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Insights Into the Origin of Carbonaceous Chondrite Organics from Their Triple Oxygen Isotope Composition

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Insights Into the Origin of Carbonaceous Chondrite Organics from Their Triple Oxygen Isotope Composition The University of Manchester Research Insights into the origin of carbonaceous chondrite organics from their triple oxygen isotope composition DOI: 10.1073/pnas.1808101115 Document Version Accepted author manuscript Link to publication record in Manchester Research Explorer Citation for published version (APA): Tartese, R., Chaussidon, M., Gurenko, A., Delarue, F., & Robert, F. (2018). Insights into the origin of carbonaceous chondrite organics from their triple oxygen isotope composition. Proceedings of the National Academy of Sciences of the United States of America. https://doi.org/10.1073/pnas.1808101115 Published in: Proceedings of the National Academy of Sciences of the United States of America Citing this paper Please note that where the full-text provided on Manchester Research Explorer is the Author Accepted Manuscript or Proof version this may differ from the final Published version. If citing, it is advised that you check and use the publisher's definitive version. General rights Copyright and moral rights for the publications made accessible in the Research Explorer are retained by the authors and/or other copyright owners and it is a condition of accessing publications that users recognise and abide by the legal requirements associated with these rights. 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Oct. 2021 1 Insights into the origin of carbonaceous chondrite organics from their triple 2 oxygen isotope composition 3 4 Romain Tartèsea,*, Marc Chaussidonb, Andrey Gurenkoc, Frédéric Delarued, François Roberte 5 6 7 aSchool of Earth and Environmental Sciences, The University of Manchester, Manchester, M13 8 9PL, UK. 9 bInstitut de Physique du Globe de Paris (IPGP), Université Sorbonne-Paris-Cité, Université Paris 10 Diderot, CNRS UMR 7154, Paris, France 11 cCentre de Recherches Pétrographiques et Géochimiques, UMR 7358, Université de Lorraine, 12 54501 Vandoeuvre-lès-Nancy, France. 13 dSorbonne Université, UPMC, CNRS, EPHE, PSL, UMR 7619 METIS, 4 place Jussieu, F-75005 14 Paris, France. 15 eInstitut de Minéralogie, de Physique des Matériaux et de Cosmochimie, Muséum National 16 d’Histoire Naturelle, Sorbonne Universités, CNRS, UPMC & IRD, 75005 Paris, France 17 18 *corresponding author: [email protected] – Tel: +44161 275 6908 19 20 Short title: O isotope composition of carbonaceous chondrite organics. 21 To be submitted to PNAS 22 Categories: Physical Sciences > Earth, Atmospheric, and Planetary Sciences 23 24 Abstract 25 Dust grains of organic matter were the main reservoir of C and N in the forming Solar System, 26 and are thus considered as an essential ingredient for the emergence of life. Yet, the physical 27 environment and the chemical mechanisms at the origin of these organic grains are still highly 28 debated. In this study we report the first high precision triple oxygen isotope composition for 29 insoluble organic matter isolated from three emblematic carbonaceous chondrites, Orgueil, 30 Murchison, and Cold Bokkeveld. These results suggest that the O isotope composition of 31 carbonaceous chondrite insoluble organic matter falls on a slope 1 correlation line in the triple 32 oxygen isotope diagram. The lack of detectable mass-dependent O isotopic fractionation, 33 indicated by the slope 1 line, suggest that the bulk of carbonaceous chondrite organics did not 34 form on asteroidal parent bodies during low temperature hydrothermal events. On the other hand, 35 these new O isotope data, together with the H and N isotope characteristics of insoluble organic 36 matter, may indicate that parent bodies of different carbonaceous chondrite types largely accreted 37 organics formed locally in the protosolar nebula, possibly by photochemical dissociation of C- 38 rich precursors. 39 40 Keywords 41 Carbonaceous chondrites; Organic matter; Oxygen isotopes; Protosolar nebula; Secondary ion 42 mass spectrometry. 43 44 Significance Statement 45 Refractory organic matter found in volatile-rich asteroidal materials essentially comprise the 46 elements C, H, O, N and S, which are thought to be important building blocks for life. 47 Characterizing the origin(s) of these organics thus constitutes a key step to constrain the origin of 48 life on Earth and appraise the habitability potential of other worlds. Yet how and where these 49 organics formed is still highly debated. In this study we have determined the oxygen isotope 50 composition of refractory organics from two families of carbonaceous chondrites. These data 51 suggest that these organics formed in the nascent Solar System, possibly through chemical 52 reactions occurring in the disk surrounding the young Sun. 53 54 \body 55 56 Introduction 57 Type 1-2 carbonaceous chondrites (CC) contain several wt.% carbon that mostly occurs as small 58 patches of organic matter (OM) dispersed in the fine-grained matrix (1). Because this OM 59 possibly played a key role in the development of life on the early Earth, its molecular structure, 60 and its chemical and isotopic compositions have been extensively investigated (see 2 and 61 references therein for a recent review). Despite this profusion of structural, chemical, and isotopic 62 information, the question of whether CC OM formed in the cold interstellar medium (e.g., 3-5), 63 in the protosolar nebula (PSN) (e.g., 6-9), or is a product of organic synthesis during 64 hydrothermalism on CC parent bodies (e.g., 10) remains highly debated, notably because the 65 extent of chemical and isotopic alteration of OM during secondary processes on CC parent bodies 66 is debated (11-15). 67 68 Oxygen is the third most abundant element in the Solar System and has three stable isotopes 16O, 69 17O and 18O. Because different fractionation laws govern interplanetary and intraplanetary 70 processes (e.g., 16), the oxygen three-isotope system can provide information that cannot be 71 accessed using other two-isotope systems of light elements such as H, C and N. In planetary 72 bodies, variations of the 17O/16O and 18O/16O ratios almost always obey the mass-dependent 73 relationship 17O ~ 0.52 × 18O1, while oxygen isotope abundance variations between Solar 74 System gas and solids are primarily governed by the mass-independent relationship 17O ~ 1.0 × 1this -notation represents deviations in parts per thousand (‰) of the 17,18O/16O ratios relative to those of the 17,18 17,18 16 17,18 16 Standard Mean Ocean Water (SMOW), according to the equation O = [( O/ O)sample/( O/ O)SMOW – 1] × 1000). 75 18O (15). Much of our understanding of how our Solar System formed and evolved is thus based 76 on O isotope studies of meteoritic materials (e.g., 16-17), and this should apply to carbonaceous 77 chondrite OM since it contains ~10-25 wt.% O (11-12). 78 79 However, determining the O isotope composition of OM is challenging since it tends to be 80 intimately mixed with O-rich silicates and oxides at a nano- to micro-scale in carbonaceous 81 chondrites (e.g., 18). Acid-maceration used to isolate the insoluble OM (IOM) fraction from 82 whole rock samples removes most of the silicates but is less effective at dissolving sulfides and 83 some refractory O-bearing oxides such as chromite, spinel, hibonite or corundum. Bulk pyrolysis 84 O isotope analysis of IOM is thus susceptible to contamination by residual mineral inclusions. To 85 constrain the triple O isotope composition of carbonaceous chondrite IOM, we integrate here 86 high spatial resolution secondary ion mass spectrometry (SIMS) data obtained using NanoSIMS 87 with high precision 17,18O/16O isotope ratios obtained using large geometry multi-collector IMS 88 1270/80 ion probes (referred as L-SIMS in the following). For each L-SIMS O isotope analysis, 89 measurement of 28Si, 32S, and 56Fe16O intensities allowed a first order filtering of data for which 90 the O signals were largely affected by contamination by residual silicate and/or oxide phases (see 91 Methods for details). The results presented here constitute the first high precision triple O isotope 92 estimates for IOM residues isolated from two emblematic carbonaceous chondrite falls, the 93 Ivuna-type (CI) Orgueil meteorite and the Mighei-type (CM) Murchison meteorite. 94 95 Results 96 The 17O and 18O values measured by L-SIMS in the Orgueil, Murchison and Cold Bokkeveld 97 IOM residues range between -23.3 ± 2.4 ‰ and +18.9 ± 2.4 ‰ and -18.0 ± 2.3 ‰ and +16.9 ± 98 2.3 ‰ (uncertainties reported at 2), respectively (Fig. 1 and SI Appendix, Table S1). Least 99 square regression through all the data yields a line defined by 17O = 1.00 (± 0.14) × 18O – 3.78 100 (± 1.35) (95% confidence level, n = 36, r2 = 0.86), which is indistinguishable from the 101 relationship known as the carbonaceous chondrite anhydrous mineral (CCAM) line (17O = 0.95 102 × 18O – 4.18) (Fig. 1). 103 104 The NanoSIMS data allow determining O isotope ratios with larger uncertainties than those 105 obtained by L-SIMS, but with higher spatial resolution, i.e., over region of interests (ROI) that 106 can be selected from ion imaging to minimize the effect of residual oxides and/or silicates, 107 located through analysis of 28Si and 56Fe16O simultaneously with O isotopes. The NanoSIMS 108 analyses obtained over 40 m2 areas in Murchison and Orgueil IOM residues show little 28Si 109 hotspots but more abundant micron size 16O-enriched areas (Figs. 2 and S2). The 16O hotspots are 110 generally associated with 56Fe16O hotspots, suggesting that magnetite and/or chromite are the 111 main mineral phases that have resisted acid-maceration treatments. 112 113 In terms of surface, these 16O-enriched ROI represent 16-18 % and 12-21 % of the total 40 m × 114 40 m areas analyzed in Murchison and Orgueil, respectively, while pure IOM ROI, defined 115 based on 16O intensity maps (see Methods), comprise 21-31 % and 18-20 % of the Murchison 116 and Orgueil analyzed areas, respectively (Fig.
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