Tracking eolian dust with helium and thorium: Impacts of grain size and provenance

Reconstructions of the deposition rate of windblown mineral dust in ocean sediments offer an important means of tracking past climate changes and of assessing the radiative and biogeochemical impacts of dust in past climates. Dust flux estimates in ocean sediments have commonly been based on the operationally defined lithogenic fraction of sediment samples. More recently, dust fluxes have been estimated from measurements of helium and thorium, as rare isotopes of these elements (He-3 and Th-230) allow estimates of sediment flux, and the dominant isotopes (He-4 and Th-232) are uniquely associated with the lithogenic fraction of marine sediments. In order to improve the fidelity of dust flux reconstructions based on He and Th, we present a survey of He and Th concentrations in sediments from dust source areas in East Asia, Australia and South America. Our data show systematic relationships between He and Th concentrations and grain size, with He concentrations decreasing and Th concentrations increasing with decreasing grain size. We find consistent He and Th concentrations in the fine fraction (<5 μm) of samples from East Asia, Australia and Central South America (Puna-Central West Argentina), with Th concentrations averaging 14 μg/g and He concentrations averaging 2 μcc STP/g. We recommend use of these values for estimating dust fluxes in sediments where dust is dominantly fine-grained, and suggest that previous studies may have systematically overestimated Th-based dust fluxes by 30%. Source areas in Patagonia appear to have lower He and Th contents than other regions, as fine fraction concentrations average 0.8 μcc STP/g and 9 μg/g for 4He and 232Th, respectively. The impact of grain size on lithogenic He and Th concentrations should be taken into account in sediments proximal to dust sources where dust grain size may vary considerably. Our data also have important implications for the hosts of He in long-traveled dust and for the 3He/4He ratio used for terrigenous He in studies of extraterrestrial He in sediments and ice. We also investigate the use of He/Th ratios as a provenance tracer. Our results suggest differences in fine fraction He/Th ratios between East Asia, Australia, central South America and Patagonia, with ratios showing a positive relationship with the geological age of source rocks. He/Th ratios may thus provide useful provenance information, for example allowing separation of Patagonian sources from Puna-Central West Argentina or Australian dust sources. He/Th ratios in open-ocean marine sediments are similar to ratios in the fine fraction of upwind dust source areas. He/Th ratios in mid-latitude South Atlantic sediments suggest that dust in this region primarily derives from the Puna-Central West Argentina region (23–32°S) rather than Patagonia (>38°S). In the equatorial Pacific, He/Th ratios are much lower than in extratropical Pacific sediments or potential source areas measured as a part of this study (East Asia, South America, Australia) for reasons that are at present unclear, complicating their use as provenance tracers in this region.

Nd, Sr and Pb isotopic composition of eolian dust deposited in the central North Pacific

The silicate fractions of recent pelagic sediments in the central north Pacific Ocean are dominated by eolian dust derived from central Asia. An 11 Myr sedimentary record at ODP Sites 885/886 at 44.7°N, 168.3°W allows the evaluation of how such dust and its sources have changed in response to late Cenozoic climate and tectonics. The extracted eolian fraction contains variable amounts (>70%) of clay minerals with subordinate quartz and plagioclase. Uniform Nd isotopic compositions (epsilon-Nd =38.6 to 310.5) and Sm/Nd ratios (0.170-0.192) for most of the 11 Myr record demonstrate a well-mixed provenance in the basins north of the Tibetan Plateau and the Gobi Desert that was a source of dust long before the oldest preserved Asian loess formed. epsilon-Nd values of up to 36.5 for samples 62.9 Ma indicate <=35 wt% admixture of a young, Kamchatka-like volcanic arc component. The coherence of Pb and Nd in the erosional cycle allows us to constrain the Pb isotopic composition of Asian loess devoid of anthropogenic contamination to 206Pb/204Pb =18.97 +/- 0.06, 207Pb/204Pb =15.67 +/- 0.02, 208Pb/204Pb =39.19 +/- 0.11. 87Sr/86Sr (0.711-0.721) and Rb/Sr ratios (0.39-1.1) vary with dust mineralogy and provide an age indication of ~250 Ma. 40Ar/39Ar ages of six dust samples are uniform around 200 Ma and match the K-Ar ages of modern dust deposited on Hawaii. These data reflect the weighted age average of illite formation. Changes from illite- smectite with significant kaolinite to illite- and chlorite-rich, kaolinite-free assemblages since the late Pliocene document changes in the intensity of chemical weathering in the source region. Such weathering evidently did not disturb the K-Ar systematics, and only induced scatter in the Rb-Sr data. We propose that when smectite forms at the expense of illite, K and Ar are quantitatively lost from what becomes smectite, but are quantitatively retained in adjacent illite layers. 40Ar/39Ar age data, therefore, are insensitive to smectite formation during chemical weathering but date the diagenetic growth of illite, the major K-bearing phase in the dust. Over the past 12 Myr, the dust flux to the north Pacific increased by more than an order of magnitude, documenting a substantial drying of central Asia. This climatic change, however, did not alter the ultimate source of the dust, and neoformational products of chemical weathering always remained subordinate to assemblages reworked by mechanical erosion in dust deposited in eastern Asia and the Pacific Ocean.

Late Cenozoic eolian dust accumulation in the eastern equatorial Pacific Ocean

Sediments recovered during Ocean Drilling Program (ODP) Leg 138 in the eastern equatorial Pacific Ocean were analyzed for variations in eolian accumulation rate and mean grain-size. Latitudinal and temporal patterns of these parameters showed important changes in the intensity of atmospheric circulation and eolian flux associated with the intertropical convergence zone (ITCZ) and suggested that eolian input parameters could be used to define its paleoposition through time. Modern atmospheric circulation in the equatorial region is weakest in the intertropical convergence zone and increases as the trade winds are approached to the north and south. Thus, the expected spatial pattern of eolian grain size would have the finest material deposited beneath the ITCZ and a coarsening of material in both directions away from this zone. Sediments from ODP Leg 138 show this pattern for much of the Pleistocene and Pliocene but, prior to about 4 Ma, begin to lose the northern coarse component suggesting that the ITCZ was located north of its present position during the late Miocene. Eolian flux records also show a latitudinal pattern of deposition associated with the position of the ITCZ that, similar to eolian grain-size variability, suggests a more northerly position of the ITCZ during the late Miocene. Overall, the regional input of eolian material to the equatorial Pacific has decreased throughout the late Neogene. This reduction in eolian input reflects climatic changes to relatively wetter conditions in the continental eolian source regions beginning during the late Pliocene.

Accumulation rates and grain sizes of eolian dust in sediments of the Intertropical Convergence Zone in the northeast Pacific

A 328 cm-long piston core (KODOS 02-01-02) collected from the northeast equatorial Pacific at 16°12'N, 125°59'W was investigated for eolian mass fluxes and grain sizes to test these proxies as a tool for the paleo-position of the Intertropical Convergence Zone (ITCZ). The eolian mass fluxes of the lower interval below 250 cm (15.5-7.6 Ma) are very uniform at 5 +/- 1 mg/cm**2/kyr, while those of the upper interval above 250 cm (from 7.6 Ma) are over 2 times higher than the lower interval at 12 +/- 1 mg/cm**2/kyr. The median grain size of the eolian dusts in the lower interval increases from 8.4 Phi to 8.0 Phi downward, while that of the upper interval varies in a narrow range from 8.8 Phi to 8.6 Phi. The determined values compare well in magnitude to those of central Pacific sediments for the upper interval and equatorial and southeast Pacific sediments for the lower interval. This result suggests a possibility that the study site had been under the influence of southeast trade winds at its earlier depositional period due to the northerly position of the ITCZ, and subsequently of the northeast trade winds for a later period when the upper sediments were deposited. This interpretation is consistent with a mineralogical and geochemical study published elsewhere that assigned the provenance of the study core dust to Central/South America for the lower interval and to Asia for the upper interval. This study suggests that the distinct differences in eolian mass flux and grain size observed across the ITCZ can be used to trace the paleo-latitude of the ITCZ.

Geochemistry of eolian dust from sediment core LL44-GPC-3

The large-diameter piston core LL44-GPC3 from the central North Pacific Ocean records continuous sedimentation of eolian dust since the Late Cretaceous. Two intervals resolved by Nd and Pb isotopic data relate to dust coming from America (prior to ~40 Ma) and dust coming from Asia (since ~40 Ma). The Intertropical Convergence Zone (ITCZ) separates these depositional regimes today and may have been at a paleolatitude of ~23°N prior to 40 Ma. Such a northerly location of the ITCZ is consistent with sluggish atmospheric circulation and warm climate for the Northern Hemisphere of the early to middle Eocene. Since ~40 Ma, correlations between Nd (~7.55 > epsilon-Nd(t) > ~10.81) and Pb (18.625 < 206/4Pb < 18.879; 15.624 < 207/4Pb < 15.666; 38.611 < 208/4Pb < 38.960; 0.8294 < 207/6Pb < 0.8389; 2.0539 < 208/6Pb < 2.0743) isotopes reflect the progressive drying of central Asia triggered by the westward retreat of the paleo-Tethys. Comparisons between the changes with time in the isotopically well-defined dust flux and Nd and Pb isotopic compositions of Pacific deep water allow one to draw two major conclusions: (1) dust-bound Nd became a resolvable contribution to Pacific seawater only after the one order of magnitude increase in dust flux starting at ~3.5 Ma. Therefore eolian Nd was unimportant for Pacific seawater Nd prior to 3.5 Ma. (2) The lack of a response of Pacific deep water Pb to this huge flux increase suggests that dust-bound Pb has never been important. Instead, mobile Pb associated with island arc volcanic exhalatives probably consists of a significant contribution to Pacific deep water Pb and possibly to seawater elsewhere far away from landmasses.

Radiogenic Hf isotopic composition of continental eolian dust in Pacific Ocean sediments

The inorganic silicate fraction extracted from bulk pelagic sediments from the North Pacific Ocean is eolian dust. It monitors the composition of continental crust exposed to erosion in Asia. 176Lu/177Hf ratios of modern dust are subchondritic between 0.011 and 0.016 but slightly elevated with respect to immature sediments. Modern dust samples display a large range in Hf isotopic composition (IC), -4.70 < epsilon-Hf < +16.45, which encompasses that observed for the time series of DSDP cores 885/886 and piston core LL44-GPC3 extending back to the late Cretaceous. Hafnium and neodymium isotopic results are consistent with a dominantly binary mixture of dust contributed from island arc volcanic material and dust from central Asia. The Hf-Nd isotopic correlation for all modern dust samples, epsilon-Hf= =0.78 epsilon-Nd = +5.66 (n =22, R**2 =0.79), is flatter than those reported so far for terrestrial reservoirs. Moreover, the variability in epsilon-Hf of Asian dust exceeds that predicted on the basis of corresponding epsilon-Nd values (34.76 epsilon-Hf < +2.5; -10.96< epsilon-Nd <-10.1). This is attributed to: (1) the fixing of an important unradiogenic fraction of Hf in zircons, balanced by radiogenic Hf that is mobile in the erosional cycle, (2) the elevated Lu/Hf ratio in chemical sediments which, given time, results in a Hf signature that is radiogenic compared with Hf expected from its corresponding Nd isotopic components, and (3) the possibility that diagenetic resetting of marine sediments may incorporate a significant radiogenic Hf component into diagenetically grown minerals such as illite. Together, these processes may explain the variability and more radiogenic character of Hf isotopes when compared to the Nd isotopic signatures of Asian dust. The Hf-Nd isotope time series of eolian dust are consistent with the results of modern dust except two samples that have extremely radiogenic Hf for their Nd (epsilon-Hf =+8.6 and +10.3, epsilon-Nd =39.5 and 39.8). These data may point to a source contribution of dust unresolved by Nd and Pb isotopes. The Hf IC of eolian dust input to the oceans may be more variable and more radiogenic than previously anticipated. The Hf signature of Pacific seawater, however, has varied little over the past 20 Myr, especially across the drastic increase of eolian dust flux from Asia around 3.5 Ma. Therefore, continental contributions to seawater Hf appear to be riverine rather than eolian. Current predictions regarding the relative proportions of source components to seawater Hf must account for the presence of a variable and radiogenic continental component. Data on the IC and flux of river-dissolved Hf to the oceans are urgently required to better estimate contributions to seawater Hf. This then would permit the use of Hf isotopes as a monitor of past changes in erosion.

Reconstructions of eolian dust accumulation in northwest African margin sediments

Reconstructions of eolian dust accumulation in northwest African margin sediments provide important continuous records of past changes in atmospheric circulation and aridity in the region. Existing records indicate dramatic changes in North African dust emissions over the last 20 ka, but the limited spatial extent of these records and the lack of high-resolution flux data do not allow us to determine whether changes in dust deposition occurred with similar timing, magnitude and abruptness throughout northwest Africa. Here we present new records from a meridional transect of cores stretching from 31°N to 19°N along the northwest African margin. By combining grain size endmember modeling with 230Th-normalized fluxes for the first time, we are able to document spatial and temporal changes in dust deposition under the North African dust plume throughout the last 20 ka. Our results provide quantitative estimates of the magnitude of dust flux changes associated with Heinrich Stadial 1, the Younger Dryas, and the African Humid Period (AHP; ~11.7-5 ka), offering robust targets for model-based estimates of the climatic and biogeochemical impacts of past changes in North African dust emissions. Our data suggest that dust fluxes between 8 and 6 ka were a factor of ~5 lower than average fluxes during the last 2 ka. Using a simple model to estimate the effects of bioturbation on dust input signals, we find that our data are consistent with abrupt, synchronous changes in dust fluxes in all cores at the beginning and end of the AHP. The mean ages of these transitions are 11.8±0.2 ka (1Sigma) and 4.9±0.2 ka, respectively.

Grain size distribution and bulk chemistry of eolian dust

Atmospheric dust samples collected along a transect off the West African coast have been investigated for their physical (grain-size distribution), mineralogical, and chemical (major elements) composition. On the basis of these data the samples were grouped into sets of samples that most likely originated from the same source area. In addition, shipboard-collected atmospheric meteorological data, modeled 4-day back trajectories for each sampling day and location, and Total Ozone Mapping Spectrometer aerosol index data for the time period of dust collection (February-March 1998) were combined and used to reconstruct the sources of the groups of dust samples. On the basis of these data we were able to determine the provenance of the various dust samples. It appears that the bulk of the wind-blown sediments that are deposited in the proximal equatorial Atlantic Ocean are transported in the lower level (>~900 hPa) NE trade wind layer, which is a very dominant feature north of the Intertropical Convergence Zone (ITCZ). However, south of the surface expression of the ITCZ, down to 5°S, where surface winds are southwesterly, we still collected sediments that originated from the north and east, carried there by the NE trade wind layer, as well as by easterly winds from higher altitudes. The fact that the size of the wind-blown dust depends not only on the wind strength of the transporting agent but also on the distance to the source hampers a direct comparison of the dust's size distributions and measured wind strengths. However, a comparison between eolian dust and terrigenous sediments collected in three submarine sediment traps off the west coast of NW Africa shows that knowledge of the composition of eolian dust is a prerequisite for the interpretation of paleorecords obtained from sediment cores in the equatorial Atlantic.

Geochemical and isotopic characterization of the Bodélé Depression dust source and implications for transatlantic dust transport to the Amazon Basin

The Bodélé Depression (Chad) in the central Sahara/Sahel region of Northern Africa is the most important source of mineral dust to the atmosphere globally. The Bodélé Depression is purportedly the largest source of Saharan dust reaching the Amazon Basin by transatlantic transport. Here, we have undertaken a comprehensive study of surface sediments from the Bodélé Depression and dust deposits (Chad, Niger) in order to characterize geochemically and isotopically (Sr, Nd and Pb isotopes) this dust source, and evaluate its importance in present and past African dust records. We similarly analyzed sedimentary deposits from the Amazonian lowlands in order to assess postulated accumulation of African mineral dust in the Amazon Basin, as well as its possible impact in fertilizing the Amazon rainforest. Our results identify distinct sources of different ages and provenance in the Bodélé Depression versus the Amazon Basin, effectively ruling out an origin for the Amazonian deposits, such as the Belterra Clay Layer, by long-term deposition of Bodélé Depression material. Similarly, no evidence for contributions from other potential source areas is provided by existing isotope data (Sr, Nd) on Saharan dusts. Instead, the composition of these Amazonian deposits is entirely consistent with derivation from in-situ weathering and erosion of the Precambrian Amazonian craton, with little, if any, Andean contribution. In the Amazon Basin, the mass accumulation rate of eolian dust is only around one-third of the vertical erosion rate in shield areas, suggesting that Saharan dust is “consumed” by tropical weathering, contributing nutrients and stimulating plant growth, but never accumulates as such in the Amazon Basin. The chemical and isotope compositions found in the Bodélé Depression are varied at the local scale, and have contrasting signatures in the “silica-rich” dry lake-bed sediments and in the “calcium-rich” mixed diatomites and surrounding sand material. This unexpected finding implies that the Bodélé Depression material is not “pre-mixed” at the source to provide a homogeneous source of dust. Rather, different isotope signatures can be emitted depending on subtle vagaries of dust-producing events. Our characterization of the Bodélé Depression components indicate that the Bodélé “calcium-rich” component, identified here, is most likely released via eolian processes of sand grain saltation and abrasion and may be significant in the overall global budget of dusts carried out by the Harmattan low-level jet during the winter.

Dust flux records from the Subarctic North Pacific

We present a new record of eolian dust flux to the western Subarctic North Pacific (SNP) covering the past 27000 years based on a core from the Detroit Seamount. Comparing the SNP dust record to the NGRIP ice core record shows significant differences in the amplitude of dust changes to the two regions during the last deglaciation, while the timing of abrupt changes is synchronous. If dust deposition in the SNP faithfully records its mobilization in East Asian source regions, then the difference in the relative amplitude must reflect climate-related changes in atmospheric dust transport to Greenland. Based on the synchronicity in the timing of dust changes in the SNP and Greenland, we tie abrupt deglacial transitions in the 230Th-normalized 4He flux record to corresponding transitions in the well-dated NGRIP dust flux record to provide a new chronostratigraphic technique for marine sediments from the SNP. Results from this technique are complemented by radiocarbon dating, which allows us to independently constrain radiocarbon paleoreservoir ages. We find paleoreservoir ages of 745 ± 140 yr at 11653 yr BP, 680 ± 228 yr at 14630 yr BP and 790 ± 498 yr at 23290 yr BP. Our reconstructed paleoreservoir ages are consistent with modern surface water reservoir ages in the western SNP. Good temporal synchronicity between eolian dust records from the Subantarctic Atlantic and equatorial Pacific and the ice core record from Antarctica supports the reliability of the proposed dust tuning method to be used more widely in other global ocean regions.