Biogenic and terrigeneous components in Pliocene-Pleistocene sediments of the equatorial Atlantic

High-resolution analyses of sediments at equatorial Atlantic Sites 662, 663, and 664 define the accumulation rates of biogenically produced CaC03 and opal and of eolian dust from North Africa over the last 3.7 m.y. The mean flux of opal increased abruptly by 60%-70% near 2.5 Ma (2.65 to 2.3 Ma), reflecting pulses of increased opal productivity along the equator due mainly to increased upwelling. The mean winter-plume dust influx from Sahelian and Saharan Africa also increased at this time by between 35% and 75%, following smaller increases earlier in the late Pliocene. The increased opal flux implies a stronger zonal component of the southern trade winds in Southern Hemisphere winter. Consistent with this wind configuration, the stronger dust flux suggests a weaker southwesterly monsoonal flow into Africa in Northern Hemisphere summer, thus increasing Sahelian aridity and winter-plume dust fluxes. Dust fluxes to the equator may possibly have also been enhanced by stronger Northern Hemisphere winter trade winds and a more southerly position of the Intertropical Convergence Zone over Africa. These late Pliocene biogenic and terrigenous flux changes coincided with the appearance of Northern Hemisphere ice sheets, implying an ultimate causal link. The immediate control on changes in tropical circulation may, however, have been changes in the Atlantic sector of the Southern Ocean. A steady background trend of increasing winter-plume dust flux occurred from the late Pliocene until the middle Pleistocene. This may reflect a progressive, tectonically induced aridification of northern and eastern Africa because of the gradual uplift of the Tibetan Plateau.

Sedimentary records of ODP Site 198-1209 on Shatsky Rise

The accumulation of wind blown (eolian) dust in deep-sea sediments reflects the aridity/humidity conditions of the continental region supplying the dust, as well as the "gustiness" of the climate system. Detailed studies of Pleistocene glacial-interglacial dust fluxes suggest changes in accumulation rates corresponding to orbital variations in solar insolation (Milankovitch cycles). While the orbital cycles found in sedimentary archives of the Pleistocene are intricately related to glacial growth and decay, similar global orbital signals recognized in deep-sea sediments of early Paleogene age, the last major greenhouse interval ~65-45 million years ago, could not have been linked to the waxing and waning of large ice sheets. Thus orbital signals recorded in early Paleogene sediments must reflect some other climate response to changes in solar insolation. To explore the potential connection between orbital forcing and the climate processes that control dust accumulation, we generated a high-resolution dust record for ~58 Myr old sediments from Shatsky Rise (ODP Site 1209, paleolatitude ~15°N-20°N). The dust accumulation data provide the first evidence of a correlation between dust flux to the deep sea and orbital cyclicity during the early Paleogene, indicating dust supply responded to insolation forcing during the last major interval of greenhouse climate. Furthermore, the relative amplitude of the dust flux response during the early Paleogene greenhouse was comparable to that during icehouse climates. Thus, subtle variations in solar insolation driven by changes in Earth's orbit about the Sun may have had a similar impact on climate during intervals of overall warmth as they did during glacial-interglacial states.

Rock magnetic, element, and color data of three sediment cores along the Senegalese continental margin

We present a suite of new high-resolution records (0-135 ka) representing pulses of aeolian, fluvial, and biogenic sedimentation along the Senegalese continental margin. A multiproxy approach based on rock magnetic, element, and color data was applied on three cores enclosing the present-day northern limit of the ITCZ. A strong episodic aeolian contribution driven by stronger winds and dry conditions and characterized by high hematite and goethite input was revealed north of 13°N. These millennial-scale dust fluxes are synchronous with North Atlantic Heinrich stadials. Fluvial clay input driven by the West African monsoon predominates at 12°N and varies at Dansgaard-Oeschger time scales while marine productivity is strongly enhanced during the African humid periods and marine isotope stage 5. From latitudinal signal variations, we deduce that the last glacial ITCZ summer position was located between core positions at 12°26' and 13°40'N. Furthermore, this work also shows that submillennial periods of aridity over northwest Africa occurred more frequently and farther south than previously thought.

Terrestrial organic matter in marine sediments of the Central Equatorial Atlantic

Terrestrial organic matter (OM) in pelagic sediments is discussed with regard to depositional processes and land-sea interactions in the modern and past glacial/interglacial Equatorial Atlantic. Special emphasis is placed on a critical evaluation of different analytical approaches (C/N, Rock-Eval Pyrolysis, stable carbon isotopes, palynology, organic petrology, and selected biomarkers) which are currently used for the qualitative and quantitative assessment of terrigenous organic carbon. If binary mixing equations are used to calculate terrestrial and marine proportions of organic carbon, we consider the definition of endmember values to be most critical since these values may be biased by a great number of independent controls. A combination of geochemical methods including optical studies (organic petrology and palynology) is therefore suggested to evaluate each individual proxy. Organic geochemical analyses performed on sediments from the modern and Late Quaternary Equatorial Atlantic evidence fluctuations in eolian supply of terrigenous OM related to changes in intensity of the trade winds. Quantification of this organic fraction leads to differing proportions depending on the approach applied, i.e. the organic carbon isotopic composition or maceral analyses. Modern distribution of terrigenous OM reveals a decrease in supply towards the basin contributing less than a fifth of the total OM in pelagic areas. Organic geochemical data indicate that sedimentation in the modern northeastern Brasil Basin is affected by lateral advection of reworked OM probably from southern source areas. Glacial/interglacial deposits from the pelagic Equatorial Atlantic (ODP Site 663), covering isotopic stages 12 and 11, reveal that deposition of terrigenous OM was higher under past glacial conditions, in correspondence to generally enhanced dust fluxes. Proportions of terrigenous OM, however, never exceed 50% of the total OM according to maceral analyses. Other estimates, recently proposed by Verardo and Ruddiman (1996), are considered to be too high probably for analytical reasons. Palynological records in the Equatorial Atlantic parallel dust records. Increased portions of grass pollen suggest the admixture of C4-plant material under modern and past glacial conditions. It is therefore assumed, as one possible interpetation, that C4-plant debris has an effect on sedimentary d13Corg and might explain differences between isotopic and microscopic quantitative estimates. Using the difference between these two records, we calculate that maximum supply of C4-material remains below 20% of the total OM for the deep modern and past glacial/interglacial Equatorial Atlantic.

Rock magnetic records and geochemical methods of sediment cores off NW Africa

Two gravity cores retrieved off NW Africa at the border of arid and subtropical environments (GeoB 13602-1 and GeoB 13601-4) were analyzed to extract records of Late Quaternary climate change and sediment export. We apply End Member (EM) unmixing to 350 acquisition curves of isothermal remanent magnetization (IRM). Our approach enables to discriminate rock magnetic signatures of aeolian and fluvial material, to determine biomineralization and reductive diagenesis. Based on the occurrence of pedogenically formed magnetic minerals in the fluvial and aeolian EMs, we can infer that goethite formed in favor to hematite in more humid climate zones. The diagenetic EM dominates in the lower parts of the cores and within a thin near-surface layer probably representing the modern Fe**2+/Fe**3+ redox boundary. Up to 60% of the IRM signal is allocated to a biogenic EM underlining the importance of bacterial magnetite even in siliciclastic sediments. Magnetosomes are found well preserved over most of the record, indicating suboxic conditions. Temporal variations of the aeolian and fluvial EMs appear to faithfully reproduce and support trends of dry and humid conditions on the continent. The proportion of aeolian to fluvial material was dramatically higher during Heinrich Stadials, especially during Heinrich Stadial 1. Dust export from the Arabian-Asian corridor appears to vary contemporaneous to increased dust fluxes on the continental margin of NW Africa emphasizing that melt-water discharge in the North Atlantic had an enormous impact on atmospheric dynamics.

He isotope, U/Th isotope, Calcium carbonate, biogenic opal, rare earth element concentrations, and grain size distribution measured on core-top sediments during SONNE cruise SO202 (INOPEX)

Eolian dust is a significant source of iron and other nutrients that are essential for the health of marine ecosystems and potentially a controlling factor of the high nutrient-low chlorophyll status of the Subarctic North Pacific. We map the spatial distribution of dust input using three different geochemical tracers of eolian dust, 4He, 232Th and rare earth elements, in combination with grain size distribution data, from a set of core-top sediments covering the entire Subarctic North Pacific. Using the suite of geochemical proxies to fingerprint different lithogenic components, we deconvolve eolian dust input from other lithogenic inputs such as volcanic ash, ice-rafted debris, riverine and hemipelagic input. While the open ocean sites far away from the volcanic arcs are dominantly composed of pure eolian dust, lithogenic components other than eolian dust play a more crucial role along the arcs. In sites dominated by dust, eolian dust input appears to be characterized by a nearly uniform grain size mode at ~4 µm. Applying the 230Th-normalization technique, our proxies yield a consistent pattern of uniform dust fluxes of 1-2 g/m**2/yr across the Subarctic North Pacific. Elevated eolian dust fluxes of 2-4 g/m**2/yr characterize the westernmost region off Japan and the southern Kurile Islands south of 45° N and west of 165° E along the main pathway of the westerly winds. The core-top based dust flux reconstruction is consistent with recent estimates based on dissolved thorium isotope concentrations in seawater from the Subarctic North Pacific. The dust flux pattern compares well with state-of-the-art dust model predictions in the western and central Subarctic North Pacific, but we find that dust fluxes are higher than modeled fluxes by 0.5-1 g/m**2/yr in the northwest, northeast and eastern Subarctic North Pacific. Our results provide an important benchmark for biogeochemical models and a robust approach for downcore studies testing dust-induced iron fertilization of past changes in biological productivity in the Subarctic North Pacific.

(Table 2) Seasonal flux data and percentages of major bulk components of total flux at the mesotrophic sediment trap site CB from 1988 - 2012

A more than two-decadal sediment trap record from the Eastern Boundary Upwelling Ecosystem (EBUE) off Cape Blanc, Mauritania, is analysed with respect to deep ocean mass fluxes, flux components and their variability on seasonal to decadal timescales. The total mass flux revealed interannual fluctuations which were superimposed by fluctuations on decadal timescales. High winter fluxes of biogenic silica (BSi), used as a measure of marine production (mostly by diatoms) largely correspond to a positive North Atlantic Oscillation (NAO) index (December-March). However, this relationship is weak. The highest positive BSi anomaly was in winter 2004-2005 when the NAO was in a neutral state. More episodic BSi sedimentation events occurred in several summer seasons between 2001 and 2005, when the previous winter NAO was neutral or even negative. We suggest that distinct dust outbreaks and deposition in the surface ocean in winter and occasionally in summer/autumn enhanced particle sedimentation and carbon export on short timescales via the ballasting effect. Episodic perturbations of the marine carbon cycle by dust outbreaks (e.g. in 2005) might have weakened the relationships between fluxes and large-scale climatic oscillations. As phytoplankton biomass is high throughout the year, any dry (in winter) or wet (in summer) deposition of fine-grained dust particles is assumed to enhance the efficiency of the biological pump by incorporating dust into dense and fast settling organic-rich aggregates. A good correspondence between BSi and dust fluxes was observed for the dusty year 2005, following a period of rather dry conditions in the Sahara/Sahel region. Large changes of all bulk fluxes occurred during the strongest El Niño-Southern Oscillation (ENSO) in 1997-1999 where low fluxes were obtained for almost 1 year during the warm El Niño and high fluxes in the following cold La Niña phase. For decadal timescales, Bakun (1990) suggested an intensification of coastal upwelling due to increased winds (''Bakun upwelling intensification hypothesis''; Cropper et al., 2014) and global climate change. We did not observe an increase of any flux component off Cape Blanc during the past 2 and a half decades which might support this. Furthermore, fluxes of mineral dust did not show any positive or negative trends over time which might suggest enhanced desertification or ''Saharan greening'' during the last few decades.

(Table 1) Insoluble aerosol concentrations and vertical fluxes at the eastern shelf of the Black Sea during breeze circulation in October 1987

Amounts of aerosols transported to the shelf surface were calculated on the basis of in situ measurements of concentrations of eolian matter (insoluble aerosol fraction) and vertical fluxes of settling dust in five areas of the Black Sea shelf from the Danube delta to the Inguri River mouth. More than 8.3 mln t of eolian matter are annually transported from the land over the shelf of the former USSR. At the same time more than 5.4 mln t are supplied to the northwestern shelf area, 1.7 mln t are supplied to the Crimean area, about 0.8 mln t are supplied to the Kerch-Taman' area, and about 0.45 mln t are supplied to the Caucasian area.

Iron (Fe) concentrations and fluxes in TALDICE ice core 0.6 to 314 ky BP

Atmospheric fluxes of iron (Fe) over the past 200 kyr are reported for the coastal Antarctic Talos Dome ice core, based on acid leachable Fe concentrations. Fluxes of Fe to Talos Dome were consistently greater than those at Dome C, with the greatest difference observed during interglacial climates. We observe different Fe flux trends at Dome C and Talos Dome during the deglaciation and early Holocene, attributed to a combination of deglacial activation of dust sources local to Talos Dome and the reorganisation of atmospheric transport pathways with the retreat of the Ross Sea ice shelf. This supports similar findings based on dust particle sizes and fluxes and Rare Earth Element fluxes. We show that Ca and Fe should not be used as quantitative proxies for mineral dust, as they all demonstrate different deglacial trends at Talos Dome and Dome C. Considering that a 20 ppmv decrease in atmospheric CO2 at the coldest part of the last glacial maximum occurs contemporaneously with the period of greatest Fe and dust flux to Antarctica, we confirm that the maximum contribution of aeolian dust deposition to Southern Ocean sequestration of atmospheric CO2 is approximately 20 ppmv.

Characteristics and aldehyde concentrations of diamond dust events near Barrow, Alaska

Diamond dust (DD) refers to tiny ice crystals that form frequently in the Polar troposphere under clear sky conditions. They provide surfaces for chemical reactions and scatter light. We have measured the specific surface area (SSA) of DD at Barrow in March-April 2009. We have also measured its chemical composition in mineral and organic ions, dissolved organic carbon (DOC), aldehydes, H2O2, and the absorption spectra of water-soluble chromophores. Mercury concentrations were also measured in spring 2006, when conditions were similar. The SSA of DD ranges from 79.9 to 223 m**2/kg . The calculated ice surface area in the atmosphere reaches 11000 (±70%) µm**2/cm**3, much higher than the aerosol surface area. However, the impact of DD on the downwelling and upwelling light fluxes in the UV and visible is negligible. The composition of DD is markedly different from that of snow on the surface. Its concentrations in mineral ions are much lower, and its overall composition is acidic. Its concentrations in aldehydes, DOC, H2O2 and mercury are much higher than in surface snows. Our interpretation is that DOC from the oceanic surface microlayer, coming from open leads in the ice off of Barrow, is taken up by DD. Active chemistry in the atmosphere takes place on DD crystal surfaces, explaining its high concentrations in aldehydes and mercury. After deposition, active photochemistry modifies DD composition, as seen from the modifications in its absorption spectra and aldehyde and H2O2 content. This probably leads to the emissions of reactive species to the atmosphere.