Rumble Douglas

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Rumble
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Douglas
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  • Preprint
    S-33 constraints on the seawater sulfate contribution in modern seafloor hydrothermal vent sulfides
    ( 2006-11-14) Ono, Shuhei ; Shanks, Wayne C. ; Rouxel, Olivier J. ; Rumble, Douglas
    Sulfide sulfur in mid-oceanic ridge hydrothermal vents is derived from leaching of basaltic-sulfide and seawater-derived sulfate that is reduced during high temperature water rock interaction. Conventional sulfur isotope studies, however, are inconclusive about the mass-balance between the two sources because 34S/32S ratios of vent fluid H2S and chimney sulfide minerals may reflect not only the mixing ratio but also isotope exchange between sulfate and sulfide. Here, we show that high-precision analysis of S-33 can provide a unique constraint because isotope mixing and isotope exchange result in different Δ33S (≡ δ33S – 0.515 δ34S) values of up to 0.04 ‰ even if δ34S values are identical. Detection of such small Δ33S differences is technically feasible by using the SF6 dual-inlet mass-spectrometry protocol that has been improved to achieve a precision as good as 0.006 ‰ (2σ). Sulfide minerals (marcasite, pyrite, chalcopyrite, and sphalerite) and vent H2S collected from four active seafloor hydrothermal vent sites, East Pacific Rise (EPR) 9-10° N, 13° N, and 21° S and Mid-Atlantic Ridge (MAR) 37° N yield Δ33S values ranging from –0.002 to 0.033 and δ34S from –0.5 to 5.3 ‰. The combined δ34S and Δ33S systematics reveal that 73 to 89 % of vent sulfides are derived from leaching from basaltic sulfide and only 11 to 27 % from seawater-derived sulfate. Pyrite from EPR 13° N and marcasite from MAR 37° N are in isotope disequilibrium not only in δ34S but also in Δ33S with respect to associated sphalerite and chalcopyrite, suggesting non-equilibrium sulfur isotope exchange between seawater sulfate and sulfide during pyrite precipitation. Seafloor hydrothermal vent sulfides are characterized by low Δ33S values compared with biogenic sulfides, suggesting little or no contribution of sulfide from microbial sulfate reduction into hydrothermal sulfides at sediment-free mid-oceanic ridge systems. We conclude that 33S is an effective new tracer for interplay among seawater, oceanic crust and microbes in subseafloor hydrothermal sulfur cycles.
  • Preprint
    Sulfur isotope evidence for microbial sulfate reduction in altered oceanic basalts at ODP Site 801
    ( 2008-01-08) Rouxel, Olivier J. ; Ono, Shuhei ; Alt, Jeffrey C. ; Rumble, Douglas ; Ludden, John
    The subsurface biosphere in the basaltic ocean crust is potentially of major importance in affecting chemical exchange between the ocean and lithosphere. Alteration of the oceanic crust commonly yields secondary pyrite that are depleted in 34S relative to igneous sulfides. Although these 34S depleted sulfur isotope ratios may point to signatures of biological fractionation, previous interpretations of sulfur isotope fractionation in altered volcanic rocks have relied on abiotic fractionation processes between intermediate sulfur species formed during basalt alteration. Here, we report results for multiple-S isotope (32S,33S,34S) compositions of altered basalts at ODP Site 801 in the western Pacific and provide evidence for microbial sulfate reduction within the volcanic oceanic crust. In-situ ion-microprobe analyses of secondary pyrite in basement rocks show a large range of δ34S values, between –45‰ and 1‰, whereas bulk rock δ34S analyses yield a more restricted range of –15.8 to 0.9‰. These low and variable δ34S values, together with bulk rock S concentrations ranging from 0.02% up to 1.28% are consistent with loss of magmatic primary mono-sulfide and addition of secondary sulfide via microbial sulfate reduction. High-precision multiple-sulfur isotope (32S/33S/34S) analyses suggest that secondary sulfides exhibit mass-dependent equilibrium fractionation relative to seawater sulfate in both δ33S and δ34S values. These relationships are explained by bacterial sulfate reduction proceeding at very low metabolic rates. The determination of the S-isotope composition of bulk altered oceanic crust demonstrates that S-based metabolic activity of subsurface life in oceanic basalt is widespread, and can affect the global S budget at the crust-seawater interface.
  • Preprint
    Multiple sulphur and iron isotope composition of detrital pyrite in Archaean sedimentary rocks : a new tool for provenance analysis
    ( 2009-06-29) Hofmann, Axel ; Bekker, Andrey ; Rouxel, Olivier J. ; Rumble, Douglas ; Master, Sharad
    Multiple S (δ34S and δ33S) and Fe (δ56Fe) isotope analyses of rounded pyrite grains from 3.1 to 2.6 Ga conglomerates of southern Africa indicate their detrital origin, which supports anoxic surface conditions in the Archaean. Rounded pyrites from Meso- to Neoarchaean gold and uranium-bearing strata of South Africa are derived from both crustal and sedimentary sources, the latter being characterised by non-mass dependent fractionation of S isotopes (Δ33S as negative as -1.35‰) and large range of Fe isotope values (δ56Fe between -1.1 and 1.2‰). Most sediment-sourced pyrite grains are likely derived from sulphide nodules in marine organic matter-rich shales, sedimentary exhalites and volcanogenic massive sulphide deposits. Some sedimentary pyrite grains may have been derived from in situ sulphidised Fe-oxides, prior to their incorporation into the conglomerates, as indicated by unusually high positive δ56Fe values. Sedimentary sulphides without significant non-mass dependent fractionation of S isotopes were also present in the source of some conglomerates. The abundance in these rocks of detrital pyrite unstable in the oxygenated atmosphere may suggest factors other than high pO2 as the cause for the absence of significant non-mass dependent fractionation processes in the 3.2 – 2.7 Ga atmosphere. Rounded pyrites from the ca. 2.6 Ga conglomerates of the Belingwe greenstone belt in Zimbabwe have strongly fractionated δ34S, Δ33S and δ56Fe values, the source of which can be traced back to black shale-hosted massive sulphides in the underlying strata. The study demonstrates the utility of combined multiple S and Fe isotope analysis for provenance reconstruction of Archaean sedimentary successions.