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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.
- ItemEstimated desert-dust ice nuclei profiles from polarization lidar: Methodology and case studies(München : European Geopyhsical Union, 2015) Mamouri, R.E.; Ansmann, A.A lidar method is presented that permits the estimation of height profiles of ice nuclei concentrations (INC) in desert dust layers. The polarization lidar technique is applied to separate dust and non-dust backscatter and extinction coefficients. The desert dust extinction coefficients σd are then converted to aerosol particle number concentrations APC280 which consider particles with radius > 280 nm only. By using profiles of APC280 and ambient temperature T along the laser beam, the profile of INC can be estimated within a factor of 3 by means of APC-T-INC parameterizations from the literature. The observed close relationship between σd at 500 nm and APC280 is of key importance for a successful INC retrieval. We studied this link by means of AERONET (Aerosol Robotic Network) sun/sky photometer observations at Morocco, Cabo Verde, Barbados, and Cyprus during desert dust outbreaks. The new INC retrieval method is applied to lidar observations of dust layers with the spaceborne lidar CALIOP (Cloud Aerosol Lidar with Orthogonal Polarization) during two overpasses over the EARLINET (European Aerosol Research Lidar Network) lidar site of the Cyprus University of Technology (CUT), Limassol (34.7° N, 33° E), Cyprus. The good agreement between the CALIOP and CUT lidar retrievals of σd, APC280, and INC profiles corroborates the potential of CALIOP to provide 3-D global desert dust APC280 and INC data sets.
- ItemDust mobilization and transport in the northern Sahara during SAMUM 2006 - A meteorological overview(Milton Park : Taylor & Francis, 2017) Knippertz, Peter; Ansmann, Albert; Althausen, Dietrich; Müller, Detlef; Tesche, Matthias; Bierwirth, Eike; Dinter, Tilman; Müller, Thomas; Von Hoyningen-Huene, Wolfgang; Schepanski, Kerstin; Wendisch, Manfred; Heinold, Bernd; Kandler, Konrad; Petzold, Andreas; Tegen, InaThe SAMUM field campaign in southern Morocco in May/June 2006 provides valuable data to study the emission, and the horizontal and vertical transports of mineral dust in the Northern Sahara. Radiosonde and lidar observations show differential advection of air masses with different characteristics during stable nighttime conditions and up to 5-km deep vertical mixing in the strongly convective boundary layer during the day. Lagrangian and synoptic analyses of selected dust periods point to a topographic channel from western Tunisia to central Algeria as a dust source region. Significant emission events are related to cold surges from the Mediterranean in association with eastward passing upper-level waves and lee cyclogeneses south of the Atlas Mountains. Other relevant events are local emissions under a distinct cut-off low over northwestern Africa and gust fronts associated with dry thunderstorms over the Malian and Algerian Sahara. The latter are badly represented in analyses from the European Centre for Medium–Range Weather Forecasts and in a regional dust model, most likely due to problems with moist convective dynamics and a lack of observations in this region. This aspect needs further study. The meteorological source identification is consistent with estimates of optical and mineralogical properties of dust samples.