area of interest. The spatial and temporal variations of near surface concentration, mass load, optical depth and emission of dust aerosols from the main source regions are reproduced by model. The main model deficiency is an overestimate of dust amounts over the source regions and an underestimate downwind of these source areas, which indicates an underestimate of dust dispersal. Over the desert source regions, the net TOA radiative forcing is positive, while it is small over the other regions as a result of high surface albedo values which reduce the short-wave radiative forcing. The net surface radiative fluxes are decreased by dust and this causes a surface cooling locally up to −1°C. The inclusion of net (short-wave and long-wave) dust radiative forcing leads to a reduction of dust emission in the East Asia source regions, which is mainly caused by an increase in local stability and a corresponding decrease in dust lifting. Our results indicate that dust effects should be included in the assessment of climate change over East Asia.
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The detection of cloudiness is investigated by means of partial and total cloud amount estimations from pyrgeometer radiation measurements and visible all-sky imager observations. The measurements have been performed in Westerland, a seaside resort on the North Sea island of Sylt, Germany, during summer 2005. <br><br> An improvement to previous studies on this subject resulting in the first time partial cloud amounts (PCAs), defined as cloud amounts without high clouds calculated from longwave downward radiation (LDR) according to the APCADA algorithm (Dürr and Philipona, 2004), are validated against both human observations from the <i>National Meteorological Servive</i> DWD at the nearby airport of Sylt and digital all-sky imaging. The aim is to establish the APCADA scheme at a coastal midlatitude site for longterm observations of cloud cover and to quantify errors resulting from the different methods of detecting cloudiness. <br><br> Differences between the resulting total cloud amounts (TCAs), defined as cloud amount for all-cloud situations, derived from the camera images and from human observations are within ±1 octa in 72% and within ±2 octa in 85% of the cases. Compared to human observations, PCA measurements, according to APCADA, underestimate the observed cloud cover in 47% of all cases and the differences are within ±1 octa in 60% and ±2 octa in 74% of all cases. Since high cirrus clouds can not be derived from LDR, separate comparisons for all cases without high clouds have been performed showing an agreement within ±1(2) octa in 73(90)% for PCA and also for camera-derived TCA. For this coastal mid-latitude site under investigation, we find similar though slightly smaller agreements to human observations as reported by Dürr and Philipona (2004). Though limited to daytime, the cloud cover retrievals from the sky imager are not really affected by cirrus clouds and provide a more reliable cloud climatology for all-cloud conditions than APCADA.
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We present a study of Saharan dust export towards the tropical North Atlantic using the regional dust emission, transport and deposition model LM-MUSCAT. Horizontal and vertical distribution of dust optical thickness, concentration, and dry and wet deposition rates are used to describe seasonality of dust export and deposition towards the eastern Atlantic for three typical months in different seasons. Deposition rates strongly depend on the vertical dust distribution, which differs with seasons. Furthermore the contribution of dust originating from the Bodélé Depression to Saharan dust over the Atlantic is investigated. A maximum contribution of Bodélé dust transported towards the Cape Verde Islands is evident in winter when the Bodélé source area is most active and dominant with regard to activation frequency and dust emission. Limitations of using satellite retrievals to estimate dust deposition are highlighted.
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Three-dimensional structures of Asian dust transport in the planetary boundary layer (PBL) and free atmosphere occurring successively during the end of May 2007 were clarified using results of space-borne backscatter lidar, Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP), and results obtained using a data-assimilated version of a dust transport model (RC4) based on a ground-based NIES lidar network. The dust layer depths and the vertical and horizontal structure simulated by RC4 agreed with those of CALIOP observations from the dust source region to the far-downstream region. Two important transport mechanisms of Asian dust in the PBL and free atmosphere were clarified: a low-level dust outbreak within the dry slot region of a well-developed low-pressure system, and formation of an elevated dust layer within the warm sector of a low-pressure system. We also represent the aging of pure dust particles using the particle depolarization ratio (PDR) at 532 nm and the color ratio (CR) at 1064 nm and 532 nm. Aerosols with high PDR were observed uniformly over the dust source region. While the dust cloud was transported to the eastern downwind regions, aerosols with low PDR and high CR occur in the layer of less than 1 km height, suggesting a mixing state of spherical aerosols and dust in the surface layer.
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We use an atmospheric general circulation model (AGCM) driven chemistry-transport model (ACTM) to simulate the evolution of sulfur hexafluoride (SF<sub>6</sub>) in the troposphere. The model results are compared with continuous measurements at 6 sites over 71° N–90° S. These comparisons demonstrate that the ACTM simulations lie within the measurement uncertainty over the analysis period (1999–2006) and capture salient features of synoptic, seasonal and interannual SF<sub>6</sub> variability. To understand transport timescales of SF<sub>6</sub> within the troposphere, transport times of air parcels from the surface to different regions of the troposphere ("age") are estimated from a simulation of an idealized tracer. The age estimation error and its sensitivity to the selection of reanalysis meteorology for ACTM nudging or the tracer transport by deep cumulus convection as represented in the model are discussed. Monthly-mean, 2-box model exchange times (τ<sub><i>ex</i></sub>) are calculated from both the observed and simulated SF<sub>6</sub> time series at the 6 observing sites and show favorable agreement, suggesting that the ACTM adequately represents large-scale interhemispheric transport. The simulated SF<sub>6</sub> variability is further investigated through decomposition of the mixing ratio time-tendency into advective, convective, and vertical diffusive components. The transport component analysis illustrates the role of each process in SF<sub>6</sub> synoptic variability at the site level and provides insight into the seasonality of τ<sub><i>ex</i></sub>.
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The MARSCHALS (Millimetre-wave Airborne Receiver for Spectroscopic CHaracterisation of Atmospheric Limb-Sounding) project has the general objectives of demonstrating the measurement capabilities of a limb viewing instrument working in the millimetre and sub-millimetre spectral regions (from 294 to 349 GHz) for the study of the Upper Troposphere – Lower Stratosphere (UTLS). MARSCHALS has flown on board the M-55 stratospheric aircraft (Geophysica) in two measurements campaigns. Here we report the results of the analysis of MARSCHALS measurements during the SCOUT-O3 campaign held in Darwin (Australia) in December 2005 obtained with MARC (Millimetre-wave Atmospheric-Retrieval Code). MARSCHALS measured vertical distributions of temperature, water vapour, ozone and nitric acid in the altitude range from 10 to 20 km in presence of clouds that obscure measurements in the middle infrared spectroscopic region. The minimum altitude at which the retrieval has been possible is determined by the high water concentration typical of the tropical region rather than the extensive cloud coverage experienced during the flight. Water has been measured from 10 km to flight altitude (~18 km) with a 10% accuracy, ozone from 14 km to flight altitude with accuracy ranging from 10% to 60%, while the retrieval of nitric acid has been possible with an accuracy not better than 40% only from 16 km to flight altitude due to the low signal to noise ratio of its emission in the analysed spectral region. The results have been validated using measurement made in a less cloudy region by MIPAS-STR, an infrared limb-viewing instrument on board the M-55, during the same flight.
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The evolution of two-dimensional drop distributions is simulated in this study using a Monte Carlo method. The stochastic algorithm of Gillespie (1976) for chemical reactions in the formulation proposed by Laurenzi et al. (2002) was used to simulate the kinetic behavior of the drop population. Within this framework, species are defined as droplets of specific size and aerosol composition. The performance of the algorithm was checked by a comparison with the analytical solutions found by Lushnikov (1975) and Golovin (1963) and with finite difference solutions of the two-component kinetic collection equation obtained for the Golovin (sum) and hydrodynamic kernels. Very good agreement was observed between the Monte Carlo simulations and the analytical and numerical solutions. A simulation for realistic initial conditions is presented for the hydrodynamic kernel. As expected, the aerosol mass is shifted from small to large particles due to collection process. This algorithm could be extended to incorporate various properties of clouds such several crystals habits, different types of soluble CCN, particle charging and drop breakup.
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We have combined the first satellite maps of the global distribution of phytoplankton functional type and new measurements of phytoplankton-specific isoprene productivities, with available remote marine isoprene observations and a global model, to evaluate our understanding of the marine isoprene source and its impacts on organic aerosol abundances. Using satellite products to scale up data on phytoplankton-specific isoprene productivity to the global oceans, we infer a mean "bottom-up" oceanic isoprene emission of 0.31±0.08 (1σ) Tg/yr. By minimising the mean bias between the model and isoprene observations in the marine atmosphere remote from the continents, we produce a "top-down" oceanic isoprene source estimate of 1.9 Tg/yr. We suggest our reliance on limited atmospheric isoprene data, difficulties in simulating in-situ isoprene production rates in laboratory phytoplankton cultures, and limited knowledge of isoprene production mechanisms across the broad range of phytoplankton communities in the oceans under different environmental conditions as contributors to this difference between the two estimates. Inclusion of secondary organic aerosol (SOA) production from oceanic isoprene in the model with a 2% yield produces small contributions (0.01–1.4%) to observed organic carbon (OC) aerosol mass at three remote marine sites in the Northern and Southern Hemispheres. Based on these findings we suggest an insignificant role for isoprene in modulating remote marine aerosol abundances, giving further support to a recently postulated primary OC source in the remote marine atmosphere.
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Experiments were conducted to investigate the effects of photo-oxidation on organic aerosol (OA) emissions from flaming and smoldering hard- and soft-wood fires under plume-like conditions. This was done by exposing the dilute emissions from a small wood stove to UV light in a smog chamber and measuring the gas- and particle-phase pollutant concentrations with a suite of instruments including a Proton Transfer Reaction Mass Spectrometer (PTR-MS), an Aerosol Mass Spectrometer (AMS) and a thermodenuder. The measurements highlight how atmospheric processing can lead to considerable evolution of the mass and volatility of biomass-burning OA. Photochemical oxidation produced substantial new OA, increasing concentrations by a factor of 1.5 to 2.8 after several hours of exposure to typical summertime hydroxyl radical (OH) concentrations. Less than 20% of this new OA could be explained using a state-of-the-art secondary organic aerosol model and the measured decay of traditional SOA precursors. The thermodenuder data indicate that the primary OA is semivolatile; at 50°C between 50 and 80% of the fresh primary OA evaporated. Aging reduced the volatility of the OA; at 50°C only 20 to 40% of aged OA evaporated. The predictions of a volatility basis-set model that explicitly tracks the partitioning and aging of low-volatility organics was compared to the chamber data. The OA production can be explained by the oxidation of low-volatility organic vapors; the model can also reproduce observed changes in OA volatility and composition. The model was used to investigate the competition between photochemical processing and dilution on OA concentrations in plumes.
