Volker Matthias

Long‐range transport of Saharan dust to northern Europe: The 11–16 October 2001 outbreak observed with EARLINET

The spread of mineral particles over southwestern, western, and central Europe resulting from a strong Saharan dust outbreak in October 2001 was observed at 10 stations of the European Aerosol Research Lidar Network (EARLINET). For the first time, an optically dense desert dust plume over Europe was characterized coherently with high vertical resolution on a continental scale. The main layer was located above the boundary layer (above 1-km height above sea level (asl)) up to 3–5-km height, and traces of dust particles reached heights of 7–8 km. The particle optical depth typically ranged from 0.1 to 0.5 above 1-km height asl at the wavelength of 532 nm, and maximum values close to 0.8 were found over northern Germany. The lidar observations are in qualitative agreement with values of optical depth derived from Total Ozone Mapping Spectrometer (TOMS) data. Ten-day backward trajectories clearly indicated the Sahara as the source region of the particles and revealed that the dust layer observed, e.g., over Belsk, Poland, crossed the EARLINET site Aberystwyth, UK, and southern Scandinavia 24–48 hours before. Lidar-derived particle depolarization ratios, backscatter- and extinction-related Angstrom exponents, and extinction-to-backscatter ratios mainly ranged from 15 to 25%, −0.5 to 0.5, and 40–80 sr, respectively, within the lofted dust plumes. A few atmospheric model calculations are presented showing the dust concentration over Europe. The simulations were found to be consistent with the network observations.

Aerosol lidar intercomparison in the framework of the EARLINET project. 3. Raman lidar algorithm for aerosol extinction, backscatter, and lidar ratio

An intercomparison of the algorithms used to retrieve aerosol extinction and backscatter starting from Raman lidar signals has been performed by 11 groups of lidar scientists involved in the European Aerosol Research Lidar Network (EARLINET). This intercomparison is part of an extended quality assurance program performed on aerosol lidars in the EARLINET. Lidar instruments and aerosol backscatter algorithms were tested separately. The Raman lidar algorithms were tested by use of synthetic lidar data, simulated at 355, 532, 386, and 607 nm, with realistic experimental and atmospheric conditions taken into account. The intercomparison demonstrates that the data-handling procedures used by all the lidar groups provide satisfactory results. Extinction profiles show mean deviations from the correct solution within 10% in the planetary boundary layer (PBL), and backscatter profiles, retrieved by use of algorithms based on the combined Raman elastic-backscatter lidar technique, show mean deviations from solutions within 20% up to 2 km. The intercomparison was also carried out for the lidar ratio and produced profiles that show a mean deviation from the solution within 20% in the PBL. The mean value of this parameter was also calculated within a lofted aerosol layer at higher altitudes that is representative of typical layers related to special events such as Saharan dust outbreaks, forest fires, and volcanic eruptions. Here deviations were within 15%.

Aerosol lidar intercomparison in the framework of the EARLINET project. 2.Aerosol backscatter algorithms

An intercomparison of aerosol backscatter lidar algorithms was performed in 2001 within the framework of the European Aerosol Research Lidar Network to Establish an Aerosol Climatology (EARLINET). The objective of this research was to test the correctness of the algorithms and the influence of the lidar ratio used by the various lidar teams involved in the EARLINET for calculation of backscatter-coefficient profiles from the lidar signals. The exercise consisted of processing synthetic lidar signals of various degrees of difficulty. One of these profiles contained height-dependent lidar ratios to test the vertical influence of those profiles on the various retrieval algorithms. Furthermore, a realistic incomplete overlap of laser beam and receiver field of view was introduced to remind the teams to take great care in the nearest range to the lidar. The intercomparison was performed in three stages with increasing knowledge on the input parameters. First, only the lidar signals were distributed; this is the most realistic stage. Afterward the lidar ratio profiles and the reference values at calibration height were provided. The unknown height-dependent lidar ratio had the largest influence on the retrieval, whereas the unknown reference value was of minor importance. These results show the necessity of making additional independent measurements, which can provide us with a suitable approximation of the lidar ratio. The final stage proves in general, that the data evaluation schemes of the different groups of lidar systems work well.

Aerosol climatology for the planetary boundary layer derived from regular lidar measurements

Regular aerosol extinction and backscatter measurements using a UV Raman Lidar have been performed for almost 3 years in Hamburg in the frame of the German Lidar Network. A set of 92 aerosol extinction and 164 aerosol backscatter profiles has been used for statistical investigations. Mean values and variances of the aerosol extinction and backscatter in the boundary layer have been calculated. Large fluctuations during the whole year have been found. The measured aerosol extinction over Hamburg shows a seasonal cycle with highest values in early fall and a second less prominent peak in spring. An analysis of the data using back trajectories showed a dependence of the aerosol extinction on the origin of the air mass. The residence time of the air mass over industrialized areas was found to be an important parameter for the measured aerosol extinction at Hamburg. However, only a small part of the total variability could be explained by the air mass origin. For 75 cases of aerosol extinction measurements under cloud-free conditions, the aerosol backscatter profile and therefore, the lidar ratio as a function of altitude could be determined. Winter measurements of the lidar ratio are often close to model results for maritime aerosol, the summer measurements are close to the model results for urban or continental aerosols. The high quality of the data has been proven by intercomparisons with other lidar systems and with star photometer measurements of the aerosol optical depth during the Lindenberg Aerosol Characterization Experiment (LACE’98) field campaign. D 2002 Elsevier Science B.V. All rights reserved.

The contribution of ship emissions to air pollution in the North Sea regions

As a consequence of the global distribution of manufacturing sites and the increasing international division of labour, ship traffic is steadily increasing and is becoming more and more important as an origin of air pollution. This study investigates the impact of ship emissions in coastal areas of the North Sea under conditions of the year 2000 by means of a regional chemistry transport model which runs on a sufficiently high resolution to study air pollution in coastal regions. It was found that northern Germany and Denmark in summer suffer from more than 50% higher sulphate, nitrate and ammonium aerosol concentrations due to contributions from ships. The implementation of a sulphur emission control area (SECA) in the North Sea, as it was implemented at the end of 2007, directly results in reduced sulphur dioxide and sulphate aerosol concentrations while nitrate aerosol concentrations are slightly increased.

Wet deposition of poly- and perfluorinated compounds in Northern Germany.

Twenty precipitation samples were taken concurrently with air samples at a northern German monitoring site over a period of 7 months in 2007 and 2008. Thirty four poly- and perfluorinated compounds (PFC) were determined in rain water samples by solid phase extraction and HPLC-MS/MS analysis. Seventeen compounds were detected in rain water with SigmaPFC concentrations ranging from 1.6 ng L(-1) to 48.6 ng L(-1). Perfluorooctanoate (PFOA) and perfluorobutanate (PFBA) were the compounds that were usually observed in highest concentrations. Calculated SigmaPFC deposition rates were between 2 and 91 ng m(-2) d(-1). These findings indicate that particle phase PFC are deposited from the atmosphere by precipitation. A relationship between PFC wet deposition and air concentration may be established via precipitation amounts. Trajectory analysis revealed that PFC concentration and deposition estimates in precipitation can only be explained if a detailed air mass history is considered.

Vertical emission profiles for Europe based on plume rise calculations.

The vertical allocation of emissions has a major impact on results of Chemistry Transport Models. However, in Europe it is still common to use fixed vertical profiles based on rough estimates to determine the emission height of point sources. This publication introduces a set of new vertical profiles for the use in chemistry transport modeling that were created from hourly gridded emissions calculated by the SMOKE for Europe emission model. SMOKE uses plume rise calculations to determine effective emission heights. Out of more than 40,000 different vertical emission profiles 73 have been chosen by means of hierarchical cluster analysis. These profiles show large differences to those currently used in many emission models. Emissions from combustion processes are released in much lower altitudes while those from production processes are allocated to higher altitudes. The profiles have a high temporal and spatial variability which is not represented by currently used profiles.

Introducing a Partitioning Mechanism for PAHs into the Community Multiscale Air Quality Modeling System and Its Application to Simulating the Transport of Benzo(a)pyrene over Europe

Into the Community Multiscale Air Quality modeling system (CMAQ) that is widely used for simulating the transport and fate of air pollutants, a new module was inserted that accounts for the partitioning of semivolatile organic compounds—in particular, polycyclic organic hydrocarbons (PAHs)—between the gaseous and the particulate phases. This PAH version of CMAQ can at this time be applied to substances that are predominantly associated with particles and can be assumed to be inert, as is the case for benzo(a)pyrene [B(a)P]. The model was set up for Europe on a grid with 54-km cell width with a nest of 18-km gridcell width located around the North Sea to simulate ambient air concentrations and depositions of B(a)P in January, April, July, and October 2000. To evaluate the quality of the simulation results, daily and monthly mean concentrations were compared with measurements from six monitoring stations. The typical ratio of modeled to measured values is circa 4 (median), which—with respect to both measurement and simulation uncertainties and problems involved when comparing measurements with simulations—proved that the PAH version of CMAQ is suitable to simulate the fate and transport of B(a)P over Europe and can serve as a starting point for models for other PAHs that additionally consider degradation.

The effect of temporal resolution of PAH emission data on transport and deposition patterns simulated with the Community Multiscale Air Quality modelling system (CMAQ)

The effect of temporal variation of polycyclic aromatic hydrocarbon (PAH) emission data on transport and deposition patterns were simulated with the Community Multiscale Air Qual- ity modelling system (CMAQ) for Europe, 54 km grid, for the year 2000. The carcinogenic benzo(a)pyrene (B(a)P) was used as a representative for the group of PAHs. The official emission data are only provided as one-year bulk emissions but the major emission sources of B(a)P vary within seasonal, diurnal and weekly cycles, respectively. The seasonal variability showed the great- est effects. However, on a regional scale diurnal cycles possessed significant effects as well. Com- parison with measured weekly average concentration indicated the same trend for simulation and observation.

Enhanced Aerosol Formation and Nutrient Deposition by Ship Emissions in North Sea Coastal Regions

This study investigates the impact of ship emissions on secondary aerosol formation in coastal areas of the North Sea under conditions of the year 2000. The regional chemistry transport model CMAQ is used with different emission data sets as input to study their impact on aerosol concentrations. It is shown that the largest effect occurs in summer, when sulphate, nitrate and ammonium concentrations may be increased by more than 50% in large areas of Denmark and Northern Germany. The use of sulphur reduced fuels results in a significant reduction of sulphate aerosols. However at the same time, nitrate aerosol concentrations increase.