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- ItemThe chemistry of OH and HO2 radicals in the boundary layer over the tropical Atlantic Ocean(München : European Geopyhsical Union, 2010) Whalley, L.K.; Furneaux, K.L.; Goddard, A.; Lee, J.D.; Mahajan, A.; Oetjen, H.; Read, K.A.; Kaaden, N.; Carpenter, L.J.; Lewis, A.C.; Plane, J.M.C.; Saltzman, E.S.; Wiedensohler, A.; Heard, D.E.Fluorescence Assay by Gas Expansion (FAGE) has been used to detect ambient levels of OH and HO2 radicals at the Cape Verde Atmospheric Observatory, located in the tropical Atlantic marine boundary layer, during May and June 2007. Midday radical concentrations were high, with maximum concentrations of 9 ×106 molecule cm−3 and 6×108 molecule cm−3 observed for OH and HO2, respectively. A box model incorporating the detailed Master Chemical Mechanism, extended to include halogen chemistry, heterogeneous loss processes and constrained by all available measurements including halogen and nitrogen oxides, has been used to assess the chemical and physical parameters controlling the radical chemistry. The model was able to reproduce the daytime radical concentrations to within the 1 σ measurement uncertainty of 20% during the latter half of the measurement period but significantly under-predicted [HO2] by 39% during the first half of the project. Sensitivity analyses demonstrate that elevated [HCHO] (~2 ppbv) on specific days during the early part of the project, which were much greater than the mean [HCHO] (328 pptv) used to constrain the model, could account for a large portion of the discrepancy between modelled and measured [HO2] at this time. IO and BrO, although present only at a few pptv, constituted ~19% of the instantaneous sinks for HO2, whilst aerosol uptake and surface deposition to the ocean accounted for a further 23% of the HO2 loss at noon. Photolysis of HOI and HOBr accounted for ~13% of the instantaneous OH formation. Taking into account that halogen oxides increase the oxidation of NOx (NO → NO2), and in turn reduce the rate of formation of OH from the reaction of HO2 with NO, OH concentrations were estimated to be 9% higher overall due to the presence of halogens. The increase in modelled OH from halogen chemistry gives an estimated 9% shorter lifetime for methane in this region, and the inclusion of halogen chemistry is necessary to model the observed daily cycle of O3 destruction that is observed at the surface. Due to surface losses, we hypothesise that HO2 concentrations increase with height and therefore contribute a larger fraction of the O3 destruction than at the surface.
- ItemCharacterisation of a new Fast CPC and its application for atmospheric particle measurements(München : European Geopyhsical Union, 2011) Wehner, B.; Siebert, H.; Hermann, M.; Ditas, F.; Wiedensohler, A.A new Fast CPC (FCPC) using butanol as working fluid has been built based on the setup described by Wang et al. (2002). In this study, we describe the new instrument. The functionality and stable operation of the FCPC in the laboratory, as well as under atmospheric conditions, is demonstrated. The counting efficiency was measured for three temperature differences between FCPC saturator and condenser, 25, 27, and 29 K, subsequently resulting in a lower detection limit between 6.1 and 8.5 nm. Above 25 nm the FCPC reached 98–100% counting efficiency compared to an electrometer used as the reference instrument. The FCPC demonstrated its ability to perform continuous measurements over a few hours in the laboratory with respect to the total particle counting. The instrument has been implemented into the airborne measurement platform ACTOS to perform measurements in the atmospheric boundary layer. Therefore, a stable operation over two hours is required. The mixing time of the new FCPC was estimated in two ways using a time series with highly fluctuating particle number concentrations. The analysis of a sharp ramp due to a concentration change results in a mixing time of 5 ms while a spectral analysis of atmospheric data demonstrates that for frequencies up to 10 Hz coherent structures can be resolved before sampling noise dominates.
- ItemVariability of black carbon mass concentrations, sub-micrometer particle number concentrations and size distributions: results of the German Ultrafine Aerosol Network ranging from city street to High Alpine locations(Amsterdam [u.a.] : Elsevier Science, 2018) Sun, J.; Birmili, W.; Hermann, M.; Tuch, T.; Weinhold, K.; Spindler, G.; Schladitz, A.; Bastian, S.; Löschau, G.; Cyrys, J.; Gu, J.; Flentje, H.; Briel, B.; Asbac, C.; Kaminski, H.; Ries, L.; Sohme, R.; Gerwig, H.; Wirtz, K.; Meinhardt, F.; Schwerin, A.; Bath, O.; Ma, N.; Wiedensohler, A.This work reports the first statistical analysis of multi-annual data on tropospheric aerosols from the German Ultrafine Aerosol Network (GUAN). Compared to other networks worldwide, GUAN with 17 measurement locations has the most sites equipped with particle number size distribution (PNSD) and equivalent black carbon (eBC) instruments and the most site categories in Germany ranging from city street/roadside to High Alpine. As we know, the variations of eBC and particle number concentration (PNC) are influenced by several factors such as source, transformation, transport and deposition. The dominant controlling factor for different pollutant parameters might be varied, leading to the different spatio-temporal variations among the measured parameters. Currently, a study of spatio-temporal variations of PNSD and eBC considering the influences of both site categories and spatial scale is still missing. Based on the multi-site dataset of GUAN, the goal of this study is to investigate how pollutant parameters may interfere with spatial characteristics and site categories. © 2019 The Authors
- ItemSize distribution, mass concentration, chemical and mineralogical composition and derived optical parameters of the boundary layer aerosol at Tinfou, Morocco, during SAMUM 2006(Milton Park : Taylor & Francis, 2017) Kandler, K.; Schütz, L.; Deutscher, C.; Ebert, M.; Hofmann, H.; Jäckel, S.; Jaenicke, R.; Knippertz, P.; Lieke, K.; Massling, A.; Petzold, A.; Schladitz, A.; Weinzierl, B.; Wiedensohler, A.; Zorn, S.; Weinbruch, S.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).