arXiv subjects

Nicolas Dauphas

Publications and source records attributed to Nicolas Dauphas.

At least 19 recordsLinked to original sources

arXiv2025

Completion of Lunar Magma Ocean Solidification at 4.43 Ga

Crystallization of the lunar magma ocean yielded a chemically unique liquid residuum named KREEP. This component is expressed as a large patch on the near side of the Moon, and a possible smaller patch in the northwest portion of the Moon's South Pole-Aitken basin on the far side. Thermal models estimate that the crystallization of the lunar magma ocean (LMO) could have spanned from 10 and 200 Myr, while studies of radioactive decay systems have yielded inconsistent ages for the completion of LMO crystallization covering over 160 Myr. Here, we show that the Moon achieved over 99 percent crystallization at 4429+/-76 Myr, indicating a lunar formation age of 4450 Myr or possibly older. Using the 176Lu-176Hf decay system (t1/2=37 Gyr), we found that the initial 176Hf/177Hf ratios of lunar zircons with varied U-Pb ages are consistent with their crystallization from a KREEP-rich reservoir with a consistently low 176Lu/177Hf ratio of 0.0167 that emerged ~140 Myr after solar system formation. The previously proposed younger model age of 4.33 Ga for the source of mare basalts (240 Myr after solar system formation) might reflect the timing of a large impact. Our results demonstrate that lunar magma ocean crystallization took place while the Moon was still battered by planetary embryos and planetesimals leftover from the main stage of planetary accretion. Study of Lu-Hf model ages for samples brought back from the South Pole-Aitken basin will help to assess the lateral continuity of KREEP and further understand its significance in the early history of the Moon.

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arXiv2024

The Ni isotopic composition of Ryugu reveals a common accretion region for carbonaceous chondrites

The isotopic compositions of samples returned from Cb-type asteroid Ryugu and Ivuna-type (CI) chondrites are distinct from other carbonaceous chondrites, which has led to the suggestion that Ryugu and CI chondrites formed in a different region of the accretion disk, possibly around the orbits of Uranus and Neptune. We show that, like for Fe, Ryugu and CI chondrites also have indistinguishable Ni isotope anomalies, which differ from those of other carbonaceous chondrites. We propose that this unique Fe and Ni isotopic composition reflects different accretion efficiencies of small FeNi metal grains among the carbonaceous chondrite parent bodies. The CI chondrites incorporated these grains more efficiently, possibly because they formed at the end of the disk's lifetime, when planetesimal formation was also triggered by photoevaporation of the disk. Isotopic variations among carbonaceous chondrites may thus reflect fractionation of distinct dust components from a common reservoir, implying CI chondrites and Ryugu may have formed in the same region of the accretion disk as other carbonaceous chondrites.

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arXiv2024

The Elemental Abundances of Ryugu: Assessment of Chemical Heterogeneities and the Nugget Effect

The Hayabusa 2 spacecraft sampled ~5.4 g of asteroid material from the Cb-type asteroid Ryugu. Initial analysis of the Ryugu materials revealed a mineralogical, chemical, and isotopic kinship to the CI chondrites. In this study, we have summarized the elemental abundances of Ryugu samples published to date, and evaluated their compositional variability associated with the CI chondrite data. The abundances of some elements (e.g., P, Ca, Mn, and rare earth elements) in individual Ryugu particles were found to show large relative dispersions compared to the other elements, presumably due to the nugget effect of aqueously formed minor secondary minerals (e.g., dolomite, apatite, magnetite, and pyrrhotite). Consequently, the mean abundances of Ryugu for these elements, calculated using currently available Ryugu data, are accompanied by a certain degree of uncertainties. We suggest establishing a consortium to determine the representative elemental abundances of Ryugu by measuring aliquots from a large homogenized powder sample that can mitigate the nugget effect. Our statistical calculation shows that at least 750 and 400 mg of homogenized samples from Chambers A and C, respectively, are needed to achieve within +/-5% compositional heterogeneity. The data obtained throughout the consortium activity complement the scientific objectives of the Hayabusa2 mission. Moreover, we anticipate that the obtained Ryugu data, coupled with the elemental abundances of CI chondrites, provide new insights into the chemical composition of the Solar System, which will be used by multidisciplinary communities, including Earth and planetary sciences, astronomy, physics, and chemistry.

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arXiv2023

Past and Present Dynamics of the Iron Biogeochemical Cycle

This chapter investigates the complexities surrounding the iron biogeochemical cycle from the Archean to present, with a focus on assessing the balance between iron sources and sinks during long periods of Earth's history with relatively invariable redox conditions, when steady state can be safely assumed. Currently, the residence time of iron in the ocean may be as short as approximately 5 years. The input flux of iron is highly sensitive to redox cycling in sediments, while its removal primarily occurs through dispersed processes of oxidation and precipitation. In the Archean, we find a significant imbalance between continental and hydrothermal inputs, which collectively contribute between 61,500 to 263,000 Gg/yr of dissolved iron to the oceans, and the most obvious sinks such as iron formations (IFs), which sequester up to ~43,000 Gg/yr of iron. A possible solution to this imbalance involves the dispersed abiotic precipitation and removal of iron as silicates, sulfides, and carbonates in marine basins. Additionally, we calculate the residence time of dissolved iron in the Archean oceans to be between 6 kyr and 3 Myr, which is significantly longer than the ocean mixing timescale. Our estimates indicate that under the anoxic Archean atmosphere, the iron cycle was more protracted than today, and the isotopic compositions and concentrations of dissolved iron were likely more uniform. Distinct water bodies were likely confined to limited areas or specific, dynamic systems with intense iron turnover, such as regions where deep-sea upwelling currents brought hydrothermal iron to photic zones rich in biotic or abiotic oxidants.

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arXiv2023

Isotopic Trichotomy of Main Belt Asteroids from Implantation of Outer Solar System Planetesimals

Recent analyses of samples from asteroid (162173) Ryugu returned by JAXA's Hayabusa2 mission suggest that Ryugu and CI chondrites formed in the same region of the protoplanetary disk, in a reservoir that was isolated from the source regions of other carbonaceous (C-type) asteroids. Here we conduct $N$-body simulations in which CI planetesimals are assumed to have formed in the Uranus/Neptune zone at $\sim15$--25 au from the Sun. We show that CI planetesimals are scattered by giant planets toward the asteroid belt where their orbits can be circularized by aerodynamic gas drag. We find that the dynamical implantation of CI asteroids from $\sim15$--25 au is very efficient with $\sim 5$\% of $\sim 100$-km planetesimals reaching stable orbits in the asteroid belt by the end of the protoplanetary gas disk lifetime. The efficiency is reduced when planetesimal ablation is accounted for. The implanted population subsequently evolved by collisions and was depleted by dynamical instabilities. The model can explain why CIs are isotopically distinct from other C-type asteroids which presumably formed at $\sim5$--10 au.

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arXiv2023

Methodologies for 176Lu-176Hf Analysis of Zircon Grains from the Moon and Beyond

Zircons are found in extraterrestrial rocks from the Moon, Mars, and some differentiated meteorite parent-bodies. These zircons are rare, often of small size, and have been affected by neutron capture induced by cosmic ray exposure. The application of the 176Lu-176Hf decay system to zircons from planetary bodies such as the Moon can help establish the chronology of large-scale differentiation processes, like the crystallization of the lunar magma ocean. Here, we present methods to measure the isotopic composition of Hf of extraterrestrial zircons dated using ID-TIMS U-Pb after chemical abrasion. We introduce a 2-stage elution scheme to separate Hf from Zr while preserving the unused Zr fraction for future isotopic analysis. The effect of neutron capture is also re-examined using the latest thermal neutron capture cross sections and epithermal resonance integrals. Our tests show that the precision of Hf isotopic analyses is close to what is theoretically attainable. We have tested this method to a limited set of zircon grains from lunar rocks returned by the Apollo missions (lunar soil 14163, fragmental polymict breccia 72275, and clast-rich breccia 14321). The model ages align with previously reported values, but further work is needed to assess the chronology of lunar magma ocean crystallization as only a handful of small zircons (5 zircons from 3 samples) were analyzed, and the precision of the analyses can be improved by measuring more and larger lunar zircon grains.

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arXiv2023

Bayesian Inference on the Isotopic Building Blocks of Mars and Earth

Isotopic anomalies provide a means of probing the materials responsible for the formation of terrestrial planets. By analyzing new iron isotopic anomaly data from Martian meteorites and drawing insights from published data for O, Ca, Ti, Cr, Fe, Ni, Sr, Zr, Mo, Ru, and Si, we scrutinize potential changes in the isotopic composition of the material accreted by Mars and Earth during their formation. A Principal Component Analysis of isotopic anomalies in meteorites identifies three main clusters (forming the three parts of the isotopic trichotomy): CI, CC=CM+CO+CV+CR, and NC=EH+EL+H+L+LL. Our results suggest that Earth is primarily an isotopic mixture of ~92% E, 6 % CI, and <2% COCV and O. Mars, on the other hand, appears to be a mixture of ~65% E, 33% O, and <2% CI and COCV. We establish that Earth's CI contribution substantially increased during the latter half of its accretion. Mars began accreting a mix of O and E but predominantly accreted E later. Mars' changing isotopic makeup during accretion can be explained if it underwent gas-driven type I migration from its origin near the O - E boundary to a location well within the E region during the first few million years of solar system history. Earth's later increased CI contribution may be attributed to the stochastic impact of an interloper carbonaceous embryo that moved inside the inner solar system region while nebular gas was still present, and subsequently participated in the stage of chaotic growth. The recent findings of Si isotopic anomalies in enstatite chondrites when compared to terrestrial rocks likely stems from insufficient correction for high-temperature equilibrium isotopic fractionation. With appropriate adjustments for this influence, both the silicate Earth and enstatite chondrites exhibit comparable Si isotopic anomalies, reaffirming a genetic link between them.

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arXiv2022

Presolar stardust in asteroid Ryugu

We have conducted a NanoSIMS-based search for presolar material in samples recently returned from C-type asteroid Ryugu as part of JAXA's Hayabusa2 mission. We report the detection of all major presolar grain types with O- and C-anomalous isotopic compositions typically identified in carbonaceous chondrite meteorites: 1 silicate, 1 oxide, 1 O-anomalous supernova grain of ambiguous phase, 38 SiC, and 16 carbonaceous grains. At least two of the carbonaceous grains are presolar graphites, whereas several grains with moderate C isotopic anomalies are probably organics. The presolar silicate was located in a clast with a less altered lithology than the typical extensively aqueously altered Ryugu matrix. The matrix-normalized presolar grain abundances in Ryugu are 4.8$^{+4.7}_{-2.6}$ ppm for O-anomalous grains, 25$^{+6}_{-5}$ ppm for SiC grains and 11$^{+5}_{-3}$ ppm for carbonaceous grains. Ryugu is isotopically and petrologically similar to carbonaceous Ivuna-type (CI) chondrites. To compare the in situ presolar grain abundances of Ryugu with CI chondrites, we also mapped Ivuna and Orgueil samples and found a total of SiC grains and 6 carbonaceous grains. No O-anomalous grains were detected. The matrix-normalized presolar grain abundances in the CI chondrites are similar to those in Ryugu: 23 $^{+7}_{-6}$ ppm SiC and 9.0$^{+5.3}_{-4.6}$ ppm carbonaceous grains. Thus, our results provide further evidence in support of the Ryugu-CI connection. They also reveal intriguing hints of small-scale heterogeneities in the Ryugu samples, such as locally distinct degrees of alteration that allowed the preservation of delicate presolar material.

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arXiv2021

Oxygen and Aluminum-Magnesium Isotopic Systematics of Presolar Nanospinel Grains from CI Chondrite Orgueil

Presolar oxide grains have been previously divided into several groups (Group 1 to 4) based on their isotopic compositions, which can be tied to several stellar sources. Much of available data was acquired on large grains, which may not be fully representative of the presolar grain population present in meteorites. We present here new O isotopic data for 74 small presolar oxide grains (~200 nm in diameter on average) from Orgueil and Al-Mg isotopic systematics for 25 of the grains. Based on data-model comparisons, we show that (i) Group 1 and Group 2 grains more likely originated in low-mass first-ascent (red giant branch; RGB) and/or second-ascent (asymptotic giant branch; AGB) red giant stars and (ii) Group 1 grains with (26Al/27Al)0 >= 5x10^-3 and Group 2 grains with (26Al/27Al)0 <= 1x10^-2 all likely experienced extra circulation processes in their parent low-mass stars but under different conditions, resulting in proton-capture reactions occurring at enhanced temperatures. We do not find any large 25Mg excess in Group 1 oxide grains with large 17O enrichments, which provides evidence that 25Mg is not abundantly produced in low-mass stars. We also find that our samples contain a larger proportion of Group 4 grains than so far suggested in the literature for larger presolar oxide grains (~400 nm). We also discuss our observations in the light of stellar dust production mechanisms.

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arXiv2021

Earth's accretion inferred from iron isotopic anomalies of supernova nuclear statistical equilibrium origin

Nucleosynthetic Fe isotopic anomalies in meteorites may be used to reconstruct the early dynamical evolution of the solar system and to identify the origin and nature of the material that built planets. Using high-precision iron isotopic data of 23 iron meteorites from nine major chemical groups we show that all iron meteorites show the same fundamental dichotomy between non-carbonaceous (NC) and a carbonaceous (CC) meteorites previously observed for other elements. The Fe isotopic anomalies are predominantly produced by variation in 54Fe, where all CC iron meteorites are characterized by an excess in 54Fe relative to NC iron meteorites. This excess in 54Fe is accompanied by an excess in 58Ni observed in the same CC meteorite groups. Together, these overabundances of 54Fe and 58Ni are produced by nuclear statistical equilibrium either in type Ia supernovae or in the Si/S shell of core-collapse supernovae. The new Fe isotopic data reveal that Earth's mantle plots on or close to correlations defined by Fe, Mo, and Ru isotopic anomalies in iron meteorites, indicating that throughout Earth's accretion, the isotopic composition of its building blocks did not drastically change. While Earth's mantle has a similar Fe isotopic composition to CI chondrites, the latter are clearly distinct from Earth's mantle for other elements (e.g., Cr and Ni) whose delivery to Earth coincided with Fe. The fact that CI chondrites exhibit large Cr and Ni isotopic anomalies relative to Earth's mantle, therefore, demonstrates that CI chondrites are unlikely to have contributed significant Fe to Earth.

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arXiv2021

Origin of the Moon

The Earth-Moon system is unusual in several respects. The Moon is roughly 1/4 the radius of the Earth - a larger satellite-to-planet size ratio than all known satellites other than Pluto's Charon. The Moon has a tiny core, perhaps with only ~1% of its mass, in contrast to Earth whose core contains nearly 30% of its mass. The Earth-Moon system has a high total angular momentum, implying a rapidly spinning Earth when the Moon formed. In addition, the early Moon was hot and at least partially molten with a deep magma ocean. Identification of a model for lunar origin that can satisfactorily explain all of these features has been the focus of decades of research.

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arXiv2019

Vapor drainage in the protolunar disk as the cause for the depletion in volatile elements of the Moon

Lunar rocks are severely depleted in moderately volatile elements such as Rb, K, and Zn relative to Earth. Identifying the cause of this depletion is important for understanding how the Earth-Moon system evolved in the aftermath of the Moon-forming giant impact. We measured the Rb isotopic compositions of lunar and terrestrial rocks to understand why moderately volatile elements are depleted in the Moon. Combining our new measurements with previous data reveals that the Moon has an 87Rb/85Rb ratio higher than Earth by +0.16 permil. This isotopic composition is consistent with evaporation of Rb into a vapor medium that was ~99 percent saturated. Evaporation under this saturation can also explain the previously documented isotopic fractionations of K, Ga, Cu and Zn of lunar rocks relative to Earth. We show that a possible setting for achieving the same saturation upon evaporation of elements with such diverse volatilities is through viscous drainage of a partially vaporized protolunar disk onto Earth. In the framework of an alpha-disk model, the alpha-viscosity needed to explain the ~99% saturation calculated here is 0.001 to 0.01, which is consistent with a vapor disk where viscosity is controlled by magnetorotational instability.

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arXiv2019

Elemental and isotopic variability in solar system materials by mixing and processing of primordial disk reservoirs

Isotope anomalies among planetary bodies provide key constraints on planetary genetics and the Solar System's dynamical evolution. However, to unlock the full potential of these anomalies for constraining the processing, mixing, and transport of material in the disk it is essential to identify the main components responsible for producing planetary-scale isotope variations, and to investigate how they relate to the isotopic heterogeneity inherited from the Solar System's parental molecular cloud. To address these issues we measured the Ti and Sr isotopic compositions of Ca,Al-rich inclusions (CAIs) from the Allende CV3 chondrite, as well as acid leachates and an insoluble residue from the Murchison CM2 chondrite, and combine these results with literature data for presolar grains, hibonites, chondrules, and bulk meteorites. Our analysis reveals that the mineral-scale nebular isotopic heterogeneity as sampled by leachates and presolar grains is largely decoupled from the planetary-scale isotope anomalies. Combining isotope anomaly data for a large number of elements reveals that the difference between non-carbonaceous (NC) and carbonaceous (CC) meteorites is the product of mixing between NC material and a nebular reservoir (termed IC) whose isotopic composition is similar to that of CAIs, but whose chemical composition is similar to bulk chondrites. In our preferred model, the distinct isotopic compositions of these two nebular reservoirs reflect an inherited heterogeneity of the solar system's parental molecular cloud core, which therefore has never been fully homogenized during collapse. Planetary-scale isotopic anomalies are thus caused by variable mixing of isotopically distinct primordial disk reservoirs, the selective processing of these reservoirs in different nebular environments, and the heterogeneous distribution of the thereby forming nebular products.

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arXiv2019

Catching Element Formation In The Act

Gamma-ray astronomy explores the most energetic photons in nature to address some of the most pressing puzzles in contemporary astrophysics. It encompasses a wide range of objects and phenomena: stars, supernovae, novae, neutron stars, stellar-mass black holes, nucleosynthesis, the interstellar medium, cosmic rays and relativistic-particle acceleration, and the evolution of galaxies. MeV gamma-rays provide a unique probe of nuclear processes in astronomy, directly measuring radioactive decay, nuclear de-excitation, and positron annihilation. The substantial information carried by gamma-ray photons allows us to see deeper into these objects, the bulk of the power is often emitted at gamma-ray energies, and radioactivity provides a natural physical clock that adds unique information. New science will be driven by time-domain population studies at gamma-ray energies. This science is enabled by next-generation gamma-ray instruments with one to two orders of magnitude better sensitivity, larger sky coverage, and faster cadence than all previous gamma-ray instruments. This transformative capability permits: (a) the accurate identification of the gamma-ray emitting objects and correlations with observations taken at other wavelengths and with other messengers; (b) construction of new gamma-ray maps of the Milky Way and other nearby galaxies where extended regions are distinguished from point sources; and (c) considerable serendipitous science of scarce events -- nearby neutron star mergers, for example. Advances in technology push the performance of new gamma-ray instruments to address a wide set of astrophysical questions.

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arXiv2017

Triggered Star Formation Inside the Shell of a Wolf-Rayet Bubble as the origin of the Solar System

A critical constraint on solar system formation is the high $^{26}$Al/$^{27}$Al abundance ratio of 5 $\times 10^{-5}$ at the time of formation, which was about 17 times higher than the average Galactic ratio, while the $^{60}$Fe/$^{56}$Fe value was about $2 \times 10^{-8}$, lower than the Galactic value. This challenges the assumption that a nearby supernova was responsible for the injection of these short-lived radionuclides into the early solar system. We show that this conundrum can be resolved if the Solar System was formed by triggered star formation at the edge of a Wolf-Rayet (W-R) bubble. Aluminium-26 is produced during the evolution of the massive star, released in the wind during the W-R phase, and condenses into dust grains that are seen around W-R stars. The dust grains survive passage through the reverse shock and the low density shocked wind, reach the dense shell swept-up by the bubble, detach from the decelerated wind and are injected into the shell. Some portions of this shell subsequently collapses to form the dense cores that give rise to solar-type systems. The subsequent aspherical supernova does not inject appreciable amounts of $^{60}$Fe into the proto-solar-system, thus accounting for the observed low abundance of $^{60}$Fe. We discuss the details of various processes within the model and conclude that it is a viable model that can explain the initial abundances of $^{26}$Al and $^{60}$Fe. We estimate that 1-16% of all Sun-like stars could have formed in such a setting of triggered star formation in the shell of a WR bubble.

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arXiv2016

Origin of uranium isotope variations in early solar nebula condensates

High temperature condensates found in meteorites display uranium isotopic variations (235U/238U) that complicate dating of the formation of the Solar System and whose origin remains mysterious. It is possible that these variations are due to decay of the short-lived radionuclide 247Cm (t1/2=15.6 Myr) into 235U but they could also be due to uranium kinetic isotopic fractionation during condensation. We report uranium isotope measurements of meteoritic refractory inclusions that reveal excesses of 235U reaching ~+6 % relative to average solar system composition, which can only be due to decay of 247Cm. This allows us to constrain the 247Cm/235U ratio at Solar System formation to (7.0 +- 1.6) x 10-5. This value provides new clues on the universality of nucleosynthetic r-process of rapid neutron capture.

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arXiv2015

Planetary and meteoritic Mg/Si and d30Si variations inherited from solar nebula chemistry

The bulk chemical compositions of planets are uncertain, even for major elements such as Mg and Si. This is due to the fact that the samples available for study all originate from relatively shallow depths. Comparison of the stable isotope compositions of planets and meteorites can help overcome this limitation. Specifically, the non-chondritic Si isotope composition of the Earth's mantle was interpreted to reflect the presence of Si in the core, which can also explain its low density relative to pure Fe-Ni alloy. However, we have found that angrite meteorites display a heavy Si isotope composition similar to the lunar and terrestrial mantles. Because core formation in the angrite parent-body (APB) occurred under oxidizing conditions at relatively low pressure and temperature, significant incorporation of Si in the core is ruled out as an explanation for this heavy Si isotope signature. Instead, we show that equilibrium isotopic fractionation between gaseous SiO and solid forsterite at 1370 K in the solar nebula could have produced the observed Si isotope variations. Nebular fractionation of forsterite should be accompanied by correlated variations between the Si isotopic composition and Mg/Si ratio following a slope of 1, which is observed in meteorites. Consideration of this nebular process leads to a revised Si concentration in the Earth's core of 3.6 (+6.0/-3.6) wt% and provides estimates of Mg/Si ratios of bulk planetary bodies.

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arXiv2015

Low 60Fe abundance in Semarkona and Sahara 99555

Iron-60 (t1/2=2.62 Myr) is a short-lived nuclide that can help constrain the astrophysical context of solar system formation and date early solar system events. A high abundance of 60Fe (60Fe/56Fe= 4x10-7) was reported by in situ techniques in some chondrules from the LL3.00 Semarkona meteorite, which was taken as evidence that a supernova exploded in the vicinity of the birthplace of the Sun. However, our previous MC-ICPMS measurements of a wide range of meteoritic materials, including chondrules, showed that 60Fe was present in the early solar system at a much lower level (60Fe/56Fe=10-8). The reason for the discrepancy is unknown but only two Semarkona chondrules were measured by MC-ICPMS and these had Fe/Ni ratios below ~2x chondritic. Here, we show that the initial 60Fe/56Fe ratio in Semarkona chondrules with Fe/Ni ratios up to ~24x chondritic is 5.4x10-9. We also establish the initial 60Fe/56Fe ratio at the time of crystallization of the Sahara 99555 angrite, a chronological anchor, to be 1.97x10-9. These results demonstrate that the initial abundance of 60Fe at solar system birth was low, corresponding to an initial 60Fe/56Fe ratio of 1.01x10-8.

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