Izumi Nakai’s research while affiliated with Tokyo University of Science and other places

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Publications (314)


Zirconium isotope composition indicates s ‐process depletion in samples returned from asteroid Ryugu
  • Article

November 2024

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75 Reads

Meteoritics & Planetary Science

Maria Schönbächler

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Nucleosynthetic isotope variations are powerful tracers to determine genetic relationships between meteorites and planetary bodies. They can help to link material collected by space missions to known meteorite groups. The Hayabusa 2 mission returned samples from the Cb‐type asteroid (162173) Ryugu. The mineralogical, chemical, and isotopic characteristics of these samples show strong similarities to carbonaceous chondrites and in particular CI chondrites. The nucleosynthetic isotope compositions of Ryugu overlap with CI chondrites for several elements (e.g., Cr, Ti, Fe, and Zn). In contrast to these isotopes, which are of predominately supernovae origin, s ‐process variations in Mo isotope data are similar to those of carbonaceous chondrites, but even more s‐ process depleted. To further constrain the origin of this depletion and test whether this signature is also present for other s ‐process elements, we report Zr isotope compositions for three bulk Ryugu samples (A0106, A0106‐A0107, C0108) collected from the Hayabusa 2 mission. The data are complemented with that of terrestrial rock reference materials, eucrites, and carbonaceous chondrites. The Ryugu samples are characterized by distinct ⁹⁶ Zr enrichment relative to Earth, indicative of a s ‐process depletion. Such depletion is also observed for carbonaceous chondrites and eucrites, in line with previous Zr isotope work, but it is more extreme in Ryugu, as observed for Mo isotopes. Since s ‐process Zr and Mo are coupled in mainstream SiC grains, these distinct s‐ process variations might be due to SiC grain depletion in the analyzed materials, potentially caused by incomplete sample digestion, because the Ryugu samples were dissolved on a hotplate only to avoid high blank levels for other elements (e.g., Cr). However, local depletion of SiC grains cannot be excluded. An alternative, equally possible scenario is that aqueous alteration redistributed anomalous, s ‐process‐depleted, Zr on a local scale, for example, into Ca‐phosphates or phyllosilicates.


Figure 1. Nickel isotope anomalies in Ryugu and CI chondrites compared to other meteorites. (A) μ 60 Ni versus μ 64 Ni, (B) μ 64 Ni versus μ 62 Ni, (C) μ 58 Ni versus μ 60 Ni. Subscripts on axis labels indicate internal normalization to either 61 Ni/ 58 Ni (A, B) or 62 Ni/ 61 Ni (C). Ryugu and CI chondrites define a distinct compositional cluster in Ni isotope space that is offset from all other carbonaceous chondrites. The grey solid line in (B) is a regression through all meteorite data with a slope of ~3 (31, 34). The red solid line in panel (C) is a regression line through all NC meteorites with a slope
Figure 3. Relation of Cr, Ti, Ni, and Fe isotope anomalies in carbonaceous chondrites and Ryugu. Also shown are mixing lines between CI chondrites and CAIs, chondrules, and FeNi metal. Tick marks indicate mass fractions of material added to or lost from (for FeNi metal) CI chondrites. The µ 54 Cr and µ 50 Ti variations among the carbonaceous chondrites can be accounted for by mixing CI chondrite-like matrix with variable amounts of chondrules and CAIs, respectively (A). These mixtures cannot reproduce the µ 60 Ni variations, which more likely reflect the heterogeneous distribution (~5 wt%) of FeNi metal characterized by positive µ 60 Ni (B, C). The Ni isotopic composition of the chondrule component in (C) is inferred from the non-matrix intercept of Fig. 2C. The linear variations of µ 60 Ni and µ 54 Fe (D) indicate that FeNi metal is likely responsible for both the observed µ 54 Fe and µ 60 Ni variations. As such, the metal should be characterized by negative µ 54 Fe values. Closed symbols in (D) represent CC iron meteorite groups. Isotopic data are
Figure 4. Cartoon illustrating the formation mechanism and accretion region of carbonaceous chondrite parent bodies. (A) The four major components of carbonaceous chondrites (chondrules, refractory inclusions, matrix, and FeNi metal) are transported through the disk towards the Sun and are trapped in a pressure maximum, which was presumably located outside the orbit of Jupiter. (B) The parent bodies of several non-CI carbonaceous chondrites (i.e., CV, CK, CO, and CM) form in this pressure maximum and incorporate different proportions of refractory inclusions, chondrules, FeNi metal, and fine-grained matrix. Owing to their small size, accretion of FeNi metal grains is inefficient in all these bodies. At the end of the disk's lifetime, nebular gas is removed via photoevaporation leading to a late burst of planetesimal formation over a wider area of the disk. CI chondrites and Ryugu form by this process and incorporate the entire background population of dust in the disk, and so accrete the small FeNi metal grains more efficiently than the other carbonaceous chondrites. CR chondrites form at about the same time but by a similar process as the
The Ni isotopic composition of Ryugu reveals a common accretion region for carbonaceous chondrites
  • Preprint
  • File available

October 2024

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219 Reads

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

September 2024

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127 Reads

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2 Citations

Science Advances

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/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/Ryugu may have formed in the same region of the accretion disk as other carbonaceous chondrites.



Disequilibrium oxygen isotope distribution among aqueously altered minerals in Ryugu asteroid returned samples

April 2024

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139 Reads

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3 Citations

Meteoritics & Planetary Science

Oxygen 3‐isotope ratios of magnetite and carbonates in aqueously altered carbonaceous chondrites provide important clues to understanding the evolution of the fluid in the asteroidal parent bodies. We conducted oxygen 3‐isotope analyses of magnetite, dolomite, and breunnerite in two sections of asteroid Ryugu returned samples, A0058 and C0002, using a secondary ion mass spectrometer (SIMS). Magnetite was analyzed by using a lower primary ion energy that reduced instrumental biases due to the crystal orientation effect. We found two groups of magnetite data identified from the SIMS pit morphologies: (1) higher δ ¹⁸ O (from 3‰ to 7‰) and ∆ ¹⁷ O (~2‰) with porous SIMS pits mostly from spherulitic magnetite, and (2) lower δ ¹⁸ O (~ −3‰) and variable ∆ ¹⁷ O (0‰–2‰) mostly from euhedral magnetite. Dolomite and breunnerite analyses were conducted using multi‐collection Faraday cup detectors with precisions ≤0.3‰. The instrumental bias correction was applied based on carbonate compositions in two ways, using Fe and (Fe + Mn) contents, respectively, because Ryugu dolomite contains higher amounts of Mn than the terrestrial standard. Results of dolomite and breunnerite analyses show a narrow range of ∆ ¹⁷ O; 0.0‰–0.3‰ for dolomite in A0058 and 0.2‰–0.8‰ for dolomite and breunnerite in C0002. The majority of breunnerite, including large ≥100 μm grains, show systematically lower δ ¹⁸ O (~21‰) than dolomite (25‰–30‰ and 23‰–27‰ depending on the instrumental bias corrections). The equilibrium temperatures between magnetite and dolomite from the coarse‐grained lithology in A0058 are calculated to be 51 ± 11°C and 78 ± 14°C, depending on the instrumental bias correction scheme for dolomite; a reliable temperature estimate would require a Mn‐bearing dolomite standard to evaluate the instrumental bias corrections, which is not currently available. These results indicate that the oxygen isotope ratios of aqueous fluids in the Ryugu parent asteroid were isotopically heterogeneous, either spatially, or temporary. Initial water ice accreted to the Ryugu parent body might have ∆ ¹⁷ O > 2‰ that was melted and interacted with anhydrous solids with the initial ∆ ¹⁷ O < 0‰. In the early stage of aqueous alteration, spherulitic magnetite and calcite formed from aqueous fluid with ∆ ¹⁷ O ~ 2‰ that was produced by isotope exchange between water (∆ ¹⁷ O > 2‰) and anhydrous solids (∆ ¹⁷ O < 0‰). Dolomite and breunnerite, along with some magnetite, formed at the later stage of aqueous alteration under higher water‐to‐rock ratios where the oxygen isotope ratios were nearly at equilibrium between fluid and solid phases. Including literature data, δ ¹⁸ O of carbonates decreased in the order calcite, dolomite, and breunnerite, suggesting that the temperature of alteration might have increased with the degree of aqueous alteration.


Hydrogen in magnetite from asteroid Ryugu

January 2024

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132 Reads

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1 Citation

Meteoritics & Planetary Science

In order to gain insights on the conditions of aqueous alteration on asteroid Ryugu and the origin of water in the outer solar system, we developed the measurement of water content in magnetite at the micrometer scale by secondary ion mass spectrometry (NanoSIMS) and determined the H and Si content of coarse‐grained euhedral magnetite grains (polyhedral magnetite) and coarse‐grained fibrous (spherulitic) magnetite from the Ryugu polished section A0058‐C1001. The hydrogen content in magnetite ranges between ~900 and ~3300 wt ppm equivalent water and is correlated with the Si content. Polyhedral magnetite has low and homogenous silicon and water content, whereas fibrous magnetite shows correlated Si and water excesses. These excesses can be explained by the presence of hydrous Si‐rich amorphous nanoinclusions trapped during the precipitation of fibrous magnetite away from equilibrium and testify that fibrous magnetite formed from a hydrous gel with possibly more than 20 wt% water. An attempt to determine the water content in sub‐μm framboids indicates that additional calibration and contamination issues must be addressed before a safe conclusion can be drawn, but hints at elevated water content as well. The high water content in fibrous magnetite, expected to be among the first minerals to crystallize at low water–rock ratio, points to the control of water content by local conditions of magnetite precipitation rather than large‐scale alteration conditions. Systematic lithological variations associated with water‐rich and water‐poor magnetite suggest that the global context of alteration may be better understood if local water concentrations are compared with millimeter‐scale distribution of the various morphologies of magnetite. Finally, the high water content in the magnetite precursor gel indicates that the initial O isotopic composition in alteration water must not have been very different from that of the earliest magnetite crystals.



Neodymium‐142 deficits and samarium neutron stratigraphy of C‐type asteroid (162173) Ryugu

December 2023

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117 Reads

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3 Citations

Meteoritics & Planetary Science

We report Nd and Sm isotopic compositions of four samples of Ryugu returned by the Hayabusa2 mission, including “A” (first touchdown) and “C” (second touchdown) samples, and several carbonaceous chondrites to evaluate potential genetic relationships between Ryugu and known chondrite groups and track the cosmic ray exposure history of Ryugu. We resolved Nd and Sm isotopic anomalies in small (<20 ng Nd and Sm) sample sizes via thermal ionization mass spectrometer using 10 ¹³ Ω amplifiers. Ryugu samples exhibit resolvable negative μ ¹⁴² Nd values consistent with carbonaceous chondrite values, suggesting that Ryugu is related to the parent bodies of carbonaceous chondrites. Ryugu's negative μ ¹⁴⁹ Sm values are the result of exposure to galactic cosmic rays, as demonstrated by the correlation between ¹⁵⁰ Sm/ ¹⁵² Sm and ¹⁴⁹ Sm/ ¹⁵² Sm ratios that fall along the expected neutron capture correlation line. The neutron fluence calculated in the “A” samples (2.75 ± 1.94 × 10 ¹⁵ n cm ⁻² ) is slightly higher compared to the “C” samples (0.95 ± 2.04 × 10 ¹⁵ n cm ⁻² ), though overlapping within measurement uncertainty. The Sm results for Ryugu, at this level of precision, thus are consistent with a well‐mixed surface layer at least to the depths from which the “A” and “C” samples derive.



Figure 1. The μ 26 Mg * (A) and μ 25 Mg (B) values of Ryugu samples and carbonaceous chondrites analyzed here. Solid symbols reflect the weighted means of several meteorite samples, whereas open symbols are individual meteorites. The weighted means include data from Larsen et al. (2011, 2016), van Kooten et al. (2016), Luu et al. (2019), and van Kooten et al. (2020). Error bars represent the internal precision (2SE) for individual samples and 95% confidence intervals for weighted means.
Figure 2. Variation diagrams showing the relationships between the μ 25 Mg values of CI chondrites, Ryugu bulk samples, and inferred Ryugu dolomite and their Ca/Mg ratios and Ca abundance. The CI chondrite μ 25 Mg value reflects the weighted mean of Orgueil, Ivuna, and Alais based on data from this study and Larsen et al. (2011) and Luu et al. (2019). The Ca abundance and Ca/Mg ratio for CI chondrites are from Palme et al. (2014). The Ca abundance and Ca/Mg ratio for the Ryugu dolomite are from Bazi et al. (2022). The μ 25 Mg value of Ryugu dolomite was determined iteratively to minimize the scatter as measured by the M.S.W.D. Using a μ 25 Mg of −1400 returns an M.S.W.D. of 1.6 and 2.6 for panels (C) and (D), respectively. Apart from CI chondrite, where we used a 95% confidence interval, all other uncertainties represent the internal precisions (2SE). For the Ryugu dolomite μ 25 Mg value, we used an uncertainty estimate of 100 ppm.
The Magnesium Isotope Composition of Samples Returned from Asteroid Ryugu

November 2023

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208 Reads

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4 Citations

The Astrophysical Journal Letters

The nucleosynthetic isotope composition of planetary materials provides a record of the heterogeneous distribution of stardust within the early solar system. In 2020 December, the Japan Aerospace Exploration Agency Hayabusa2 spacecraft returned to Earth the first samples of a primitive asteroid, namely, the Cb-type asteroid Ryugu. This provides a unique opportunity to explore the kinship between primitive asteroids and carbonaceous chondrites. We report high-precision μ ²⁶ Mg* and μ ²⁵ Mg values of Ryugu samples together with those of CI, CM, CV, and ungrouped carbonaceous chondrites. The stable Mg isotope composition of Ryugu aliquots defines μ ²⁵ Mg values ranging from –160 ± 20 ppm to –272 ± 30 ppm, which extends to lighter compositions relative to Ivuna-type (CI) and other carbonaceous chondrite groups. We interpret the μ ²⁵ Mg variability as reflecting heterogeneous sampling of a carbonate phase hosting isotopically light Mg ( μ ²⁵ Mg ∼ –1400 ppm) formed by low temperature equilibrium processes. After correcting for this effect, Ryugu samples return homogeneous μ ²⁶ Mg* values corresponding to a weighted mean of 7.1 ± 0.8 ppm. Thus, Ryugu defines a μ ²⁶ Mg* excess relative to the CI and CR chondrite reservoirs corresponding to 3.8 ± 1.1 and 11.9 ± 0.8 ppm, respectively. These variations cannot be accounted for by in situ decay of ²⁶ Al given their respective ²⁷ Al/ ²⁴ Mg ratios. Instead, it requires that Ryugu and the CI and CR parent bodies formed from material with a different initial ²⁶ Al/ ²⁷ Al ratio or that they are sourced from material with distinct Mg isotope compositions. Thus, our new Mg isotope data challenge the notion that Ryugu and CI chondrites share a common nucleosynthetic heritage.


Citations (61)


... This observation appears consistent with the idea that Earth accreted roughly the second half of its mass from material akin to CI chondrites, which are presumed to represent the composition of pebbles from the outer disk. However, Hopp et al. (2022) have shown that in this case the BSE should also have a CI chondrite-like isotope composition for Ni (another siderophile element with similar siderophility as Fe), yet CI chondrites have the largest 64 Ni anomaly (compared to the BSE) among all meteorites (Spitzer et al., 2024). In general, the use of µ 54 Fe to trace the provenance of Earth's accreted material is difficult because the NC and CC domains overlap for µ 54 Fe, unlike for Ni isotopes (see Fig. 8 in Hopp et al., 2022, for a µ 54 Fe vs. µ 64 Ni diagram). ...

Reference:

Did the terrestrial planets of the Solar System form by pebble accretion?
The Ni isotopic composition of Ryugu reveals a common accretion region for carbonaceous chondrites
  • Citing Article
  • September 2024

Science Advances

... The different carbonaceous chondrites classes are approximately located on a single line in (Nakanishi et al. 2023), which plot outside the axis range used here. This CC-line also includes the primitive CI chondrites, marked with a bold blue cross (Burkhardt et al. 2011, although Dauphas et al. (2002b reports an off-set value). ...

Nucleosynthetic s-Process Depletion in Mo from Ryugu samples returned by Hayabusa2

Geochemical Perspectives Letters

... Other values measured for CM2 Murchison, Murray, Aguas Zarcas, CI Orgueil, and C2 ung Tarda at similar weight scales are shown for comparison of chemical composition. However, there is a variation of~0.1‰ in the Mg isotopic composition of Ryugu 35 . Such variation is explained by the varying amount of carbonates in each aliquot 18 , indicating the effect of taking only small aliquots. ...

The Magnesium Isotope Composition of Samples Returned from Asteroid Ryugu

The Astrophysical Journal Letters

... Third, this study was conducted on multiple bulk samples and therefore does not directly place a limit on the formation age of any particular grain, such that it requires the demonstration of isotopic equilibration of the samples. We note as well that an alteration age of 5.2 [+1.8, 1.4; 2σ] Ma was reported by Yokoyama, Wadhwa, et al. (2023) using ICP-MS but that this age suffers some of the same limitations. Therefore, we consider that these studies, while important, do not conclusively distinguish between the two interpretations of the SIMS ages. ...

Water circulation in Ryugu asteroid affected the distribution of nucleosynthetic isotope anomalies in returned sample

Science Advances

... The parent body size estimates are less conclusive due to the lack of data but they fall into the range of typical sizes estimated for early solar system planetesimals 52 . Of note is a size contrast to the sub-10 km radius parent body of Ryugu that was derived based on porosity modeling 13 and supported by later studies 53,54 . ...

The Oxygen Isotopic Composition of Samples Returned from Asteroid Ryugu with Implications for the Nature of the Parent Planetesimal

The Planetary Science Journal

... However, most of the large carbonaceous grains deviate by >2σ in at least one of these isotopic systems (Supplementary Table 1). Both the highest 15 N and 13 C enrichments are observed in grains with an IL functional group chemistry, while the two measured grains with HA functional chemistry contain depletions in both 15 N and 13 C. Similar simultaneous large isotopic depletions in both 15 N and 13 C were previously observed in Ryugu carbonaceous grains 8,35 . In carbonaceous meteorite samples, correlated 15 N and 13 C depletions have been observed in carbonaceous grains within many primitive chondrites, A TEM image of sample C0109-11 8 containing two carbonaceous grains (A1 and A2). ...

Abundant presolar grains and primordial organics preserved in carbon-rich exogenous clasts in asteroid Ryugu

Science Advances

... Ryugu samples show a close affinity with CI carbonaceous chondrites, which are the most chemically primitive, the most hydrated and organic-rich groups of asteroidal materials [3][4][5][6][7][8] . The accretion region of the parent body is probably beyond the H 2 O and CO 2 snow lines (3-4 au) and possibly beyond the orbit of Jupiter 4,7,[9][10][11] , where numerous icy planetesimals could have formed 12 . Therefore, Ryugu samples offer valuable insights into the evolution and water activity of outer Solar System bodies, including icy bodies that may possess habitable water environments. ...

Carbonate record of temporal change in oxygen fugacity and gaseous species in asteroid Ryugu

... The coevolutionary outline hypothesized here is also supported by the observations of secondary mineral assemblages and altered vein formations 38,[47][48][49] (Fig. 9). For a comparative investigation of those findings, the origin of Ryugu's water within the history of the parent body will be elucidated in subsequent studies 38,[50][51][52] . As a notable opportunity in 2023, NASA's OSIRIS-REx (Origins, Spectral Interpretation, Resource Identification and Security-Regolith Explorer) spacecraft returned the carbonaceous asteroid (101955) Bennu sample to Earth 53 . ...

Hydrogen Isotopic Composition of Hydrous Minerals in Asteroid Ryugu

The Astrophysical Journal Letters

... Ryugu samples show a close affinity with CI carbonaceous chondrites, which are the most chemically primitive, the most hydrated and organic-rich groups of asteroidal materials [3][4][5][6][7][8] . The accretion region of the parent body is probably beyond the H 2 O and CO 2 snow lines (3-4 au) and possibly beyond the orbit of Jupiter 4,7,[9][10][11] , where numerous icy planetesimals could have formed 12 . Therefore, Ryugu samples offer valuable insights into the evolution and water activity of outer Solar System bodies, including icy bodies that may possess habitable water environments. ...

Oxygen isotopes of anhydrous primary minerals show kinship between asteroid Ryugu and comet 81P/Wild2

Science Advances

... An important recent discovery is the finding of nucleosynthetic isotope anomalies for the moderately volatile element Zn (Martins et al., 2023;Paquet et al., 2022;Savage et al., 2022;Steller et al., 2022). For Zn, the BSE has a mixed NC-CC composition, indicating that ~70% of terrestrial Zn derives from the NC, and ~30% from the CC reservoir (Savage et al., 2022;Steller et al., 2022). ...

Contribution of Ryugu-like material to Earth’s volatile inventory by Cu and Zn isotopic analysis

Nature Astronomy