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The impact of different boundary layer source regions in Asia on the chemical composition of the Asian monsoon anticyclone, considering its intraseasonal variability in 2012, is analysed by simulations of the Chemical Lagrangian Model of the Stratosphere (CLaMS) using artificial emission tracers. The horizontal distribution of simulated CO, O3, and artificial emission tracers for India/China are in good agreement with patterns found in satellite measurements of O3 and CO by the Aura Microwave Limb Sounder (MLS). Using in addition, correlations of artificial emission tracers with potential vorticity demonstrates that the emission tracer for India/China is a very good proxy for spatial distribution of trace gases within the Asian monsoon anticyclone. The Asian monsoon anticyclone constitutes a horizontal transport barrier for emission tracers and is highly variable in location and shape. From the end of June to early August, a northward movement of the anticyclone and, during September, a strong broadening of the spatial distribution of the emission tracer for India/China towards the tropics are found. In addition to the change of the location of the anticyclone, the contribution of different boundary source regions to the composition of the Asian monsoon anticyclone in the upper troposphere strongly depends on its intraseasonal variability and is therefore more complex than hitherto believed. The largest contributions to the composition of the air mass in the anticyclone are found from northern India and Southeast Asia at a potential temperature of 380 K. In the early (mid-June to mid-July) and late (September) period of the 2012 monsoon season, contributions of emissions from Southeast Asia are highest; in the intervening period (early August), emissions from northern India have the largest impact. Our findings show that the temporal variation of the contribution of different convective regions is imprinted in the chemical composition of the Asian monsoon anticyclone. Air masses originating in Southeast Asia are found both within and outside of the Asian monsoon anticyclone because these air masses experience, in addition to transport within the anticyclone, upward transport at the southeastern flank of the anticyclone and in the tropics. Subsequently, isentropic poleward transport of these air masses occurs at around 380 K with the result that the extratropical lowermost stratosphere in the Northern Hemisphere is flooded by the end of September with air masses originating in Southeast Asia. Even after the breakup of the anticyclonic circulation (around the end of September), significant contributions of air masses originating in India/China are still found in the upper troposphere over Asia. Our results demonstrate that emissions from India, China, and Southeast Asia have a significant impact on the chemical composition of the lowermost stratosphere of the Northern Hemisphere, in particular at the end of the monsoon season in September/October 2012.

The Asian summer monsoon provides an important pathway of tropospheric source gases and pollution into the lower stratosphere. This transport is characterized by deep convection and steady upwelling, combined with confinement inside a large-scale anticyclonic circulation in the upper troposphere and lower stratosphere (UTLS). In this paper, we show that a barrier to horizontal transport along the 380 K isentrope in the monsoon anticyclone can be determined from a local maximum in the gradient of potential vorticity (PV), following methods developed for the polar vortex (e.g., Nash et al., 1996). The monsoon anticyclone is dynamically highly variable and the maximum in the PV gradient is weak, such that additional constraints are needed (e.g., time averaging). Nevertheless, PV contours in the monsoon anticyclone agree well with contours of trace gas mixing ratios (CO, O3) and mean age from model simulations with a Lagrangian chemistry transport model (CLaMS) and satellite observations from the Microwave Limb Sounder (MLS) instrument. Hence, the PV-based transport barrier reflects the separation between air inside the core of the anticyclone and the background atmosphere well. For the summer season 2011 we find an average PV value of 3.6 PVU for the transport barrier in the anticyclone on the 380 K isentrope.

We present the first stage of a new online-coupled global to regional-scale modeling framework for the simulation of the spatiotemporal evolution of aerosols and trace gases. The underlying meteorological model is the new nonhydrostatic model system ICON (ICOsahedral Nonhydrostatic) which allows a local grid refinement with two-way interactions between the grids. We develop the extension ART (Aerosol and Reactive Trace gases) with the goal of simulating interactions between trace substances and the state of the atmosphere. Within this paper, we present the basic equations and give an overview of the physical parameterizations as well as numerical methods we use. First applications of the new model system for trace gases, monodisperse particles and polydisperse particles are shown. The simulated distribution of two very short-lived substances (VSLS), bromoform (CHBr3) and dibromomethane (CH2Br2) reflecting the fast upward transport shows a good agreement with observations and previous model studies. Also, the shape of the simulated tropical profiles is well reproduced. As an example for the treatment of monodisperse particles we present the simulated ash plume of the Eyjafjallajökull eruption in April 2010. Here, a novel approach for the source function is applied. The pattern of the simulated distribution of volcanic ash particles shows a good agreement with previous studies. As an example for the treatment of a polydisperse aerosol, where number densities and mass concentrations are accounted for, we simulated the annual emissions of sea salt. We obtain a total emission flux of 26.0 Pg yr−1 and an emission flux of particles with diameter less than 10 μm of 7.36 Pg yr−1.

The three-dimensional quantification of small-scale processes in the upper troposphere and lower stratosphere is one of the challenges of current atmospheric research and requires the development of new measurement strategies. This work presents the first results from the newly developed Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) obtained during the ESSenCe (ESa Sounder Campaign) and TACTS/ESMVal (TACTS: Transport and composition in the upper troposphere/lowermost stratosphere, ESMVal: Earth System Model Validation) aircraft campaigns. The focus of this work is on the so-called dynamics-mode data characterized by a medium-spectral and a very-high-spatial resolution. The retrieval strategy for the derivation of two- and three-dimensional constituent fields in the upper troposphere and lower stratosphere is presented. Uncertainties of the main retrieval targets (temperature, O3, HNO3, and CFC-12) and their spatial resolution are discussed. During ESSenCe, high-resolution two-dimensional cross-sections have been obtained. Comparisons to collocated remote-sensing and in situ data indicate a good agreement between the data sets. During TACTS/ESMVal, a tomographic flight pattern to sense an intrusion of stratospheric air deep into the troposphere was performed. It was possible to reconstruct this filament at an unprecedented spatial resolution of better than 500 m vertically and 20 × 20 km horizontally.

Variations in the mixing ratio of trace gases of tropospheric origin entering the stratosphere in the tropics are of interest for assessing both troposphere to stratosphere transport fluxes in the tropics and the impact of these transport fluxes on the composition of the tropical lower stratosphere. Anomaly patterns of carbon monoxide (CO) and long-lived tracers in the lower tropical stratosphere allow conclusions about the rate and the variability of tropical upwelling to be drawn. Here, we present a simplified chemistry scheme for the Chemical Lagrangian Model of the Stratosphere (CLaMS) for the simulation, at comparatively low numerical cost, of CO, ozone, and long-lived trace substances (CH4, N2O, CCl3F (CFC-11), CCl2F2 (CFC-12), and CO2) in the lower tropical stratosphere. For the long-lived trace substances, the boundary conditions at the surface are prescribed based on ground-based measurements in the lowest model level. The boundary condition for CO in the lower troposphere (below about 4 km) is deduced from MOPITT measurements. Due to the lack of a specific representation of mixing and convective uplift in the troposphere in this model version, enhanced CO values, in particular those resulting from convective outflow are underestimated. However, in the tropical tropopause layer and the lower tropical stratosphere, there is relatively good agreement of simulated CO with in situ measurements (with the exception of the TROCCINOX campaign, where CO in the simulation is biased low ≈10–15 ppbv). Further, the model results (and therefore also the ERA-Interim winds, on which the transport in the model is based) are of sufficient quality to describe large scale anomaly patterns of CO in the lower stratosphere. In particular, the zonally averaged tropical CO anomaly patterns (the so called "tape recorder" patterns) simulated by this model version of CLaMS are in good agreement with observations, although the simulations show a too rapid upwelling compared to observations as a consequence of the overestimated vertical velocities in the ERA-Interim reanalysis data set. Moreover, the simulated tropical anomaly patterns of N2O are in good agreement with observations. In the simulations, anomaly patterns of CH4 and CFC-11 were found to be very similar to those of N2O; for all long-lived tracers, positive anomalies are simulated because of the enhanced tropical upwelling in the easterly shear phase of the quasi-biennial oscillation.

Enhanced tropospheric trace gases such as CO, CH4 and H2O and reduced stratospheric O3 were measured in situ in the lowermost stratosphere over northern Europe on 26 September 2012 during the TACTS aircraft campaign. The measurements indicate that these air masses clearly differ from the stratospheric background. The calculation of 40-day backward trajectories with the trajectory module of the CLaMS model shows that these air masses are affected by the Asian monsoon anticyclone. Some air masses originate from the boundary layer in Southeast Asia/West Pacific and are rapidly lifted (1–2 days) within a typhoon up to the outer edge of the Asian monsoon anticyclone. Afterwards, the air parcels are entrained by the anticyclonic circulation of the Asian monsoon. The subsequent long-range transport (8–14 days) of enhanced water vapour and pollutants to the lowermost stratosphere in northern Europe is driven by eastward transport of tropospheric air from the Asian monsoon anticyclone caused by an eddy shedding event. We found that the combination of rapid uplift by a typhoon and eastward eddy shedding from the Asian monsoon anticyclone is a novel fast transport pathway that may carry boundary emissions from Southeast Asia/West Pacific within approximately 5 weeks to the lowermost stratosphere in northern Europe.

In situ measurements with a four-channel stratospheric condensation particle counter (CPC) were conducted at up to 20 km altitude on board the aircraft M-55 Geophysica from Kiruna, Sweden, in January through March (EUPLEX 2003, RECONCILE 2010) and in December (ESSenCe 2011). During all campaigns air masses from the upper stratosphere and mesosphere were subsiding inside the Arctic winter vortex, thus initializing a transport of refractory aerosol into the lower stratosphere (Θ < 500 K). The strength and extent of this downward transport varied between the years depending on the dynamical evolution of the vortex. Inside the vortex and at potential temperatures Θ ≥ 450 K around 11 submicron particles per cm3 were generally detected. Up to 8 of these 11 particles per cm3 were found to contain thermo-stable (at 250 °C) residuals with diameters of 10 nm to about 1 μm. Particle mixing ratios (150 mg−1) and fractions of non-volatile particles (75% of totally detected particles) exhibited highest values in air masses having the lowest content of nitrous oxide (70 nmol mol−1 of N2O). This indicates that refractory aerosol originates from the upper stratosphere or the mesosphere. Derived from the mixing ratio of the simultaneously measured long-lived tracer N2O, an empirical index serves to differentiate probed air masses according to their origin: inside the vortex, the vortex edge region, or outside the vortex. Previously observed high fractions of refractory submicron aerosol in the 2003 Arctic vortex were ascribed to unusually strong subsidence during that winter. However, measurements under perturbed vortex conditions in 2010 and during early winter in December 2011 revealed similarly high values. Thus, the abundance of refractory aerosol in the lower stratosphere within the Arctic vortices appears to be a regular feature rather than the exception. During December, the import from aloft into the lower stratosphere appears to be developing; thereafter the abundance of refractory aerosol inside the vortex reaches its highest levels in March. The correlations of refractory aerosol with N2O suggest that, apart from mean subsidence, diabatic dispersion inside the vortex significantly contributes to the transport of particles to the Arctic lower stratosphere. A measurement-based estimate of the total mass of refractory aerosol inside the vortex is provided for each campaign. Based on the derived increase of particle mass in the lower stratospheric vortex (100–67 hPa pressure altitude) by a factor of 4.5 between early and late winter, we estimate the total mass of mesospheric particles deposited over the winter 2009/2010 in the entire Arctic vortex to range between 77 × 103 and 375 × 106 kg. This estimate is compared with the expected atmospheric influx of meteoritic material (110 ± 55 × 103 kg per day). Such estimates at present still hold considerable uncertainties, which are discussed in this article. Nevertheless, the results enable placing constraints on the shape of the so far unknown size distribution of refractory aerosol within the vortex.

In January 2010 and December 2011, synoptic-scale polar stratospheric cloud (PSC) fields were probed during seven flights of the high-altitude research aircraft M-55 Geophysica within the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interaction) and the ESSenCe (ESSenCe: ESA Sounder Campaign) projects. Particle size distributions in a diameter range between 0.46 and 40μm were recorded by four different optical in situ instruments. Three of these particle instruments are based on the detection of forward-scattered light by single particles. The fourth instrument is a grayscale optical array imaging probe. Optical particle diameters of up to 35μm were detected with particle number densities and total particle volumes exceeding previous Arctic measurements. Also, gas-phase and particle-bound NOy was measured, as well as water vapor concentrations. The optical characteristics of the clouds were measured by the remote sensing lidar MAL (Miniature Aerosol Lidar) and by the in situ backscatter sonde MAS (Multiwavelength Aerosol Scatterometer), showing the synoptic scale of the encountered PSCs. The particle mode below 2μm in size diameter has been identified as supercooled ternary solution (STS) droplets. The PSC particles in the size range above 2μm in diameter are considered to consist of nitric acid hydrates, and the particles' high HNO3 content was confirmed by the NOy instrument. Assuming a particle composition of nitric acid trihydrate (NAT), the optically measured size distributions result in particle-phase HNO3 mixing ratios exceeding available stratospheric values. Therefore the measurement uncertainties concerning probable overestimations of measured particle sizes and volumes are discussed in detail. We hypothesize that either a strong asphericity or an alternate particle composition (e.g., water ice coated with NAT) could explain our observations. In particular, with respect to the denitrification by sedimentation of large HNO3-containing particles, generally considered to be NAT, our new measurements raise questions concerning composition, shape and nucleation pathways. Answering these would improve the numerical simulation of PSC microphysical processes like cloud particle formation, growth and denitrification, which is necessary for better predictions of future polar ozone losses, especially under changing global climate conditions. Generally, it seems that the occurrence of large NAT particles – sometimes termed "NAT rocks" – are a regular feature of synoptic-scale PSCs in the Arctic.

An extended version of the German operational weather forecast model was used to simulate the ash dispersion during the eruption of the Eyjafjallajökull. As an operational forecast was launched every 6 hours, a time-lagged ensemble was obtained. Sensitivity runs show the ability of the model to simulate thin ash layers when an increased vertical resolution is used. Calibration of the model results with measured data allows for a quantitative forecast of the ash concentration. After this calibration an independent comparison of the simulated number concentration of 3 μm particles and observations at Hohenpeißenberg gives a correlation coefficient of 0.79. However, this agreement could only be reached after additional modifications of the emissions. Based on the time lagged ensemble the conditional probability of violation of a certain threshold is calculated. Improving the ensemble technique used in our study such probabilities could become valuable information for the forecasters advising the organizations responsible for the closing of the airspace.

The upper troposphere/lower stratosphere (UTLS) represents an important part of the climate system. Even small changes in the composition and dynamic structure of this region have significant radiative effects. Quantifying the underlying physical and chemical processes therefore represents a crucial task. Currently, there is a lack of UTLS observations with sufficient three-dimensional resolution. The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) aircraft instrument addresses this observational lack by providing observations of numerous trace constituents as well as temperature and cloud structures with an unprecedented combination of vertical resolution (up to 300 m) and horizontal resolution (about 30 km &times 30 km). As a result, important scientific questions concerning stratosphere–troposphere exchange, the occurrence of subvisible cirrus clouds in the lowermost stratosphere (LMS), polar chemistry, and gravity wave processes can be addressed, as reviewed in this paper.

Online coupled mesoscale meteorology atmospheric chemistry models have undergone a rapid evolution in recent years. Although mainly developed by the air quality modelling community, these models are also of interest for numerical weather prediction and regional climate modelling as they can consider not only the effects of meteorology on air quality, but also the potentially important effects of atmospheric composition on weather. Two ways of online coupling can be distinguished: online integrated and online access coupling. Online integrated models simulate meteorology and chemistry over the same grid in one model using one main time step for integration. Online access models use independent meteorology and chemistry modules that might even have different grids, but exchange meteorology and chemistry data on a regular and frequent basis. This article offers a comprehensive review of the current research status of online coupled meteorology and atmospheric chemistry modelling within Europe. Eighteen regional online coupled models developed or being used in Europe are described and compared. Topics discussed include a survey of processes relevant to the interactions between atmospheric physics, dynamics and composition; a brief overview of existing online mesoscale models and European model developments; an analysis on how feedback processes are treated in these models; numerical issues associated with coupled models; and several case studies and model performance evaluation methods. Finally, this article highlights selected scientific issues and emerging challenges that require proper consideration to improve the reliability and usability of these models for the three scientific communities: air quality, numerical meteorology modelling (including weather prediction) and climate modelling. This review will be of particular interest to model developers and users in all three fields as it presents a synthesis of scientific progress and provides recommendations for future research directions and priorities in the development, application and evaluation of online coupled models.

A volatility basis set (VBS) approach for the simulation of secondary organic aerosol (SOA) formation is incorporated in the online coupled atmospheric model system COSMO-ART and applied over Europe during the EUCAARI May 2008 campaign. Organic aerosol performance is improved when compared to the default SOA module of COSMO-ART (SORGAM) against high temporal resolution aerosol mass spectrometer ground measurements. The impact of SOA on the overall radiative budget was investigated. The mean direct surface radiative cooling averaged over Europe is −1.2 W m−2, representing approximately 20% of the total effect of aerosols on the radiative budget. However, responses are not spatially correlated with the radiative forcing, due to the nonlinear interactions among changes in particle chemical composition, water content, size distribution and cloud cover. These interactions initiated~by the effect of SOA on radiation are found to result even in a positive forcing in specific areas. Further model experiments showed that the availability of nitrogen oxides slightly affects SOA production, but that the aging rate constant used in the VBS approximation and boundary concentrations assumed in the model should be carefully selected. The aging of SOA is found to reduce hourly nitrate levels by up to 30%, while the condensation of inorganic species upon pre-existing, SOA-rich particles results in a monthly average increase of 5% in sulfate and ammonium formation in the accumulation mode.

We investigated the impact of mineral dust particles on clouds, radiation and atmospheric state during a strong Saharan dust event over Europe in May 2008, applying a comprehensive online-coupled regional model framework that explicitly treats particle microphysics and chemical composition. Sophisticated parameterizations for aerosol activation and ice nucleation, together with two-moment cloud microphysics are used to calculate the interaction of the different particles with clouds depending on their physical and chemical properties. The impact of dust on cloud droplet number concentration was found to be low, with just a slight increase in cloud droplet number concentration for both uncoated and coated dust. For temperatures lower than the level of homogeneous freezing, no significant impact of dust on the number and mass concentration of ice crystals was found, though the concentration of frozen dust particles reached up to 100 l−1 during the ice nucleation events. Mineral dust particles were found to have the largest impact on clouds in a temperature range between freezing level and the level of homogeneous freezing, where they determined the number concentration of ice crystals due to efficient heterogeneous freezing of the dust particles and modified the glaciation of mixed phase clouds. Our simulations show that during the dust events, ice crystals concentrations were increased twofold in this temperature range (compared to if dust interactions are neglected). This had a significant impact on the cloud optical properties, causing a reduction in the incoming short-wave radiation at the surface up to −75 W m−2. Including the direct interaction of dust with radiation caused an additional reduction in the incoming short-wave radiation by 40 to 80 W m−2, and the incoming long-wave radiation at the surface was increased significantly in the order of +10 W m−2. The strong radiative forcings associated with dust caused a reduction in surface temperature in the order of −0.2 to −0.5 K for most parts of France, Germany, and Italy during the dust event. The maximum difference in surface temperature was found in the East of France, the Benelux, and Western Germany with up to −1 K. This magnitude of temperature change was sufficient to explain a systematic bias in numerical weather forecasts during the period of the dust event.

The online-coupled, regional chemistry transport model COSMO-ART is evaluated for periods in all seasons against several measurement datasets to assess its ability to represent gaseous pollutants and ambient aerosol characteristics over the European domain. Measurements used in the comparison include long-term station observations, satellite and ground-based remote sensing products, and complex datasets of aerosol chemical composition and number size distribution from recent field campaigns. This is the first time these comprehensive measurements of aerosol characteristics in Europe are used to evaluate a regional chemistry transport model. We show a detailed analysis of the simulated size-resolved chemical composition under different meteorological conditions. Mean, variability and spatial distribution of the concentrations of O3 and NOx are well reproduced. SO2 is found to be overestimated, simulated PM2.5 and PM10 levels are on average underestimated, as is AOD. We find indications of an overestimation of shipping emissions. Time evolution of aerosol chemical composition is captured, although some biases are found in relative composition. Nitrate aerosol components are on average overestimated, and sulfates underestimated. The accuracy of simulated organics depends strongly on season and location. While strongly underestimated during summer, organic mass is comparable in spring and autumn. We see indications for an overestimated fractional contribution of primary organic matter in urban areas and an underestimation of SOA at many locations. Aerosol number concentrations compare well with measurements for larger size ranges, but overestimations of particle number concentration with factors of 2–5 are found for particles smaller than 50 nm. Size distribution characteristics are often close to measurements, but show discrepancies at polluted sites. Suggestions for further improvement of the modeling system consist of the inclusion of a revised secondary organic aerosols scheme, aqueous-phase chemistry and improved aerosol boundary conditions. Our work sets the basis for subsequent studies of aerosol characteristics and climate impacts with COSMO-ART, and highlights areas where improvements are necessary for current regional modeling systems in general.

To cope with the world's growing demand for energy, a large number of coal-fired power plants are currently in operation or under construction. To prevent environmental damage from acidic sulphur and particulate emissions, many such installations are equipped with flue gas cleaning technology that reduces the emitted amounts of sulphur dioxide (SO2) and nitrogen dioxide (NO2). However, the consequences of this technology for aerosol emissions, and in particular the regional scale impact on cloud microphysics, have not been studied until now. We performed airborne investigations to measure aerosol size distributions in the air masses downwind of coal-fired power installations. We show how the current generation of clean technology reduces the emission of sulphur and fine particulate matter, but leads to an unanticipated increase in the direct emission of ultrafine particles (1–10 nm median diameter) which are highly effective precursors of cloud condensation nuclei (CCN). Our analysis shows how these additional ultrafine particles probably modify cloud microphysics, as well as precipitation intensity and distribution on a regional scale downwind of emission sources. Effectively, the number of small water droplets might be increased, thus reducing the water available for large droplets and rain formation. The possible corresponding changes in the precipitation budget with a shift from more frequent steady rain to occasionally more vigorous rain events, or even a significant regional reduction of annual precipitation, introduce an unanticipated risk for regional climate and agricultural production, especially in semi-arid climate zones.

We have extended the coupled mesoscale atmosphere and chemistry model COSMO-ART to account for the transformation of aerosol particles into cloud condensation nuclei and to quantify their interaction with warm cloud microphysics on the regional scale. The new model system aims to fill the gap between cloud resolving models and global scale models. It represents the very complex microscale aerosol and cloud physics as detailed as possible, whereas the continental domain size and efficient codes will allow for both studying weather and regional climate. The model system is applied in a first extended case study for Europe for a cloudy five day period in August 2005. The model results show that the mean cloud droplet number concentration of clouds is correlated with the structure of the terrain, and we present a terrain slope parameter TS to classify this dependency. We propose to use this relationship to parameterize the probability density function, PDF, of subgrid-scale cloud updraft velocity in the activation parameterizations of climate models. The simulations show that the presence of cloud condensation nuclei (CCN) and clouds are closely related spatially. We find high aerosol and CCN number concentrations in the vicinity of clouds at high altitudes. The nucleation of secondary particles is enhanced above the clouds. This is caused by an efficient formation of gaseous aerosol precursors above the cloud due to more available radiation, transport of gases in clean air above the cloud, and humid conditions. Therefore the treatment of complex photochemistry is crucial in atmospheric models to simulate the distribution of CCN. The mean cloud droplet number concentration and droplet diameter showed a close link to the change in the aerosol. To quantify the net impact of an aerosol change on the precipitation we calculated the precipitation susceptibility β for the whole model domain over a period of two days with an hourly resolution. The distribution function of β is slightly skewed to positive values and has a mean of 0.23. Clouds with a liquid water path LWP of approximately 0.85 kg m−2 are on average most susceptible to aerosol changes in our simulations with an absolute value of β of 1. The average β for LWP between 0.5 kg m−2 and 1 kg m−2 is approximately 0.4.

For the past 200 years, the field of aerobiology has explored the abundance, diversity, survival and transport of micro-organisms in the atmosphere. Micro-organisms have been explored as passive and severely stressed riders of atmospheric transport systems. Recently, an interest in the active roles of these micro-organisms has emerged along with proposals that the atmosphere is a global biome for microbial metabolic activity and perhaps even multiplication. As part of a series of papers on the sources, distribution and roles in atmospheric processes of biological particles in the atmosphere, here we describe the pertinence of questions relating to the potential roles that air-borne micro-organisms might play in meteorological phenomena. For the upcoming era of research on the role of air-borne micro-organisms in meteorological phenomena, one important challenge is to go beyond descriptions of abundance of micro-organisms in the atmosphere toward an understanding of their dynamics in terms of both biological and physico-chemical properties and of the relevant transport processes at different scales. Another challenge is to develop this understanding under contexts pertinent to their potential role in processes related to atmospheric chemistry, the formation of clouds, precipitation and radiative forcing. This will require truly interdisciplinary approaches involving collaborators from the biological and physical sciences, from disciplines as disparate as agronomy, microbial genetics and atmosphere physics, for example.

We used the comprehensive model system COSMO-ART to quantify the impact of mineral dust on the radiative fluxes, the temperature and the feedback between dust particles and their emissions. We simulated two dust storms over West Africa in March 2006 and in June 2007. Simulations with and without coupling of the actual dust concentration with the radiative fluxes and the thermodynamics were carried out for each case. The model results for the 2006 case were compared with observations of the AMMA campaign. At the surface the shortwave radiative effect of mineral dust can be described by a linear relation between the changes in net surface radiation and the aerosol optical depth (AOD). For an AOD at 450 nm of 1 the average shortwave radiation reduction amounts −140 W m−2 during noon. The longwave radiative effect of mineral dust is nonlinear, with an average increase of +70 W m−2 for an AOD (450 nm) of 1. At the top of the atmosphere the effect of the dust layer with an AOD of 1 on radiative fluxes is not as significant as at the surface. It is slightly positive for the shortwave and approximately 26 W m−2 for the longwave radiation. The height range and the extension of the dust layer determine the effect of dust particles on the 2 m temperature. When the dust layer is attached to the surface and lasts for several days it leads to an increase of the surface temperature even during daytime. In case of an elevated dust layer there is a decrease in 2 m temperature of up to 4 K during noon. It is shown, that the temperature changes caused by mineral dust may result in horizontal temperature gradients which also modify near surface winds. Since surface wind thresholds decide the uptake of dust from the surface, a feedback on total emission fluxes is established. The coupled model provides an increase in the total emission fluxes of dust particles by about 16% during the dust storm in March 2006 and 25% during the dust episode in June 2007.

A new fully online coupled model system developed for the evaluation of the interaction of aerosol particles with the atmosphere on the regional scale is described. The model system is based on the operational weather forecast model of the Deutscher Wetterdienst. Physical processes like transport, turbulent diffusion, and dry and wet deposition are treated together with photochemistry and aerosol dynamics using the modal approach. Based on detailed calculations we have developed parameterisations to examine the impact of aerosol particles on photolysis and on radiation. Currently the model allows feedback between natural and anthropogenic aerosol particles and the atmospheric variables that are initialized by the modification of the radiative fluxes. The model system is applied to two summer episodes, each lasting five days, with a model domain covering Western Europe and adjacent regions. The first episode is characterised by almost cloud free conditions and the second one by cloudy conditions. The simulated aerosol concentrations are compared to observations made at 700 stations distributed over Western Europe. For each episode two model runs are performed; one where the feedback between the aerosol particles and the atmosphere is taken into account and a second one where the feedback is neglected. Comparing these two sets of model runs, the radiative feedback on temperature and other variables is evaluated. In the cloud free case a clear correlation between the aerosol optical depth and changes in global radiation and temperature is found. In the case of cloudy conditions the pure radiative effects are superposed by changes in the liquid water content of the clouds due to changes in the thermodynamics of the atmosphere. In this case the correlation between the aerosol optical depth and its effects on temperature is low. However, on average a decrease in the 2 m temperature is still found. For the area of Germany we found on average for both cases a reduction in the global radiation of about 6 W m2, a decrease of the 2 m temperature of 0.1 K, and a reduction in the daily temperature range of −0.13 K.

Satellite observations show that the enormous solar proton events (SPEs) in October–November 2003 had significant effects on the composition of the stratosphere and mesosphere in the polar regions. After the October–November 2003 SPEs and in early 2004, significant enhancements of NOx(=NO+NO2) in the upper stratosphere and lower mesosphere in the Northern Hemisphere were observed by several satellite instruments. Here we present global full chemistry calculations performed with the CLaMS model to study the impact of mesospheric NOx intrusions on Arctic polar ozone loss processes in the stratosphere. Several model simulations are preformed with different upper boundary conditions for NOx at 2000 K potential temperature (≈50 km altitude). In our study we focus on the impact of the non-local production of NOx, which means the downward transport of enhanced NOx from the mesosphere to the stratosphere. The local production of NOx in the stratosphere is neglected. Our findings show that intrusions of mesospheric air into the stratosphere, transporting high burdens of NOx, affect the composition of the Arctic polar region down to about 400 K (≈17–18 km). We compare our simulated NOx and O3 mixing ratios with satellite observations by ACE-FTS and MIPAS processed at IMK/IAA and derive an upper limit for the ozone loss caused by enhanced mesospheric NOx. Our findings show that in the Arctic polar vortex (equivalent lat.>70° N) the accumulated column ozone loss between 350–2000 K potential temperature (≈14–50 km altitude) caused by the SPEs in October–November 2003 in the stratosphere is up to 3.3 DU with an upper limit of 5.5 DU until end of November. Further, we found that about 10 DU, but in any case lower than 18 DU, accumulated ozone loss additionally occurred until end of March 2004 caused by the transport of mesospheric NOx-rich air in early 2004. The solar-proton-produced NOx above 55 km due to the SPEs of October–November 2003 had a negligibly small impact on ozone loss processes through the end of November in the lower stratosphere (350–700 K≈14–27 km). The mesospheric NOx intrusions in early 2004 yielded a lower stratospheric ozone loss of about 3.5 DU, and clearly lower than 6.5 DU through the end of March. Overall, the non-local production of NOx is an additional variability in the existing variations of the ozone loss observed in the Arctic.

Statistical analyses of data from ground-based sun photometer stations in Central Europe are presented. All stations are part of the Aerosol Robotic Network (AERONET), and only data of the highest data quality level 2.0 has been applied. The averages by weekday of Aerosol Optical Thickness (AOT) at a wavelength of 440 nm of 12 of the 14 stations in the investigation area show a weekly periodicity with lowest values on Sunday and Monday, but greatest values from Wednesday until Saturday, that is significant at least on a 90% level. The stations in Germany and in Greater Paris show weekly cycles with ranges of about 20% on average. In Northern Italy and Switzerland this range is about 10% on average. By applying several checks, we exclude that the weekly cycles were caused by a maintenance effect or by different retrieval conditions as a consequence of a weekly cycle in cloud cover. The corresponding weekly cycle of anthropogenic gaseous and particulate emissions leads us to the conclusion of the anthropogenic origin of the weekly AOT cycle. Since these AOT patterns are derived from the reduction of the direct sun radiation by the columnar atmospheric aerosol, this result represents strong evidence for an anthropogenic direct aerosol effect on shortwave radiation. Furthermore, this study makes a first contribution to the understanding and explanation of recently observed weekly periodicities in meteorological variables as temperature in Germany.

The importance of radical-molecule complexes for atmospheric chemistry has been discussed in recent years. In particular, the existence of a ClO·O2 and ClOx water radical complexes like ClO·H2O, OClO·H2O, OClO·(H2O)2, and ClOO·H2O could play a role in enhancing the ClO dimer (Cl2O2) formation and therefore may constitute an important intermediate in polar stratospheric ozone loss cycles. Model simulations performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS) will be presented to study the role of radical complexes on polar stratospheric ozone loss processes. The model simulations are performed for the Arctic winter 2002/2003 at a level of 500 K potential temperature and the results are compared to observed ozone loss rates determined by the Match technique. Moreover, recently reported values for the equilibrium constant of the ClO dimer formation are used to restrict the number of possible model results caused by large uncertainties about radical complex chemistry. Our model simulations show that the potential impact of ClO·O2 on polar ozone loss processes is small (dO3/dt≪0.5 ppb/sunlight h) provided that the ClO·O2 complex is only weakly stable. Assuming that the binding energies of the ClOx water complexes are much higher than theoretically predicted an enhancement of the ozone loss rate by up to ≈0.5 ppb/sunlight h is simulated. Because it is unlikely that the ClOx water complexes are much more stable than predicted we conclude that these complexes have no impact on polar stratospheric ozone loss processes. Although large uncertainties about radical complex chemistry exist, our findings show that the potential impact of ClOx radical molecule complexes on polar stratospheric ozone loss processes is very small considering pure gas-phase chemistry. However the existence of ClOx radical-molecule complexes could possibly explain discrepancies for the equilibrium constant of the ClO dimer formation found between recent laboratory and stratospheric measurements.

Chlorine monoxide (ClO) plays a key role in stratospheric ozone loss processes at midlatitudes. We present two balloon-borne in situ measurements of ClO conducted in northern hemisphere midlatitudes during the period of the maximum of total inorganic chlorine loading in the atmosphere. Both ClO measurements were conducted on board the TRIPLE balloon payload, launched in November 1996 in León, Spain, and in May 1999 in Aire sur l'Adour, France. For both flights a ClO daylight and night-time vertical profile was derived over an altitude range of approximately 15-35 km. ClO mixing ratios are compared to model simulations performed with the photochemical box model version of the Chemical Lagrangian Model of the Stratosphere (CLaMS). Simulations along 24-hour backward trajectories were performed to study the diurnal variation of ClO in the midlatitude lower stratosphere. Model simulations for the flight launched in Aire sur l'Adour 1999 show an excellent agreement with the ClO measurements. For the flight launched in León 1996, an overall good agreement is found, whereas the flight is characterized by a more complex dynamical situation due to a possible mixture of vortex and non-vortex air. We note that for both flights at solar zenith angles greater than 86°-87° simulated ClO mixing ratios are higher than observed ClO mixing ratios. However, the present findings indicate that no substantial uncertainties exist in midlatitude chlorine chemistry of the stratosphere.

The aging of soot is one of the key uncertainties in the estimation of both the direct and indirect climate effect. While freshly emitted soot is initially hydrophobic and externally mixed, it can be transferred into an internal mixture by coagulation, condensation or photochemical processes. These aging processes affect the hygroscopic qualities and hence the growth behaviour, the optical properties and eventually the lifetime of the soot particles. However, due to computational limits the aging of soot in global climate models is often only parameterised by an estimated turnover rate resulting in a lifetime of soot of several days. Hence, the aging process of soot is one of the key uncertainties governing the burden and effect of black carbon. In this study, we discuss the time scale on which diesel soot is transferred from an external to an internal mixture based on the results of our simulations with a comprehensive mesoscale model. For daytime conditions during summer condensation of sulphuric acid is dominant and the aging process occurs on a time scale of τ =8h close to the sources and τ =2h above the source region. During winter comparable time scales are found but ammonium nitrate becomes more important. During night time condensation is not effective. Then coagulation is the most important aging process and our results show time scales between 10h and 40h.