Antarctic ice cores preserve the record of past aerosols, an important proxy of past atmospheric chemistry. Here we present the aerosol compositions of sulphate and chloride particles in the Talos Dome (TD) ice core from the Holocene and Last Glacial Period. We find that the main salt types of both periods are NaCl, Na2SO4 and CaSO4, indicating that TD ice contains relatively abundant sea salt (NaCl) from marine primary particles. By evaluating the molar ratio of NaCl to Na2SO4, we show that about half of the sea salt does not undergo sulphatisation during late Holocene. Compared to in inland Antarctica, the lower sulphatisation rate at TD is probably due to relatively little contact between sea salt and sulphuric acid. This low contact rate can be related to a reduced time of reaction for marine-sourced aerosol before reaching TD and/or to a reduced post-depositional effect from the higher accumulation rate at TD. Many sulphate and chloride salts are adhered to silicate minerals. The ratio of sulphate-adhered mineral to particle mass and the corresponding ratio of chloride-adhered mineral both increase with increasing dust concentration. Also, the TD ice appears to contain Ca(NO3)(2) or CaCO3 particles, thus differing from aerosol compositions in inland Antarctica, and indicating the proximity of peripheral regions to marine aerosols. / <p>AuthorCount:9;</p>

This research focuses on aircraft observational studies of aerosol-cloud interactions in cumulus clouds. The data were collected in the summer of 2004, the spring of 2007 and the mid-winter and spring of 2008 in Texas, central Saudi Arabia and Istanbul, Turkey, respectively. A set of 24 pairs of sub-cloud aerosol and cloud penetration data are analyzed. Measurements of fine and coarse mode aerosol concentrations from 3 different instruments were combined and fitted with lognormal distributions. The fit parameters of the lognormal distributions are compared with cloud droplet effective radii retrieved from 260 cloud penetrations. Cloud condensation nuclei (CCN) measurements for a subset of 10 cases from the Istanbul region are compared with concentrations predicted from aerosol size distributions. Ammonium sulfate was assumed to represent the soluble component of aerosol with dry sizes smaller than 0.5 mm and sodium chloride for aerosol larger than 0.5 mm. The measured CCN spectrum was used to estimate the soluble fraction. The correlations of the measured CCN concentration with the predicted CCN concentration were strong (R2 > 0.89) for supersaturations of 0.2, 0.3 and 0.6%. The measured concentrations were typically consistent with an aerosol having a soluble fraction between roughly 0.5 and 1.0, suggesting a contribution of sulfate or some other similarly soluble inorganic compound. The predicted CCN were found to vary by +or-3.7% when the soluble fraction was varied by 0.1. Cumulative aerosol concentrations at cutoff dry diameters of 1.1, 0.1 and 0.06 mm were found to be correlated with cloud condensation nuclei concentrations but not with maximum cloud base droplet concentrations. It is also shown that in some cases the predominant mechanisms involved in the formation of precipitation were altered and modified by the aerosol properties. This study suggests that CCN-forced variations in cloud droplet number concentration can change the effective radius profile and the type of precipitation hydrometeors. These differences may have a major impact on the global hydrological cycle and energy budget.

Ein mobiler Aerosolstandard für ultrafeine Partikel wurde als neue Möglichkeit zur Qualitätskontrolle für innovative Umweltmessungen in Luftgütemessnetzen entwickelt. Die Bestimmung der Anzahl ultrafeiner Partikel in Ergänzung zur Überwachung von Feinstaub PM10 oder PM2.5 eröffnet neue Möglichkeiten, die Luftqualität zukünftig besser beurteilen zu können. Ultrafeine Partikel sind ein zweckmäßiger Indikator, um z. B. die positive Wirkung einer Umweltzone in Luftreinhalteplänen nachzuweisen.

Convective and long-range transport of air mass controls the global distributions and impacts of the pollutants generated in limited source regions. However, an observational characterization of such transport based on long-term satellite data has been difficult in part because adequate satellite measurements were not available until recent years and lack of an automated method for identifying the transport pathways. My dissertation addresses this problem through three steps: First, I developed a method to automate the identification of two pathways that are responsible for the transport of biomass burning generated tracers from the surface to the upper troposphere (UT). I focused on carbon monoxide (CO) because it has a relatively long lifetime in the atmosphere, and thus it is commonly used as a tracer of convective and long-range mass transport. Next, I applied this method to investigate the relative importance of the two pathways in determining the seasonal pattern of UT CO distribution. Results show that the seasonality of CO concentrations in the tropical UT mainly reflects the seasonality of the “local convection” pathway, because the “local convection” pathway typically transports significantly more CO to the UT than the “advection within the lower troposphere followed by convective transport” pathway. Then, I investigated the impacts of transport pathways on the interannual variation of tropical UT CO concentration. Results show that the interannual variation of CO in the tropical UT is dominated by UT CO anomaly over Southeast Asia related to the El Niño-Southern Oscillation, and the average mass of CO transported per event of “local convection” is the factor that accounts for the UT CO difference between two El Niño periods. After that, I began to address the transport of more complex pollutants such as aerosols. First, the seasonal and diurnal variations of the vertical distributions of aerosol properties were characterized through a statistical analysis of aerosol profile data. Then, the transport pathways associated with the aerosol layer at the tropopause level over Asian area during boreal summer were investigated through back-trajectory model analyses. Three major pathways were found and the occurrence frequency of each pathway was analyzed and discussed. / text

The influence of anthropogenic emissions on aerosol distributions and the hydrological cycle are examined with a focus on monsoon precipitation over the Indian subcontinent, during January 2001 to December 2005, using the European Centre for Medium-Range Weather Forecasts-Hamburg (ECHAM5.5) general circulation model extended by the Hamburg Aerosol Module (HAM). The seasonal variability of aerosol optical depth (AOD) retrieved from the MODerate Resolution Imaging Spectroradiometer (MODIS) on board the Terra and Aqua satellite is broadly well simulated (R 0.6–0.85) by the model. The spatial distribution and seasonal cycle of the precipitation observed over the Indian region are reasonably well simulated (R 0.5 to 0.8) by the model, while in terms of absolute magnitude, the model underestimates precipitation, in particular in the south-west (SW) monsoon season. The model simulates significant anthropogenic aerosol-induced changes in clear-sky net surface solar radiation (dimming greater than -7 W m-2), which agrees well with the observed trends over the Indian region. A statistically significant decreasing precipitation trend is simulated only for the SWmonsoon season over the central-north Indian region, which is consistent with the observed seasonal trend over the Indian region. In the model, this decrease results from a reduction in convective precipitation, where there is an increase in stratiform cloud droplet number concentration (CDNC) and solar dimming that resulted from increased stability and reduced evaporation. Similarities in spatial patterns suggest that surface cooling, mainly by the aerosol indirect effect, is responsible for this reduction in convective activity. When changes in large-scale dynamics are allowed by slightly disturbing the initial state of the atmosphere, aerosol absorption in addition leads to a further stabilization of the lower troposphere, further reducing convective precipitation.

The Second Aerosol Characterization Experiment (ACE-2) data set along with ECMWF reanalysis meteorological fields provided the basis for the single column model (SCM) simulations, performed as part of the PACE (Parameterization of the Aerosol Indirect Climatic Effect) project. Six different SCMs were used to simulate ACE-2 case studies of clean and polluted cloudy boundary layers, with the objective being to identify limitations of the aerosol/cloud/radiation interaction schemes within the range of uncertainty in in situ, reanalysis and satellite retrieved data. The exercise proceeds in three steps. First, SCMs are configured with the same fine vertical resolution as the ACE-2 in situ data base to evaluate the numerical schemes for prediction of aerosol activation, radiative transfer and precipitation formation. Second, the same test is performed at the coarser vertical resolution of GCMs to evaluate its impact on the performance of the parameterizations. Finally, SCMs are run for a 24–48 hr period to examine predictions of boundary layer clouds when initialized with large-scale meteorological fields. Several schemes were tested for the prediction of cloud droplet number concentration (N). Physically based activation schemes using vertical velocity show noticeable discrepancies compared to empirical schemes due to biases in the diagnosed cloud base vertical velocity. Prognostic schemes exhibit a larger variability than the diagnostic ones, due to a coupling between aerosol activation and drizzle scavenging in the calculation of N. When SCMs are initialized at a fine vertical resolution with locally observed vertical profiles of liquid water, predicted optical properties are comparable to observations. Predictions however degrade at coarser vertical resolution and are more sensitive to the mean liquid water path than to its spatial heterogeneity. Predicted precipitation fluxes are severely underestimated and improve when accounting for sub-grid liquid water variability. Results from the 24–48 hr runs suggest that most models have problems in simulating boundary layer cloud morphology, since the large-scale initialization fields do not accurately reproduce observed meteorological conditions. As a result, models significantly overestimate optical properties. Improved cloud morphologies were obtained for models with subgrid inversions and subgrid cloud thickness schemes. This may be a result of representing subgrid scale effects though we do not rule out the possibility that better large-forcing data may also improve cloud morphology predictions.

In this paper we analyse aerosol loading and its direct radiative effects over the Bay of Bengal (BoB) and Arabian Sea (AS) regions for the Integrated Campaign on Aerosols, gases and Radiation Budget (ICARB) undertaken during 2006, using satellite data from the MODerate Resolution Imaging Spectroradiometer (MODIS) on board the Terra and Aqua satellites, the Aerosol Index from the Ozone Monitoring Instrument (OMI) on board the Aura satellite, and the European-Community Hamburg (ECHAM5.5) general circulation model extended by Hamburg Aerosol Module (HAM). By statistically comparing with large-scale satellite data sets, we firstly show that the aerosol properties measured during the ship-based ICARB campaign and simulated by the model are representative for the BoB and AS regions and the pre-monsoon season. In a second step, the modelled aerosol distributions were evaluated by a comparison with the measurements from the ship-based sunphotometer, and the satellite retrievals during ICARB. It is found that the model broadly reproduces the observed spatial and temporal variability in aerosol optical depth (AOD) over BoB and AS regions. However, AOD was systematically underestimated during high-pollution episodes, especially in the BoB leg. We show that this underprediction of AOD is mostly because of the deficiencies in the coarse mode, where the model shows that dust is the dominant component. The analysis of dust AOD along with the OMI Aerosol Index indicate that missing dust transport that results from too low dust emission fluxes over the Thar Desert region in the model caused this deficiency. Thirdly, we analysed the spatio-temporal variability of AOD comparing the ship-based observations to the large-scale satellite observations and simulations. It was found that most of the variability along the track was from geographical patterns, with a minor influence by single events. Aerosol fields were homogeneous enough to yield a good statistical agreement between satellite data at a 1° spatial, but only twice-daily temporal resolution, and the shipbased sunphotometer data at a much finer spatial, but dailyaverage temporal resolution. Examination of the satellite data further showed that the year 2006 is representative for the five-year period for which satellite data were available. Finally, we estimated the clear-sky solar direct aerosol radiative forcing (DARF). We found that the cruise represents well the regional-seasonal mean forcings. Constraining simulated forcings using the observed AOD distributions yields a robust estimate of regional-seasonal mean DARF of −8.6, −21.4 and +12.9Wm−2 at the top of the atmosphere (TOA), at the surface (SUR) and in the atmosphere (ATM), respectively, for the BoB region, and over the AS, of, −6.8, −12.8, and +6Wm−2 at TOA, SUR, and ATM, respectively.

Global climate change is considered to be one of the most serious concerns of humankind (United Nations, 1992; United Nations, 2002). Anthropogenic greenhouse gases and aerosols impact considerably the energy balance of the Earth system, possibly provoking adverse effects on social, ecological, and economical equilibria. This is one of the main reasons why the understanding of the Earth’s climate system is of major importance. If better predictions of the response of the climate system to anthropogenic perturbations were available, political decisions against negative impacts could be taken, and social adaptations to changed climate conditions would be possible.

This study describes two projects involving recent research on atmospheric ammonia. The first project investigates differences in modelling techniques of aerosol acidity using data from two recent field campaigns. Our results show that allowing or disallowing gas-particle partitioning in the Extended Aerosol Inorganic Model (E-AIM) changed the average modelled aerosol activity of H+ from one campaign by seven orders of magnitude and that disallowing gas-particle partitioning may not accurately represent the chemical state of the aerosols. The second project investigates the interference of reduced nitrogen in commercial chemiluminescent nitrogen oxide monitors with molybdenum oxide catalytic converters. This phenomenon is strongly dependent on the temperature of the catalytic converter. Our results show these instruments can have high conversion efficiencies of gaseous NH3 and NH4+ salts to NO at typical reported converter temperatures, but conversion efficiency varies between instruments and may be the result of uncertainty in reported converter temperature.

This study describes two projects involving recent research on atmospheric ammonia. The first project investigates differences in modelling techniques of aerosol acidity using data from two recent field campaigns. Our results show that allowing or disallowing gas-particle partitioning in the Extended Aerosol Inorganic Model (E-AIM) changed the average modelled aerosol activity of H+ from one campaign by seven orders of magnitude and that disallowing gas-particle partitioning may not accurately represent the chemical state of the aerosols. The second project investigates the interference of reduced nitrogen in commercial chemiluminescent nitrogen oxide monitors with molybdenum oxide catalytic converters. This phenomenon is strongly dependent on the temperature of the catalytic converter. Our results show these instruments can have high conversion efficiencies of gaseous NH3 and NH4+ salts to NO at typical reported converter temperatures, but conversion efficiency varies between instruments and may be the result of uncertainty in reported converter temperature.