Bernadett Weinzierl

Size distribution, mass concentration, chemical and mineralogical composition and derived optical parameters of the boundary layer aerosol at Tinfou, Morocco, during SAMUM 2006

During the SAMUM 2006 field campaign in southern Morocco, physical and chemical properties of desert aerosols were measured. Mass concentrations ranging from 30μgm−3 for PM2.5 under desert background conditions up to 300 000μgm−3 for total suspended particles (TSP) during moderate dust storms were measured. TSP dust concentrations are correlated with the local wind speed, whereasPM10 andPM2.5 concentrations are determined by advection from distant sources. Size distributions were measured for particles with diameter between 20 nm and 500μm (parametrizations are given). Two major regimes of the size spectrum can be distinguished. For particles smaller than 500 nm diameter, the distributions show maxima around 80 nm, widely unaffected of varying meteorological and dust emission conditions. For particles larger than 500 nm, the range of variation may be up to one order of magnitude and up to three orders of magnitude for particles larger than 10μm. The mineralogical composition of aerosol bulk samples was measured by X-ray powder diffraction. Major constituents of the aerosol are quartz, potassium feldspar, plagioclase, calcite, hematite and the clay minerals illite, kaolinite and chlorite. A small temporal variability of the bulk mineralogical composition was encountered. The chemical composition of approximately 74 000 particles was determined by electron microscopic single particle analysis. Three size regimes are identified: for smaller than 500 nm in diameter, the aerosol consists of sulphates and mineral dust. For larger than 500 nm up to 50μm, mineral dust dominates, consisting mainly of silicates, and—to a lesser extent—carbonates and quartz. For diameters larger than 50μm, approximately half of the particles consist of quartz. Time series of the elemental composition show a moderate temporal variability of the major compounds. Calcium-dominated particles are enhanced during advection from a prominent dust source in Northern Africa (Chott El Djerid and surroundings). The particle aspect ratio was measured for all analysed particles. Its size dependence reflects that of the chemical composition. For larger than 500 nm particle diameter, a median aspect ratio of 1.6 is measured. Towards smaller particles, it decreases to about 1.3 (parametrizations are given). From the chemical/mineralogical composition, the aerosol complex refractive index was determined for several wavelengths from ultraviolet to near-infrared. Both real and imaginary parts show lower values for particles smaller than 500 nm in diameter (1.55–2.8 × 10−3i at 530 nm) and slightly higher values for larger particles (1.57–3.7 × 10−3i at 530 nm).

Processes influencing ozone levels in Alaskan forest fire plumes during long-range transport over the North Atlantic

[1] A case of long-range transport of a biomass burning plume from Alaska to Europe is analyzed using a Lagrangian approach. This plume was sampled several times in the free troposphere over North America, the North Atlantic and Europe by three different aircraft during the IGAC Lagrangian 2K4 experiment which was part of the ICARTT/ ITOP measurement intensive in summer 2004. Measurements in the plume showed enhanced values of CO, VOCs and NOy, mainly in form of PAN. Observed O-3 levels increased by 17 ppbv over 5 days. A photochemical trajectory model, CiTTyCAT, was used to examine processes responsible for the chemical evolution of the plume. The model was initialized with upwind data and compared with downwind measurements. The influence of high aerosol loading on photolysis rates in the plume was investigated using in situ aerosol measurements in the plume and lidar retrievals of optical depth as input into a photolysis code (Fast-J), run in the model. Significant impacts on photochemistry are found with a decrease of 18% in O-3 production and 24% in O-3 destruction over 5 days when including aerosols. The plume is found to be chemically active with large O-3 increases attributed primarily to PAN decomposition during descent of the plume toward Europe. The predicted O-3 changes are very dependent on temperature changes during transport and also on water vapor levels in the lower troposphere which can lead to O-3 destruction. Simulation of mixing/dilution was necessary to reproduce observed pollutant levels in the plume. Mixing was simulated using background concentrations from measurements in air masses in close proximity to the plume, and mixing timescales ( averaging 6.25 days) were derived from CO changes. Observed and simulated O-3/CO correlations in the plume were also compared in order to evaluate the photochemistry in the model. Observed slopes change from negative to positive over 5 days. This change, which can be attributed largely to photochemistry, is well reproduced by multiple model runs even if slope values are slightly underestimated suggesting a small underestimation in modeled photochemical O-3 production. The possible impact of this biomass burning plume on O-3 levels in the European boundary layer was also examined by running the model for a further 5 days and comparing with data collected at surface sites, such as Jungfraujoch, which showed small O-3 increases and elevated CO levels. The model predicts significant changes in O-3 over the entire 10 day period due to photochemistry but the signal is largely lost because of the effects of dilution. However, measurements in several other BB plumes over Europe show that O-3 impact of Alaskan fires can be potentially significant over Europe.

Saharan Mineral Dust Experiments SAMUM-1 and SAMUM-2: What have we learned?

Two comprehensive field campaigns were conducted in 2006 and 2008 in the framework of the Saharan Mineral Dust Experiment (SAMUM) project. The relationship between chemical composition, shape morphology, size distribution and optical effects of the dust particles was investigated. The impact of Saharan dust on radiative transfer and the feedback of radiative effects upon dust emission and aerosol transport were studied. Field observations (ground-based, airborne and remote sensing) and modelling results were compared within a variety of dust closure experiments with a strong focus on vertical profiling. For the first time, multiwavelength Raman/polarization lidars and an airborne high spectral resolution lidar were involved in major dust field campaigns and provided profiles of the volume extinction coefficient of the particles at ambient conditions (for the full dust size distribution), of particle-shape-sensitive optical properties at several wavelengths, and a clear separation of dust and smoke profiles allowing for an estimation of the single-scattering albedo of the biomass-burning aerosol. SAMUM–1 took place in southern Morocco close to the Saharan desert in the summer of 2006, whereas SAMUM–2 was conducted in Cape Verde in the outflow region of desert dust and biomass-burning smoke from western Africa in the winter of 2008. This paper gives an overview of the SAMUM concept, strategy and goals, provides snapshots (highlights) of SAMUM–2 observations and modelling efforts, summarizes main findings of SAMUM–1 and SAMUM–2 and finally presents a list of remaining problems and unsolved questions.

Airborne measurements of dust layer properties, particle size distribution and mixing state of Saharan dust during SAMUM 2006

The Saharan Mineral Dust Experiment (SAMUM) was conducted in May/June 2006 in southern Morocco. As part of SAMUM, airborne in situ measurements of the particle size distribution in the diameter range 4 nm < Dp < 100 μm were conducted. The aerosol mixing state was determined below Dp < 2.5 μm. Furthermore, the vertical structure of the dust layers was investigated with a nadir-looking high spectral resolution lidar (HSRL). The desert dust aerosol exhibited two size regimes of different mixing states: below 0.5 μm, the particles had a non-volatile core and a volatile coating; larger particles above 0.5 μm consisted of non-volatile components and contained light absorbing material. In all cases, particles larger than 10 μm were present, and in 80% of the measurements no particles larger than 40 μm were present. The abundance of large particles showed almost no height dependence. The effective diameter Deff in the dust plumes investigated showed two main ranges: the first range of Deff peaked around 5 μm and the second range of Deff around 8 μm. The two ranges of Deff suggest that it may be inadequate to use one average effective diameter or one parametrization for a typical dust size distribution.

Saharan dust absorption and refractive index from aircraft-based observations during SAMUM 2006

During the Saharan Mineral Dust Experiment (SAMUM) conducted in summer 2006 in southeast Morocco, the complex refractive index of desert dust was determined from airborne measurements of particle size distributions and aerosol absorption coefficients at three different wavelengths in the blue (467 nm), green (530 nm) and red (660 nm) spectral regions. The vertical structure of the dust layers was analysed by an airborne high spectral resolution lidar (HSRL). The origin of the investigated dust layers was estimated from trajectory analyses, combined with Meteosat 2nd Generation (MSG) scenes and wind field data analyses. The real part n of the dust refractive index was found almost constant with values between 1.55 and 1.56, independent of the wavelength. The values of the imaginary part k varied between the blue and red spectral regions by a factor of three to ten depending on the dust source region. Absolute values of k ranged from 3.1 × 10−3 to 5.2 × 10−3 at 450 nm and from 0.3 × 10−3 to 2.5 × 10−3 at 700 nm. Groupings of k values could be attributed to different source regions.

Operational prediction of ash concentrations in the distal volcanic cloud from the 2010 Eyjafjallajökull eruption

[1] During the 2010 eruption of Eyjafjallajokull, improvements were made to the modeling procedure at the Met Office, UK, enabling peak ash concentrations within the volcanic cloud to be estimated. In this paper we describe the ash concentration forecasting method, its rationale and how it evolved over time in response to new information and user requirements. The change from solely forecasting regions of ash to also estimating peak ash concentrations required consideration of volcanic ash emission rates, the fraction of ash surviving near-source fall-out, and the relationship between predicted mean and local peak ash concentrations unresolved by the model. To validate the modeling procedure, predicted peak ash concentrations are compared against observations obtained by ground-based and research aircraft instrumentation. This comparison between modeled and observed peak concentrations highlights the many sources of error and the uncertainties involved. Despite the challenges of predicting ash concentrations, the ash forecasting method employed here is found to give useful guidance on likely ash concentrations. Predicted peak ash concentrations lie within about one and a half orders of magnitude of the observed peak concentrations. A significant improvement in the agreement between modeled and observed values is seen if a buffer zone, accounting for positional errors in the predicted ash cloud, is used. Sensitivity of the predicted ash concentrations to the source properties (e.g., the plume height and the vertical distribution of ash at the source) is assessed and in some cases, seemingly minor uncertainties in the source specification have a large effect on predicted ash concentrations.

Solar radiative effects of a Saharan dust plume observed during SAMUM assuming spheroidal model particles

The solar optical properties of Saharan mineral dust observed during the Saharan Mineral Dust Experiment (SAMUM) were explored based on measured size-number distributions and chemical composition. The size-resolved complex refractive index of the dust was derived with real parts of 1.51–1.55 and imaginary parts of 0.0008–0.006 at 550 nm wavelength. At this spectral range a single scattering albedo ωo and an asymmetry parameter g of about 0.8 were derived. These values were largely determined by the presence of coarse particles. Backscatter coefficients and lidar ratios calculated with Mie theory (spherical particles) were not found to be in agreement with independently measured lidar data. Obviously the measured Saharan mineral dust particles were of non-spherical shape. With the help of these lidar and sun photometer measurements the particle shape as well as the spherical equivalence were estimated. It turned out that volume equivalent oblate spheroids with an effective axis ratio of 1:1.6 matched these data best. This aspect ratio was also confirmed by independent single particle analyses using a scanning electron microscope. In order to perform the non-spherical computations, a database of single particle optical properties was assembled for oblate and prolate spheroidal particles. These data were also the basis for simulating the non-sphericity effects on the dust optical properties: ωo is influenced by up to a magnitude of only 1% and g is diminished by up to 4% assuming volume equivalent oblate spheroids with an axis ratio of 1:1.6 instead of spheres. Changes in the extinction optical depth are within 3.5%. Non-spherical particles affect the downwelling radiative transfer close to the bottom of the atmosphere, however, they significantly enhance the backscattering towards the top of the atmosphere: Compared to Mie theory the particle non-sphericity leads to forced cooling of the Earth-atmosphere system in the solar spectral range for both dust over ocean and desert.

Microphysical and optical properties of dust and tropical biomass burning aerosol layers in the Cape Verde region—an overview of the airborne in situ and lidar measurements during SAMUM-2

In the framework of the Saharan Mineral Dust Experiment (SAMUM) airborne High Spectral Resolution Lidar and in situ measurements of the particle size, aerosol mixing state and absorption coefficient were conducted. Here, the properties of mineral dust and tropical biomass burning layers in the Cape Verde region in January/February 2008 are investigated and compared with the properties of fresh dust observed in May/June 2006 close the Sahara. In the Cape Verde area, we found a complex stratification with dust layers covering the altitude range below 2 km and biomass burning layers aloft. The aerosol type of the individual layers was classified based on depolarization and lidar ratios and, in addition, on in situ measured Ångström exponents of absorption åap. The dust layers had a depth of 1.3 ± 0.4 km and showed a median åap of 3.95. The median effective diameter Deff was 2.5 μm and the dust layers over Cape Verde yielded clear signals of aging: large particles were depleted due to gravitational settling and the accumulation mode diameter was shifted towards larger sizes as a result of coagulation. The tropical biomass layers had a depth of 2.0 ± 1.1 km and were characterized by a median åap of 1.34. They always contained a certain amount of large dust particles and showed a median Deff of 1.1 μm and a fine mode Deff,fine of 0.33. The dust and biomass burning layers had a median aerosol optical depth (AOD) of 0.23 and 0.09, respectively. The median contributions to the AOD of the total atmospheric column below 10 km were 75 and 37%, respectively.

Spatial distribution and optical properties of Saharan dust observed by airborne high spectral resolution lidar during SAMUM 2006

Airborne measurements of pure Saharan dust extinction and backscatter coefficients, the corresponding lidar ratio and the aerosol optical thickness (AOT) have been performed during the Saharan Mineral Dust Experiment 2006, with a high spectral resolution lidar. Dust layers were found to range from ground up to 4–6 km above sea level (asl). Maximum AOT values at 532 nm, encountered within these layers during the DLR Falcon research flights were 0.50–0.55. A significant horizontal variability of the AOT south of the High Atlas mountain range was observed even in cases of a well-mixed dust layer. High vertical variations of the dust lidar ratio of 38–50 sr were observed in cases of stratified dust layers. The variability of the lidar ratio was attributed to dust advection from different source regions. The aerosol depolarization ratio was about 30% at 532 nm during all measurements and showed only marginal vertical variations.

State of Mixing, Shape Factor, Number Size Distribution, and Hygroscopic Growth of the Saharan Anthropogenic and Mineral Dust Aerosol at Tinfou, Morocco

The Saharan Mineral Dust Experiment (SAMUM) was conducted in May and June 2006 in Tinfou, Morocco. A H-TDMA system and a H-DMA-APS system were used to obtain hygroscopic properties of mineral dust particles at 85% RH. Dynamic shape factors of 1.11, 1.19 and 1.25 were determined for the volume equivalent diameters 720, 840 and 960 nm, respectively. During a dust event, the hydrophobic number fraction of 250 and 350 nm particles increased significantly from 30 and 65% to 53 and 75%, respectively, indicating that mineral dust particles can be as small as 200 nm in diameter. Lognormal functions for mineral dust number size distributions were obtained from total particle number size distributions and fractions of hydrophobic particles. The geometric mean diameter for Saharan dust particles was 715 nm during the dust event and 570 nm for the Saharan background aerosol. Measurements of hygroscopic growth showed that the Saharan aerosol consists of an anthropogenic fraction (predominantly non natural sulphate and carbonaceous particles) and of mineral dust particles. Hygroscopic growth and hysteresis curve measurements of the ‘more’ hygroscopic particle fraction indicated ammonium sulphate as a main component of the anthropogenic aerosol. Particles larger than 720 nm in diameter were completely hydrophobic meaning that mineral dust particles are not hygroscopic.