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  • 1
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    Isotopic composition of atmospheric nitrate in a tropical marine boundary layer (2013)
    National Academy of Sciences
    In:  PNAS Proceedings of the National Academy of Sciences of the United States of America, 110 (44). pp. 17668-17673.
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    Publikationsdatum: 2014-01-27
    Beschreibung: Long-term observations of the reactive chemical composition of the tropical marine boundary layer (MBL) are rare, despite its crucial role for the chemical stability of the atmosphere. Recent observations of reactive bromine species in the tropical MBL showed unexpectedly high levels that could potentially have an impact on the ozone budget. Uncertainties in the ozone budget are amplified by our poor understanding of the fate of NOx (= NO + NO2), particularly the importance of nighttime chemical NOx sinks. Here, we present year-round observations of the multiisotopic composition of atmospheric nitrate in the tropical MBL at the Cape Verde Atmospheric Observatory. We show that the observed oxygen isotope ratios of nitrate are compatible with nitrate formation chemistry, which includes the BrNO3 sink at a level of ca. 20 ± 10% of nitrate formation pathways. The results also suggest that the N2O5 pathway is a negligible NOx sink in this environment. Observations further indicate a possible link between the NO2/NOx ratio and the nitrogen isotopic content of nitrate in this low NOx environment, possibly reflecting the seasonal change in the photochemical equilibrium among NOx species. This study demonstrates the relevance of using the stable isotopes of oxygen and nitrogen of atmospheric nitrate in association with concentration measurements to identify and constrain chemical processes occurring in the MBL.
    Materialart: Article , PeerReviewed
    DOI: 10.1073/pnas.1216639110
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  • 2
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    Attenuation of sinking particulate organic carbon flux through the mesopelagic ocean (2015)
    National Academy of Sciences
    In:  PNAS Proceedings of the National Academy of Sciences of the United States of America, 112 (4). pp. 1089-1094.
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    Publikationsdatum: 2021-04-23
    Beschreibung: The biological carbon pump, which transports particulate organic carbon (POC) from the surface to the deep ocean, plays an important role in regulating atmospheric carbon dioxide (CO2) concentrations. We know very little about geographical variability in the remineralization depth of this sinking material and less about what controls such variability. Here we present previously unpublished profiles of mesopelagic POC flux derived from neutrally buoyant sediment traps deployed in the North Atlantic, from which we calculate the remineralization length scale for each site. Combining these results with corresponding data from the North Pacific, we show that the observed variability in attenuation of vertical POC flux can largely be explained by temperature, with shallower remineralization occurring in warmer waters. This is seemingly inconsistent with conclusions drawn from earlier analyses of deep-sea sediment trap and export flux data, which suggest lowest transfer efficiency at high latitudes. However, the two patterns can be reconciled by considering relatively intense remineralization of a labile fraction of material in warm waters, followed by efficient downward transfer of the remaining refractory fraction, while in cold environments, a larger labile fraction undergoes slower remineralization that continues over a longer length scale. Based on the observed relationship, future increases in ocean temperature will likely lead to shallower remineralization of POC and hence reduced storage of CO2 by the ocean.
    Materialart: Article , PeerReviewed
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    DOI: 10.1073/pnas.1415311112
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  • 3
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    Real-time monitoring of picomolar concentrations of iron(II) in marine waters using automated flow injection-chemiluminescence instrumentation (2002)
    American Chemistry Society
    In:  Environmental Science and Technology, 36 (21). pp. 4600-4607.
    Details
    Publikationsdatum: 2016-12-19
    Beschreibung: A shipboard-deployable, flow-injection (FI) based instrument for monitoring iron(II) in surface marine waters is described. It incorporates a miniature, low-power photon-counting head for measuring the light emitted from the iron-(II)-catalyzed chemiluminescence (CL) luminol reaction. System control, signal acquisition, and data processing are performed in a graphical programming environment. The limit of detection for iron(II) is in the range 8-12 pmol L-1 (based on 3s of the blank), and the precision over the range 8-1000 pmol L-1 varies between 0.9 and 7.6 (n = 4). Results from a day-night deployment during a north-to-south transect of the Atlantic Ocean and a daytime transect in the Sub-Antarctic Front are presented together with ancillary temperature, salinity, and irradiance data. The generic nature of the components used to assemble the instrument make the technology readily transferable to other laboratories and the modular construction makes it easy to adapt the system for use with other CL chemistries.
    Materialart: Article , PeerReviewed
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    DOI: 10.1021/es020045v
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  • 4
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    Species kinetics and heterogeneous reactivity of dissolved CU in natural freshwaters (2002)
    American Chemistry Society
    In:  Environmental Science and Technology, 36 (5). pp. 914-920.
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    Publikationsdatum: 2016-12-19
    Beschreibung: Using high specific activity 64Cu 2+ as radiotracer, the distribution kinetics among Cu species were established in natural organic-rich freshwaters under steady-state conditions, i.e., with minimal disturbance of existing equilibria. Study sites with contrasting suspended particulate matter (SPM) characteristics were investigated. Our analytical protocol allowed the differentiation between the following Cu species: SPM associated Cu, dissolved reactive (free and labile) Cu, and organically complexed Cu. The data obtained were successfully evaluated by compartmental analysis, which showed the importance of organically complexed Cu in freshwaters, and the dominant role of the interactions between organically complexed Cu and SPM in a SPM-rich water. The kinetic 64Cu measurements indicated that the attainment of equilibrium between dissolved reactive and organically complexed Cu took ca. 〈1-2 h, and 4-15 h for the interaction between dissolved organically complexed and SPM associated Cu. The kinetic study was augmented by voltammetric measurements of the dissolved (stable) Cu equilibrium speciation conditions in the natural waters. These measurements showed that the waters contained very low cupric ion concentrations (10 -12-10 -15 M), with more than 99.9 of the dissolved Cu complexed by strong organic ligands (conditional stability constants: 10 13.4- 10 15.4.
    Materialart: Article , PeerReviewed
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    DOI: 10.1021/es010109m
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  • 5
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    Predominance of heavily calcified coccolithophores at low CaCO3 saturation during winter in the Bay of Biscay (2012)
    National Academy of Sciences
    In:  PNAS Proceedings of the National Academy of Sciences of the United States of America, 109 (23). pp. 8845-8849.
    Details
    Publikationsdatum: 2014-01-27
    Beschreibung: Coccolithophores are an important component of the Earth system, and, as calcifiers, their possible susceptibility to ocean acidification is of major concern. Laboratory studies at enhanced pCO2 levels have produced divergent results without overall consensus. However, it has been predicted from these studies that, although calcification may not be depressed in all species, acidification will produce "a transition in dominance from more to less heavily calcified coccolithophores"Ridgwell A, et al., (2009) Biogeosciences 6:2611-2623. A recent observational study Beaufort L, et al., (2011) Nature 476:80-83 also suggested that coccolithophores are less calcified in more acidic conditions.We present the results of a large observational study of coccolithophore morphology in the Bay of Biscay. Samples were collected once a month for over a year, along a 1,000-km-long transect. Our data clearly show that there is a pronounced seasonality in the morphotypes of Emiliania huxleyi, the most abundant coccolithophore species. Whereas pH and CaCO 3saturation are lowest in winter, the E. huxleyi population shifts from 〈10% (summer) to >90% (winter) of the heavily calcified form. However, it is unlikely that the shifts in carbonate chemistry alone caused the morphotype shift. Our finding that the most heavily calcified morphotype dominates when conditions are most acidic is contrary to the earlier predictions and raises further questions about the fate of coccolithophores in a high-CO2 world.
    Materialart: Article , PeerReviewed
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    DOI: 10.1073/pnas.1117508109
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  • 6
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    Hydroxamate siderophores: Occurrence and importance in the Atlantic Ocean (2008)
    American Chemistry Society
    In:  Environmental Science and Technology, 42 (23). pp. 8675-8680.
    Details
    Publikationsdatum: 2017-10-24
    Beschreibung: Siderophores are chelates produced by bacteria as part of a highly specific iron uptake mechanism. They are thought to be important in the bacterial acquisition of iron in seawater and to influence iron biogeochemistry in the ocean. We have identified and quantified two types of siderophores in seawater samples collected from the Atlantic Ocean. These siderophores were identified as hydroxamate siderophores, both ferrioxamine species representative of the more soluble marine siderophores characterized to date. Ferrioxamine G was widely distributed in surface waters throughout the Atlantic Ocean, while ferrioxamine E had a more varied distribution. Total concentrations of the two siderophores were between 3 and 20 pM in the euphotic zone. If these compounds are fully complexed in seawater, they represent approximately 0.2-4.6 of the 〈0.2 μm iron pool. Our data confirm that siderophore-mediated iron acquisition is important for marine heterotrophic bacteria and indicate that siderophores play an important role in the oceanic biogeochemical cycling of iron. © 2008 American Chemical Society.
    Materialart: Article , PeerReviewed
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    DOI: 10.1021/es801884r
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  • 7
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    Chemical speciation of dissolved Cu, Ni, and Co in a contaminated estuary in southwest Spain and its influence on plankton communities (2007)
    American Chemistry Society
    In:  Environmental Science and Technology, 41 (12). pp. 4214-4220.
    Details
    Publikationsdatum: 2017-10-24
    Beschreibung: Four surveys of the Huelva Estuary in southwest Spain and its sources, the Tinto and the Odiel Rivers, were carried out between 1996 and 1998. The surveys investigated the impact of metalliferous mining of sulfide-rich ores in the catchment area on metal speciation, metal concentrations in a macrophyte, and phytoplankton diversity and abundance. Chemical speciation measurements in the lower Tinto Estuary showed that metals were predominantly electrochemically labile (>99 of total dissolved Cu, Co, and Ni at 10 μM Cu, 424 nM Co, and 500 nM Ni, S = 28). Concentrations of Cu complexing ligands and free cupric ions Cu2+ in the Gulf of Cádiz ranged between 5.3 and 38 nM and 0.2-7.9 pM, respectively, with conditional stability constants of the ligands of log K′CuL = 11.7-12.6. At enhanced dissolved Cu concentrations in the lower Huelva Estuary, Cu complexing ligands were saturated with Cu, resulting in nanomolar Cu2+, which increased upstream. Metal tissue concentrations of the macrophyte Blindingia marginata were high, and a clear relationship between dissolved labile Cu and macrophyte tissue Cu concentrations was observed. A low biodiversity was observed in the Huelva system (Shannon-Wiener indices (H) typically 〈0.2). Nevertheless, the maximum biomass was observed in the lower Tinto Estuary, which showed high labile metal and nutrient concentrations and a low biodiversity (H 〈 0.02), thereby suggesting adaptation through evolutionary processes of the phytoplankton community to the harsh conditions. © 2007 American Chemical Society.
    Materialart: Article , PeerReviewed
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    DOI: 10.1021/es063042h
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  • 8
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    Seasonal ITCZ migration dynamically controls the location of the (sub)tropical Atlantic biogeochemical divide (2014)
    National Academy of Sciences
    In:  PNAS Proceedings of the National Academy of Sciences of the United States of America, 111 (4). pp. 1438-1442.
    Details
    Publikationsdatum: 2021-04-23
    Beschreibung: Inorganic nitrogen depletion restricts productivity in much of the low-latitude oceans, generating a selective advantage for diazotrophic organisms capable of fixing atmospheric dinitrogen (N2). However, the abundance and activity of diazotrophs can in turn be controlled by the availability of other potentially limiting nutrients, including phosphorus (P) and iron (Fe). Here we present high-resolution data (∼0.3°) for dissolved iron, aluminum, and inorganic phosphorus that confirm the existence of a sharp north–south biogeochemical boundary in the surface nutrient concentrations of the (sub)tropical Atlantic Ocean. Combining satellite-based precipitation data with results from a previous study, we here demonstrate that wet deposition in the region of the intertropical convergence zone acts as the major dissolved iron source to surface waters. Moreover, corresponding observations of N2 fixation and the distribution of diazotrophic Trichodesmium spp. indicate that movement in the region of elevated dissolved iron as a result of the seasonal migration of the intertropical convergence zone drives a shift in the latitudinal distribution of diazotrophy and corresponding dissolved inorganic phosphorus depletion. These conclusions are consistent with the results of an idealized numerical model of the system. The boundary between the distinct biogeochemical systems of the (sub)tropical Atlantic thus appears to be defined by the diazotrophic response to spatial–temporal variability in external Fe inputs. Consequently, in addition to demonstrating a unique seasonal cycle forced by atmospheric nutrient inputs, we suggest that the underlying biogeochemical mechanisms would likely characterize the response of oligotrophic systems to altered environmental forcing over longer timescales.
    Materialart: Article , PeerReviewed
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    Format: text
    DOI: 10.1073/pnas.1318670111
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