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Uranium interference is a major problem in conventional 238Pu analysis. In RIMS, a slight detuning of the resonance laser extinguishes the Pu signal so that the 238U interference can be accurately quantified and subtracted.

Timing Solar System formation The oldest solids that formed in the Solar System are calcium-aluminium–rich inclusions (CAIs), small metallic droplets that were later incorporated into meteorites. The ages of CAIs are conventionally taken as the age of the Solar System, but which exact moment in star formation they correspond to has been unclear. Brennecka et al. measured molybdenum isotope ratios in CAIs and found a wide range of origins in both the inner and outer Solar System. They propose that CAIs formed from heterogeneous material accreting from the presolar nebula and that the ages of CAIs coincide with the Sun's transition from a protostar to a pre–main sequence star. Science , this issue p. 837

Significance Understanding the history of volatile species such as water in the Earth–Moon system is a major objective of planetary science. In this work, we use the moderately volatile element Rb, which has a long-lived isotope ( 87 Rb) that decays to 87 Sr, to show that lunar volatile element depletion was not caused by the Moon-forming impact. The Rb–Sr systematics of lunar rocks mandate that the bodies involved in the impact that formed the Earth–Moon system were depleted in volatile elements relative to the bulk solar system prior to the impact. As such, Earth’s relatively small proportion of water is either primarily indigenous or was added after the Giant Impact from a source that contained essentially no moderately volatile elements.

Calcium-aluminum-rich inclusions (CAIs) are the first solids to form in the early Solar System, and they exhibit nucleosynthetic anomalies in many isotope systems. The overwhelming majority of isotopic data for CAIs has been limited to inclusions from the CV chondrite Allende and a select few other CV, CO, CM, and ordinary chondrites. It is therefore important to ascertain whether previously reported values for CAIs are representative of the broader CAI-forming region and to make a more rigorous assessment of the extent and implications of isotopic heterogeneity in the early Solar System. Here, we report the mass-independent Ti isotopic compositions of a suite of 23 CAIs of diverse petrologic and geochemical types, including 11 from Allende and 12 from seven other CV3 and CK3 chondrites; the data for CAIs from CK chondrites represent the first reported measurements of Ti isotope compositions of refractory inclusions from this meteorite class. The resolved variation in the mass-independent Ti isotopic compositions of these CAIs indicates that the CAI-forming region of the early Solar System preserved isotopic variability at their time of formation. Nevertheless, the range of Ti isotope compositions reported here for CAIs from CV and CK chondrites falls within the range observed in previously analyzed CAIs from CV, CO, CM, and ordinary chondrites. This implies that CAIs from CV, CK, CO, CM, and ordinary chondrites originated from a common nebular source reservoir characterized by mass-independent isotopic variability in Ti (and other select elements). We further interpret these data to indicate that the Ti isotope anomalies in CAIs represent the isotopic signatures of supernova components in presolar grains that were incorporated into the Solar System in an initially poorly mixed reservoir that was progressively homogenized over time. We conclude that the differing degrees of isotopic variability observed for different elements in normal CAIs are the result of distinct carrier phases and that these CAIs were likely formed towards the final stages of homogenization of the large-scale isotopic heterogeneity that initially existed in the solar nebula.

The last thirty years of cosmochemistry and planetary science have shown that one major Solar System reservoir is vastly undersampled in the available suite of extra-terrestrial materials, namely small bodies that formed in the outer Solar System (>10 AU). Because various dynamical evolutionary processes have modified their initial orbits (e.g., giant planet migration, resonances), these objects can be found today across the entire Solar System as P/D near-Earth and main-belt asteroids, Jupiter and Neptune Trojans, comets, Centaurs, and small (diameter < 200 km) trans-Neptunian objects. This reservoir is of tremendous interest, as it is recognized as the least processed since the dawn of the Solar System and thus the closest to the starting materials from which the Solar System formed. Some of the next major breakthroughs in planetary science will come from studying outer Solar System samples (volatiles and refractory constituents) in the laboratory. Yet, this can only be achieved by an L-class mission that directly collects and returns to Earth materials from this reservoir. It is thus not surprising that two White Papers advocating a sample return mission of a primitive Solar System small body (ideally a comet) were submitted to ESA in response to its Voyage 2050 call for ideas for future L-class missions in the 2035-2050 time frame. One of these two White Papers is presented in this article., Experimental Astronomy, 54 (2-3), ISSN:0922-6435, ISSN:1572-9508

Description, CAIs, the oldest solids in the Solar System, probably formed further away from the Sun than previously thought., Calcium-aluminum–rich inclusions (CAIs) in meteorites carry crucial information about the environmental conditions of the nascent Solar System prior to planet formation. Based on models of 50V–10Be co-production by in-situ irradiation, CAIs are considered to have formed within ~0.1 AU from the proto-Sun. Here, we present vanadium (V) and strontium (Sr) isotopic co-variations in fine- and coarse-grained CAIs and demonstrate that kinetic isotope effects during partial condensation and evaporation best explain V isotope anomalies previously attributed to solar particle irradiation. We also report initial excesses of 10Be and argue that CV CAIs possess essentially a homogeneous level of 10Be, inherited during their formation. Based on numerical modeling of 50V–10Be co-production by irradiation, we show that CAI formation during protoplanetary disk build-up likely occurred at greater heliocentric distances than previously considered, up to planet-forming regions (~1AU), where solar particle fluxes were sufficiently low to avoid substantial in-situ irradiation of CAIs.

Calcium-aluminum-rich inclusions (CAIs) are the oldest dated materials that provide crucial information about the isotopic reservoirs present in the early Solar System. For a variety of elements, CAIs have isotope compositions that are uniform yet distinct from later formed solid material. However, despite being the most abundant metal in the Solar System, the isotopic composition of Fe in CAIs is not well constrained. In an attempt to determine the Fe isotopic compositions of CAIs, we combine extensive work from a previously studied CAI sample set with new isotopic work characterizing mass-dependent and mass-independent (nucleosynthetic) signatures in Mg, Ca, and Fe. This investigation includes work on three mineral separates of the Allende CAI Egg 2. For all isotope systems investigated, we find that in general, fine-grained CAIs exhibit light mass-dependent isotopic signatures relative to terrestrial standards, whereas igneous CAIs have heavier isotopic compositions relative to the fine-grained CAIs. Importantly, the mass-dependent Fe isotope signatures of bulk CAIs show a range of both light (fine-grained CAIs) and heavy (igneous CAIs) isotopic signatures relative to bulk chondrites, suggesting that Fe isotope signatures in CAIs largely derive from mass fractionation events such as condensation and evaporation occurring in the nebula. Such signatures show that a significant portion of the secondary alteration experienced by CAIs, particularly prevalent in fine-grained inclusions, occurred in the nebula prior to accretion into their respective parent bodies. Regarding nucleosynthetic Fe isotope signatures, we do not observe any variation outside of analytical uncertainty in bulk CAIs compared to terrestrial standards. In contrast, all three Egg 2 mineral separates display resolved mass-independent excesses in (56)Fe compared to terrestrial standards. Furthermore, we find that the combined mass-dependent and nucleosynthetic Fe isotopic compositions of the Egg 2 mineral separates are well correlated, likely indicating that Fe indigenous to the CAI is mixed with less anomalous Fe, presumably from the solar nebula. Thus, these reported nucleosynthetic anomalies may point in the direction of the original Fe isotope composition of the CAI-forming region, but they likely only provide a minimum isotopic difference between the original mass-independent Fe isotopic composition of CAIs and that of later formed solids.

Isotopic anomalies in chondrules hold important clues about the dynamics of mixing and transport processes in the solar accretion disk. These anomalies have been interpreted to indicate either disk-wide transport of chondrules or local heterogeneities of chondrule precursors. However, all previous studies relied on isotopic data for a single element (either Cr, Ti, or O), which does not allow distinguishing between source and precursor signatures as the cause of the chondrules isotope anomalies. Here we obtained the first combined O, Ti, and Cr isotope data for individual chondrules from enstatite, ordinary, and carbonaceous chondrites. We find that chondrules from non-carbonaceous (NC) chondrites have relatively homogeneous {\Delta}17O, {\epsilon}50Ti, and {\epsilon}54Cr, which are similar to the compositions of their host chondrites. By contrast, chondrules from carbonaceous chondrites (CC) have more variable compositions. Although the compositions of the analyzed CC and NC chondrules may overlap for either {\epsilon}50Ti, {\epsilon}54Cr, or {\Delta}17O, in multi-isotope space none of the CC chondrules plot in the compositional field of NC chondrites, and no NC chondrule plots within the field of CC chondrites. As such, our data reveal a fundamental isotopic difference between NC and CC chondrules, which is inconsistent with a disk-wide transport of chondrules across and between the NC and CC reservoirs. Instead, the isotopic variations among CC chondrules reflect local precursor heterogeneities, which most likely result from mixing between NC-like dust and a chemically diverse dust component that was isotopically similar to CAIs and AOAs.The same mixing processes, but on a larger, disk-wide scale, were likely responsible for establishing the distinct isotopic compositions of the NC and CC reservoirs, which represent in inner and outer disk, respectively., Comment: 1 Table 5 Figures Supplementary Materials: 1 Table, 1Figure

Uranium ore is mined and milled to produce uranium ore concentrate (UOC), a regulated product of the nuclear fuel cycle. Diversion of UOC from the fuel cycle into possible weapons production is a key concern in global nonproliferation efforts. As such, the ability to trace the origin of seized nuclear materials is imperative to law enforcement efforts. Although isotopic signatures of UOCs have proven fruitful to pinpoint sample provenance, new isotopic signatures are needed because most existing isotopic signatures are not indicative of the original ore body from which the U is derived. In this work, we developed a new method to separate samarium (Sm) from a U-rich sample matrix and report the first Sm isotope compositions of 32 UOCs derived from a variety of worldwide uranium mines. Relative to terrestrial standards, approximately half the UOCs have resolved and anticorrelated 149Sm-150Sm isotope compositions, consistent with the capture of thermal neutrons by 149Sm in the ore body. The UOCs with anomalous Sm isotope compositions tend to derive from older (~>1.5Ga) and higher-grade ore bodies, although other factors, such as the presence of neutron moderators like water, also play a role. Nonetheless, the Sm isotope compositions of UOCs directly reflects the neutron fluence over the history of the original ore body and can be used to discern different geologic conditions associated with that ore body. As such, this work demonstrates the potential use of Sm isotopes as a novel nuclear forensics signature for origin assessment of UOCs.

Understanding the relationships between and among chondritic components of various chondrite groups is of prime importance for deciphering the dynamics of material transport and planetary accretion in the early Solar System. Here we obtain insights into these processes and the reservoirs present by investigating the nucleosynthetic Ti isotopic signatures of individual Ca,Al-rich inclusions (CAIs) and Na–Al-rich chondrules from ordinary and CO chondrites. This specific type of chondrule is of interest as it is thought to have incorporated refractory, CAI-like material as precursors. Our data show that CAIs from ordinary and CO chondrites exhibit 50Ti excesses that are indistinguishable from CV CAIs, and thus indicate a common source reservoir for refractory inclusions in ordinary, CO, and CV chondrites. Na–Al-rich chondrules from CO chondrites also show 50Ti excesses, indicating the presence of CAIs from this reservoir in the precursor materials of CO chondrules. In contrast, Na–Al-rich chondrules from ordinary chondrites show no 50Ti excesses and are indistinguishable from the bulk values for ordinary chondrites. Thus, known CAIs cannot have been the refractory precursor of the Na–Al-rich chondrules in ordinary chondrites. Consequently, within the accretion region of the ordinary chondrites, two different types of refractory components must have existed: (1) a 50Ti-enriched refractory component that is present as CAIs and either arrived at the accretion region of the ordinary chondrites after chondrule formation, or was only present in insignificant amounts, and (2) another type of refractory material without a 50Ti excess, which was involved as precursor in the chondrule formation process. Our data thus imply that refractory components with condensation signatures must have formed in at least two isotopically distinct nebular regions. These may be related to non-carbonaceous and carbonaceous source regions, that is, the inner and outer Solar System, divided by the early formation of Jupiter.

The oldest dated solids in our Solar System, calcium–aluminum-rich inclusions (CAIs), contain isotopic anomalies in a whole suite of elements relative to later formed Solar System materials. Previous work has reported differences in the proportions of nucleosynthetic components between CAIs and terrestrial rocks as a function of mass. However, the nucleosynthetic fingerprint of the CAI-forming region is still lacking significant data in the heavier mass range (A > 154). Therefore, we present the first erbium (Er) and ytterbium (Yb) isotopic data along with hafnium (Hf) isotopic compositions in a wide variety of CAIs derived from a variety of CV and CK chondrites. This work presents new methods for Er and Yb isotopic investigation that were explored using both thermal ionization mass spectrometry (TIMS) and multicollector inductively coupled plasma mass spectrometry (MC-ICPMS). Relative to terrestrial rock standards, CAIs—regardless of host rock, petrologic or chemical classification—have uniform and resolvable Er, Yb, and Hf isotopic compositions. The CAI isotopic patterns correspond to r-process deficits (or s-process excesses) relative to terrestrial values of 9 ppm for Er, 18 ppm for Yb, and 17 ppm for Hf. This new Er, Yb, and Hf data help complete the nucleosynthetic fingerprint of the CAI-forming region, further highlighting the systematic difference between the CAIs and later formed bulk planetary bodies. Such a systematic difference between CAIs and terrestrial rocks cannot be caused by different amounts of any known single presolar phase but is likely the result of a well-mixed reservoir made of diverse stellar sources.

The crystallization ages of planetary crustal material (given by basaltic meteorites) and planetary cores (given by iron meteorites) provide fiducial marks for the progress of planetary formation, and thus, the absolute ages of these objects fundamentally direct our knowledge and understanding of planet formation and evolution. The lone precise absolute age of planetary core material was previously obtained on troilite inclusions from the IVA iron meteorite Muonionalusta. This previously reported Pb–Pb age of 4565.3 ± 0.1 Ma—assuming a 238U/235U =137.88—only post-dated the start of the Solar System by approximately 2–3 million years, and mandated fast cooling of planetary core material. Since an accurate Pb–Pb age requires a known 238U/235U of the sample, we have measured both 238U/235U and Pb isotopic compositions of troilite inclusions from Muonionalusta. The measured 238U/235U of the samples range from ∼137.84 to as low as ∼137.22, however based on Pb and U systematics, terrestrial contamination appears pervasive and has affected samples to various extents for Pb and U. The cause of the relative 235U excess in one sample does not appear to be from terrestrial contamination or the decay of short-lived 247Cm, but is more likely from fractionation of U isotopes during metal–silicate separation during core formation, exacerbated by the extreme U depletion in the planetary core. Due to limited Pb isotopic variation and terrestrial disturbance, no samples of this study produced useful age information; however the clear divergence from the previously assumed 238U/235U of any troilite in Muonionalusta introduces substantial uncertainty to the previously reported absolute age of the sample without knowledge of the 238U/235U of the sample. Uncertainties associated with U isotope heterogeneity do not allow for definition of a robust age of solidification and cooling for the IVA core. However, one sample of this work—paired with previous work using short-lived radionuclides—suggests that the cooling age of the IVA core may be significantly younger than previously thought. This work indicates the metallic cores of protoplanetary bodies solidified no earlier than the first ∼5–10 million years of the Solar System.

Mars probably accreted within the first 10 million years of Solar System formation and likely underwent magma ocean crystallization and crust formation soon thereafter. To assess the nature and timescales of these large-scale mantle differentiation processes we applied the short-lived 182 Hf– 182 W and 146 Sm– 142 Nd chronometers to a comprehensive suite of martian meteorites, including several shergottites, augite basalt NWA 8159, orthopyroxenite ALH 84001 and polymict breccia NWA 7034. Compared to previous studies the 182 W data are significantly more precise and have been obtained for a more diverse suite of martian meteorites, ranging from samples from highly depleted to highly enriched mantle and crustal sources. Our results show that martian meteorites exhibit widespread 182 W/ 184 W variations that are broadly correlated with 142 Nd/ 144 Nd, implying that silicate differentiation (and not core formation) is the main cause of the observed 182 W/ 184 W differences. The combined 182 W– 142 Nd systematics are best explained by magma ocean crystallization on Mars within ∼20–25 million years after Solar System formation, followed by crust formation ∼15 million years later. These ages are indistinguishable from the I–Pu–Xe age for the formation of Mars' atmosphere, indicating that the major differentiation of Mars into mantle, crust, and atmosphere occurred between 20 and 40 million years after Solar System formation and, hence, earlier than previously inferred based on Sm–Nd chronometry alone.

Although there is limited direct evidence for supernova input into the nascent Solar System, many models suggest it formed by the gravitational collapse of a molecular cloud that was triggered by a nearby supernova. Existing lines of evidence, mostly in the form of short-lived radionuclides present in the early Solar System, are potentially consistent with this hypothesis, but still allow for alternative explanations. Since the natural production of 126Sn is thought to occur only in supernovae and this isotope has a short half-life (126Sn→126Te, t1/2 = 235 ky), the discovery of extant 126Sn would provide unequivocal proof of supernova input to the early Solar System. Previous attempts to quantify the initial abundance of 126Sn by examining Sn-Te systematics in early solids have been hampered by difficulties in precisely measuring Te isotope ratios in these materials. Thus, here we describe a novel technique that uses hydride generation to dramatically increase the ionization efficiency of Te—an approximately 30-fold increase over previous work. This introduction system, when coupled to a MC-ICPMS, enables high-precision Te isotopic analyses on samples with

Molybdenum (Mo) stable isotopes hold great potential to investigate the processes involved in planetary formation and differentiation. However their use is currently hampered by the lack of understanding of the dominant controls driving mass-dependent fractionations at high temperature. Here we investigate the role of magmatic processes and mantle source heterogeneities on the Mo isotope composition of Mid-Ocean Ridges Basalts (MORBs) using samples from two contrasting ridge segments: (1) the extremely fast spreading Pacific–Antarctic (66–41°S) section devoid of plume influence and; (2) the slow spreading Mohns–Knipovich segment (77–71°N) intercepted by the Jan Mayen Plume (71°N). We show that significant variations in Mo stable isotope composition exist in MORBs with δ98/95Mo ranging from − 0.24 ‰ to + 0.15 ‰ (relative to NIST SRM3134). The absence of correlation between δ98/95Mo and indices of magma differentiation or partial melting suggests a negligible impact of these processes on the isotopic variations observed. On the other hand, the δ98/95Mo variations seem to be associated with changes in radiogenic isotope signatures and rare earth element ratios (e.g., (La/Sm)N), suggesting mantle source heterogeneities as a dominant factor for the δ98/95Mo variations amongst MORBs. The heaviest Mo isotope compositions correspond to the most enriched signatures, suggesting that recycled crustal components are isotopically heavy compared to the uncontaminated depleted mantle. The uncontaminated depleted mantle shows slightly sub-chondritic δ98/95Mo, which cannot be produced by core formation and, therefore, more likely result from extensive anterior partial melting of the mantle. Consequently, the primitive δ98/95Mo composition of the depleted mantle appears overprinted by the effects of both partial melting and crustal recycling.

Astrobiology is the science that seeks to understand the story of life in our universe. Astrobiology includes investigation of the conditions that are necessary forlife to emerge and flourish, the origin of life, the ways that life has evolved and adaptedto the wide range of environmental conditions here on Earth, the search for life beyondEarth, the habitability of extraterrestrial environments, and consideration of the future oflife both here on Earth and elsewhere. It therefore requires knowledge of physics,chemistry and biology, and many more specialized scientific areas including astronomy,geology, planetary science, microbiology, atmospheric science and oceanography. Fil: Domagal Goldman, Shawn D.. National Aeronautics And Space Administration; Estados Unidos Fil: Wright, Katherine. University Of Bristol; Reino Unido Fil: Adamala, Katarzyna. University Of Minnesota; Estados Unidos Fil: Antonio, Marina. Washington State University. School Of Earth & Environmental Sciences; Estados Unidos Fil: Arino de la Rubia, Leigh. University Of New South Wales; Australia Fil: Carter Bond, Jade. University Of New South Wales; Australia Fil: Dartnell, Lewis. University Of Leicester; Reino Unido Fil: Goldman, Aaron. Oberlin College; Reino Unido Fil: Paulino Lima, Ivan Glaucio. National Aeronautics And Space Administration; Estados Unidos Fil: Lynch, Kennda. Colorado School; Estados Unidos Fil: Naud, Marie Eve. Université Du Québec A Montreal; Canadá Fil: Singer, Kelsi. Southwest Research Institute; Estados Unidos Fil: Abrevaya, Ximena Celeste. Consejo Nacional de Investigaciónes Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Astronomía y Física del Espacio. - Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Astronomía y Física del Espacio; Argentina Fil: Anderson, Rika. University of Washington; Estados Unidos Fil: Arney, Giada. University of Washington; Estados Unidos Fil: Atri, Dimitra. International Centre Of Theoretical Science. Tata Institute Of Fundamental Research; España Fil: Azua Bustos, Armando. Pontificia Universidad Católica de Chile; Chile Fil: Bowman, Jeff. Lamont Doherty Earth Observatory; Estados Unidos Fil: Brazelton, William. University of Utah; Estados Unidos Fil: Brennecka, Gregory. Westfalische Wilhelms Universitat; Alemania Fil: Carns, Regina. University of Washington; Estados Unidos Fil: Chopra, Adytia. Australian National University; Australia Fil: Collangelo Lillis, Jess. McGill University; Estados Unidos Fil: Crockett, Christopher. University Of Carnegie Mellon; Estados Unidos Fil: DeMarines, Julia. University Of Carnegie Mellon; Estados Unidos Fil: Frank, Elizabeth. University Of Carnegie Mellon; Estados Unidos Fil: Frantz, Carie. University of Washington; Estados Unidos Fil: Galante, Douglas. Brazilian Synchrotron Light Laboratory; Brasil Fil: Glass, Jennifer. Georgia Institute Of Techology; Estados Unidos Fil: Gleeson, Damhait. Instituto Nacional de Tecnica Aeroespacial; España

The significant reorganization of the early Solar System due to giant planet migration has hampered our understanding of where planetary bodies formed. Previously employed proxies for reconstructing the primordial planetary architecture, such as water content or oxidation state, are complicated by post-accretionary processes. Here we investigate basaltic achondrites for their nucleosynthetic isotope signatures in the elements neodymium (Nd) and zirconium (Zr) and show that they are—similar to previously investigated chondritic meteorites—characterized by a relative deficit in isotopes produced by the s-process of nucleosynthesis. Importantly, these data are well correlated with nucleosynthetic signatures observed in other elements, demonstrating that s-process matter was heterogeneously distributed throughout the early Solar System. By comparing these isotopic signatures with potential proxies for Solar System reconstruction and computer modeling, we here argue that this isotopic heterogeneity in bulk meteoritic materials is linked to the original heliocentric distance of formation. Such scaling of nucleosynthetic signatures with heliocentric distance could permit reconstruction of the primordial architecture of the Solar System by ‘cosmolocating’ the accretion orbits of meteoritic parent bodies as a function of incorporated s-process matter.

High precision Sm−Nd isotopic analyses have been completed on a suite of 11 martian basaltic meteorites in order to better constrain the age of silicate differentiation on Mars associated with the formation of their mantle sources. These data are used to evaluate the merits and disadvantages of various mathematical approaches that have been employed in previous work on this topic. Ages determined from the Sm−Nd isotopic systematics of individual samples are strongly dependent on the assumed Nd isotopic composition of the bulk planet. This assumption is problematic given differences observed between the Nd isotopic composition of Earth and chondritic meteorites and the fact that these materials are both commonly used to represent bulk planetary Nd isotopic compositions. Ages determined from the slope of 146Sm−142Nd whole rock isochrons are not dependent on the assumed 142Nd/144Nd ratio of the planet, but require the sample suite to be derived from complementary, contemporaneously-formed reservoirs. In this work, we present a mathematical expression that defines the age of formation of the source regions of such a suite of samples that is based solely on the slope of a 143Nd−142Nd whole rock isochron and is also independent of any a priori assumptions regarding the bulk isotopic composition of the planet. This expression is also applicable to mineral isochrons and has been used to successfully calculate 143Nd−142Nd model crystallization ages of early refractory solids as well as lunar samples. This permits ages to be obtained using only Nd isotopic measurements without the need for 147Sm/144Nd isotope dilution determinations. When used in conjunction with high-precision Nd isotopic measurements completed on martian meteorites this expression yields an age of formation of the martian basaltic meteorite source regions of 4504 ± 6 Ma. Because the Sm−Nd model ages for the formation of martian source regions are commonly interpreted to record the age at which large scale mantle reservoirs formed during planetary differentiation associated with magma ocean solidification, the age determined here implies that magma ocean solidification occurred several tens of millions of years after the beginning of the Solar System. Recent thermal models, however, suggest that Mars-sized bodies cool rapidly in less than ∼5 Ma after accretion ceases, even in the presence of a thick atmosphere. Assuming these models are correct, an extended period of accretion is necessary to provide a mechanism to keep portions of the martian mantle partially molten until 4504 Ma. Late accretional heating of Mars could either be associated with protracted accretion occurring at a quasi-steady state or alternatively be associated with a late giant impact. If this scenario is correct, then accretion of Mars-sized bodies takes up to 60 Ma and is likely to be contemporaneous with the core formation and possibly the onset of silicate differentiation. This further challenges the concept that isotopic equilibrium is attained during primordial evolution of planets, and may help to account for geochemical evidence implying addition of material into planetary interiors after core formation was completed.

The early evolution of planetesimals and planets can be constrained using variations in the abundance of neodymium-142 ((142)Nd), which arise from the initial distribution of (142)Nd within the protoplanetary disk and the radioactive decay of the short-lived samarium-146 isotope ((146)Sm). The apparent offset in (142)Nd abundance found previously between chondritic meteorites and Earth has been interpreted either as a possible consequence of nucleosynthetic variations within the protoplanetary disk or as a function of the differentiation of Earth very early in its history. Here we report high-precision Sm and Nd stable and radiogenic isotopic compositions of four calcium-aluminium-rich refractory inclusions (CAIs) from three CV-type carbonaceous chondrites, and of three whole-rock samples of unequilibrated enstatite chondrites. The CAIs, which are the first solids formed by condensation from the nebular gas, provide the best constraints for the isotopic evolution of the early Solar System. Using the mineral isochron method for individual CAIs, we find that CAIs without isotopic anomalies in Nd compared to the terrestrial composition share a (146)Sm/(144)Sm-(142)Nd/(144)Nd isotopic evolution with Earth. The average (142)Nd/(144)Nd composition for pristine enstatite chondrites that we calculate coincides with that of the accessible silicate layers of Earth. This relationship between CAIs, enstatite chondrites and Earth can only be a result of Earth having inherited the same initial abundance of (142)Nd and chondritic proportions of Sm and Nd. Consequently, (142)Nd isotopic heterogeneities found in other CAIs and among chondrite groups may arise from extrasolar grains that were present in the disk and incorporated in different proportions into these planetary objects. Our finding supports a chondritic Sm/Nd ratio for the bulk silicate Earth and, as a consequence, chondritic abundances for other refractory elements. It also removes the need for a hidden reservoir or for collisional erosion scenarios to explain the (142)Nd/(144)Nd composition of Earth.

A handful of events, such as the condensation of refractory inclusions and the formation of chondrules, represent important stages in the formation and evolution of the early solar system and thus are critical to understanding its development. Compared to the refractory inclusions, chondrules appear to have a protracted period of formation that spans millions of years. As such, understanding chondrule formation requires a catalog of reliable ages, free from as many assumptions as possible. The Pb-Pb chronometer has this potential; however, because common individual chondrules have extremely low uranium contents, obtaining U-corrected Pb-Pb ages of individual chondrules is unrealistic in the vast majority of cases at this time. Thus, in order to obtain the most accurate 238U/235U ratio possible for chondrules, we separated and pooled thousands of individual chondrules from the Allende meteorite. In this work, we demonstrate that no discernible differences exist in the 238U/235U compositions between chondrule groups when separated by size and magnetic susceptibility, suggesting that no systematic U-isotope variation exists between groups of chondrules. Consequently, chondrules are likely to have a common 238U/235U ratio for any given meteorite. A weighted average of the six groups of chondrule separates from Allende results in a 238U/235U ratio of 137.786 ± 0.004 (±0.016 including propagated uncertainty on the U standard [Richter et al. 2010]). Although it is still possible that individual chondrules have significant U isotope variation within a given meteorite, this value represents our best estimate of the 238U/235U ratio for Allende chondrules and should be used for absolute dating of these objects, unless such chondrules can be measured individually.

Bunburra Rockhole is a unique basaltic achondrite that has many mineralogical and petrographic characteristics in common with the noncumulate eucrites, but differs in its oxygen isotope composition. Here, we report a study of the mineralogy, petrology, geochemistry, and chronology of Bunburra Rockhole to better understand the petrogenesis of this meteorite and compare it to the eucrites. The geochemistry of bulk samples and of pyroxene, plagioclase, and Ca-phosphate in Bunburra Rockhole is similar to that of typical noncumulate eucrites. Chronological data for Bunburra Rockhole indicate early formation, followed by slow cooling and perhaps multiple subsequent heating events, which is also similar to some noncumulate eucrites. The 26 Al- 26 Mg extinct radionuclide chronometer was reset in Bunburra Rockhole after the complete decay of 26 Al, but a slight excess in the radiogenic 26 Mg in a bulk sample allows the determination of a model 26 Al- 26 Mg age that suggests formation of the parent melt for this meteorite from its source magma within the first ~3 Ma of the beginning of the solar system. The 207 Pb- 206 Pb absolute chronometer is also disturbed in Bunburra Rockhole minerals, but a whole-rock isochron provides a re-equilibration age of ~4.1 Ga, most likely caused by impact heating. The mineralogy, geochemistry, and chronology of Bunburra Rockhole demonstrate the similarities of this achondrite to the eucrites, and suggest that it formed from a parent melt with a composition similar to that for noncumulate eucrites and subsequently experienced a thermal history and evolution comparable to that of eucritic basalts. This implies the formation of multiple differentiated parent bodies in the early solar system that had nearly identical bulk elemental compositions and petrogenetic histories, but different oxygen isotope compositions inherited from the solar nebula.

One way to study the original building blocks of the Solar System is to investigate primitive meteorites and their components. Specifically, isolating these meteorites' individual components via sequential acid leaching can reveal isotopically diverse material present in the early Solar System, which can provide new insights into the mixing and transport processes that eventually led to planet formation. Such isotopic differences in the components are likely to be found in heavy rare earth elements, such as dysprosium (Dy), erbium (Er), and ytterbium (Yb), because their isotopes have different nucleosynthetic production pathways and the elements have significant differences in volatility; however, these specific elements have yet to be thoroughly investigated in the field of cosmochemistry. As such, we present the first combined Dy, Er, and Yb isotope compositions of sequential acid leachates from the Murchison meteorite, along with multiple bulk meteorites from different taxonomic classes. This work also presents a new method to separate, purify, and accurately measure Dy isotopes. Here we show that resolved Dy, Er, and Yb isotope variations in most bulk meteorites are due to neutron capture processes. However, Dy and Er isotopic compositions of bulk Murchison and Murchison leachates stem from the additions or depletions of a nucleosynthetic component formed by the s-process, most likely mainstream silicon carbide (SiC) grains. In contrast, the Yb isotope compositions of bulk Murchison and Murchison leachates display either unresolved or relatively small isotope anomalies. The disparate isotopic behavior between Dy-Er and Yb likely reflects their differing volatilities, with Dy and Er condensing/incorporating into the mainstream SiC grains, whereas the less refractory Yb remains in the gas phase during SiC formation. This work suggests that Yb is hosted in a non-SiC presolar carrier phase and, furthermore, that mainstream SiC grains may be the primary source of isotopic variation in bulk meteorites.

We report 182W and 142Nd isotopic compositions, 187Re–187Os systematics, and abundances of highly siderophile elements (HSE: Re, Os, Ir, Ru, Rh, Pt, Pd, and Au) for a suite of komatiites and basalts from the ∼ 3.3 Ga Ruth Well Formation and the ∼ 3.45 Ga Warrawoona Group of the Pilbara Craton, Western Australia. The 182W compositions from all samples are indistinguishable from each other, and more radiogenic than modern bulk silicate Earth, with a mean μ182W value of + 9.1 ± 4.2 (2SD). By contrast, the 142Nd values for all samples are indistinguishable from each other and terrestrial standards, with a mean μ142Nd value of − 1.6 ± 3.2 (2SD). The 146Sm–142Nd and 187Re–187Os systematics are consistent with chondritic Sm/Nd and Re/Os ratios in the mantle source during the lifetime of 182Hf, and the observed 182W excesses therefore cannot be accounted for by early Hf–W fractionation by magma ocean processes, neither by silicate liquid-crystal fractionation nor by high P–T metal-silicate equilibration. The estimated abundances of HSE in the mantle source, however, are significantly lower than modern bulk silicate Earth, with only 51 ± 9 % (1SD) of modern bulk silicate Earth abundances. These results are consistent with a partial lack of late-accreted material within the Pilbara source at ∼ 3.3 Ga to account for the 182W excesses. Further, widespread 182W excesses of similar magnitude in other Archean mantle-derived rocks worldwide strongly suggests that a common process, most likely incomplete addition of late-accreted material, was responsible. The apparent mismatch between late-accreted 182W–HSE systematics for some other localities likely reflects either the inherent difficulties associated with estimating source HSE abundances, and/or dissociation of W and HSE by mantle processes. Finally, the combined average 182W–HSE systematics of Archean samples indicate that the pre-late accretion BSE likely had a μ182W value similar to that of the lunar mantle, which strongly suggests post-giant impact Earth–Moon equilibration and indicates that the Moon formed after 182Hf extinction.

The recent witnessed fall of the meteorite Tissint represents the delivery of a pristine new sample from the surface of Mars. This meteorite provides an unprecedented opportunity to study a variety of aspects about the planet's evolution. Using the Rb-Sr and Sm-Nd isotopic systems, we determined that Tissint, a depleted shergottite, has a crystallization age of 574 20 Ma, an initial e 143 Nd =+ 42.2 0.5, and an initial 87 Sr/ 86 Sr = 0.700760 11. These initial Nd and Sr isotopic compositions suggest that Tissint originated from a mantle source on Mars that is distinct from the source reservoirs of the other Martian meteorites. The known crystallization ages, geochemical characteristics, ejection ages, and ejection dynamics of Tissint and other similarly grouped Martian meteorites suggest that they are likely derived from a source crater up to approximately 90 km in diameter with an age of approximately 1 Ma that is located on terrain that is approximately 600 million years old.

Geochemical data from late Archean sedimentary rocks point to photosynthetic O 2 production and at least intermittent occurrences of locally mild oxidative weathering and surface ocean oxygenation (“oxygen oases”) prior to the early Paleoproterozoic Great Oxidation Event. For example, distinctive authigenic enrichments of Mo and Re in euxinic (anoxic and sulfidic) black shales are best explained by the oxidative mobilization of these metals from crustal sulfide minerals and their accumulation as oxyanions in seawater. In contrast, it is not clear if low U enrichments in the same shales reflect negligible oxidation of U from the upper crust or a very small oceanic U inventory that was derived from oxidative U mobilization. Here, we report U isotope data for the 2.50 Ga Mt. McRae Shale (Hamersley basin, Western Australia), which provides a more sensitive test for the presence or absence of authigenic U compared to U concentrations and enrichment factors normalized to average shale or upper crustal compositions (that may not be representative of the local detrital composition). We find instances where the U isotope composition in the upper Mt. McRae Shale (δ 238 U = − 0.2 to 0.0‰ relative to standard SRM950a) is isotopically heavier than average upper crust (δ 238 U = − 0.31 ± 0.14 [2SD] based on granitoids and basalts). The high δ 238 U values point to U isotope fractionation in the late Archean marine environment and hence indicate the presence of a small amount of dissolved U in seawater and authigenic U in the Mt. McRae Shale. Volume-dependent equilibrium isotope fractionation during the reduction of dissolved U VI to insoluble U IV , like that observed in the modern Black Sea, may explain the high δ 238 U signatures if U removal from bottom waters was not quantitative. Alternatively, quantitative U removal would require that late Archean seawater had high δ 238 U, which could have arisen from the preferential sequestration of 235 U to Fe (oxyhydr)oxide minerals elsewhere in the Hamersley basin. The supracrustal δ 238 U signatures are associated with some of the highest Mo and Re enrichments in the Mt. McRae Shale as well as distinctive Mo, S and N isotope signatures that are indicative of mild environmental oxygenation. Hence, our findings suggest that small amounts of U were oxidatively mobilized from the upper crust at 2.50 Ga. Unlike Mo and Re, however, U oxidation may not have occurred on land. Instead, we hypothesize that oxidative U mobilization occurred by submarine weathering in an oxygen oasis.

The isotopic composition of our Solar System reflects the blending of materials derived from numerous past nucleosynthetic events, each characterized by a distinct isotopic signature. We show that the isotopic compositions of elements spanning a large mass range in the earliest formed solids in our Solar System, calcium-aluminum-rich inclusions (CAIs), are uniform, and yet distinct from the average Solar System composition. Relative to younger objects in the Solar System, CAIs contain positive r-process anomalies in isotopes A140 and negative r-process anomalies in isotopes A140. This fundamental difference in the isotopic character of CAIs around mass 140 necessitates (i) the existence of multiple sources for r-process nucleosynthesis and (ii) the injection of supernova material into a reservoir untapped by CAIs. A scenario of late supernova injection into the protoplanetary disk is consistent with formation of our Solar System in an active star-forming region of the galaxy.

International audience; Northwest Africa (NWA) 8159 is an augite-rich shergottite, with a mineralogy dominated by Ca-, Fe-rich pyroxene, plagioclase, olivine, and magnetite. NWA 8159 crystallized from an evolved melt of basaltic composition under relatively rapid conditions of cooling, likely in a surface lava flow or shallow sill. Redox conditions experienced by the melt shifted from relatively oxidizing (with respect to known Martian lithologies, similar to QFM) on the liquidus to higher oxygen fugacity (similar to QFM + 2) during crystallization of the groundmass, and under subsolidus conditions. This shift resulted in the production of orthopyroxene and magnetite replacing olivine phenocryst rims. NWA 8159 contains both crystalline and shock-amorphized plagioclase (An(5062)), often observed within a single grain; based on known calibrations we bracket the peak shock pressure experienced by NWA 8159 to between 15 and 23 GPa. The bulk composition of NWA 8159 is depleted in LREE, as observed for Tissint and other depleted shergottites; however, NWA 8159 is distinct from all other martian lithologies in its bulk composition and oxygen fugacity. We obtain a Sm-Nd formation age of 2.37 +/- 0.25 Ga for NWA 8159, which represents an interval in Mars geologic time which, until recently, was not represented in the other martian meteorite types. The bulk rock Sm-147/Nd-144 value of 0.37 +/- 0.02 is consistent with it being derived directly from its source and the high initial epsilon(143)(Nd) value indicates this source was geochemically highly depleted. Cr, Nd, and W isotopic compositions further support a unique mantle source. While the rock shares similarities with the 2.4-Ga NWA 7635 meteorite, there are notable distinctions between the two meteorites that suggest differences in mantle source compositions and conditions of crystallization. Nevertheless, the two samples may be launch-paired. NWA 8159 expands the known basalt types, ages and mantle sources within the Mars sample suite to include a second igneous unit from the early Amazonian.(C) 2017 Elsevier Ltd. All rights reserved.

The nuclear field shift (NFS) is an isotope shift in atomic energy levels caused by a combination of differences in nuclear size and shape and electron densities at the nucleus. The effect of NFS in isotope fractionation was theoretically established by Bigeleisen in 1996 [Bigeleisen J. (1996) J. Am. Chem. Soc. 118:3676–3680] and has been analytically measured in laboratory chemical exchange reactions. More recently, some isotopic variations of heavy elements (Hg, Tl, U) measured in natural systems as well as isotopic anomalies measured for lower-mass elements in meteorites have been attributed to the NFS effect. These isotopic variations open up new and exciting fields of investigations in Earth sciences. In this paper, we review the different natural systems in which NFS has been proposed to be the origin of isotopic variations.

Events occurring within the first 10 million years of the Solar System’s approximately 4.5 billion-year history, such as formation of the first solids, accretion, and differentiation of protoplanetary bodies, have determined the evolutionary course of our Solar System and the planetary bodies within it. The application of high-resolution chronometers based on short-lived radionuclides is critical to our understanding of the temporal sequence of these critical events. However, to map the relative ages from such chronometers onto the absolute time scale, they must be “anchored” to absolute ages of appropriate meteoritic materials using the high-precision lead–lead (Pb–Pb) chronometer. Previously reported Pb–Pb dates of the basaltic angrite meteorites, some of which have been used extensively as time anchors, assumed a constant 238 U/ 235 U ratio (= 137.88). In this work, we report measurements of 238 U/ 235 U ratios in several angrites that are distinct from the previously assumed value, resulting in corrections to the Pb–Pb ages of ≥1 million years. There is no resolvable variation in the 238 U/ 235 U ratio among the angrite bulk samples or mineral separates, suggesting homogeneity in the U isotopic composition of the angrite parent body. Based on these measurements, we recalculated the Pb–Pb age for the commonly used anchor, the D’Orbigny angrite, to be 4563.37 ± 0.25 Ma. An adjustment to the Pb–Pb age of a time anchor (such as D’Orbigny) requires a corresponding correction to the “model ages” of all materials dated using that anchor and a short-lived chronometer. This, in turn, has consequences for accurately defining the absolute timeline of early Solar System events.

Periods of oceanic anoxia have had a major influence on the evolutionary history of Earth and are often contemporaneous with mass extinction events. Changes in global (as opposed to local) redox conditions can be potentially evaluated using U system proxies. The intensity and timing of oceanic redox changes associated with the end-Permian extinction horizon (EH) were assessed from variations in 238 U/ 235 U ( δ 238 U) and Th/U ratios in a carbonate section at Dawen in southern China. The EH is characterized by shifts toward lower δ 238 U values (from -0.37‰ to -0.65‰), indicative of an expansion of oceanic anoxia, and higher Th/U ratios (from 0.06 to 0.42), indicative of drawdown of U concentrations in seawater. Using a mass balance model, we estimate that this isotopic shift represents a sixfold increase in the flux of U to anoxic facies, implying a corresponding increase in the extent of oceanic anoxia. The intensification of oceanic anoxia coincided with, or slightly preceded, the EH and persisted for an interval of at least 40,000 to 50,000 y following the EH. These findings challenge previous hypotheses of an extended period of whole-ocean anoxia prior to the end-Permian extinction.

We report elemental abundances and the isotopic systematics of the short-lived 26Al–26Mg (half-life of ∼0.73 Ma) and long-lived U–Pb radiochronometers in the ungrouped basaltic meteorite Northwest Africa (NWA) 2976. The bulk geochemical composition of NWA 2976 is clearly distinct from that of the eucrites and angrites, but shows broad similarities to that of the paired NWA 001 and 2400 ungrouped achondrites indicating that it is likely to also be paired with these two samples. The major and trace element abundances in NWA 2976 further indicate that it formed by extensive melting and magmatic fractionation processes on its parent body. The Al–Mg and Pb–Pb isotope systematics indicate that this meteorite represents the earliest stages of crust formation on a differentiated parent body in the early Solar System. The absolute Pb–Pb internal isochron age of NWA 2976, obtained from acid leaching residues of three whole-rock samples and two pyroxene separates, is 4562.89 ± 0.59 Ma (MSWD = 0.02). This Pb–Pb age is calculated using the measured 238U/235U ratio of a NWA 2976 whole-rock of 137.751 ± 0.018 (2σ) which was determined relative to the recently revised value of 137.840 ± 0.008 for the SRM 950a U isotope standard. The Al–Mg systematics reveal the presence of 26Mg isotopic anomalies produced by the decay of 26Al with an (26Al/27Al)0 of (3.94 ± 0.16) × 10−7, and indicate a time of formation of 0.26 ± 0.18 Ma after the D’Orbigny angrite. Using the revised Pb–Pb age of 4563.36 ± 0.34 Ma for the D’Orbigny anchor (corrected for its U isotopic composition), we deduce an Al–Mg model age of 4563.10 ± 0.38 Ma for NWA 2976, which is consistent with its Pb–Pb internal isochron age. The concordance of the Pb–Pb and Al–Mg chronometers, when taking into account the differences in the U isotopic compositions of the D’Orbigny and NWA 2976 achondrites (whose parent bodies likely formed in distinct regions of early Solar System as indicated by their different oxygen isotopic compositions), implies that 26Al was homogeneously distributed in the early Solar System. It also suggests that igneous processes on planetesimals, as represented by the formation of various basaltic meteorite groups that likely originated on distinct parent bodies (e.g., eucrites and angrites, as well as ungrouped achondrites), were widespread throughout the protoplanetary disk within the first ∼5 Ma of the history of the Solar System.

As the earliest dated solids, calcium–aluminum-rich inclusions (CAIs) provide a unique window into the early solar system. However, for many elements, CAIs have been shown to exhibit a very different nucleosynthetic isotope signature from that of later-formed bulk meteorites. To explore this critical difference between solar system materials, we investigate a broad set of CAI samples for both mass-dependent and non-mass-dependent (nucleosynthetic) isotope variations in the siderophile element nickel (Ni). We find that fine-grained CAIs show little if any mass-dependent Ni isotopic fractionation, whereas coarse-grained inclusions exhibit a broad range of isotopically heavy signatures. Because mass-dependent variations appear to be coupled with nucleosynthetic anomalies in CAIs, a part of this Ni isotope variability could be due to thermal processing that acted on these samples. Nucleosynthetic Ni isotopic signatures show that CAIs share a genetic heritage with carbonaceous meteorites and provide a clear distinction from the isotopic reservoirs occupied by terrestrial Ni and non-carbonaceous meteorites. However, whereas nucleosynthetic Ni isotope heterogeneity in previously investigated bulk meteorites was ascribed to variation in the neutron-poor isotope 58Ni, we here find that CAI signatures require variability in other, more neutron-rich Ni isotopes. Taken in aggregate with previous work, this highlights a change in the nucleosynthetic character from CAIs to later-formed solids that cannot be explained by variable admixture of a single presolar phase or material from a specific supernova shell. Instead, these data reveal the complex evolution of the solar system, including blending and reprocessing of matter from several generations and types of stars.

Precise measurement of the 238 U/ 235 U ratio in geologic samples is now possible with modern techniques and mass spectrometers. Natural variations in this ratio have been shown in previous studies. In this study, data obtained from uranium ore concentrates of mining facilities around the world show clear evidence that the depositional redox environment in which uranium is precipitated is the primary factor affecting 238 U/ 235 U fractionation. Low-temperature uranium deposits are, on average, isotopically ∼ 0.4‰ heavier than uranium deposited at high temperatures or by non-redox processes. 238 U/ 235 U ratios coupled with 235 U/ 234 U ratios in the same sample provide evidence that the redox transition (U VI → U IV ) at low temperatures is the primary mechanism of 238 U/ 235 U fractionation and that aqueous alteration plays a very limited, if any, role in fractionation of the 238 U/ 235 U ratio. The isotopic variation of U is therefore a potential signature that can be used to trace the origin of uranium ore concentrate.

Precise knowledge of the abundances of short-lived radionuclides at the start of the solar system leads to fundamental information about the stellar environment of solar system formation. Previous investigations of the short-lived system (t 1/2 = 2.3 Ma) have resulted in a range of calculated initial amounts of 135Cs, with most estimates elevated to a level that requires extraneous input of material to the protoplanetary disk. Such an array of proposed 135Cs/133Cs initial solar system values has severely restricted the system's use as both a possible chronometer and as an informant about supernovae input. However, if 135Cs was as abundant in the early solar system as previously proposed, the resulting deficits in its daughter product 135Ba would be easily detectable in volatile-depleted parent bodies (i.e., having sub-chondritic Cs/Ba) from the very early solar system. In this work, we show that angrites and eucrites, which were volatile-depleted within ~1 million years of the start of the solar system, do not possess deficits in 135Ba compared to other planetary bodies. From this, we calculate an upper limit for the initial 135Cs/133Cs of 2.8 × 10−6, well below previous estimates. This significantly lower initial 135Cs/133Cs ratio now suggests that all of the 135Cs present in the early solar system was inherited simply from galactic chemical evolution and no longer requires an addition from an external stellar source such as an asymptotic giant branch star or SN II, corroborating evidence from several other short-lived radionuclides.

Previous work has shown uranium (U) isotope fractionation between natural ferromanganese crusts and seawater. Understanding the mechanism that causes (238)U/(235)U fractionation during adsorption to ferromanganese oxides is a critical step in the utilization of (238)U/(235)U as a tracer of U adsorption reactions in groundwater as well as a potential marine paleoredox proxy. We conducted U adsorption experiments using synthetic K-birnessite and U-bearing solutions. These experiments revealed a fractionation matching that observed between seawater and natural ferromanganese sediments: adsorbed U is isotopically lighter by ∼0.2‰ (δ(238/235)U) than dissolved U. As the redox state of U does not change during adsorption, a difference in the coordination environment between dissolved and adsorbed U is likely responsible for this effect. To test this hypothesis, we analyzed U adsorbed to K-birnessite in our experimental study using extended X-ray absorption fine structure (EXAFS) spectroscopy, to obtain information about U coordination in the adsorbed complex. Comparison of our EXAFS spectra with those for aqueous U species reveals subtle, but important, differences in the U-O coordination shell between dissolved and adsorbed U. We hypothesize that these differences are responsible for the fractionation observed in our experiments as well as for some U isotope variations in nature.

How to Get a Date Radiometric dating relies on measuring the abundance of a radioactive isotope and/or its decay products. By knowing a decay rate and an isotopic starting abundance—both assumed to be constant—an age is determined. Using high-resolution mass spectrometry, Brennecka et al. (p. 449 , published online 31 December; see the Perspective by Connelly ) show that the known starting abundance of 238 U and 235 U isotopes in meteorites, which decay into 206 Pb and 207 Pb, respectively, is actually quite variable. Trace amounts of 247 Cm in the early solar system may have unexpectedly contributed additional 235 U, skewing the ratio. Pb-Pb dating, the method commonly used to date early solar system materials, may thus need a correction of up to 5 million years.

Insights into the earliest stages of our Solar System can be derived from its oldest dated solids, calcium-aluminum-rich inclusions (CAIs). In particular, investigating isotopic anomalies of nucleosynthetic origin in CAIs offers potential clues to the genetic heritage of refractory inclusions and the reservoir(s) involved in their formation. To this point, however, nucleosynthetic anomalies in refractory inclusions have almost exclusively been recognized in (1) relatively large CAIs from CV3 chondrites, employing chemical purification and high-precision mass spectrometry, or (2) from sub-mm-sized hibonite-rich objects (e.g., PLACs, SHIBs) from the Murchison CM2 chondrite using much less precise in-situ techniques. Whereas the latter have been shown to be highly anomalous in their isotopic compositions, their genetic connection to ‘regular’ CAIs from carbonaceous chondrites remains poorly understood. Here, we aim to address this issue by taking advantage of a new technique that allows for high-precision analysis of sub-mm-sized inclusions. Using this method, we report Ti isotope anomalies in a suite of twelve CAIs from five different CO carbonaceous chondrites, as well as ten refractory inclusions from the CM2 chondrite Jbilet Winselwan using MC-ICPMS. We find that these CO and CM CAIs exhibit Ti isotopic compositions very similar to those of previously investigated CV3 (and of two CK3) CAIs, suggesting a fundamental genetic relationship of CAIs found within these chondrite groups. As such, our data indicates that CAIs from various groups of carbonaceous chondrites formed from similar matter and in a single region of the solar nebula (i.e., derived from a single common CAI-formation region). Collectively, these data show evidence of large-scale transport of CAIs over a significant range of heliocentric distances, covering at least the accretion areas of the CV, CK, CO, and CM chondrites. In addition, we report two inclusions consisting of hibonite-rich crystal aggregates from Jbilet Winselwan that exhibit highly irregular nucleosynthetic Ti signatures, implying a distinct origin from the aforementioned CAIs. These inclusions may represent an earlier generation of refractory material, perhaps more akin to the previously mentioned PLACs and/or SHIBs.

Nucleosynthetic isotope anomalies are powerful tracers to determine the provenance of meteorites and their components, and to identify genetic links between these materials. Here we show that chondrules and matrix separated from the Allende CV3 chondrite have complementary nucleosynthetic Mo isotope anomalies. These anomalies result from the enrichment of a presolar carrier enriched in s -process Mo into the matrix, and the corresponding depletion of this carrier in the chondrules. This carrier most likely is a metal and so the uneven distribution of presolar material probably results from metal–silicate fractionation during chondrule formation. The Mo isotope anomalies correlate with those reported for W isotopes on the same samples in an earlier study, suggesting that the isotope variations for both Mo and W are caused by the heterogeneous distribution of the same carrier. The isotopic complementary of chondrules and matrix indicates that both components are genetically linked and formed together from one common reservoir of solar nebula dust. As such, the isotopic data require that most chondrules formed in the solar nebula and are not a product of protoplanetary impacts. Allende chondrules and matrix together with bulk carbonaceous chondrites and some iron meteorites (groups IID, IIIF, and IVB) show uniform excesses in 92 Mo, 95 Mo, and 97 Mo that result from the addition of supernova material to the solar nebula region in which these carbonaceous meteorites formed. Non-carbonaceous meteorites (enstatite and ordinary chondrites as well as most iron meteorites) do not contain this material, demonstrating that two distinct Mo isotope reservoirs co-existed in the early solar nebula that remained spatially separated for several million years. This separation was most likely achieved through the formation of the gas giants, which cleared the disk between the inner and outer solar system regions parental to the non-carbonaceous and carbonaceous meteorites. The Mo isotope dichotomy of meteorites provides a new means to determine the provenance of meteoritic and planetary materials, and to assess genetic links between chondrites and differentiated meteorites.

Calcium-aluminum-rich inclusions (CAIs) are the oldest dated materials in the Solar System and numerous previous studies have revealed nucleosynthetic anomalies relative to terrestrial rock standards in many isotopic systems. However, most of the isotopic data from CAIs has been limited to the Allende meteorite and a handful of other CV3 chondrites. To better constrain the isotopic composition of the CAI-forming region, we report the first Sr, Mo, Ba, Nd, and Sm isotopic compositions of two CAIs hosted in the CK3 desert meteorites NWA 4964 and NWA 6254 along with two CAIs from the CV3 desert meteorites NWA 6619 and NWA 6991. After consideration of neutron capture processes and the effects of hot-desert weathering, the Sr, Mo, Ba, Nd, and Sm stable isotopic compositions of the samples show clearly resolvable nucleosynthetic anomalies that are in agreement with previous results from Allende and other CV meteorites. The extent of neutron capture, as manifested by shifts in the observed 149Sm-150Sm isotopic composition of the CAIs is used to estimate the neutron fluence experienced by some of these samples and ranges from 8.40 × 1013 to 2.11 × 1015 n/cm2. Overall, regardless of CAI type or host meteorite, CAIs from CV and CK chondrites have similar nucleosynthetic anomalies within analytical uncertainty. We suggest the region that CV and CK CAIs formed was largely uniform with respect to Sr, Mo, Ba, Nd, and Sm isotopes when CAIs condensed and that CAIs hosted in CV and CK meteorites are derived from the same isotopic reservoir.