Mixing of mineral dust with urban pollution aerosol over Dakar (Senegal): Impact on dust physico-chemical and radiative properties.

In the framework of the Saharan Mineral Dust Experiment (SAMUM) in 2008, the mixing of the urban pollution plume of Dakar (Senegal) with mineral dust was studied in detail using the German research aircraft Falcon which was equipped with a nadir-looking high spectral resolution lidar (HSRL) and extensive aerosol in situ instrumentation. The mineral dust layer as well as the urban pollution plume were probed remotely by the HSRL and in situ. Back trajectory analyses were used to attribute aerosol samples to source regions.We found that the emission from the region of Dakar increased the aerosol optical depth (532 nm) from approximately 0.30 over sea and over land east of Dakar to 0.35 in the city outflow. In the urban area, local black carbon (BC) emissions, or soot respectively, contributed more than 75% to aerosol absorption at 530 nm. In the dust layer, the single-scattering albedo at 530 nm was 0.96 â�� 0.99, whereas we found a value of 0.908 �± 0.018 for the aerosol dominated by urban pollution. After 6h of transport over the North Atlantic, the externally mixed mode of secondary aerosol particles had almost completely vanished, whereas the BC agglomerates (soot) were still externally mixed with mineral dust particles

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 °aap. The dust layers had a depth of 1.3 ± 0.4 km and showed a median °aap 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 °aap 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

Enhancement of the aerosol direct radiative effect by semi-volatile aerosol components: airborne measurements in North-Western Europe

A case study of atmospheric aerosol measurements exploring the impact of the vertical distribution of aerosol chemical composition upon the radiative budget in North-Western Europe is presented. Sub-micron aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) on both an airborne platform and a ground-based site at Cabauw in the Netherlands. The examined period in May 2008 was characterised by enhanced pollution loadings in North-Western Europe and was dominated by ammonium nitrate and Organic Matter (OM). Both ammonium nitrate and OM were observed to increase with altitude in the atmospheric boundary layer. This is primarily attributed to partitioning of semi-volatile gas phase species to the particle phase at reduced temperature and enhanced relative humidity. Increased ammonium nitrate concentrations in particular were found to strongly increase the ambient scattering potential of the aerosol burden, which was a consequence of the large amount of associated water as well as the enhanced mass. During particularly polluted conditions, increases in aerosol optical depth of 50–100% were estimated to occur due to the observed increase in secondary aerosol mass and associated water uptake. Furthermore, the single scattering albedo was also shown to increase with height in the boundary layer. These enhancements combined to increase the negative direct aerosol radiative forcing by close to a factor of two at the median percentile level. Such increases have major ramifications for regional climate predictions as semi-volatile components are often not included in aerosol models. The results presented here provide an ideal opportunity to test regional and global representations of both the aerosol vertical distribution and subsequent impacts in North-Western Europe. North-Western Europe can be viewed as an analogue for the possible future air quality over other polluted regions of the Northern Hemisphere, where substantial reductions in sulphur dioxide emissions have yet to occur. Anticipated reductions in sulphur dioxide in polluted regions will result in an increase in the availability of ammonia to form ammonium nitrate as opposed to ammonium sulphate. This will be most important where intensive agricultural practises occur. Our observations over North-Western Europe, a region where sulphur dioxide emissions have already been reduced, indicate that failure to include the semi-volatile behaviour of ammonium nitrate will result in significant errors in predicted aerosol direct radiative forcing. Such errors will be particularly significant on regional scales

Spectroscopic investigations of a semi-synthetic [FeFe] hydrogenase with propane di-selenol as bridging ligand in the binuclear subsite: comparison to the wild type and propane di-thiol variants

[FeFe] Hydrogenases catalyze the reversible conversion of H2 into electrons and protons. Their catalytic site, the H-cluster, contains a generic [4Fe–4S]H cluster coupled to a [2Fe]H subsite [Fe2(ADT)(CO)3(CN)2]2−, ADT = µ(SCH2)2NH. Heterologously expressed [FeFe] hydrogenases (apo-hydrogenase) lack the [2Fe]H unit, but this can be incorporated through artificial maturation with a synthetic precursor [Fe2(ADT)(CO)4(CN)2]2−. Maturation with a [2Fe] complex in which the essential ADT amine moiety has been replaced by CH2 (PDT = propane-dithiolate) results in a low activity enzyme with structural and spectroscopic properties similar to those of the native enzyme, but with simplified redox behavior. Here, we study the effect of sulfur-to-selenium (S-to-Se) substitution in the bridging PDT ligand incorporated in the [FeFe] hydrogenase HydA1 from Chlamydomonas reinhardtii using magnetic resonance (EPR, NMR), FTIR and spectroelectrochemistry. The resulting HydA1-PDSe enzyme shows the same redox behavior as the parent HydA1-PDT. In addition, a state is observed in which extraneous CO is bound to the open coordination site of the [2Fe]H unit. This state was previously observed only in the native enzyme HydA1-ADT and not in HydA1-PDT. The spectroscopic features and redox behavior of HydA1-PDSe, resulting from maturation with [Fe2(PDSe)(CO)4(CN)2]2−, are discussed in terms of spin and charge density shifts and provide interesting insight into the electronic structure of the H-cluster. We also studied the effect of S-to-Se substitution in the [4Fe–4S] subcluster. The reduced form of HydA1 containing only the [4Fe–4Se]H cluster shows a characteristic S = 7/2 spin state which converts back into the S = 1/2 spin state upon maturation with a [2Fe]–PDT/ADT complex

Multiple star systems in the Orion nebula

This is the author accepted manuscript. The final fersion is available from EDP Sciences via the DOI in this record.This work presents an interferometric study of the massive-binary fraction in the Orion Trapezium cluster with the recently comissioned GRAVITY instrument. We observed a total of 16 stars of mainly OB spectral type. We find three previously unknown companions for θ1 Ori B, θ2 Ori B, and θ2 Ori C. We determined a separation for the previously suspected companion of NU Ori. We confirm four companions for θ1 Ori A, θ1 Ori C, θ1 Ori D, and θ2 Ori A, all with substantially improved astrometry and photometric mass estimates. We refined the orbit of the eccentric high-mass binary θ1 Ori C and we are able to derive a new orbit for θ1 Ori D. We find a system mass of 21.7 M⊙ and a period of 53 days. Together with other previously detected companions seen in spectroscopy or direct imaging, eleven of the 16 high-mass stars are multiple systems. We obtain a total number of 22 companions with separations up to 600 AU. The companion fraction of the early B and O stars in our sample is about two, significantly higher than in earlier studies of mostly OB associations. The separation distribution hints toward a bimodality. Such a bimodality has been previously found in A stars, but rarely in OB binaries, which up to this point have been assumed to be mostly compact with a tail of wider companions. We also do not find a substantial population of equal-mass binaries. The observed distribution of mass ratios declines steeply with mass, and like the direct star counts, indicates that our companions follow a standard power law initial mass function. Again, this is in contrast to earlier findings of flat mass ratio distributions in OB associations. We excluded collision as a dominant formation mechanism but find no clear preference for core accretion or competitive accretion.Marie Skłodowska-Curie Grant AgreementFCT-PortugalERC Starting Gran

Orbit-related sea level errors for TOPEX altimetry at seasonal to decadal timescales

Interannual to decadal sea level trends are indicators of climate variability and change. A major source of global and regional sea level data is satellite radar altimetry, which relies on precise knowledge of the satellite's orbit. Here, we assess the error budget of the radial orbit component for the TOPEX/Poseidon mission for the period 1993 to 2004 from a set of different orbit solutions. The errors for seasonal, interannual (5-year), and decadal periods are estimated on global and regional scales based on radial orbit differences from three state-of-the-art orbit solutions provided by different research teams: the German Research Centre for Geosciences (GFZ), the Groupe de Recherche de Géodésie Spatiale (GRGS), and the Goddard Space Flight Center (GSFC). The global mean sea level error related to orbit uncertainties is of the order of 1 mm (8 % of the global mean sea level variability) with negligible contributions on the annual and decadal timescales. In contrast, the orbit-related error of the interannual trend is 0.1 mm yr−1 (27 % of the corresponding sea level variability) and might hamper the estimation of an acceleration of the global mean sea level rise. For regional scales, the gridded orbit-related error is up to 11 mm, and for about half the ocean the orbit error accounts for at least 10 % of the observed sea level variability. The seasonal orbit error amounts to 10 % of the observed seasonal sea level signal in the Southern Ocean. At interannual and decadal timescales, the orbit-related trend uncertainties reach regionally more than 1 mm yr−1. The interannual trend errors account for 10 % of the observed sea level signal in the tropical Atlantic and the south-eastern Pacific. For decadal scales, the orbit-related trend errors are prominent in a several regions including the South Atlantic, western North Atlantic, central Pacific, South Australian Basin, and the Mediterranean Sea. Based on a set of test orbits calculated at GFZ, the sources of the observed orbit-related errors are further investigated. The main contributors on all timescales are uncertainties in Earth's time-variable gravity field models and on annual to interannual timescales discrepancies of the tracking station subnetworks, i.e. satellite laser ranging (SLR) and Doppler Orbitography and Radiopositioning Integrated by Satellite (DORIS)

Dust mobilization and aerosol transport from West Africa to Cape Verde-a meteorological overview of SAMUM-2

The second field campaign of the SAharan Mineral dUst experiMent (SAMUM-2) was performed between 15 January and 14 February 2008 at the airport of Praia, Cape Verde, and provided valuable information to study the westward transport of Saharan dust and the mixing with biomass-burning smoke and sea-salt aerosol. Here lidar, meteorological, and particle measurements at Praia, together with operational analyses, trajectories, and satellite and synoptic station data are used to give an overview of the meteorological conditions and to place other SAMUM-2 measurements into a large-scale context. It is demonstrated that wintertime dust conditions at Cape Verde are closely related to the movement and intensification of mid-latitude high-pressure systems and the associated pressure gradients at their southern flanks. These cause dust emission over Mauritania, Mali, and Niger, and subsequent westward transport to Cape Verde within about 1-5 d. Dust emissions often peak around midday, suggesting a relation to daytime mixing of momentum from nocturnal low-level jets to the surface. The dust layer over Cape Verde is usually restricted to the lowest 1.5 km of the atmosphere. During periods with near-surface wind speeds about 5.5 ms -1, a maritime aerosol layer develops which often mixes with dust from above. On most days, the middle levels up to about 5 km additionally contain smoke that can be traced back to sources in southern West Africa. Above this layer, clean air masses are transported to Cape Verde with the westerly flow at the southern side of the subtropical jet. The penetration of extra-tropical disturbances to low latitudes can bring troposphere-deep westerly flow and unusually clean conditions to the region

Mineral dust observed with AERONET Sun photometer, Raman lidar, and in situ instruments during SAMUM 2006: Shape-independent particle properties

Aerosol Robotic Network (AERONET) Sun photometer observations were carried out at Ouarzazate, Morocco, during the Saharan Mineral Dust Experiment (SAMUM) 2006. Data from one measurement day, 19 May 2006, are used to derive particle optical and microphysical parameters with AERONET's latest version of light-scattering model for non-spherical particle geometry. In our analysis we also make use of a novel measurement channel at 1638 nm wavelength. We compare the results to data products obtained by airborne high-spectral-resolution lidar, several ground-based Raman lidar, and airborne and ground-based in situ measurement platforms. We chose that specific measurement day because the dust plume was vertically well mixed. Extinction coefficients from AERONET Sun photometer and lidar observations and in situ measurements agree well. ngstrm exponents from Sun photometer and lidar are in close agreement, too. Airborne in situ measurements of dust particle size distributions show larger effective radii than inferred from the AERONET data. Complex refractive indices that are derived with the AERONET algorithm differ from the values obtained with different independent techniques employed in our study. The single-scattering albedo was derived from the airborne observations of particle size distributions and complex refractive indices. Single-scattering albedo differs to the value inferred from the AERONET data. The differences may be attributed to the different effective radii that we obtained from the various techniques. The differences between the data products from the various measurement platforms, however, cannot be generalized, as we could only test data for one measurement day. An analysis of additional measurements is under way