Steven J. Goldstein

Chemical and isotopic constraints on the generation and transport of magma beneath the East Pacific Rise

Abstract Interpretation of U-series disequilibria in midocean ridge basalts is highly dependent on the bulk partition coefficients for U and Th and therefore the mineralogy of the mantle source. Distinguishing between the effect of melting processes and variable source compositions on measured disequilibria (238U-230Th-226Ra and 235U-231Pa) requires measurement of the radiogenic isotopes Hf, Nd, Sr, and Pb. Here, we report measurements of 238U-230Th-226Ra and 235U-231Pa disequilibria; Hf, Nd, Sr, and Pb isotopic; and major and trace element compositions for a suite of 20 young midocean ridge basalts from the East Pacific Rise axis between 9°28′ and 9°52′N. All of the samples were collected within the axial summit trough using the submersible Alvin. The geological setting and observational data collected during sampling operations indicate that all the rocks are likely to have been erupted from 1991 to 1992 or within a few decades of that time. In these samples, 230Th excesses and 226Ra excesses are variable and inversely correlated. Because the eruption ages of the samples are much less than the half-life of 226Ra, this inverse correlation between 230Th and 226Ra excesses can be considered a primary feature of these lavas. For the lava suite analyzed in this study, 226Ra and 230Th excesses also vary with lava composition: 226Ra excesses are negatively correlated with Na8 and La/Yb and positively correlated with Mg#. Conversely, 230Th excesses are positively correlated with Na8 and La/Yb and negatively correlated with Mg#. Th/U, 230Th/232Th, and 230Th excesses are also variable and correlated to one another. 231Pa excesses are large but relatively constant and independent of Mg#, La/Yb, Th/U, and Na8. The isotope ratios 143Nd/144Nd, 176Hf/177Hf, 87Sr/86Sr, and 208Pb/206Pb are constant within analytical uncertainty, indicating that they were derived from a common source. The source is homogeneous with respect to parent/daughter ratios Lu/Hf, Sm/Nd, Rb/Sr, and Th/U; therefore, the measured variations of Th/U, 230Th, and 226Ra excesses and major and trace element compositions in these samples are best explained by polybaric melting of a homogeneous source, not by mixing of compositionally distinct sources.

Porosity of the melting zone and variations in the solid mantle upwelling rate beneath Hawaii: inferences from 238U-230Th-226Ra and 235U-231Pa disequilibria

Abstract Measurements of 238U-230Th-226Ra and 235U-231Pa disequilibria in a suite of tholeiitic-to-basanitic lavas provide estimates of porosity, solid mantle upwelling rate and melt transport times beneath Hawaii. The observation that (230Th/238U) > 1 indicates that garnet is required as a residual phase in the magma sources for all of the lavas. Both chromatographic porous flow and dynamic melting of a garnet peridotite source can adequately explain the combined U-Th-Ra and U-Pa data for these Hawaiian basalts. For chromatographic porous flow, the calculated maximum porosity in the melting zone ranges from 0.3–3% for tholeiites and 0.1–1% for alkali basalts and basanites, and solid mantle upwelling rates range from 40 to 100 cm yr−1 for tholeiites and from 1 to 3 cm yr−1 for basanites. For dynamic melting, the escape or threshold porosity is 0.5–2% for tholeiites and 0.1–0.8% for alkali basalts and basanites, and solid mantle upwelling rates range from 10 to 30 cm yr−1 for tholeiites and from 0.1 to 1 cm yr−1 for basanites. Assuming a constant melt productivity, calculated total melt fractions range from 15% for the tholeiitic basalts to 3% for alkali basalts and basanites.

Th and U isotopic systematics of basalts from the Juan de Fuca and Gorda Ridges by mass spectrometry

We have developed a mass spectrometric technique for the measurement of 230Th/232Th ratios in young volcanic rocks. We show that we can measure 230Th/232Th ratios on MORB samples of ∼- 1 gram with an accuracy and reproducibility of 0.5–1.0%. This represents an improvement of at least a factor of 5–10 in sample size and precision over conventional alpha spectrometry methods. Using this technique, we have measured distinct excesses of230Th activity relative to238U activity for axial samples from the Juan de Fuca (JDF) and Gorda Ridges. These enrichments are 13–15% but range up to 40% in one sample. Low boron concentrations and 234U/238U ratios corresponding to secular equilibrium verify the absence of detectable seawater contamination. From this we infer that primary magmatic processes are the source of the measured230Th activity excesses, and that Th is indeed more incompatible than U during partial melting of MORB sources. 230Th/232Th activity ratios for the axial samples from JDF appear to be relatively high for uncontaminated MORB, ranging from 1.35 to 1.41. From this we infer that the JDF basalts formed from a uniform source highly depleted in Th relative to U (Th/Uwt= 2.15–2.25). One Gorda axial sample has a somewhat lower 230Th/232Th activity ratio of 1.31, suggesting formation from a source only slightly less depleted (Th/U= 2.32 ± 0.02). Based on the small range in 30Th/232Th ratios for axial basalts from JDF, dating off-axis JDF basalts may be feasible.

Mechanisms of Magma Generation Beneath Hawaii and Mid-Ocean Ridges: Uranium/Thorium and Samarium/Neodymium Isotopic Evidence

Measurements of uranium/thorium and samarium/neodymium isotopes and concentrations in a suite of Hawaiian basalts show that uranium/thorium fractionation varies systematically with samarium/neodymium fractionation and major-element composition; these correlations can be understood in terms of simple batch melting models with a garnet-bearing peridotite magma source and melt fractions of 0.25 to 6.5 percent. Midocean ridge basalts shows a systematic but much different relation between uranium/thorium fractionation and samarium/neodymium fractionation, which, although broadly consistent with melting of a garnet-bearing peridotite source, requires a more complex melting model.

Geochronology and petrogenesis of MORB from the Juan de Fuca and Gorda ridges by 238U– 230Th disequilibrium

A highly precise mass spectrometric method of analysis was used to determine238U—234U—230Th—232Th in axial and off-axis basalt glasses from Juan de Fuca (JDF) and Gorda ridges. Initial230Th activity excesses in the axial samples range from 3 to 38%, but generally lie within a narrow range of 12 to 15%. Secondary alteration effects were evaluated usingδ234U and appear to be negligible; hence the230Th excesses are magmatic in origin. Direct dating of MORB was accomplished by measuring the decrease in excess230Th in off-axis samples.238U—230Th ages progressively increase with distance from axis. Uncertainties in age range from 10 to 25 ka for U—Th ages of 50 to 200 ka. The full spreading rate based on U—Th ages for Endeavour segment of JDF is 5.9 ± 1/2 cm/yr, with asymmetry in spreading between the Pacific (4.0 ± 0.6 cm/yr) and JDF (1.9 ± 0.6 cm/yr) plates. For northern Gorda ridge, the half spreading rate for the JDF plate is found to be 3.0 ± 0.4 cm/yr. These rates are in agreement with paleomagnetic spreading rates and topographic constraints. This suggests that assumptions used to determine ages, including constancy of initial 230Th/232Th ratio over time, are generally valid for the areas studied. Samples located near the axis of spreading are typically younger than predicted by these spreading rates, which most likely reflects recent volcanism within a 1–3 km wide zone of crustal accretion. Initial230Th/232Th ratios and230Th activity were also used to examine the recent Th/U evolution and extent of melting of mantle sources beneath these ridges. A negative anomaly in 230Th/232Th for Axial seamount lavas provides the first geochemical evidence of a mantle plume source for Axial seamount and the Cobb-Eickelberg seamount chain and indicates recent depletion of other JDF segment sources. Large230Th activity excesses for lavas from northern Gorda ridge and Endeavour segment indicate formation from a lower degree of partial melting than other segments. An inverse correlation between230Th excess and 230Th/232Th for each ridge indicates that these lower degree melts formed from slightly less depleted sources than higher degree melts. Uniformity in230Th excess for other segments suggests similarity in processes of melt formation and mixing beneath most of the JDF-Gorda ridge area. The average initial230Th/232Th activity ratio of 1.31 for the JDF-Gorda ridge area is in agreement with the predicted value of 1.32 from the Th—Sr isotope mantle array.

231Pa and230Th chronology of mid-ocean ridge basalts

Mass spectrometric measurements of235U231Pa and238U230Th disequilibria are used to further constrain processes producing U-series disequilibria in young mid-ocean ridge basalts (MORB) and to determine eruption ages for samples from 9–10°N East Pacific Rise and Juan de Fuca-Gorda ridges.231Pa/235U activity ratios for axial basalts are large and relatively uniform within ridge segments. The systematically large231Pa/235U,230Th/238U, and226Ra/230Th activity ratios in MORB are inconsistent with simple equilibrium melting models and crustal contamination or seawater alteration processes. More complicated melting processes involving disequilibrium or heterogeneous melting of mantle sources and disequilibrium transport of melts to the crust could produce the large U-series disequilibria in MORB. 231Pa and230Th model ages were determined by estimating initial231Pa/235U and230Th/232Th ratios from axial samples and by assuming constancy of these ratios over time. All231Pa and230Th ages agree to ±0–7 ka for samples with ages of 0–130 ka. These concordant ages validate the model assumptions of the two dating methods and suggest that mantle sources and melt generation processes have been uniform for these areas during the past 130 ka. Consequently,231Pa and230Th age-dates can be used to quantify the temporal and spatial dependence of volcanism at oceanic spreading centers during the past 375 ka.

Techniques for Measuring Uranium-series Nuclides: 1992–2002

Advances in geochemistry and geochronology are often closely linked to development of new technologies for improved measurement of elemental and isotopic abundance. At the beginning of the past decade, thermal ionization mass spectrometric (TIMS) methods were just beginning to be applied for long-lived uranium-series nuclide measurement (Edwards et al. 1987; Goldstein et al. 1989; Bard et al. 1990), with considerable advances in measurement speed, precision, and sensitivity over decay-counting methods. This opened up a vast number of applications in uranium-series geochronology and geochemistry of young sediments, volcanic rocks, and aqueous systems. Over the past decade there have continued to be advances in thermal ionization techniques, and the advent of alternative mass spectrometric methods, particularly multi-collector inductively coupled plasma mass spectrometry (MC-ICPMS), has continued to improve the quality of uranium-series studies. So the past decade has been a particularly dynamic time for not only development of mass spectrometric techniques, but initiation of other methods related to long-lived uranium-series nuclide measurement. In the area of sample preparation, further development of microwave digestion methods had led to advances in speed and cost of analysis. In chemical separations, development of extraction chromatographic resins for isolating specific elements have simplified many separation problems and consequently improved analytical characteristics including sensitivity, speed of analysis, waste generation, and cost. With regard to instrumental analysis, advances in both decay-counting and mass spectrometry instrumentation have improved either measurement sensitivity or precision, speed of analysis, or analytical cost. One could argue that instrumental developments will continue to drive scientific breakthroughs in the application of uranium-series nuclides as tracers and chronometers in the earth and other sciences. In this chapter we discuss improvements documented in the literature over the past decade in these areas and others. Chemical procedures, decay-counting spectroscopy, and mass spectrometric techniques published prior to 1992 were …

226Ra-230Th disequilibrium in axial and off-axis mid-ocean ridge basalts☆

The authors describe [sup 226]Ra-[sup 230]Th disequilibrium in mid-ocean ridge basalt (MORB) glasses from the Juan de Fuca, Gorda, and East Pacific ridges. These first mass spectrometric measurements of [sup 226]Ra in MORB glasses at sub-picogram abundance levels confirm the large excesses over [sup 230]Th determined by radon-emanation techniques and alpha spectrometry. All off-axis MORB glasses have [sup 226]Ra-[sup 230]Th and [sup 234]U-[sup 238]U in secular equilibrium. This suggests that magmatic processes, not secondary post-eruption alteration, generate [sup 238]U-series disequilibrium in these MORB. Least evolved, N-MORB from axial valleys have ([sup 226]Ra/[sup 230]Th) between 2.2-2.3. Differentiated and enriched E-type MORB have consistently low ([sup 226]Ra/[sup 230]Th) ratios compared with N-MORB from the same ridge sections. Ra-Th fractionation may be less pronounced, or magma residence-transit periods may be long for differentiated MORB. Also, E-MORB may be generated by different melt extraction volumes and rates. Estimated [sup 226]Ra-[sup 230]Th ages for N-MORB agree with location on and off ridge segments, and with Th-U model ages. These preliminary results show that [sup 226]Ra-[sup 230]Th disequilibrium could be used to quantify volcanic episodicity at ocean ridges. 39 refs., 6 figs., 4 tabs.

Uranium-series and radiocarbon geochronology of deep-sea corals: implications for Southern Ocean ventilation rates and the oceanic carbon cycle

We present new uranium-series and radiocarbon measurements for deep-sea corals from the Southern Ocean. These data are used to reconstruct ventilation ages, both at present and at the end of the last glacial period approximately 16 500 years ago. We apply an improved two-component mixing approach to correct uranium-series dates for contaminant thorium and protactinium present in oxide coatings. Calculated seawater radiocarbon values for contemporary samples decrease with depth in the water column and agree with direct seawater radiocarbon measurements for this area. This indicates that deep-sea corals can accurately record seawater radiocarbon distributions. Two of three glacial samples experienced open-system uranium-series systematics, however, a third sample from the Drake Passage yields concordant thorium and protactinium dates as well as seawater values for initial 234U/238U. This coral yields a ventilation age that is approximately 20–40% greater than modern values for its location. This increase is consistent with published deep-sea coral and calibrated planktonic–benthic foraminifera radiocarbon data, suggesting that the glacial oceans as a whole may have been substantially less ventilated, presumably due to decreased formation of North Atlantic Deep Water. An overall decrease in oceanic mixing rates could have contributed to lower dissolved carbon in surface ocean water and lower atmospheric pCO2 during the past glacial period.

Uranium-series age constraints on lavas from the axial valley of the Mid-Atlantic Ridge, MARK area

Abstract Mass spectrometric measurements of 230 Th– 226 Ra, 235 U– 231 Pa and 238 U– 230 Th disequilibria are used to determine eruption ages for four mid-ocean ridge basalts from the median valley of the Mid-Atlantic Ridge south of the Kane Fracture Zone (MARK area). Three samples were collected across-axis on the Axial Volcanic Ridge (i.e. the Neovolcanic Ridge) near the Snake Pit hydrothermal mound, and one sample was collected near the crest of Serocki Volcano ∼50 km south of Snake Pit. ( 226 Ra)/( 230 Th) and ( 230 Th)/( 238 U) activity ratios are low and uniform for all four samples, while ( 231 Pa)/( 235 U) activity ratios are elevated and somewhat more variable. Age constraints suggest that these lavas, from the most robust volcanic edifices in the MARK area, are 10 000–20 000 yr old. The age data are used to evaluate the efficacy of commonly used age estimate scales based on qualitative indicators (e.g. sediment cover, glass quality) and to begin to quantify the temporal and spatial dependence of volcanic, tectonic and hydrothermal processes at slow-spreading oceanic ridges.