David Ulfbeck

Origin of Nucleosynthetic Isotope Heterogeneity in the Solar Protoplanetary Disk

Stable-isotope variations exist among inner solar system solids, planets, and asteroids, but their importance is not understood. We report correlated, mass-independent variations of titanium-46 and titanium-50 in bulk analyses of these materials. Because titanium-46 and titanium-50 have different nucleosynthetic origins, this correlation suggests that the presolar dust inherited from the protosolar molecular cloud was well mixed when the oldest solar system solids formed, but requires a subsequent process imparting isotopic variability at the planetary scale. We infer that thermal processing of molecular cloud material, probably associated with volatile-element depletions in the inner solar system, resulted in selective destruction of thermally unstable, isotopically anomalous presolar components, producing residual isotopic heterogeneity. This implies that terrestrial planets accreted from thermally processed solids with nonsolar isotopic compositions.

Evidence for a Late Supernova Injection of 60Fe into the Protoplanetary Disk

High-precision 60Fe-60Ni isotope data show that most meteorites originating from differentiated planetesimals that accreted within 1 million years of the solar systems formation have 60Ni/58Ni ratios that are ∼25 parts per million lower than samples from Earth, Mars, and chondrite parent bodies. This difference indicates that the oldest solar system planetesimals formed in the absence of 60Fe. Evidence for live 60Fe in younger objects suggests that 60Fe was injected into the protoplanetary disk ∼1 million years after solar system formation, when 26Al was already homogeneously distributed. Decoupling the first appearance of 26Al and 60Fe constrains the environment where the Suns formation could have taken place, indicating that it occurred in a dense stellar cluster in association with numerous massive stars.

Rapid and highly reproducible analysis of rare earth elements by multiple collector inductively coupled plasma mass spectrometry

Abstract A method has been developed for the rapid chemical separation and highly reproducible analysis of the rare earth elements (REE) by isotope dilution analysis by means of a multiple collector inductively coupled plasma mass spectrometer (MC-ICP-MS). This technique is superior in terms of the analytical reproducibility or rapidity of analysis compared with quadrupole ICP-MS or with thermal ionization mass spectrometric isotope dilution techniques. Samples are digested by standard hydrofluoric–nitric acid–based techniques and spiked with two mixed spikes. The bulk REE are separated from the sample on a cation exchange column, collecting the middle-heavy and light REE as two groups, which provides a middle-heavy REE cut with sufficient separation of the light from the heavier REE to render oxide interferences trivial, and a Ba-free light REE cut. The heavy (Er-Lu), middle (Eu-Gd), and light REE (La-Eu) concentrations are determined by three short (1 to 2 min) analyses with a CETAC Aridus desolvating nebulizer introduction system. Replicate digestions of international rock standards demonstrate that concentrations can be reproduced to

Rapid sample digestion by fusion and chemical separation of Hf for isotopic analysis by MC-ICPMS

A new method for rapid sample digestion and efficient chemical separation of Hf and REE from rock samples for precise isotopic analysis is presented. Samples are digested by fusion in the presence of a lithium borate flux at 1100 degrees C and dissolved whilst molten in dilute nitric or hydrochloric acid. Prior to chemical separation using ion exchange techniques, Li and B from the flux material and Si from the sample are separated from the remaining major elements, REE and high field strength elements (HFSE) in the sample by Fe-hydroxide co-precipitation. The chemical separation of Hf is a two-stage procedure designed to first remove the remaining matrix elements (e.g. Fe, Ba) in the sample using standard cation exchange techniques, followed by separation of Hf from the REE and HFSE on TEVA extraction chromatographic resin. Hf yields are >90% and total procedural blanks are ca. 50 pg. Hf isotope ratios of a synthetic standard solution and replicate digestions of international rock standards BHVO-1 and BCR-1 measured on multi-collector inductively coupled plasma mass spectrometer (MC-ICPMS) reproduce similarly to </=50 ppm (2 S.D.). The following elemental ratios are routinely obtained for elements, which interfere isobarically or may affect the ionisation and/or fractionation behaviour of Hf during analysis: (176)Yb/(176)Hf<0.0001; (176)Lu/(176)Hf<0.00001; Ti/Hf<0.05. This technique also provides a means of separating Nd from the REE fraction for isotopic analysis and, potentially, may be adapted for measurement of Lu/Hf ratios by isotope dilution techniques.

Hydrothermal-metasomatic and tectono-metamorphic processes in the Isua supracrustal belt (West Greenland): A multi-isotopic investigation of their effects on the Earth's oldest oceanic crustal sequence

Abstract Despite superimposed metamorphic overprinting and metasomatic alterations, primary volcanic features remain preserved in low-strain domains of mafic volcanic sequences in the western Isua supracrustal belt (ISB, West Greenland). These basaltic successions represent the hitherto oldest known fragments of oceanic crust on Earth. Early Archean metasomatic fluids, rich in light rare earth elements (LREE), Th, U, Pb, Ba, and alkalies, invaded the supracrustal package and distinctively altered the basaltic sequences. Field relationships, source characteristics traced by Pb isotopes, and geochronological results provide indications that these fluids were genetically related to the emplacement of tonalite sheets into the ISB between 3.81 and 3.74 Ga ago. Subsequent early Archean metamorphism homogenized the mixed primary and metasomatic mineral parageneses of these metavolcanic rocks. Allanite occurs as the most characteristic and critical secondary metasomatic-metamorphic phase and is developed in macroscopically discernible zones of increased metsomatic alteration, even in domains of low strain. Because of its high concentration of LREE, Th, and U, this secondary mineral accounts for much of the disturbances recorded by the Sm-Nd and Th-U-Pb isotope systematics of the pillowed metabasalts. The supracrustal sequences were tectono-metamorphically affected to varying degrees during a late Archean, ∼2.6- to 2.8-Ga-old event, also recognized in the adjacent gneiss terranes of the Isuakasia area. The degree to which bulk rocks were isotopically reequilibrated is directly dependent on the different relative contributions of allanite-hosted parent-daughter elements to the overall whole-rock mass budget of the respective isotope systems. Although low-strained (initially only weakly metasomatized) pillow basalts remained more or less closed with respect to the U-Pb and Rb-Sr systems since ∼3.74 Ga, the Sm-Nd system appears to have been partially opened on a whole-rock scale during the late Archean event. This diversified behavior of the whole-rock isotope systems with respect to late Archean overprinting is explained by the combination of mass budget contributions of the respective elements added during metasomatism and the partial opening of metasomatic macroenvironments during late Archean recrystallization processes with associated renewed fluid flow. In reactivated zones of high strain, where primary metasomatic alteration is most prominently developed, late Archean partial resetting also of the U-Pb isotope system on a whole-rock scale occurred. This is consistent with an apparent late Archean age of kyanite, which initially crystallized during the early Archean metamorphism. Its age is controlled by the U-Pb systematics of allanite inclusions, which have exchanged their isotopic properties during the tectono-metamorphic event that overprinted the oceanic crustal sequence at Isua more than 1000 myr later. These results underline the need for care in the interpretation of whole-rock geochemical data from polymetamorphic rocks in general, and from the Isua oceanic crustal sequences in particular, to constrain isotopic models of early Earth’s evolution. Likewise, this study cautions against the indiscriminate use of geochemical data of metavolcanic rocks from Isua to infer models for geotectonic settings relevant for their formation.