# Origin of the mass-dependent germanium isotopic continuum in the early Solar System

Béatrice Luais, Guillaume Florin

► To cite this version:

Béatrice Luais, Guillaume Florin. Origin of the mass-dependent germanium isotopic continuum in the early Solar System. Earth and Planetary Science Letters, 2025, 672, pp.119663. 10.1016/j.epsl.2025.119663. hal-05362993

HAL Id: hal-05362993

https://hal.science/hal-05362993v1

Submitted on 13 Nov 2025

HAL is a multi-disciplinary open access
archive for the deposit and dissemination of sci-
entific research documents, whether they are pub-
lished or not. The documents may come from
teaching and research institutions in France or
abroad, or from public or private research centers.

L'archive ouverte pluridisciplinaire HAL, est
destinée au dépôt et à la diffusion de documents
scientifiques de niveau recherche, publiés ou non,
émanant des établissements d'enseignement et de
recherche français ou étrangers, des laboratoires
publics ou privés.

<figure><img src="image_1.png" /></figure>

Distributed under a Creative Commons Attribution 4.0 International License
# Origin of the mass-dependent germanium isotopic continuum in the early Solar System

Béatrice Luais<fnref n="1" />* and Guillaume Florin<fnref n="2" />*

*Corresponding authors E-mail: <beatrice.luais@univ-lorraine.fr>; <guillaume.florin@uca.fr>

<https://doi.org/10.1016/j.epsl.2025.119663>

Received 29 March 2025; Received in revised form 28 September 2025; Accepted 1 October 2025;

Available online 25 October 2025

## Abstract

The warm, reduced, volatile-poor inner Solar System and cold, oxidized, volatile-rich outer Solar System are characterized by neutron-poor and neutron-rich isotopic anomalies, respectively. Nucleosynthetic isotopic anomalies recorded in meteorites, asteroidal bodies, and planets are thus indicative of their regions of formation. However, whether these reservoirs evolved as closed systems or underwent some degree of intermixing remains uncertain. Here, we report new high-precision mass-dependent germanium isotopic compositions revealing that carbonaceous chondrites exhibit higher and more variable δ<sup>74/70</sup>Ge values than ordinary chondrites, defining a strong continuous trend in both Ge concentrations and isotopic compositions. We highlight that similar strong correlations with matrix mass fraction occur across all chondrite groups, but that the non-carbonaceous (NCC, inner Solar System)–carbonaceous (CC, outer Solar System) dichotomy observed in ε<sup>48</sup>Ca, ε<sup>54</sup>Cr, ε<sup>50</sup>Ti, and ε<sup>64</sup>Ni nucleosynthetic anomalies is maintained. In the δ<sup>74/70</sup>Ge vs. ε<sup>48</sup>Ca, ε<sup>54</sup>Cr, ε<sup>50</sup>Ti, and ε<sup>64</sup>Ni spaces, two distinct mixing lines are resolved within both the NCC and CC reservoirs, between NCC and CC-type chondrules and CI-type matrix. Extending the NCC-CI chondrite correlation to primitive achondrites, main-group pallasites, and the mantles of Mars and Earth reveals that these silicate

<footnote n="1">¹ Université de Lorraine, CNRS, CRPG, F-54000, Nancy, France</footnote>

<footnote n="2">² Laboratoire Magmas et Volcans, Université Clermont Auvergne, CNRS, IRD, OPGC, F-63000, Clermont-Ferrand, France</footnote>
reservoirs plot away from the OC-Cl mixing lines, highlighting the possible existence of a neutron-poor
matrix component in the inner Solar System. Overall, the Ge isotopic systematics of the Solar System
suggest that chondrules and their matrices did not form exclusively in a single reservoir, but rather
formed throughout the inner and outer Solar System.

**Keywords:** Chondrites, Germanium isotopes, Nucleosynthetic anomalies, Solar System formation, Planets
# 1. Introduction

Knowledge of the processes that produced the primitive components of the Solar System is of great importance for identifying the materials from which planetary bodies formed. Among these primitive components, CI-type carbonaceous chondrites (CCs) are chemically the most primitive chondritic material; they contain most elements in relative abundances similar to those of the solar photosphere (Lodders et al., 2009). In contrast, the other CC groups (Braukmüller et al., 2018; Davis et al., 2006), ordinary chondrites (OCs) (Wasson and Chou, 1974), and the bulk silicate Earth (BSE; Fegley et al., 2020) exhibit a progressive depletion of volatile elements in the order CI >> CM > CO > CV-CR > BSE > OC.

The reason for the progressive depletion of volatile elements in chondrites is the subject of long-standing debate (e.g. Braukmüller et al., 2018; Davis et al., 2006; Palme et al., 1988; Wai and Wasson, 1977). In particular, depletions of moderately volatile elements (MVEs; $750 \text{ K} < T_{50\%} < 1250 \text{ K}$, where $T_{50\%}$ is the temperature at which 50% of an element is condensed from a gas of solar composition) differ from those of highly volatile elements (HVES; $T_{50\%} < 750 \text{ K}$; Wood et al., 2019) in that relative HVE depletions are unfractionated, like the relative abundances in CI chondrites (Palme et al., 1988). This difference presumably resulted from the addition of a CI-like component to nearly HVE-free material (Braukmüller et al., 2018). The distinct MVE and HVE depletions in chondrites have been attributed to (i) early volatile loss prior to condensation in the nebula (Wai and Wasson, 1977); (ii) incomplete condensation-evaporation (Palme et al., 1988); and (iii) matrix-chondrule mixing (Braukmüller et al., 2018; Hellmann et al., 2020).

Recently, a model involving incomplete condensation and/or matrix-chondrule mixing was proposed to explain the CC trends because matrix abundances in CCs correlate with MVE and HVE stable isotopic systems ($\delta^{66}\text{Zn}, \delta^{87}\text{Rb}, \delta^{128}\text{Te}$), as well as with oxygen ($\Delta^{17}\text{O}$) and nucleosynthetic anomalies ($\varepsilon^{50}\text{Ti}, \varepsilon^{50}\text{Ca}, \varepsilon^{54}\text{Cr}$) (Braukmüller et al., 2018; Hellmann et al., 2020; Nie et al., 2021). In essence, the model involves the mixing of a CI-type volatile-rich matrix with volatile-depleted “chondrule” components (Alexander 2019a, 2019b; Braukmüller et al., 2018; Palme et al., 1988). Indeed, heterogeneities among nucleosynthetic isotopic anomalies for several elements in chondrites have revealed a dichotomy between carbonaceous-type (CCs) and non-carbonaceous-type chondrites (NCCs) (Trinquier et al., 2007; Warren, 2011), representative of outer and inner Solar System reservoirs, respectively. This dichotomy has further fuelled debates over the natures of these anomalies and their carrier phases (Ek et al., 2019; Jansen et al., 2024; Kruijer et al., 2017; Lichtenberg et al., 2021; Torrano et al., 2024), the dynamics of the formation of these reservoirs (Jacquet et al., 2019), and the dynamics of mass transport between them. Coupling nucleosynthetic anomalies as tracers of protoplanetary disk material sources with stable isotopic systems constraining specific thermodynamic conditions in the inner and outer Solar System (Hellmann et al., 2020; Luck et al., 2005; Nie et al., 2023) is expected to provide strong constraints on the establishment and early evolution of the Solar System’s structure. However, such advances have been precluded by the lack of correlation between the mass-dependant isotopic systems studied so far and nucleosynthetic anomalies (Hu et al., 2023; Koefoed et al., 2023; Nie et al., 2023) from CCs to NCCs. Accordingly, the predominant physical/chemical processes occurring within source regions in the protoplanetary disk remain unconstrained.

Germanium is a moderately siderophile and volatile element ($T_{50\%} = 830 \text{ K}$; Wood et al., 2019), filling a gap in cosmochemical affinities between volatile lithophile elements ($T_{50\%}$ of K = 993 K > Rb = 752 K > Zn = 704 K) and volatile siderophile elements ($T_{50\%}$ of Te = 650 K). Here, we report data on
chondrites, achondrites, and known planetary reservoirs alongside data from OCs (Florin et al., 2020) and bencubbinite chondrites (CBs) (Florin et al., 2021) to elucidate the behaviour of Ge in primitive outer and inner Solar System materials. Based on our results, we constrain the causes of the correlations between nucleosynthetic anomalies and volatile element fractionations in chondrites (Trinquier et al., 2009), and, hence, the dynamics of interactions between the inner and outer Solar System.

## 2. Samples and analytical methods

We selected twenty-four chondrites (eleven carbonaceous chondrites of CO, CV, CM, C-Ung, Cl, and CB<sub>a-b</sub> types; thirteen ordinary chondrites, including six H, five L, and two LL types), as well as one main-group pallasite, one primitive achondrite (winonaite), one Martian meteorite, and two terrestrial rocks (Table S1). These samples were analysed in bulk at high-precision for their germanium contents and germanium stable isotopic compositions from the same powder or solution using the ThermoFischer ICP-MS X7 and the NeptunePlus HG-MC-ICP-MS at the CRPG (Nancy, France), following established chemical preparation and separation procedures and measurement techniques described by Luais (2007, 2012) (see Supplementary Information, Materials and Analytical Methods). Samples' germanium contents are reported in µg/g (±10%, 2SD) and their mass-dependent Ge isotopic compositions in delta notation relative to the NIST3120a standard (δ<sup>74/70</sup>Ge [%] = ((<sup>74</sup>Ge/<sup>70</sup>Ge)<sub>sample</sub>/(<sup>74</sup>Ge/<sup>70</sup>Ge)<sub>NIST3120a</sub> - 1) × 1000, ± 2σ SD).

## 3. Continuous germanium isotopic trend among chondrites

Analytical data are reported in Figure 1 and Table 1. Our main observation is that chondrites do not exhibit constant Ge isotopic compositions. Instead, compared to the restricted variations in OCs (-0.65‰ in H-type to -0.29‰ in LL-type chondrites), CCs exhibit a large range of δ<sup>74/70</sup>Ge values, from = -0.65‰ in HaH237 (CBb) to +0.55‰ in Ornans (CO), +0.90‰ in Orgueil (Cl), and +1.04‰ in Bencubbin (CBa). In the δ<sup>74/70</sup>Ge vs. Ge concentration plot (Fig. 2), OCs and CCs (respectively representative of inner and outer Solar System materials; Warren, 2011) together describe a continuous and well-constrained positive correlation. OCs exhibit a restricted range of Ge concentrations and isotopic compositions that lie on an extension of the CC trend, but towards lower Ge concentrations and isotopic compositions ([Ge] = 9–16 µg/g, δ<sup>74/70</sup>Ge = -0.33 ± 0.10‰ to -0.51 ± 0.06‰) (Florin et al., 2020). Amongst the CC groups, Ge concentrations and δ<sup>74/70</sup>Ge values are positively correlated from CB<sub>b</sub> samples to CVs ([Ge] = 16 µg/g, δ<sup>74/70</sup>Ge = -0.25 ± 0.05‰) and Cls ([Ge] = 32 µg/g; δ<sup>74/70</sup>Ge = +0.90 ± 0.06‰); OCs are consistent within uncertainties once the percentage of matrix is taken in account (as discussed Section 3.2, see Fig. 4a,b). OCs show small variations that can be associated with redox heterogeneity within the OC reservoirs (Florin et al., 2020), defining a trend orthogonal to that of the CC groups. However, the lack of any gap between the Ge concentrations and isotopic compositions of the two groups indicates that a single major process similarly affected both parts of the forming Solar System.
<table><caption>Table 1: Germanium elemental and isotopic compositions of chondrites, one winonaite, one main-group pallasite, one Martian meteorite and two Earth samples. Isotopic values are reported according to NIST3120a.</caption><thead><tr><th>Group</th><th>Meteorite</th><th>Petrographic Group</th><th>δ<sup>72/70</sup>Ge ‰</th><th>±2σ SD</th><th>δ<sup>73/70</sup>Ge ‰</th><th>±2s SD</th><th>δ<sup>74/70</sup>Ge ‰</th><th>±2s SD</th><th>n</th><th>References</th><th>Ge µg/g</th><th>±2σ</th><th>References</th></tr></thead><tbody><tr><td colspan="13"><strong>Carbonaceous chondrites</strong></td></tr><tr><td>CI</td><td>Orgueil</td><td>1</td><td>-0.46</td><td>0.05</td><td>-0.66</td><td>0.09</td><td>0.9</td><td>0.06</td><td>7</td><td></td><td>32.4</td><td>1.62</td><td>Fouché & Smales (1967); Kallemeyn & Wasson (1981)</td></tr><tr><td>C2-ung.</td><td>Tagish Lake</td><td>2</td><td>0.38</td><td>0.06</td><td>0.56</td><td>0.09</td><td>0.74</td><td>0.09</td><td>3</td><td></td><td>25</td><td>1.25</td><td></td></tr><tr><td>CV</td><td>Allende</td><td>3</td><td>0.07</td><td>0.11</td><td>0.09</td><td>0.07</td><td>0.1</td><td>0.12</td><td>10</td><td></td><td>16</td><td>0.8</td><td>Fouché & Smales (1967); Wasson & Kallemeyn (1988)</td></tr><tr><td></td><td>NWA 5943</td><td>3</td><td>0</td><td>0.04</td><td>-0.06</td><td>0.11</td><td>-0.04</td><td>0.04</td><td>3</td><td></td><td>16.8</td><td>0.84</td><td></td></tr><tr><td></td><td><u>Mean CV</u></td><td></td><td><u>0.03</u></td><td><u>0.07</u></td><td><u>0.01</u></td><td><u>0.15</u></td><td><u>0.03</u></td><td><u>0.14</u></td><td></td><td></td><td><u>16.4</u></td><td><u>1.16</u></td><td></td></tr><tr><td>CM</td><td>Murray</td><td>2</td><td>0.35</td><td>0.01</td><td>0.53</td><td>0.09</td><td>0.66</td><td>0.04</td><td>4</td><td></td><td>25.7</td><td>1.29</td><td>Fouché & Smales (1967)</td></tr><tr><td></td><td>Mukundpura</td><td>2</td><td>0.21</td><td>0.03</td><td>0.31</td><td>0.03</td><td>0.43</td><td>0.03</td><td>3</td><td></td><td>22.7</td><td>1.14</td><td></td></tr><tr><td></td><td>NWA 10126</td><td>2</td><td>0.26</td><td>0.08</td><td>0.37</td><td>0.09</td><td>0.5</td><td>0.11</td><td>3</td><td></td><td>22.3</td><td>1.12</td><td></td></tr><tr><td></td><td><u>Mean CM</u></td><td></td><td><u>0.27</u></td><td><u>0.08</u></td><td><u>0.4</u></td><td><u>0.13</u></td><td><u>0.53</u></td><td><u>0.14</u></td><td></td><td></td><td><u>23.6</u></td><td><u>2.04</u></td><td></td></tr><tr><td>CO</td><td>Ornans</td><td>3.4</td><td>-0.12</td><td>0.05</td><td>-0.2</td><td>0.07</td><td>-0.25</td><td>0.05</td><td>4</td><td></td><td>20.2</td><td>1.01</td><td>Fouché & Smales (1967); Kallemeyn et al. (1981)</td></tr><tr><td>CBa</td><td>Gjuba</td><td></td><td>0.53</td><td>0.12</td><td>0.76</td><td>0.32</td><td>0.97</td><td>0.32</td><td>8</td><td>Florin et al. (2021)</td><td>1.11</td><td>0.11</td><td>Florin et al. (2021)</td></tr><tr><td></td><td>Bencubbin</td><td></td><td>0.58</td><td>0.09</td><td>0.76</td><td>0.25</td><td>1.04</td><td>0.09</td><td>5</td><td>Florin et al. (2021)</td><td>0.91</td><td>0.18</td><td>Florin et al. (2021)</td></tr><tr><td></td><td><u>Mean CBa</u></td><td></td><td><u>0.56</u></td><td><u>0.05</u></td><td><u>0.76</u></td><td><u>0</u></td><td><u>1.01</u></td><td><u>0.07</u></td><td></td><td>Florin et al. (2021)</td><td><u>1.01</u></td><td><u>0.23</u></td><td>Florin et al. (2021)</td></tr><tr><td>CBb</td><td>HaH 237</td><td></td><td>-0.29</td><td>0.14</td><td>-0.59</td><td>0.39</td><td>-0.65</td><td>0.1</td><td>3</td><td>Florin et al. (2021)</td><td>1.34</td><td>0.13</td><td>Florin et al. (2021)</td></tr><tr><td colspan="13"><strong>Non-Carbonaceous chondrites</strong></td></tr><tr><td>H</td><td>Sharps</td><td>3.4</td><td>-0.29</td><td>0.06</td><td>-0.49</td><td>0.15</td><td>-0.59</td><td>0.04</td><td>3</td><td>Florin et al. (2020)</td><td>12.1</td><td>0.61</td><td>Florin et al. (2020)</td></tr><tr><td></td><td>Dhajala</td><td>3.8</td><td>-0.16</td><td>0.06</td><td>-0.25</td><td>0.12</td><td>-0.37</td><td>0.15</td><td>8</td><td>Florin et al. (2020)</td><td>15.2</td><td>0.76</td><td>Florin et al. (2020)</td></tr><tr><td></td><td>St Marguerite</td><td>4</td><td>-0.23</td><td>0.06</td><td>-0.37</td><td>0.11</td><td>-0.47</td><td>0.09</td><td>4</td><td>Florin et al. (2020)</td><td>10.3</td><td>0.52</td><td>Florin et al. (2020)</td></tr><tr><td></td><td>Allegan</td><td>5</td><td>-0.2</td><td>0.07</td><td>-0.33</td><td>0.1</td><td>-0.55</td><td>0.04</td><td>3</td><td>Florin et al. (2020)</td><td>22.2</td><td>1.11</td><td>Florin et al. (2020)</td></tr><tr><td></td><td>Guareña</td><td>6</td><td>-0.23</td><td>0.09</td><td>-0.38</td><td>0.13</td><td>-0.51</td><td>0.16</td><td>11</td><td>Florin et al. (2020)</td><td>21.4</td><td>1.07</td><td>Florin et al. (2020)</td></tr><tr><td></td><td>Kernouvé</td><td>6</td><td>-0.29</td><td>0.12</td><td>-0.45</td><td>0.17</td><td>-0.56</td><td>0.17</td><td>10</td><td>Florin et al. (2020)</td><td>13.6</td><td>0.68</td><td>Florin et al. (2020)</td></tr><tr><td></td><td><u>Mean H</u></td><td></td><td><u>-0.23</u></td><td><u>0.04</u></td><td><u>-0.38</u></td><td><u>0.07</u></td><td><u>-0.51</u></td><td><u>0.06</u></td><td></td><td></td><td><u>15.8</u></td><td><u>1.94</u></td><td></td></tr><tr><td>L</td><td>Julesburg</td><td>3.6</td><td>-0.15</td><td>0.05</td><td>-0.25</td><td>0.1</td><td>-0.3</td><td>0.12</td><td>6</td><td></td><td>8.7</td><td>0.87</td><td></td></tr><tr><td></td><td>Herdaz</td><td>3.7</td><td>-0.15</td><td>0.04</td><td>-0.27</td><td>0.05</td><td>-0.31</td><td>0.05</td><td>5</td><td></td><td>12.3</td><td>0.62</td><td></td></tr><tr><td></td><td>Bjurbole (metal)</td><td>4</td><td>-0.16</td><td>0.03</td><td>-0.24</td><td>0.04</td><td>-0.32</td><td>0.02</td><td>3</td><td>Florin et al. (2020)</td><td>10.2</td><td>0.51</td><td>Florin et al. (2020)</td></tr><tr><td></td><td>Vouillé</td><td>6</td><td>-0.13</td><td>0.02</td><td>-0.22</td><td>0.05</td><td>-0.26</td><td>0.05</td><td>3</td><td></td><td>10.9</td><td>0.55</td><td></td></tr><tr><td></td><td>Afianello</td><td>6</td><td>-0.13</td><td>0.07</td><td>-0.26</td><td>0.08</td><td>-0.28</td><td>0.14</td><td>4</td><td></td><td>8.33</td><td>0.83</td><td></td></tr></tbody></table>
<table><tbody><tr><td></td><td>Tourrines-la-Grosse</td><td>6</td><td>-0.16</td><td>0.07</td><td>-0.26</td><td>0.11</td><td>-0.27</td><td>0.12</td><td>4</td><td></td><td>n.a.</td><td>n.a.</td></tr><tr><td></td><td><u>Mean L</u></td><td></td><td><u>-0.15</u></td><td><u>0.01</u></td><td><u>-0.25</u></td><td><u>0.02</u></td><td><u>-0.29</u></td><td><u>0.02</u></td><td></td><td></td><td><u>10.09</u></td><td><u>1.67</u></td></tr><tr><td rowspan="3">LL</td><td>Semarkona</td><td>3</td><td>-0.19</td><td>0.03</td><td>-0.32</td><td>0.05</td><td>-0.38</td><td>0.09</td><td>3</td><td></td><td>7.15</td><td>0.72</td></tr><tr><td>Parnallee</td><td>3.6</td><td>-0.17</td><td>0.07</td><td>-0.29</td><td>0.18</td><td>-0.29</td><td>0.08</td><td>7</td><td>Florin et al. (2020)</td><td>5.98</td><td>0.6</td></tr><tr><td><u>Mean LL</u></td><td></td><td><u>-0.18</u></td><td><u>0.02</u></td><td><u>-0.3</u></td><td><u>0.03</u></td><td><u>-0.33</u></td><td><u>0.1</u></td><td></td><td></td><td><u>9</u></td><td><u>1.27</u></td></tr><tr><td colspan="12"><strong>Primitive achondrites</strong></td></tr><tr><td>Winonaite</td><td>Pontlyfni</td><td></td><td>0.42</td><td>0.06</td><td>0.59</td><td>0.05</td><td>0.79</td><td>0.08</td><td>5</td><td></td><td>28.3</td><td>1.41</td></tr><tr><td><strong>Main group pallasite</strong></td><td>Seymchan (olivine)</td><td></td><td>0.11</td><td>0.02</td><td>0.17</td><td>0.04</td><td>0.21</td><td>0.13</td><td>2</td><td></td><td>0.06</td><td>0.02</td></tr><tr><td><strong>Mars mantle</strong></td><td>Nakhla (cpx cumulate)</td><td></td><td>0.15</td><td>0.02</td><td>0.2</td><td>0.1</td><td>0.32</td><td>0.07</td><td>5</td><td></td><td>2.29</td><td>0.23</td></tr><tr><td colspan="12"><strong>Terrestrial geostandards</strong></td></tr><tr><td>Peridotite</td><td>San Carlos olivine</td><td></td><td>0.34</td><td>0.02</td><td>0.49</td><td>0.05</td><td>0.66</td><td>0.06</td><td>3</td><td>Florin et al. (2020), this study<sup>a</sup></td><td>0.89</td><td>0.18</td></tr><tr><td rowspan="3">Basaltic crust</td><td>BIR-1</td><td></td><td>0.33</td><td>0.07</td><td>0.43</td><td>0.13</td><td>0.61</td><td>0.09</td><td>23</td><td>Florin et al. (2020), Luais (2012)</td><td>1.52</td><td>0.15</td></tr><tr><td>BIR-1 bomb digestion 150°C</td><td></td><td>0.32</td><td>0.03</td><td>0.47</td><td>0.1</td><td>0.62</td><td>0.07</td><td>2</td><td>Florin et al. (2021), this study<sup>a</sup></td><td>1.5</td><td>0.15</td></tr><tr><td>BIR-1 ashing 500°C</td><td></td><td>0.36</td><td>0.01</td><td>0.55</td><td>0.11</td><td>0.69</td><td>0.05</td><td>2</td><td></td><td></td><td></td></tr></tbody></table>

<footnote><sup>a</sup> The long-term reproducibility on silicate geostandard BIR-1 is 0.09 ‰ (2σ SD) based on 24 measurements. This is similar to the long-term reproducibility of 0.1 ‰ observed for the synthetic Ge standart solution (JMC, Aldrich) based on 70 measurements.</footnote>
## 3.1. Germanium isotopic variations in chondrites compared to other mass-dependent isotopic systems

### 3.1.1 *The carbonaceous chondrites*

The Ge isotopic compositions of CCs are positively correlated ($R^2$ > 0.97) with the mass-dependant isotopic fractionations of other elements with similar or lower $T_{50\%}$, such as Te, Zn, and Rb, as well as V, which has a higher $T_{50\%}$ (Fig. 3). Correlations are less constrained ($R^2$ < 0.7) with other elements of higher $T_{50\%}$ that are siderophile (Ga), chalcophile (Cu), or lithophile (K, Si) (Fig. 3). CI-type chondrites consistently have heavier isotopic values (except Si) than other CCs containing lower proportions of matrix. Because Ge isotopes correlate with elements of distinct chemical behaviors, it is questionable whether these trends toward light isotopic compositions in mass-dependent isotopic systems, as seen in the chondrule-rich chondrites, could result from parent-body alteration processes such as aqueous alteration and/or thermal metamorphism (Rb, K) or sulfide destabilization (Te, Zn, Cu). The less constrained Ge-K correlation ($R^2$ = 0.11) compared to that of Ge-Rb ($R^2$ = 0.87) (Fig. 3) reveals the small range of K isotopic variations within the CC group, consistent with the scattered Rb-K isotopic correlations attributed to K mobility on their parent bodies (Nie et al., 2021, 2023; Hu et al., 2024). In detail, the Ge-K isotopic trend probably results from the fact that mean values were calculated for each sub-group to minimize K isotopic dispersion within some chondrite sub-groups, for example in COs and CVs (Nie et al., 2021) and Cls (Hu et al., 2024). Such intra-group variabilities could result from the redistribution of K during variable degrees of fluid-mediated alteration or thermal metamorphism on the parent body (Nie et al., 2021; Hu et al. 2024). In some cases, these intra-group variations vary according to the element and CC group (e.g., $\delta^{130}$Te by 1.8‰ only in CKs and $\delta^{66}$Zn by <0.2‰ in CVs, both due to thermal metamorphism) whereas the remaining isotopic variations are minor (<0.1‰ for Te and Zn in Cls, CMs, and COs) and therefore unlikely to result from secondary processes (Morton et al., 2024). Indeed, Pringle et al. (2017) dismissed aqueous alteration as the cause of Zn isotopic variations in CCs because this process should result in Zn losses in matrix-rich chondrites like Cls, whereas these chondrites are actually richer in Zn; this is also the case for Ge elemental and isotopic characteristics in Cls.

Instead, Pringle et al. (2017) argued that the removal of sulfides containing isotopically heavy Zn may account for the light Zn isotopic compositions of chondrules. Indeed, the amount of mildly chalcophile elements (Zn, Ge, Te) hosted in sulfide, silicate, and/or metal phases in chondrites strongly influences the effects of secondary processes on the larger isotopic budget. For example, Te is incorporated into sulfide and metal, but Zn is preferentially partitioned into metal and silicate compared to sulfide (Morton et al., 2024), leaving unconstrained the extent to which the fraction of sulfide removed can affect the isotopic composition of an entire chondrite (Morton et al., 2024). In chondrites, Ge is mainly hosted in metal, is depleted in sulfide by 3 and 4 orders of magnitude compared to silicate and metal, respectively, and sulfides have light Ge isotopic compositions (Florin et al., 2020, 2023). Therefore, although Ge isotopes are positively correlated with Zn and Te isotopes, it is improbable that the trend toward light Ge isotopic compositions from Cls to COs and CVs can result from the removal of isotopically light sulfides. The strong and statistically significant correlations between Ge isotopes (siderophile) and chalcophile (Te, Zn), moderately siderophile (Cu), and lithophile (Rb, V) isotopes, regardless of their chemical affinity and degree of volatility/refractoriness (Te < Zn < Rb < Cu << V) impose that the main cause of Ge isotopic fractionations in carbonaceous chondrites cannot be sensu lato parent-body alteration. Nonetheless, the uniform depletion of MVEs
in CCs (Braukmüller et al., 2025), regardless of their geochemical behaviors, precludes the idea that chondrules or their precursors lost different elements through distinct processes. Although we cannot exclude that alteration processes have affected some specific elemental and isotopic systems, the impact of such processes on the overall Ge isotopic variations in CCs was minor.

The lack of any significant effect of parent-body alteration on the observed $\delta^{74/70}$Ge values implies that the CC correlation is attributable to protoplanetary processes. When Ge mass fractions are reported against those of elements with various geochemical behaviors (Fig. S1), no trend can be identified with refractory lithophile elements (Mg/Si, V/Si, Alexander, 2019a, b), and all chondrites display sub-chondritic ratios. When compared to elements with transitional volatility, such as Fe, poor correlations are obtained. These correlations progressively improve when compared with non-siderophile volatile elements (Zn/Si, Te/Si), and all chondrites display super-chondritic ratios. This strongly supports that Ge isotopic variations are significantly controlled by volatility (Fig. S2) and we concur with most previous studies that these correlated isotopic variations primarily reflect mixtures between chondrite matrices and variable amounts of chondrule components (Nie et al., 2021; Hellmann et al., 2020; Pringle et al., 2017).

### 3.1.2 The non-carbonaceous chondrites

The correlation obtained for CCs in Ge vs. $\delta^{74/70}$Ge space can be extended to OC compositions, which show a restricted range of distinctively lower Ge isotopic compositions (Fig. 2). These small Ge and $\delta^{74/70}$Ge variations in OCs are thought to reflect constrained Ge fractionation during the accretion and evolution of the OC parent bodies. Whereas CI-CM-CO-CV chondrites are characteristically more oxidized and contain low amounts of metal (from <0.1 to 5 vol.%; Krot et al., 2014), OC parent bodies are more reduced and contain substantial amounts of FeNi metal (8.4, 4.1, and 2.1 vol.% from H to L and LL types; Krot et al., 2014). Because Ge is primarily contained in metal, it remains immobile both during metal-silicate redistribution via closed-system metamorphism and during shock events (Florin et al., 2020; Florin et al., 2023). Consequently, neither thermal metamorphism nor impacts on OC parent bodies in low-gravity environments can produce significant Ge isotopic fractionations (Florin et al., 2020). Conversely, the larger isotopic variations of low-$T_{50\%}$ elements (Te, Zn, Rb) among OCs, reflecting either isotopic redistribution during metamorphism or impact-related volatility (Hellmann et al., 2021; Nie et al., 2023), render any correlation with Ge isotopes poorly defined. Therefore, in contrast to other HVEs and MVEs, Ge tends to preserve the isotopic signature of pre-accretionary heating events inherited from nebular processes (Florin et al., 2020). Additionally, beyond these intra-group variations, offsets toward lower alkali (Rb, K) isotopic values and higher chalcophile (Te, Cu) isotopic values in OCs define a compositional gap with respect to the CC trend (Fig. 3). In contrast, Ge is the only element that defines a high precision continuous elemental and isotopic trend between OCs and CCs, although Ga and Si (higher $T_{50\%}$) also show these trends but at lower definition. These observations highlight the effect of isotopic perturbations on the OC parent bodies (Hellmann et al., 2021; Koefoed et al., 2023; Nie et al., 2023).

The important outcome of these results is that the $\delta^{74/70}$Ge vs. [Ge] trend likely reflects a large-scale process in the early Solar System, rather than the evolution of individual parent bodies (Florin et al., 2020). Therefore, Ge appears to be a key element for understanding the isotopic variations between chondrite groups. The distinct stable isotopic compositions of the inner and outer Solar
System, combined with the highly defined δ<sup>74/70</sup>Ge vs. [Ge] correlation, support that similar processes responsible for these isotopic variations could have occurred in both regions. Conversely, as these regions were characterized by distinct thermodynamic conditions (temperature, redox state, and volatile element contents) that would affect Ge isotopic fractionations, we suggest that the observed δ<sup>74/70</sup>Ge values were acquired before the formation of the distinct inner and outer reservoirs.

## 3.2. Explaining δ<sup>74/70</sup>Ge variations using chondrule-matrix mixing models

Unlike previously described mass-dependent isotopic variations of elements with distinct behaviors in CCs and/or NCCs (Hellmann et al., 2020, 2021; Koefoed et al., 2023; Nie et al., 2021), Ge is one of the few elements (alongside Si) that exhibits continuous trends with positive correlations (*R*² > 0.8) between concentrations, isotopic compositions, and matrix abundances in both the OC and CC groups (Fig. 4a,b). Among the OCs, Ge contents are more scattered than in CCs, with OCs defining an endmember composition close to that of chondrules (Fig. 4b). Because Ge is mainly hosted in the metal phase (Florin et al., 2020), we attribute this small scatter to the heterogeneous distribution of metal grains among OC groups. However, the similar highly siderophile element compositions of OC metal grains suggest a common homogeneous source, with the variable metal abundances among H, L, and LL groups arising from the redistribution of this initially homogeneous batch within the OC reservoir (Florin et al., 2023). The observed variations of Ge contents among OCs are therefore likely the results of a physical sorting process that is unlikely to have fractionated Ge isotopes (see Florin et al., 2020 for details). This interpretation is supported by (1) the fact that the average Ge content of OC samples plots on the regression line in Ge vs. matrix fraction space (Fig. 4a), (2) the excellent agreement between OC δ<sup>74/70</sup>Ge values and the CC trend (Fig. 4b), (3) and the consistency of the δ<sup>74/70</sup>Ge vs. Ge<sub>average</sub> data in OCs in the mixing model (Fig. 4c).

The composition of the matrix-poor (chondrule) component can be determined by extrapolating the linear regression to 0 wt.% matrix (Fig. 4; see Supplementary information, Linear regression and Mixing model), as done previously for Te (Hellmann et al., 2020). We estimate [Ge] = 10.74 ± 4.5 µg/g and δ<sup>74/70</sup>Ge = -0.49 ± 0.19‰ for the non-matrix component, consistent with the chondrule composition previously measured in OC chondrites ([Ge] = 11.95 ± 0.59 µg/g; δ<sup>74/70</sup>Ge = -0.31 ± 0.10‰; Florin et al., 2020). Taking the CI group as a proxy for the matrix component and using the newly calculated chondrule component, we calculate a mixing model reproducing the entire range of [Ge] and δ<sup>74/70</sup>Ge variations in chondrites (Fig. 4c; see Supplementary Information, Linear regression and Mixing model). This model indicates that the average bulk compositions of the studied chondrite groups arise from the binary mixing of a Ge-depleted, isotopically light chondrule component and a Ge-rich, isotopically heavy matrix-rich component. However, the low-temperature matrix is oxidized and volatile-rich, whereas the high-temperature chondrules are reduced and relatively volatile-depleted (Hezel et al., 2018). Accordingly, whether the matrix and chondrules are complementary or not (Hezel et al., 2018), their formation environments must have been spatiotemporally distinct, raising the question of where the components came from, how this mixing occurred, and how they acquired their distinct compositions.

The distinctive δ<sup>74/70</sup>Ge compositions of chondrite matrices and chondrules may help answer these questions because δ<sup>74/70</sup>Ge variations can be linked with the high temperatures and subsequent cooling rates typical of most thermally processed chondrules and their precursors (Jones et al., 2018).
Peak temperatures during chondrule formation or heating events range from 1200 to 2000 °C, sufficient to at least partially evaporate most MVEs. Moreover, petrographic evidence suggests that chondrule cooling rates could have reached 3000 °C/h, fast enough to trigger the kinetic recondensation of MVEs, theoretically favoring the condensation of light isotopes (Richter, 2004). This preferential recondensation of light isotopes following the chondrule forming event(s) is supported by the light δ²⁹Si compositions observed in Type I chondrules (Villeneuve et al., 2020).

The ability of δ⁷⁴/⁷⁰Ge to record this process has been further demonstrated using the CB_b chondrite groups, formed by kinetic condensation from a gas of Cl-like composition (Florin et al., 2021). When reported alongside with the full δ⁷⁴/⁷⁰Ge range of OCs and CCs, the δ⁷⁴/⁷⁰Ge compositions of CB_b groups compare very well with the non-matrix components (Fig. 4c). Therefore, as a first-order estimate, we suggest that the overall enrichment of light isotopes in chondrules was acquired through partial disequilibrium recondensation of a gas produced during the melting and partial evaporation of chondrules or their precursors having an initial Cl-like δ⁷⁴/⁷⁰Ge composition, as suggested by Nie et al. (2021) for Rb and K. To preserve this light signature, the gaseous residue of partial condensation must have been efficiently removed from the non-matrix reservoir. Conversely, the heavy δ⁷⁴/⁷⁰Ge signature of the matrix component might be considered as the starting composition. Accordingly, we attribute the evolution toward lighter δ⁷⁴/⁷⁰Ge values from Cls to OCs to increasing chondrule-to-matrix ratios during mixing and the thermal processing that these components experienced within the protoplanetary disk.

### 4. Correlations between δ⁷⁴/⁷⁰Ge variations and nucleosynthetic anomalies

A key point of our study is the continuum of δ⁷⁴/⁷⁰Ge values throughout the chondrite forming regions, despite the distinct δ⁷⁴/⁷⁰Ge values of the two main inner and outer Solar System reservoirs. The restricted range of δ⁷⁴/⁷⁰Ge values in the inner reservoir (Florin et al., 2020) can be expanded by considering new δ⁷⁴/⁷⁰Ge data from early differentiated and achondritic planetesimals, as well as planetary mantles (pallasites, winonaites, Mars, Earth; Fig. 1). Regardless of the element, coupling isotopic anomalies and mass-dependent δ⁷⁴/⁷⁰Ge values reveals that objects formed in the inner Solar System have light δ⁷⁴/⁷⁰Ge values, positive Δ¹⁷O values (Yurimoto et al., 2007), and neutron-poor nucleosynthetic anomalies (Trinquier et al., 2007) (Figs. 5, S3). Conversely, outer Solar System objects have heavy δ⁷⁴/⁷⁰Ge values, negative Δ¹⁷O values (Clayton and Mayeda, 1999), and neutron-rich nucleosynthetic anomalies (Trinquier et al., 2007) (Fig. 5). Unlike mixing within δ⁷⁴/⁷⁰Ge-[Ge]-matrix spaces, distinct ε⁴⁸Ca, ε⁵⁴Cr, ε⁵⁰Ti, ε⁶⁴Ni, ε⁹⁶Zr nucleosynthetic anomalies lead to distinct trends for CC and NCC groups in δ⁷⁴/⁷⁰Ge vs. isotopic anomaly diagrams (Fig. 5), whereas CCs and OCs define nearly continuous δ⁷⁴/⁷⁰Ge vs. ε⁴⁰K (Fig. S3) and µ³⁰Si trends (Fig. 5). We highlight that within the CC group, δ⁷⁴/⁷⁰Ge values are strongly correlated with oxygen isotopic anomalies (Fig. S3)—produced by isotope-selective photo-dissociation of CO in the solar nebula (Clayton, 2003 and reference therein) or the molecular cloud—and with nucleosynthetic anomalies of iron-group elements (ε⁴⁸Ca, ε⁵⁴Cr, ε⁵⁰Ti, ε⁶⁴Ni) (Schiller et al., 2015). In contrast, δ⁷⁴/⁷⁰Ge values are not well correlated with nucleosynthetic anomalies of major (µ⁵⁴Fe), volatile (µ⁶⁶Zn, ε⁴⁰K) or heavier elements (ε⁹²Mo, ε¹⁰⁰Ru) (Fig. S3).

The Ge isotopic compositions and Ti, Cr, Ni, and Ca nucleosynthetic anomalies of the inner Solar System reservoirs define a trend in which OCs have the lightest δ⁷⁴/⁷⁰Ge values and nucleosynthetic anomalies (ε⁵⁰Ti, ε⁵⁴Cr, ε⁶²Ni, ε⁴⁸Ca) and the heaviest Δ¹⁷O values. This trend progresses towards
main-group pallasites, to Martian nakhlites, and the Earth's mantle, then to primitive achondrites (winonaites), which have the heaviest $\delta^{74/70}$Ge values near those of CI-CM chondrites (Figs. 2 and 5). The higher condensation temperatures of Cr, Ti, Ni, and Ca ($T_{50\%} > 1350$ K) relative to Ge ($T_{50\%} = 830$ K) (Wood et al., 2019) likely imply that Ge was still in a gaseous state when the former elements had already condensed, implying that solids in the protoplanetary disk had acquired their Cr, Ti, Ni, and Ca isotopic compositions prior to their Ge isotopic compositions. Therefore, the mixing of chondrules and matrix highlighted in $\delta^{74/70}$Ge-[Ge] space (Fig. 4c) must have occurred after Ge, Cr, Ti, Ni, and Ca condensation. As such, if the $\delta^{74/70}$Ge-[Ge] mixing trend resulted from intensive exchanges between the inner and outer Solar System, nucleosynthetic anomalies should describe a single trend with $\delta^{74/70}$Ge variations from NCC to CC groups. The significant gap between the $^{50}$Ti, $^{54}$Cr, $^{62}$Ni and $^{48}$Ca values of the highest NCC composition and CI chondrites precludes intense mixing between NCC and CC reservoirs, as supported by recent findings (Palme and Mezger, 2024).

Dynamic exchanges between the inner and outer Solar System reservoirs have been recently investigated using Fe nucleosynthetic anomalies. Schiller et al. (2020) and Hopp et al. (2022) demonstrated that similar $\mu^{54}$Fe values between CI-type chondrites from the outer reservoirs and OCs and the mantles of Earth and Mars from NC reservoirs would be indicative of the accretion of CI-like material in the inner disk, even identifying a CI-type carbonaceous chondritic reservoir in the outermost Solar System (Hopp et al., 2022).

Additional constraints on interactions between the inner and outer Solar System arise from Si nucleosynthetic anomalies, $\mu^{30}$Si, in chondrites and planetary mantles (Onyett et al., 2023). The heterogeneous $\mu^{30}$Si values of porphyritic chondrules from the CV group, which contain preserved $\mu^{30}$Si-depleted cores surrounded by $\mu^{30}$Si-positive rims, could provide evidence for chondrule migration from the inner to the outer Solar System, followed by the accretion of CI-like dust and subsequent reheating (i.e. recycling) (Onyett et al., 2024; Van Kooten et al., 2021). We highlight a continuum $\mu^{30}$Si-$\delta^{74/70}$Ge trend between NC and CC chondrites that is subparallel to that between achondrites and planets (Fig. 5), suggesting that exchanges between NC and CC reservoirs were possible. Because Ge and Si have similar chemical behaviors in mineral lattices, the gradient in $\mu^{30}$Si-$\delta^{74/70}$Ge space from CCs to OCs, opposed to the discontinuity in the $\varepsilon^{50}$Ti, $\varepsilon^{54}$Cr, $\varepsilon^{62}$Ni, and $\varepsilon^{48}$Ca vs. $\delta^{74/70}$Ge trends, could reflect that Si nucleosynthetic anomalies and Ge are hosted by the same specific carrier phases, or phases that experienced similar migration events, that are distinct from those that host Ti, Cr, Ni, and Ca anomalies. This would also indicate that Ge isotopic composition and Si isotopic anomalies can be retained after post-accretion and magmatic evolution. The timing of exchanges between the inner and outer Solar System remains difficult to constrain. Correlations of both $\mu^{30}$Si and $\delta^{74/70}$Ge with the accretion ages of the respective chondrites (Fig. 5e; Onyett et al., 2023) would favor the progressive modification of the composition of infalls over time in the disk (Bizzarro et al., 2025). However, it remains unclear if this process affected the NC groups, particularly as they accreted earlier than the CC groups (Sugiura and Fujiya, 2014).

Based on these arguments, we model the $\varepsilon^{54}$Cr and $\varepsilon^{60}$Ni vs. $\delta^{74/70}$Ge trends in CCs as the mixing of neutron-rich, heavy-$\delta^{74/70}$Ge matrix with chondrules that migrated from the inner to the outer Solar System but mostly record a neutron-rich composition (compared to OCs) and light $\delta^{74/70}$Ge values (Fig. 5, Table S4). For $\varepsilon^{50}$Ti and $\varepsilon^{48}$Ca, refractory inclusions must be added to the chondrule-matrix assemblage to explain the negative correlation observed in CCs (Hellmann et al., 2023), although this does not seem to influence $\delta^{74/70}$Ge values. For the NCC reservoir, a neutron-poor chondrule pole with light $\delta^{74/70}$Ge values similar to those of OCs is directly constrained by the isotopic composition of OC
chondrules (Florin et al., 2020) (Figs. 4, 5). For Ti and Ca, the lack of any significant amounts of refractory inclusions in OCs explains the reverse mixing trend compared to CCs. The heavy $\delta^{74/70}\text{Ge}$ pole of the inner Solar System remains to be identified.

**5. Causes of $\delta^{74/70}\text{Ge}$ variations in the inner Solar System**

In this section, we investigate whether the origin of the high-$\delta^{74/70}\text{Ge}$ matrix pole of the NCC reservoir originated from the inner or outer Solar System by focusing on planetary mantles and primitive achondrites. It has been suggested that the Earth accreted from 5% to >25% CC material (Steller et al., 2022; Bizzarro et al., 2025), such that inner Solar System objects could reflect a mixing of neutron-poor (i.e. enstatite-like chondrites) and neutron-rich components (i.e. CI-like matrix). In that case, the heavier $\delta^{74/70}\text{Ge}$ values of the mantles of Earth, Mars, and the pallasite parent bodies than predicted by the OC-CI mixing line (Fig. 5) could reflect isotopic fractionation during metal-silicate differentiation or early devolatilization during accretion, while maintaining constant Cr and Ti anomalies; that is, any Ge isotopic fractionation results in a purely horizontal shift in isotope anomaly diagrams. Based on the OC-CI mixing line, we can therefore delimit a range of hypothetical initial bulk Earth $\delta^{74/70}\text{Ge}$ values from of +0.28‰ (based on the $\epsilon^{54}\text{Cr}$ and $\epsilon^{50}\text{Ti}$ diagrams) to -0.06‰ (based on the $\epsilon^{64}\text{Ni}$ diagram) (Fig. 5). To assess the viability of this assumption, we performed mass balance calculations to quantify the $\delta^{74/70}\text{Ge}$ values of the bulk Earth, taking into account: (1) the Earth's core-to-mantle mass fraction; (2) measured Ge isotopic values of the silicate Earth ($\delta^{74/70}\text{Ge}$ = +0.53 to +0.59 ± 0.16‰; Luais, 2012), with those of Earth's core taken as those of magmatic iron meteorites as proxies for planetary cores ($\delta^{74/70}\text{Ge}$= +1.41 ± 0.22‰; Luais, 2007, 2012); and (3) calculated Ge concentrations of the bulk Earth ($[\text{Ge}]_{\text{bulk-Earth}}$ = 7–15 ppm), bulk silicate Earth ($[\text{Ge}]_{\text{BSE}}$ = 1–1.5 ppm), and Earth's core ($[\text{Ge}]_{\text{core}}$ = 20–45ppm) (Fischer and McDonough, 2025; Kargel and Lewis, 1993; Righter et al. 2011). Despite the highly variable Ge contents of these reservoirs, we calculate a heavy $\delta^{74/70}\text{Ge}$ range for the bulk Earth of +1.27 to +1.40‰, which is notably heavier than the BSE and plots far away from the OC-CI mixing line and the hypothetical $\delta^{74/70}\text{Ge}$ range from +0.28‰ to -0.06‰ (Fig. 5).

It is important to note that the selected ranges of $[\text{Ge}]_{\text{bulk-Earth}}$ and $[\text{Ge}]_{\text{core}}$ are not the key parameters for deriving the Ge isotopic composition of the bulk Earth, which was dominantly controlled by the isotopic compositions of iron meteorites, the main host of Ge. In addition, during magma ocean stages, evaporation processes driven by the surface gravity of planets could have further fractionated the residual mantle toward heavier values. Indeed, the extent of K isotopic fractionation on the Earth (large planetary size, high surface gravity) is smaller than that on Mars, the Moon, or Vesta (Tian et al., 2020). However, the heavier $\delta^{74/70}\text{Ge}_{\text{Earth}}$ values compared to $\delta^{74/70}\text{Ge}_{\text{Mars}}$ reported here is inconsistent with this interpretation. Therefore, core formation or large-scale evaporation processes do not satisfactorily explain the $\delta^{74/70}\text{Ge}$ composition of the mantles of Earth and Mars. Instead, the heavier $\delta^{74/70}\text{Ge}$ values of the Earth may reflect the direct contribution of a CI-like matrix component with a nucleosynthetic composition distinct from that of the CCs.

In comparison to planetary mantles, winonaites are primitive achondrites that underwent limited differentiation processes and exhibit higher $\delta^{74/70}\text{Ge}$ values farthest from the OC-CI mixing lines. They are weakly shocked and contain chondrule relics and 10–30 wt.% metal (Benedix et al., 1998). The texture of the metal in winonaites indicates melting at the Fe and Ni–FeS cotectic (Kullerud, 1963), which is too cool for extensive silicate melting, suggesting that the winonaite parent body experienced limited partial melting and no melt migration (Benedix et al., 1998). The complex
characteristics of winonaites result from their level of MVE depletion, which is intermediate between
CMs and Cls (Collinet and Grove, 2020), even though their major element compositions are closer to
OCs and ECs (e.g. Hunt et al., 2017). The pristine nature of winonaites is supported by their CM- and
Tagish Lake-normalized Ge contents of around 1 (Ge<sub>win</sub>/Ge<sub>CM</sub>/Mg = 1.04; Ge<sub>win</sub>/Ge<sub>TL</sub>/Mg = 0.90),
indicating that neither thermal metamorphism nor evaporation significantly modified their bulk
compositions. Furthermore, winonaite Ge systematics plot precisely on the chondrule-matrix mixing
line, in between Cls, CM and Tagish Lake (Fig. 4c, Table 1). Therefore, their parent body precursor was
rich in MVEs, with CI-like matrix material (>70 wt.% matrix). However, two major points contradict
this CI-TL inheritance: (1) ε<sup>54</sup>Cr, ε<sup>50</sup>Ti, and ε<sup>48</sup>Ca nucleosynthetic anomalies indicate that winonaites
have compositions characteristic of the NCC group (Fig. 5); and (2) as for oxygen isotopes (Clayton and
Mayeda, 1996), winonaite δ<sup>74/70</sup>Ge values of 0.79‰ (Table 1) indicate a genetic link with IAB non-
magmatic Fe-meteorites (Luais 2007, 2012) of the NCC group (Kruijer et al., 2017). Accordingly, three
possibilities remain: (1) the NCC reservoir contained some CC components (and vice versa), and
winonaites are direct evidence that CCs contaminated the inner Solar System; (2) winonaites' heavy
δ<sup>74/70</sup>Ge values result from the partial loss of their volatiles; or (3) a neutron-poor CI-like matrix
material was present in the inner Solar System at the time of winonaite accretion, implying that the
inner Solar System contained more volatiles than is commonly assumed. If the winonaite parent
body's enrichment in volatile elements resulted from contamination by CI material originating from
the outer Solar System—either by the inward-drifting of outer Solar System materials (Schiller et al.,
2020) or the outward migration of inner Solar System materials—the nucleosynthetic anomalies in
winonaites should be significantly higher than observed, as for CV chondrules (Onyett et al., 2024; Van
Kooten et al., 2021). However, their ε<sup>54</sup>Cr and ε<sup>48</sup>Ca nucleosynthetic anomalies are lower than the OC
chondrule pole (Fig. 5a, d), as for ε<sup>50</sup>Ti in main-group pallasites (Fig. 5c) or ε<sup>48</sup>Ca in Mars and Earth (Fig.
5d), and therefore cannot be explained by the accretion of neutron-rich CI material. Therefore, we
propose that resolving these inconsistencies necessitates the existence of a neutron-poor CI-like
matrix component.

A unique matrix component with CI-like nucleosynthetic anomalies cannot reproduce all inner
Solar System isotopic characteristics and the dichotomy within δ<sup>74/70</sup>Ge vs ε<sup>50</sup>Ti, ε<sup>54</sup>Cr, ε<sup>62</sup>Ni, and ε<sup>66</sup>Ca
spaces (Fig. 5) while maintaining the δ<sup>74/70</sup>Ge-[Ge]-matrix correlation (Fig. 4c) and the CI to OC
continuum in δ<sup>74/70</sup>Ge vs. µ<sup>30</sup>Si space (Fig. 5). Thus, we propose that the matrix component that
contributed to the isotopic signatures of inner Solar System planetary mantles and achondrites had a
CI-like Ge isotopic composition, but varied neutron-poor nucleosynthetic anomalies compared to the
outer Solar System, whether or not the inner and outer Solar System were separated by a barrier. In
our model, the nucleosynthetic signature of the inner Solar System matrix should record the evolution
of the disk composition at its time of formation. Using the ε<sup>54</sup>Cr-δ<sup>74/70</sup>Ge diagram as an example (Fig.
5a), the NC mixing trend can be reproduced by considering a matrix-rich component characterized by
a ε<sup>54</sup>Cr anomaly lower than that of the CC matrix and intermediate between CC matrix-free silicates
and OC chondrules (Fig. 5); i.e., ε<sup>54</sup>Cr<sub>CI</sub> > ε<sup>54</sup>Cr<sub>CC-chondrules</sub> > ε<sup>54</sup>Cr<sub>NC-matrix</sub> > ε<sup>54</sup>Cr<sub>OC-chondrules</sub>.

A CI-type component with lower ε<sup>54</sup>Cr and μ<sup>30</sup>Si nucleosynthetic anomalies than the CI-type
matrix has been identified in the matrices of dark clasts in CR-type carbonaceous chondrites (Van
Kooten et al., 2024). These Outer Disk dark (ODD) clasts are characterized by μ<sup>30</sup>Si = 4.7 and ε<sup>54</sup>Cr =
1.25 ± 0.09, lower than the values for Cls (Fig. 5a, e) and approaching the ε<sup>54</sup>Cr value of CB<sub>a</sub>-type metal-
rich carbonaceous chondrites (1.09). This low-ε<sup>54</sup>Cr and low-μ<sup>30</sup>Si component has been interpreted as
the late infall of material from the outermost Solar System, and such inward drifting would have
established the variability of the CC trend of the outer Solar System (Van Kooten et al., 2024); i.e., the late infalling material would have accreted later. The correlation between $\delta^{74/70}\text{Ge}$ and the age of parent body accretion suggests that the $\delta^{74/70}\text{Ge}$ values of late infalling material also plots along this trend, toward the high $\delta^{74/70}\text{Ge}$ values of the chondrite trend (Fig. 5f). In the $\varepsilon^{54}\text{Cr}-\delta^{74/70}\text{Ge}$ plot, this component does not align with the low $\varepsilon^{54}\text{Cr}$ pole of the CC trend and therefore cannot explain our $\varepsilon^{54}\text{Cr}-\delta^{74/70}\text{Ge}$ trend (Fig. 5a). These observations are inconsistent with the idea that CI-type bodies were contaminated with ODD material (Bizzarro et al., 2025).

Nonetheless, the $\delta^{74/70}\text{Ge}-\mu^{30}\text{Si}$ continuum from Cls to OCs (Fig. 5e) suggests that some exchanges occurred between the reservoirs. This implies that the mixing of matrix and non-matrix components was progressive, being a function of time and spatial location. This seems consistent with the view that a multi-component mixing model can explain the entirety of variations among chondrites and planetary mantles (Bizzarro et al., 2025, and reference therein). Regardless of the carrier phases of nucleosynthetic anomalies, the discontinuities within $\delta^{74/70}\text{Ge}$ vs. $\varepsilon^{50}\text{Ti}$, $\varepsilon^{54}\text{Cr}$, $\varepsilon^{62}\text{Ni}$, and $\varepsilon^{66}\text{Ca}$ spaces along with the $\delta^{74/70}\text{Ge}-[\text{Ge}]$-matrix correlation remains puzzling, because an isotopic continuum similar to that in $\mu^{30}\text{Si}-\delta^{74/70}\text{Ge}$ space should exist for these other nucleosynthetic tracers. We propose that at the time of accretion of achondrites, protoplanetary bodies, and the OC parent bodies, the inner Solar System was mostly free of any neutron-rich CI-matrix component, instead hosting an intermediate “neutron-poor” CI-like matrix component.

# 6. Summary and Conclusions

We reported new mass-dependent Ge isotopic compositions for bulk carbonaceous and ordinary chondrites, pallasite olivines, primitive achondrites, and Martian meteorites. Unlike earlier mass-dependent isotopic studies, we highlighted a continuum from CCs to OCs in $\delta^{74/70}\text{Ge}-[\text{Ge}]$-matrix % space, suggesting a mixing between a light-$\delta^{74/70}\text{Ge}$ chondrule component and a heavy-$\delta^{74/70}\text{Ge}$ matrix component. We proposed that these chondrule $\delta^{74/70}\text{Ge}$ values were inherited from similar processes occurring in both the inner and outer solar system, specifically disequilibrium condensation after partial evaporation of the MVE host in chondrule precursors that might have had CI-like compositions.

The mixing of chondrules and matrix components while preserving the NCC-CC nucleosynthetic dichotomy within $\delta^{74/70}\text{Ge}$ vs. $\varepsilon^{50}\text{Ti}$, $\varepsilon^{54}\text{Cr}$, $\varepsilon^{62}\text{Ni}$, and $\varepsilon^{66}\text{Ca}$ spaces requires minimal mixing between the outer and inner Solar System reservoirs. Yet, the $\delta^{74/70}\text{Ge}-\mu^{30}\text{Si}$ continuum in chondrites suggest that some such exchanges must have occurred. Therefore, to resolve these inconsistencies, we suggested that a neutron-poor matrix component existed in the inner Solar System. Accordingly, regions of the inner Solar System must have been thermodynamically favorable for the preservation of volatile-rich matrix components; otherwise OCs and CCs would not define a single correlation between $\delta^{74/70}\text{Ge}$, $[\text{Ge}]$ and matrix %. This conclusion suggests that some of Earth's volatiles may have originated from the inner Solar System.

# Data and materials availability

Samples were obtained from museums and private collections. Sample reference numbers are listed in Table S1. All data shown in figures or used for modelling are listed in Tables 1 and S3-S4, and are available on request.
**CRediT authorship contribution statement**

**Béatrice Luais:** Writing – review & editing, Writing – original draft, Validation, Resources, Project administration, Methodology, Investigation, Funding acquisition, Formal analysis, Data curation, Conceptualization.
**Guillaume Florin:** Writing – review & editing, Writing – original draft, Validation, Resources, Methodology, Investigation, Formal analysis, Data curation, Conceptualization.

**Declaration of Competing interests**

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

**Acknowledgments**

We gratefully thank M. Gounelle and the Comité de Gestion at the Muséum National d'Histoire Naturelle (Paris), T. McCoy and J. Hoskin at the Smithsonian National Museum of Natural History (Washington, D.C.), A. Nieto Codina at the Museo Nacional de Ciencias Naturales (Madrid), L. Vacher and J. Karl for providing meteorite samples. Damien Cividini is warmly thanked for his valuable assistance on the NeptunePlus MC-ICP-MS at CRPG, and Robert Dennen for careful editing of the manuscript. We also thank D.C. Hezel for giving us access to the ChondruleDB. B.L. was supported by the ANR – FRANCE (French National Research Agency) for its financial support of the PlanetGEM project (Grant # ANR-21-CE49-0011), and G.F. for a Post-doctorate funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) – Project-ID 263649064 – TRR 170. This is CRPG communication n° 2877.

**References**

Alexander, C. M. O. D., 2019a. Quantitative models for the elemental and isotopic fractionations in chondrites: The carbonaceous chondrites. *Geochim. Cosmochim. Acta* 254, 277-309

Alexander, C. M. O. D., 2019b. Quantitative models for the elemental and isotopic fractionations in the chondrites: The non-carbonaceous chondrites. *Geochim. Cosmochim. Acta* 254, 246-276

Benedix, G. K., McCoy, T. J., Keil, K., Bogard, D. D., Garrison, D. H., 1998. A petrologic and isotopic study of winonaites: evidence for early partial melting, brecciation, and metamorphism. *Geochim. Cosmochim. Acta* 62, 2535-2553.

Bizzarro, M., Johansen, A., & Dorn, C. 2025. The cosmochemistry of planetary systems. *Nature Reviews Chemistry*, 1-19.

Braukmüller, N., Wombacher, F., Hezel, D. C., Escoube, R., Münker, C., 2018. The chemical composition of carbonaceous chondrites: Implications for volatile element depletion, complementarity and alteration. *Geochim. Cosmochim. Acta* 239, 17-48.

Braukmüller, N., Funk, C., Abouchami, W., Pickard, H., Rehkämper, M., Bragagni, A., ... & Wombacher, F. (2025). Moderately volatile elements in chondrites record chondrule formation, two-component mixing and redistribution on parent bodies. *Geochimica et Cosmochimica Acta*, 393, 43-62.

Clayton, R. N., 2003. Oxygen isotopes in meteorites. In: Treatise on Geochemistry v eds. H.D. Holland & K.K. Turekian (Elsevier), 1, 129, 711.
Clayton, R. N., Mayeda, T. K., 1996. Oxygen isotope studies of achondrites. Geochim. Cosmochim. Acta 60, 1999-2017.

Clayton, R. N., Mayeda, T. K., 1999. Oxygen isotope studies of carbonaceous chondrites. Geochim. Cosmochim. Acta 63, 2089-2104

Collinet, M., Grove, T. L., 2020. Formation of primitive achondrites by partial melting of alkali-undepleted planetesimals in the inner solar system. Geochim. Cosmochim. Acta 277, 358-376.

Davis, A. M., Binzel, R. P., Walker, R. M., Cameron, A. G. W., 2006. Volatile evolution and loss" in Meteorites and the Early Solar System II, D. S. Lauretta, H. Y. McSween, Eds. (University of Arizona Press), 295-308.

Ek, M., Hunt, A. C., Lugaro, M., Schönbächler, M., 2019. The origin of s-process isotope heterogeneity in the solar protoplanetary disk. Nat. Astro. 4, 273-281.

El Korh, A., Luais, B., Boiron, M.-C., Deloule, E., Cividini, D., 2017. Investigation of Ge and Ga exchange behaviour and Ge isotopic fractionation during subduction zone metamorphism. Chem. Geol. 449, 165-181

Escoube, R., Rouxel, O.J., Luais, B., Ponzevera, E., Donard, O.F.X., 2012. Intercomparison study of germanium isotope composition of geological and reference materials. Geostand. Geoanal. Res. 36, 149-159.

Fegley, B., Lodders, K., Jacobson, N. S., 2020. Volatile element chemistry during accretion of the Earth. Geochemistry 80, 125594.

Fischer, R. A., McDonough, W. F., 2025. Earth's core composition and core formation" in Treatise on Geochemistry (Third edition), A. Anbar, D. Weis, Eds. (Elsevier, Oxford, 2025), pp. 17-71.

Florin, G., Luais, B., Alard, O., Rushmer, T., 2021. Condensation and evaporation processes during CB chondrite formation: Insights from Ge isotopes and highly siderophile element abundances. Meteorit. Planet. Sci. 56, 1191-1211.

Florin, G., Luais, B., Rushmer, T., Alard, O., 2020. Influence of redox processes on the germanium isotopic composition of ordinary chondrites. Geochim. Cosmochim. Acta 269, 270-291.

Florin G., Alard O., Luais B., Rushmer T., 2023. Abundances of siderophile elements in H-chondrite metal grains: Implications for the origin of metal in unequilibrated ordinary chondrites. Geochim. Cosmochim. Acta 341, 1-15.

Fouché, K. F., Smales, A. A., 1967. The distribution of trace elements in chondritic meteorites. 1. Gallium, germanium and indium. Chem. Geol. 2, 5-33.

Hellmann, J. L., Hopp, T., Burkhardt, C., Becker, H., Fischer-Gödde, M., Kleine, T., 2021. Tellurium isotope cosmochemistry: Implications for volatile fractionation in chondrite parent bodies and origin of the late veneer. Geochim. Cosmochim. Acta 309, 313-328.

Hellmann, J. L., Hopp, T., Burkhardt, C., Kleine, T., 2020. Origin of volatile element depletion among carbonaceous chondrites. Earth Planet. Sci. Lett. 549, 116508

Hellmann, J. L., Schneider, J. M., Wölfer, E., Drążkowska, J., Jansen, C. A., Hopp, T., ... Kleine, T., 2023. Origin of isotopic diversity among carbonaceous chondrites. The Astrophys. Journ. Lett. 946(2), L34.

Hezel, D. C., Harak, M., Libourel, G., 2018. Composition of chondrules and matrix and their complementary relationship in chondrites" in Chondrules 4, 91-121.

Hopp, T., Dauphas, N., Abe, Y., Aléon, J., O'D. Alexander, C. M., Amari, S., ... & Yurimoto, H. (2022). Ryugu's nucleosynthetic heritage from the outskirts of the Solar System. Science Advances, 8(46), eadd8141.
Hu, Y., Moynier, F., Yang, X., 2023. Volatile-depletion processing of the building blocks of Earth and Mars as recorded by potassium isotopes. Earth Planet. Sci. Lett. 620, 118319.

Hu, Y., Moynier, F., Dai, W., Paquet, M., Yokoyama, T., Abe, Y., ... & Yurimoto, H., 2024. Pervasive aqueous alteration in the early Solar System revealed by potassium isotopic variations in Ryugu samples and carbonaceous chondrites. *Icarus*, *409*, 115884

Hunt, A. C., Benedix, G. K., Hammond, S. J., Bland, P. A., Rehkämper, M., Kreissig, K., Strekopytov, S., 2017. A geochemical study of the winonaites: Evidence for limited partial melting and constraints on the precursor composition. *Geochim. Cosmochim. Acta* 199, 13-30.

Jacquet, E., Pignatale, F. C., Chaussidon, M., Charnoz, S., 2019. Fingerprints of the protosolar cloud collapse in the solar system. *Ii. Nucleosynthetic anomalies in meteorites. The Astrophys. Journ. Lett.* 884, 32-43.

Jansen, C. A., Burkhardt, C., Marrocchi, Y., Schneider, J. M., Wölfer, E., Kleine, T., 2024. Condensate evolution in the solar nebula inferred from combined Cr, Ti, and O isotope analyses of amoeboid olivine aggregates. *Earth Planet. Sci. Lett.* 627.

Jones, R. H., Villeneuve, J., Libourel, G., 2018. "Thermal histories of chondrules" in Chondrules, Eds S. S. Russell, H. C. Connolly, Jr., & A.N. Krot (Cambridge University Press, UK) 3, 57-90,

Kargel, J. S., Lewis, J. S., 1993. The Composition and Early Evolution of Earth. *Icarus* 105, 1-25.

Kalllemeyn, G. W., Wasson, J. T., 1981. The compositional classification of chondrites—I. The carbonaceous chondrite groups. *Geochim. Cosmochim. Acta* 45, 1217-1230.

Koefoed, P., Barrat, J.-A., Pravdivtseva, O., Alexander, C. M. O. D., Lodders, K., Ogliore, R., Wang, K., 2023. The potassium isotopic composition of CI chondrites and the origin of isotopic variations among primitive planetary bodies. *Geochim. Cosmochim. Acta* 358, 49-60.

Krot, A. N., Keil, K., Scott, E. R. D., Goodrich, C. A., Weisberg, M. K., 2014. Classification of meteorites and their genetic relationships. *Meteorites and Cosmochemical Processes, Volume 1, Treatise on Geochemistry (2nd Edition)*. Elsevier, Edited by Andrew M. Davis, p.1-63.

Kruijer, T. S., Burkhardt, C., Budde, G., Kleine, T., 2017. Age of Jupiter inferred from the distinct genetics and formation times of meteorites. *Proc. Natl. Acad. Sci.* 114, 6712-6716.

Kullerud, G., 1963. The Fe-Ni-S system, in: *Annual Reviews of the Geophysical Laboratory (The Carnegie Institution of Washington, Washington)*, 175-189.

Lichtenberg, T., Dra Zkowska, J., Schonbachler, M., Golabek, G. J., Hands, T. O., 2021. Bifurcation of planetary building blocks during Solar System formation. *Science* 371, 365-370

Lodders, K., Palme, H., Gail, H. P., 2009. Abundances of the elements in the Solar System" in Solar System, J. E. Trümper, Ed. (Springer-Verlag Berlin Heidelberg, 2009), vol. 4B, (34), pp. 712-770.

Luais, B., 2007. Isotopic fractionation of germanium in iron meteorites: Significance for nebular condensation, core formation and impact processes. *Earth Planet. Sci. Lett.* 262, 21-36.

Luais, B., 2012. Germanium chemistry and MC-ICPMS isotopic measurements of Fe–Ni, Zn alloys and silicate matrices: Insights into deep Earth processes. *Chem. Geol.* 334, 295-311.

Luck, J.-M., Othman, D. B., Albarède, F., 2005. Zn and Cu isotopic variations in chondrites and iron meteorites: Early solar nebula reservoirs and parent-body processes. *Geochim. Cosmochim. Acta* 69, 5351-5363.

Mahan, B., Moynier, F., Beck, P., Pringle, E. A., & Siebert, J. (2018). A history of violence: Insights into post-accretionary heating in carbonaceous chondrites from volatile element abundances, Zn isotopes and water contents. *Geochim. Cosmochim. Acta* 220, 19-35
Morton, E. M., Pickard, H., Wombacher, F., Huang, Y., Palk, E., Martins, R., ... & Rehkämper, M. (2024). Volatile Element Depletion of Carbonaceous Chondrites—Insights from Mass-dependent Zinc, Cadmium, and Tellurium Isotope Variations. Astrophys. Journ. 977(1), 53.

Nie, N. X., Chen, X. Y., Hopp, T., Hu, J. Y., Zhang, Z. J., Teng, F. Z., ... Dauphas, N., 2021. Imprint of chondrule formation on the K and Rb isotopic compositions of carbonaceous meteorites. Science. Adv. 7, eabl3929

Nie, N. X., Chen, X. Y., Zhang, Z. J., Hu, J. Y., Liu, W., Tissot, F. L., ... Dauphas, N., 2023. Rubidium and potassium isotopic variations in chondrites and Mars: Accretion signatures and planetary overprints. Geochim. Cosmochim. Acta 344, 207-229

Onyett, I. J., Schiller, M., Makhatadze, G. V., Deng, Z., Johansen, A., & Bizzarro, M., 2023. Silicon isotope constraints on terrestrial planet accretion. Nature, 619(7970), 539-544.

Onyett, I. J., Schiller, M., Stokholm, M., Bollard, J., & Bizzarro, M. (2024). Silicon isotope compositions of chondritic components: Insights into early disk processes. Earth Planet. Sci. Lett. 646, 1189-1208.

Palme, H., Larimer, J. W., and Lipschutz, M. E., 1988. Moderately volatile elements, in: Kerridge, J. F., Matthews, M. S. (Eds), Meteorites and the early solar system. Tucson, AZ, University of Arizona Press, 436-461.

Palme, H., Mezger, K., 2024. Nucleosynthetic isotope variations in chondritic meteorites and their relationship to bulk chemistry. Meteorit. Planet. Sci. 59, 382-394.

Pringle, E. A., & Moynier, F. (2017). Rubidium isotopic composition of the Earth, meteorites, and the Moon: Evidence for the origin of volatile loss during planetary accretion. *Earth and Planetary Science Letters, 473*, 62-70.

Richter, F. M., 2004. Timescales determining the degree of kinetic isotope fractionation by evaporation and condensation. Geochim. Cosmochim. Acta 68, 4971-4992.

Righter, K., King, C., Danielson, L., Pando, K., Lee, C. T., 2011. Experimental determination of the metal/silicate partition coefficient of Germanium: Implications for core and mantle differentiation. Earth Planet. Sci. Lett. 304, 379-388.

Schiller, M., Bizzarro, M., & Siebert, J, 2020. Iron isotope evidence for very rapid accretion and differentiation of the proto-Earth. Science. Adv 6(7), eaay7604.

Schiller, M., Paton, C., Bizzarro, M., 2015. Evidence for nucleosynthetic enrichment of the protosolar molecular cloud core by multiple supernova events. Geochim. Cosmochim. Acta 149, 88-102.

Sugiura, N., & Fujiya, W. (2014). Correlated accretion ages and ε54Cr of meteorite parent bodies and the evolution of the solar nebula. Meteorit. Planet. Sci. 49(5), 772-787.

Steller, T., Burkhardt, C., Yang, C., Kleine, T., 2022. Nucleosynthetic zinc isotope anomalies reveal a dual origin of terrestrial volatiles. Icarus 386, 115171.

Tian, Z., Jolliff, B. L., Korotev, R. L., Fegley Jr, B., Lodders, K., Day, J. M., Chen, H., Wang, K., 2020. Potassium isotopic composition of the Moon. Geochim. Cosmochim. Acta 280, 263-280.

Torrano, Z. A., Alexander, C. M. O. D., Carlson, R. W., Render, J., Brennecka, G. A., Bullock, E. S., 2024. A common isotopic reservoir for amoeboid olivine aggregates (AOAs) and calcium-aluminum-rich inclusions (CAIs) revealed by Ti and Cr isotopic compositions. Earth Planet. Sci. Lett. 627, 1185-1198.

Trinquier, A., Birck, J. L., Allegre, C. J., 2007. Widespread ⁵⁴Cr Heterogeneity in the Inner Solar System. The Astrophys. Journ. 655, 1179-1185

Trinquier, A., Elliott, T., Ulfbeck, D., Coath, C., Krot, A. N., Bizzarro, M., 2009. Origin of nucleosynthetic isotope heterogeneity in the solar protoplanetary disk. Science 324, 374-376.
Van Kooten, E., Schiller, M., Moynier, F., Johansen, A., Haugbølle, T., & Bizzarro, M. (2021). Hybrid accretion of carbonaceous chondrites by radial transport across the jupiter barrier. The Astrophys. Journ. 910(1), 70.

Van Kooten, E., Zhao, X., Franchi, I., Tung, P. Y., Fairclough, S., Walmsley, J., ... & Bizzarro, M. (2024). The nucleosynthetic fingerprint of the outermost protoplanetary disk and early Solar System dynamics. Science. Adv 10(24), eadp1613.

Villeneuve, J., Marrocchi, Y., & Jacquet, E. (2020). Silicon isotopic compositions of chondrule silicates in carbonaceous chondrites and the formation of primordial solids in the accretion disk. Earth Planet. Sci. Lett. 542, 116318.

Wai, C. M., Wasson, J. T., 1977. Nebular condensation of moderately volatile elements and their abundances in ordinary chondrites. Earth Planet. Sci. Lett. 36, 1-13.

Warren, P. H., 2011. Stable-isotopic anomalies and the accretionary assemblage of the Earth and Mars: A subordinate role for carbonaceous chondrites. Earth Planet. Sci. Lett. 311, 93-100

Wasson, J. T., Chou, C.-L., 1974. Fractionation of moderately volatile elements in ordinary chondrites. Meteoritics 9, 69-84.

Wasson, J. T., Kallemeyn, G. W., 1988. Compositions of chondrites. Philosophical Transactions of the Royal Society of London. Series A, Mathematical and Physical Sciences 325, 535-544.

Wood, B. J., Smythe, D. J., Harrison, T., 2019. The condensation temperatures of the elements: A reappraisal. Am. Min. 104, 844-856

Yurimoto, H., Kuramoto, K., Krot, A. N., Scott, E. R. D., Cuzzi, J. N., Thiemens, M. H., & Lyons, J. R., 2007. Origin and Evolution of Oxygen-Isotopic Compositions of the Solar System, in: Reipurth, B., D. Jewitt, D., Keil, K. (Eds.), Protostars and Planets V. Tucson, AZ, University of Arizona Press, 849-862.
<table><caption>Figure 1</caption><thead><tr><th></th><th></th><th></th><th></th></tr></thead><tbody><tr><td rowspan="5">Carbonaceous (CC)</td><td>CI-Orgueil</td><td></td><td rowspan="10">Chondrites and Primitive bodies</td></tr><tr><td>C2-Ung</td><td></td></tr><tr><td>CM</td><td></td></tr><tr><td>CV</td><td></td></tr><tr><td>CO</td><td></td></tr><tr><td rowspan="2">Ordinary (OC)</td><td>CBb</td><td>CBa</td></tr><tr><td>LL</td><td></td></tr><tr><td rowspan="3">Achondrite</td><td>L</td><td></td></tr><tr><td>H</td><td></td></tr><tr><td>Winonaite</td><td></td></tr><tr><td>MG Pallasite</td><td>Seymchan</td><td></td></tr><tr><td>Mars</td><td>Nakhlite</td><td></td><td rowspan="5">Planetary reservoirs</td></tr><tr><td rowspan="3">Earth</td><td>Eclogite- amphibolite</td><td></td></tr><tr><td>Basaltic crust</td><td></td></tr><tr><td>Ultramafics</td><td></td></tr><tr><td>Magmatic Fe-Meteorites</td><td></td><td></td></tr></tbody></table>

**Figure 1:** Ge isotopic compositions of carbonaceous chondrites, ordinary chondrites, one achondrite (winonaite), olivine from one main group pallasite, a Martian meteorite (Nakhlite), and new data for Earth reference samples (BIR-1 basalt and San Carlos olivine). For comparison, literature data are reported for CB meteorites (Florin et al. 2020; Florin et al., 2021), iron meteorites (Luais, 2007, 2012), and the Earth's mantle, basaltic crust and metamorphosed basaltic crust (Luais, 2012; El Korh et al., 2017). The green vertical line and shaded band represent the average bulk silicate Earth composition (δ<sup>74/70</sup>Ge = +0.53 ± 0.16‰) and the brown line and shaded band represent the average composition of magmatic iron meteorites (δ<sup>74/70</sup>Ge = +1.41 ± 0.22‰)
<figure><img src="image_2.png" /><figcaption>Figure 2</figcaption></figure>

**Figure 2:** Variations in δ<sup>74/70</sup>Ge vs [Ge] space for CC chondrites (CI, TL, CM, CV, CO, CBa, CBb) and OC chondrites (H, L, LL) (all chondrites shown as circles), and a winonaite, a main group pallasite (MGP), and the mantles of Mars and Earth (squares). Individual samples are in light blue (CC), red (OC), green (Earth), and orange (MGP); the dark green symbol represents the Earth's average basaltic crust and mantle composition (Luais, 2012; Escoube et al., 2012; El Korh et al., 2017). The black dashed line is the linear regression through CC and OC chondrites, excluding CB; the gray band is the 2 sigma standard deviation confidence interval (2σ SD). The empty red circle represents the average measured chondrule compositions (Florin et al., 2020). Win., winonaite; TL, Tagish Lake; MGP, main-group pallasite. Errors bars are 2σ SD.
<figure><img src="image_3.png" /><figcaption>Figure 3</figcaption></figure>

**Figure 3:** Mass-dependent isotopic values (‰) of δ¹²⁸Te, δ⁶⁶Zn, δ⁸⁰Rb, δ⁴¹K, δ⁷¹Ga, δ⁶⁵Cu, and δ⁵¹V vs. δ⁷⁴/⁷⁰Ge for chondrites and the Earth. The estimated CC chondrule compositions are indicated when available. Elements are ordered by decreasing volatility (expressed as T₅₀%) from top left to bottom right (T₅₀% values are reported in the top-right of each panel). For Ge, the T₅₀% = 883 K. The best correlation coefficients are seen for Te, Zn, Rb, V. Are excluded from these correlations samples with anomalous isotopic variations (e.g. high δ⁶⁶Zn in CM2, Mahan et al., 2018) due to very high degree of aqueous alteration, as well as Cd isotopes because of large variations up to 6‰ in CV and CO groups due to thermal metamorphism (Morton et al., 2024). Symbols and line colors are as in Figure 1, and reported data are average compositions. Data and references for mass-dependent isotopic compositions are listed in Table S3.
<figure><img src="image_4.png" /></figure>

**Figure 4:** Average [Ge] and δ<sup>74/70</sup>Ge values vs. matrix for each chondrite group. Blue full circles are CC mean values; the dark red filled circle is the average OC composition, and the pale filled red circles the average compositions of each individual group. (A, B) The black dashed line is the linear regression through CC and OC chondrites, excluding CBs. The gray bands indicate the 2 sigma standard deviation confidence interval (2SD). Empty red and black circles represent measured chondrule compositions (Florin et al., 2020) and those calculated by linear regression, respectively. (C) Variations in δ<sup>74/70</sup>Ge vs. [Ge] for carbonaceous chondrites and ordinary chondrites (circles), a winonaite, a main-group pallasite, and the mantles of Mars and Earth (squares). The modeled dark line indicate mixing between a matrix of CI composition, and the calculated chondrules, in 10% increments. Matrix fractions are from Hellmann et al. (2020) and Alexander (2019a, b). Win., winonaite; TL, Tagish Lake; MGP, main-group pallasite. Errors bars are 2σ SD. Further symbol descriptions are provided in Figures 2 and 3.
<figure><img src="image_5.png" /><figcaption>Figure 5</figcaption></figure>

**Figure 5:** Variations of ε⁵⁴Cr, ε⁶⁴Ni, ε⁵⁰Ti, ε⁴⁸Ca, and μ³⁰Si nucleosynthetic anomalies vs. mass-dependent δ⁷⁴/⁷⁰Ge values. A-B-C-D: Empty green circles are measured chondrule compositions from Florin et al. (2020); empty blue (CC) and red (OC) diamonds are calculated chondrule compositions (see Tables S3 and S4 for data, parameters, and references). No measured ε⁶⁴Ni or ε⁴⁸Ca values are available in the literature for CC and NC chondrules. Solid lines are mixing models between the CC matrix (CI composition) and chondrule end-members. Red shaded areas delimited by dashed lines in the NC region represent the ranges of compositions obtained using chondrule-matrix mixing models, assuming a hypothetical NC matrix with intermediate composition in terms of nucleosynthetic anomalies (see text for details). In (E), the blue and black lines are regression lines fitted through CCs only and all chondrite groups, respectively. F) Accretion time after CAIs formation reported against the δ⁷⁴/⁷⁰Ge values. Outer Disk Dark (ODD) clast composition at μ³⁰Si = 4.7±1.8 ppm and ε⁵⁴Cr = 1.25±0.09 ppm in panels A and E as defined by Van Kooten et al. (2024). Other symbols are as in Figure 2.
Supplementary materials

Origin of the mass-dependent germanium isotopic continuum
in the early Solar System

Béatrice Luais<fnref n="1" />* and Guillaume Florin<fnref n="2" />*

*Corresponding authors Email: [beatrice.luais@univ-lorraine.fr](mailto:beatrice.luais@univ-lorraine.fr) ; [guillaume.florin@uca.fr](mailto:guillaume.florin@uca.fr)

The PDF file includes:

Materials and Analytical Methods

Linear Regression and Mixing Model

Tables S1 to S4

Figures S1 to S3

Supplementary References

# 1. Materials and Analytical methods

Sample preparation

The samples selected for this study were obtained as rock chips from Museums and private collections (Table S1). The required quantity of processed samples is based on their Ge contents: about 300 mg for CCs, OCs, and primitive achondrites, and 200-300 mg for the Martian meteorite and terrestrial samples. In the case of pallasite samples, olivine was mechanically separated from the metal phase and hand-picked under a binocular microscope to obtain about 1 g of pure olivine separates.
Rock chips and olivine grain samples were first cleaned with diluted 0.2M HNO3 for 5 min in an ultrasonic bath, rinsed in ultrapure water (18.2 MΩ) for 3 min, then with ultrapure acetone for 5 min

<footnote n="1">¹Université de Lorraine, CNRS, CRPG, F-54000, Nancy, France</footnote>

<footnote n="2">²Laboratoire Magmas et Volcans, Université Clermont Auvergne, CNRS, IRD, OPGC, F-63000, Clermont-Ferrand, France</footnote>
before being dried in a laminar flow hood. Cleaned samples were crushed to a fine-grained powder in an agate mortar that was previously cleaned with dilute acid and is specifically dedicated to silicate meteorite samples. After careful homogenization of the powder, we divided it into two splits: one for elemental analysis by ThermoFischer ICP-MS X7 at the SARM and the other one for isotopic analysis by NeptunePlus MC-ICP-MS at the CRPG.

<table><caption>**Table S1** – Meteorite names and references</caption><thead><tr><th>Groups</th><th>Meteorite name</th><th>Reference number</th><th>Museums / Sources</th></tr></thead><tbody><tr><td colspan="4"><strong>Carbonaceous chondrites</strong></td></tr><tr><td>CI</td><td>Orgueil</td><td>MNHN 234</td><td>Muséum National d'Histoire Naturelle Paris</td></tr><tr><td>C2-ung.</td><td>Tagish Lake</td><td>PC</td><td></td></tr><tr><td>CV</td><td>Allende</td><td>MNHN 02811</td><td>Muséum National d'Histoire Naturelle Paris</td></tr><tr><td></td><td>NWA 5943</td><td>PC</td><td></td></tr><tr><td>CM</td><td>Murray</td><td>USNM 1769 98</td><td>Smithsonian Institution of Washington</td></tr><tr><td></td><td>Mukundpura</td><td>PC</td><td></td></tr><tr><td></td><td>NWA 10126</td><td>PC</td><td></td></tr><tr><td>CO</td><td>Ornans</td><td>MNHN 581 PE1</td><td>Muséum National d'Histoire Naturelle Paris</td></tr><tr><td>CB</td><td>Gjuba (CBa)</td><td>USNM 7075</td><td>Smithsonian Institution of Washington</td></tr><tr><td></td><td>Bencubbin (CBa)</td><td>USNM 5717 2</td><td>Smithsonian Institution of Washington</td></tr><tr><td></td><td>HaH 237 (CBb)</td><td></td><td>J. Karl, Meteorite seller</td></tr><tr><td colspan="4"><strong>Non-Carbonaceous chondrites</strong></td></tr><tr><td>H</td><td>Sharps</td><td>USNM 640</td><td>Smithsonian Institution of Washington</td></tr><tr><td></td><td>Dhajala</td><td>USNM 5832</td><td>Smithsonian Institution of Washington</td></tr><tr><td></td><td>Ste. Marguerite</td><td>MNHN 3290</td><td>Muséum National d'Histoire Naturelle Paris</td></tr><tr><td></td><td>Allegan</td><td>USNM 215</td><td>Smithsonian Institution of Washington</td></tr><tr><td></td><td>Guareña</td><td>MNCN</td><td>Museo Nacional de Ciencias Naturales, Madrid</td></tr><tr><td></td><td>Kernouvé</td><td></td><td>Smithsonian Institution of Washington</td></tr><tr><td>L</td><td>Julesburg</td><td>MNHN 3346</td><td>Muséum National d'Histoire Naturelle Paris</td></tr><tr><td></td><td>Herdaz</td><td>MNHN 2132</td><td>MNHN-Paris</td></tr><tr><td></td><td>Bjurbole (metal)</td><td>USNM 6705</td><td>Muséum National d'Histoire Naturelle Paris</td></tr><tr><td></td><td>Vouillé</td><td>MNHN 148</td><td>Muséum National d'Histoire Naturelle Paris</td></tr><tr><td></td><td>Afianello</td><td>MNHN 855</td><td>Muséum National d'Histoire Naturelle Paris</td></tr><tr><td></td><td>Tourrines-la Grosse</td><td>MNHN 181</td><td>Muséum National d'Histoire Naturelle Paris</td></tr><tr><td>LL</td><td>Semarkona</td><td>USNM 1805</td><td>Smithsonian Institution of Washington</td></tr><tr><td></td><td>Parnallee</td><td>USNM 1613</td><td>Smithsonian Institution of Washington</td></tr><tr><td colspan="4"><strong>Primitive achondrites</strong></td></tr><tr><td>Winonaite</td><td>Pontlyfni</td><td>BM.1975,M6</td><td>National History Museum, London</td></tr><tr><td>Main group pallasite</td><td>Seymchan (olivine)</td><td>INCA 5147</td><td>Kachalin D., Meteorite seller</td></tr><tr><td>Mars mantle (Nakhlite)</td><td>Nakhla (cpx cumulate)</td><td>BM.1913,25</td><td>National History Museum, London</td></tr></tbody></table>

**Abreviations:** MNCN, Museo Nacional de Ciencias Naturales, Madrid; MNHN, Muséum National d'Histoire Naturelle, Paris; USNM, United States National Museum, Washington; IB, Impact Breccia; PC: Sample provided by L. G. Vacher.
The volatile behavior of germanium necessitates specific precautions during chemical processing. All procedures must be performed at temperatures below 65°C to prevent germanium loss. Additionally, the use of HCl and HClO₄ acids is prohibited, as they can lead to Ge loss through the formation of volatile GeCl₄ species (Luais, 2012).

Carbonaceous chondrites have high carbon contents at the wt.% level. In our samples, carbon content ranged from 0.29 wt.% in Allende CV-type to 2.8 wt.% in Orgueil CI-type. Such high carbon contents can induce difficulties during sample digestion and the chromatographic purification of Ge. Therefore, specific pre-digestion processing was applied to powdered carbonaceous chondrite samples before the digestion steps. Namely, powdered samples were first placed in a furnace in individual platinum crucibles and heated to 500 °C for carbon combustion (ashing). This process does not induce any isotopic fractionation of Ge (Qi et al., 2011) (see BIR-1 ashing values, Table S2).

Sample digestion and the chromatographic purification of germanium were performed followed the procedures reported in Luais (2012). All chemical reagents used were of high purity: HF and HNO₃ acids from SeaStar™, and 18.2 MΩ deionized water. Carbonaceous chondrites, achondrites, Martian meteorites, pallasite olivines and geostandard sample powders were dissolved in 3:1 mixtures of 28 M HF-15 M HNO₃ acids in screw-top Teflon vials on a hot plate at 65°C to avoid any loss of volatile Ge, with alternating ultrasonic and hot plate steps, during several days until complete dissolution. In contrast, ordinary chondrites powders cannot successfully dissolve in screw-top Teflon vials at 65°C on hot plate. Instead, they were dissolved at higher temperature (160°C) and pressure (25 bars) in pure PTFE/TFM BOLA digestion vessels (Bohlender GmbH®) (Luais et al., 2009), which does not allow Ge evaporation (Florin et al., 2020; Luais, 2007). The solutions were then transferred into screw-top Teflon vials. The total dissolution of the samples was evaluated visually and validated when obtaining a white cloudy solution free of any sample powder solid particles, resulting from the formation of Al-Mg-Ca-fluorides that do not incorporate Ge (Luais, 2012). Several steps of centrifugation and leaching with 28 M HF leads to complete Ge recovery in the supernatant fraction (Luais, 2012). The Ge-bearing solution was evaporated to dryness, then dissolved in 1 M HF for subsequent germanium isolation through two steps: resin-exchange chromatography columns. The 1 M HF sample solution was first introduced through an AG 1-X8 anion exchange resin (chloride form, 200–400 mesh, 2 mL) and the Ge fraction was eluted with 0.2 M HNO₃ and evaporated at 65 °C on a hot plate. The dry residue was taken up in 0.5cc HNO₃ (0.5 M) for further purification through an AG 50W-X8 cationic-exchange resin (hydrogen form, 200–400 mesh, 2 mL), and Ge was then collected with 2 mL HNO₃ (0.5 M). The total chemistry procedure results in a nearly full yield of Ge on various matrices (>95%). The obtained Ge fraction was then ready for preparation for MC-ICPMS analysis. Chemistry blanks and a geostandard sample (BIR-1
Icelandic basalt) were processed together with meteorite samples to evaluate the long-term reproducibility and accuracy of Ge chemistry.

## Germanium elemental measurements

For a large number of meteorites, no bulk germanium concentration data have been reported in the literature. About 100 mg of bulk powder samples of the ordinary chondrites, a winonaite, Martian meteorite, and pallasite olivine were analyzed for trace elemental compositions at the SARM analytical facility (Service Analytique des Roches et des Minéraux, CRPG-Nancy) following routine LiBO₂ alkaline fusion dissolution techniques, and using a ThermoFischer ICP-MS X7 instrument (Carignan et al., 2001). Errors associated with the Ge measurements are <5% at 1 µg/g for our sample concentrations. For pallasite olivine containing < 50 ηg/g Ge, to improve the accuracy on these extremely low Ge concentrations, measurements of Ge abundances were performed using the standard addition method, with an estimated error of 20%.

For some carbonaceous chondrite samples with limited amounts of available material (NWA 6418, Mukundpura, NWA10126, Tagish Lake), the Ge elemental compositions were obtained using dedicated sample solutions for NeptunePlus MC-ICP-MS isotopic measurements, and by comparing sample intensities to reference materials (BIR-1), in-house standards (Ge-Aldrich, Ge-JMC), and bracketing standards (NIST3120a) of known concentrations.

## MC-ICP-MS isotopic measurements

Ge isotopic measurements were performed using the NeptunePlus MC-ICP-MS coupled with a Hydride Generator Introduction System (HGIS-HGX-200 Teledyne CETAC Technologies) at the CRPG-Nancy. This technique removes isobaric interferences from elements that do not form hydrides (e.g. ⁷⁰Zn on ⁷⁰Ge, ⁵⁶Fe¹⁶O on ⁷²Ge, ⁵⁷Fe¹⁶O on ⁷³Ge, and ⁵⁸Ni¹⁶O on ⁷⁴Ge, as well as Ar dimers), avoiding matrix effects. This results in a gain in signal sensitivity by at least a factor of 30, which is required for high precision routine isotopic measurements of 10–20 ng Ge for one measurement (Florin et al., 2020; Luais, 2007; 2012). Given the absence of interferences, analyses were performed in static mode at low mass resolution (M/ΔM = 400) with a Ni skimmer, and sampler cones in standard geometrical configuration. To allow for Zn monitoring, the Faraday cups were arranged as follows: Low3 (⁶⁸Zn), Low2 (⁶⁹Ga), Low1 (⁷⁰Ge), Axial (⁷¹Ga), High1 (⁷²Ge), High2 (⁷³Ge), High3 (⁷⁴Ge), allowing the possibility for Zn monitoring. Tuning parameters, e.g. gas flow rates of the ICP-MS and the Hydride Generator Introduction System (HGIS), torch positions, and ion lenses, were optimized by measuring the NIST SRM 3120a Ge standard solution (Luais, 2007; 2012). Analyses were carried out on diluted 10 ppb
samples and standard solutions, with beam intensities matching to within 7% between samples and
standards, giving an average ⁷⁴Ge beam intensity of 2.5 V during the course of this study. Washing
sequence between measurements include 200 s washout with 0.5 M HNO₃, followed by 240s rinse in
1 M HNO₃ and 120 s in 0.5 M HNO₃ blank solution. After washing, measurements of a 0.5 M HNO₃
blank solution (180 s on-peak integration time) were taken before each sample and standard
measurement to check the procedural blank level. Data acquisition procedures for standards and
samples consisted of 40 cycles of 8 s integration time, giving an internal precision better than 5
ppm/amu (2SE).

We used the sample-standard-bracketing method with the NIST 3120a Ge standard solution to encompass analytical mass bias. ⁷²Ge/⁷⁰Ge, ⁷³Ge/⁷⁰Ge, and ⁷⁴Ge/⁷⁰Ge ratios are expressed in delta notation relative to the NIST 3120a Ge standard measured before and after each sample: ‰ δₓGe = ((ₓGe/⁷⁰Ge)ₘₚ₉/(_ₓGe/⁷⁰Ge)ₙₘ₉ - 1) × 1000. At least three to five replicates were required to achieve external reproducibilities less than about 0.1‰ (2σ SD)

The total procedural blank level for germanium, including chemistry and MC-ICP-MS
measurements, ranged between 70 and 200 pg during the course of this study, which represents 0.1–
0.3% of the chemically processed Ge. During each measurement session, we used JMC Ge (1000 ppm
ICP standard solution, lot # 301230S, Johnson Matthey, Germany) and Aldrich Ge (10200 ppm ICP
standard solution, lot # 01704KZ, Aldrich Chemical Co., USA) as secondary standards to evaluate the
accuracy and long-term reproducibility of Ge isotopic measurements. Average values for JMC and
Aldrich Ge standard solutions yielded δ<sup>74</sup>Ge = -0.31 ± 0.09‰ (n = 68) and δ<sup>74</sup>Ge = -1.97 ± 0.09‰ (n =
67), respectively (2σ SD) (Table S2). We also measured the BIR-1 geostandard that we processed along
with the samples according to the three different digestion procedures used for silicate samples. Data
were consistent within errors for Ge isotopic values, emphasizing the accuracy of the Ge chemistry
procedures: δ<sup>74</sup>Ge = 0.61 ± 0.09‰ (n = 24) for classical digestion in screw-top Teflon vials on a hot
plate at 65°C, δ<sup>74</sup>Ge = 0.62 ± 0.07‰ (n = 2) for BOLA digestion pressure vessels at 150 °C, and δ<sup>74</sup>Ge =
0.69 ± 0.05‰ (n = 2) for the furnace ashing treatment before digestion (Table S2). All these values are
in full agreement with previously published data (Florin et al., 2020; Luais, 2007, 2012). The long-term
reproducibility of germanium isotopic measurements on JMC and Aldrich standard solutions is 0.1‰,
consistent with the reproducibility range of 0.02 to 0.1‰ observed in meteorite samples (Table S2).
<table><caption>Table S2. Germanium isotopic compositions of geostandards and standards</caption><thead><tr><th>Geostandard name</th><th>Date</th><th>δ<sup>72/70</sup>Ge<sub>NIST3120a</sub><br>‰</th><th>±2σ SD</th><th>δ<sup>73/70</sup>Ge<sub>NIST3120a</sub><br>‰</th><th>±2σ SD</th><th>δ<sup>74/70</sup>Ge<sub>NIST3120a</sub><br>‰</th><th>±2σ SD</th></tr></thead><tbody><tr><td><strong>BIR-1</strong></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td rowspan="24">Hotplate digestion</td><td>December-2017</td><td>0.29</td><td></td><td>0.38</td><td></td><td>0.56</td><td></td></tr><tr><td></td><td>0.35</td><td></td><td>0.41</td><td></td><td>0.60</td><td></td></tr><tr><td>January-2018</td><td>0.35</td><td></td><td>0.52</td><td></td><td>0.68</td><td></td></tr><tr><td>May-2018</td><td>0.32</td><td></td><td>0.40</td><td></td><td>0.60</td><td></td></tr><tr><td></td><td>0.28</td><td></td><td>0.36</td><td></td><td>0.54</td><td></td></tr><tr><td>June-2018</td><td>0.35</td><td></td><td>0.52</td><td></td><td>0.68</td><td></td></tr><tr><td></td><td>0.36</td><td></td><td>0.48</td><td></td><td>0.59</td><td></td></tr><tr><td></td><td>0.30</td><td></td><td>0.36</td><td></td><td>0.54</td><td></td></tr><tr><td></td><td>0.37</td><td></td><td>0.48</td><td></td><td>0.62</td><td></td></tr><tr><td></td><td>0.30</td><td></td><td>0.38</td><td></td><td>0.56</td><td></td></tr><tr><td>July-2018</td><td>0.32</td><td></td><td>0.43</td><td></td><td>0.60</td><td></td></tr><tr><td></td><td>0.32</td><td></td><td>0.44</td><td></td><td>0.62</td><td></td></tr><tr><td></td><td>0.31</td><td></td><td>0.39</td><td></td><td>0.57</td><td></td></tr><tr><td></td><td>0.38</td><td></td><td>0.46</td><td></td><td>0.67</td><td></td></tr><tr><td></td><td>0.30</td><td></td><td>0.45</td><td></td><td>0.67</td><td></td></tr><tr><td>August-2018</td><td>0.31</td><td></td><td>0.37</td><td></td><td>0.56</td><td></td></tr><tr><td></td><td>0.35</td><td></td><td>0.44</td><td></td><td>0.65</td><td></td></tr><tr><td></td><td>0.33</td><td></td><td>0.48</td><td></td><td>0.56</td><td></td></tr><tr><td></td><td>0.29</td><td></td><td>0.38</td><td></td><td>0.56</td><td></td></tr><tr><td></td><td>0.35</td><td></td><td>0.41</td><td></td><td>0.60</td><td></td></tr><tr><td></td><td>0.31</td><td></td><td>0.40</td><td></td><td>0.60</td><td></td></tr><tr><td>November-2018</td><td>0.38</td><td></td><td>0.60</td><td></td><td>0.77</td><td></td></tr><tr><td><strong>Average</strong></td><td></td><td><strong>0.33</strong></td><td><strong>0.06</strong></td><td><strong>0.44</strong></td><td><strong>0.13</strong></td><td><strong>0.62</strong></td><td><strong>0.13</strong></td></tr><tr><td rowspan="3">Bomb digestion 150°C</td><td>May-2018</td><td>0.33</td><td></td><td>0.50</td><td></td><td>0.64</td><td></td></tr><tr><td>August-2018</td><td>0.31</td><td></td><td>0.43</td><td></td><td>0.59</td><td></td></tr><tr><td><strong>Average</strong></td><td><strong>0.32</strong></td><td><strong>0.03</strong></td><td><strong>0.47</strong></td><td><strong>0.10</strong></td><td><strong>0.62</strong></td><td><strong>0.07</strong></td></tr><tr><td rowspan="2">Ashing 500°C</td><td>September-2020</td><td>0.37</td><td></td><td>0.59</td><td></td><td>0.67</td><td></td></tr><tr><td></td><td>0.36</td><td></td><td>0.51</td><td></td><td>0.71</td><td></td></tr><tr><td><strong>Average</strong></td><td></td><td><strong>0.36</strong></td><td><strong>0.01</strong></td><td><strong>0.55</strong></td><td><strong>0.11</strong></td><td><strong>0.69</strong></td><td><strong>0.05</strong></td></tr><tr><td><strong>San Carlos Olivine</strong></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td rowspan="8">December-2017</td><td></td><td>0.37</td><td></td><td>0.57</td><td></td><td>0.77</td><td></td></tr><tr><td></td><td>0.35</td><td></td><td>0.45</td><td></td><td>0.69</td><td></td></tr><tr><td></td><td>0.35</td><td></td><td>0.39</td><td></td><td>0.67</td><td></td></tr><tr><td></td><td>0.36</td><td></td><td>0.46</td><td></td><td>0.72</td><td></td></tr><tr><td></td><td>0.34</td><td></td><td>0.49</td><td></td><td>0.71</td><td></td></tr><tr><td></td><td>0.34</td><td></td><td>0.43</td><td></td><td>0.66</td><td></td></tr><tr><td></td><td>0.37</td><td></td><td>0.51</td><td></td><td>0.74</td><td></td></tr><tr><td>June-2018</td><td>0.34</td><td></td><td>0.51</td><td></td><td>0.68</td><td></td></tr><tr><td></td><td>0.34</td><td></td><td>0.49</td><td></td><td>0.67</td><td></td></tr><tr><td></td><td>0.33</td><td></td><td>0.46</td><td></td><td>0.63</td><td></td></tr><tr><td><strong>Average</strong></td><td></td><td><strong>0.35</strong></td><td><strong>0.03</strong></td><td><strong>0.55</strong></td><td><strong>0.10</strong></td><td><strong>0.69</strong></td><td><strong>0.08</strong></td></tr></tbody></table>
<table><thead><tr><th>Standard name</th><th>Date</th><th>δ<sup>72/70</sup>Ge<sub>NIST3120a</sub><br>‰</th><th>±2σ SD</th><th>δ<sup>73/70</sup>Ge<sub>NIST3120a</sub><br>‰</th><th>±2σ SD</th><th>δ<sup>74/70</sup>Ge<sub>NIST3120a</sub><br>‰</th><th>±2σ SD</th></tr></thead><tbody><tr><td rowspan="24">Aldrich</td><td rowspan="12">December-2017</td><td>-1.05</td><td></td><td>-1.58</td><td></td><td>-2.00</td><td></td></tr><tr><td>-1.04</td><td></td><td>-1.48</td><td></td><td>-2.02</td><td></td></tr><tr><td>-1.04</td><td></td><td>-1.56</td><td></td><td>-1.98</td><td></td></tr><tr><td>-1.02</td><td></td><td>-1.47</td><td></td><td>-1.95</td><td></td></tr><tr><td>-1.00</td><td></td><td>-1.50</td><td></td><td>-1.94</td><td></td></tr><tr><td>-1.02</td><td></td><td>-1.54</td><td></td><td>-1.99</td><td></td></tr><tr><td>-1.01</td><td></td><td>-1.47</td><td></td><td>-1.95</td><td></td></tr><tr><td>-1.00</td><td></td><td>-1.48</td><td></td><td>-1.93</td><td></td></tr><tr><td>-0.99</td><td></td><td>-1.47</td><td></td><td>-1.97</td><td></td></tr><tr><td>-1.05</td><td></td><td>-1.58</td><td></td><td>-1.98</td><td></td></tr><tr><td>-1.01</td><td></td><td>-1.59</td><td></td><td>-1.94</td><td></td></tr><tr><td>-1.04</td><td></td><td>-1.56</td><td></td><td>-2.07</td><td></td></tr><tr><td>-1.01</td><td></td><td>-1.52</td><td></td><td>-1.98</td><td></td></tr><tr><td>-1.04</td><td></td><td>-1.54</td><td></td><td>-2.02</td><td></td></tr><tr><td>-1.03</td><td></td><td>-1.53</td><td></td><td>-1.98</td><td></td></tr><tr><td>-1.01</td><td></td><td>-1.49</td><td></td><td>-1.96</td><td></td></tr><tr><td>-0.99</td><td></td><td>-1.56</td><td></td><td>-2.01</td><td></td></tr><tr><td>-1.03</td><td></td><td>-1.50</td><td></td><td>-2.00</td><td></td></tr><tr><td>-1.02</td><td></td><td>-1.56</td><td></td><td>-1.98</td><td></td></tr><tr><td>-1.00</td><td></td><td>-1.52</td><td></td><td>-1.99</td><td></td></tr><tr><td>-1.01</td><td></td><td>-1.50</td><td></td><td>-1.99</td><td></td></tr><tr><td>-0.97</td><td></td><td>-1.49</td><td></td><td>-1.95</td><td></td></tr><tr><td>-1.04</td><td></td><td>-1.55</td><td></td><td>-1.98</td><td></td></tr><tr><td>-1.00</td><td></td><td>-1.55</td><td></td><td>-1.96</td><td></td></tr><tr><td>-1.02</td><td></td><td>-1.56</td><td></td><td>-1.97</td><td></td></tr><tr><td>-1.01</td><td></td><td>-1.50</td><td></td><td>-1.95</td><td></td></tr><tr><td>-1.03</td><td></td><td>-1.55</td><td></td><td>-2.02</td><td></td></tr><tr><td rowspan="6">January-2018</td><td>-1.01</td><td></td><td>-1.47</td><td></td><td>-1.95</td><td></td></tr><tr><td>-1.02</td><td></td><td>-1.57</td><td></td><td>-1.99</td><td></td></tr><tr><td>-0.99</td><td></td><td>-1.52</td><td></td><td>-1.94</td><td></td></tr><tr><td>-0.97</td><td></td><td>-1.47</td><td></td><td>-1.95</td><td></td></tr><tr><td>-1.01</td><td></td><td>-1.50</td><td></td><td>-1.99</td><td></td></tr><tr><td>-1.02</td><td></td><td>-1.58</td><td></td><td>-2.01</td><td></td></tr><tr><td rowspan="8">April-2018</td><td>-1.06</td><td></td><td>-1.61</td><td></td><td>-2.07</td><td></td></tr><tr><td>-1.04</td><td></td><td>-1.63</td><td></td><td>-2.06</td><td></td></tr><tr><td>-0.96</td><td></td><td>-1.44</td><td></td><td>-1.94</td><td></td></tr><tr><td>-1.00</td><td></td><td>-1.56</td><td></td><td>-2.00</td><td></td></tr><tr><td>-0.99</td><td></td><td>-1.48</td><td></td><td>-1.94</td><td></td></tr><tr><td>-1.03</td><td></td><td>-1.58</td><td></td><td>-1.99</td><td></td></tr><tr><td>-1.01</td><td></td><td>-1.48</td><td></td><td>-2.02</td><td></td></tr><tr><td>-1.02</td><td></td><td>-1.52</td><td></td><td>-1.99</td><td></td></tr><tr><td rowspan="4">September-2018</td><td>-1.00</td><td></td><td>-1.43</td><td></td><td>-1.95</td><td></td></tr><tr><td>-0.99</td><td></td><td>-1.50</td><td></td><td>-1.95</td><td></td></tr><tr><td>-0.96</td><td></td><td>-1.42</td><td></td><td>-1.89</td><td></td></tr><tr><td>-1.01</td><td></td><td>-1.52</td><td></td><td>-1.99</td><td></td></tr></tbody></table>
<table><thead><tr><th>Standard name</th><th>Date</th><th>δ<sup>72/70</sup>Ge<sub>NIST3120a</sub><br>‰</th><th>±2σ SD</th><th>δ<sup>73/70</sup>Ge<sub>NIST3120a</sub><br>‰</th><th>±2σ SD</th><th>δ<sup>74/70</sup>Ge<sub>NIST3120a</sub><br>‰</th><th>±2σ SD</th></tr></thead><tbody><tr><td rowspan="24">Aldrich</td><td rowspan="12">October-2018</td><td>-0.94</td><td></td><td>-1.42</td><td></td><td>-1.78</td><td></td></tr><tr><td>-0.99</td><td></td><td>-1.49</td><td></td><td>-1.94</td><td></td></tr><tr><td>-1.00</td><td></td><td>-1.47</td><td></td><td>-1.92</td><td></td></tr><tr><td>-1.02</td><td></td><td>-1.48</td><td></td><td>-1.96</td><td></td></tr><tr><td>-1.03</td><td></td><td>-1.53</td><td></td><td>-1.99</td><td></td></tr><tr><td>-1.02</td><td></td><td>-1.49</td><td></td><td>-1.95</td><td></td></tr><tr><td>-0.99</td><td></td><td>-1.49</td><td></td><td>-1.93</td><td></td></tr><tr><td>-1.02</td><td></td><td>-1.56</td><td></td><td>-1.99</td><td></td></tr><tr><td>-0.98</td><td></td><td>-1.47</td><td></td><td>-1.92</td><td></td></tr><tr><td>-1.03</td><td></td><td>-1.50</td><td></td><td>-1.99</td><td></td></tr><tr><td>-1.00</td><td></td><td>-1.52</td><td></td><td>-1.97</td><td></td></tr><tr><td>-0.96</td><td></td><td>-1.46</td><td></td><td>-1.87</td><td></td></tr><tr><td>-0.95</td><td></td><td>-1.45</td><td></td><td>-1.91</td><td></td></tr><tr><td rowspan="6">January-2019</td><td>-0.97</td><td></td><td>-1.57</td><td></td><td>-1.89</td><td></td></tr><tr><td>-1.05</td><td></td><td>-1.69</td><td></td><td>-1.97</td><td></td></tr><tr><td>-1.00</td><td></td><td>-1.47</td><td></td><td>-1.98</td><td></td></tr><tr><td>-1.02</td><td></td><td>-1.67</td><td></td><td>-2.00</td><td></td></tr><tr><td>-1.04</td><td></td><td>-1.53</td><td></td><td>-1.99</td><td></td></tr><tr><td>-0.99</td><td></td><td>-1.33</td><td></td><td>-1.90</td><td></td></tr><tr><td rowspan="4">September-2020</td><td>-1.03</td><td></td><td>-1.51</td><td></td><td>-1.98</td><td></td></tr><tr><td>-1.01</td><td></td><td>-1.48</td><td></td><td>-1.95</td><td></td></tr><tr><td>-0.98</td><td></td><td>-1.49</td><td></td><td>-1.91</td><td></td></tr><tr><td>-1.00</td><td></td><td>-1.46</td><td></td><td>-1.94</td><td></td></tr><tr><td>Average</td><td></td><td><b>-1.01</b></td><td><b>0.05</b></td><td><b>-1.51</b></td><td><b>0.12</b></td><td><b>-1.97</b></td><td><b>0.09</b></td></tr><tr><td rowspan="24">JMC</td><td rowspan="24">December-2017</td><td>-0.15</td><td></td><td>-0.10</td><td></td><td>-0.32</td><td></td></tr><tr><td>-0.16</td><td></td><td>-0.19</td><td></td><td>-0.35</td><td></td></tr><tr><td>-0.16</td><td></td><td>-0.12</td><td></td><td>-0.34</td><td></td></tr><tr><td>-0.13</td><td></td><td>-0.19</td><td></td><td>-0.27</td><td></td></tr><tr><td>-0.18</td><td></td><td>-0.19</td><td></td><td>-0.35</td><td></td></tr><tr><td>-0.16</td><td></td><td>-0.21</td><td></td><td>-0.33</td><td></td></tr><tr><td>-0.13</td><td></td><td>-0.17</td><td></td><td>-0.27</td><td></td></tr><tr><td>-0.18</td><td></td><td>-0.28</td><td></td><td>-0.39</td><td></td></tr><tr><td>-0.14</td><td></td><td>-0.14</td><td></td><td>-0.26</td><td></td></tr><tr><td>-0.12</td><td></td><td>-0.20</td><td></td><td>-0.30</td><td></td></tr><tr><td>-0.13</td><td></td><td>-0.13</td><td></td><td>-0.27</td><td></td></tr><tr><td>-0.12</td><td></td><td>-0.21</td><td></td><td>-0.26</td><td></td></tr><tr><td>-0.12</td><td></td><td>-0.15</td><td></td><td>-0.24</td><td></td></tr><tr><td>-0.10</td><td></td><td>-0.15</td><td></td><td>-0.22</td><td></td></tr><tr><td>-0.16</td><td></td><td>-0.21</td><td></td><td>-0.30</td><td></td></tr><tr><td>-0.15</td><td></td><td>-0.23</td><td></td><td>-0.35</td><td></td></tr><tr><td>-0.12</td><td></td><td>-0.14</td><td></td><td>-0.24</td><td></td></tr><tr><td>-0.16</td><td></td><td>-0.22</td><td></td><td>-0.32</td><td></td></tr><tr><td>-0.16</td><td></td><td>-0.24</td><td></td><td>-0.33</td><td></td></tr><tr><td>-0.18</td><td></td><td>-0.23</td><td></td><td>-0.33</td><td></td></tr><tr><td>-0.18</td><td></td><td>-0.24</td><td></td><td>-0.32</td><td></td></tr><tr><td>-0.15</td><td></td><td>-0.18</td><td></td><td>-0.30</td><td></td></tr></tbody></table>
<table><thead><tr><th>Standard name</th><th>Date</th><th>δ<sup>72/70</sup>Ge<sub>NIST3120a</sub><br>‰</th><th>±2σ SD</th><th>δ<sup>73/70</sup>Ge<sub>NIST3120a</sub><br>‰</th><th>±2σ SD</th><th>δ<sup>74/70</sup>Ge<sub>NIST3120a</sub><br>‰</th><th>±2σ SD</th></tr></thead><tbody><tr><td rowspan="24">JMC</td><td rowspan="4">January-2018</td><td>-0.17</td><td></td><td>-0.2</td><td></td><td>-0.34</td><td></td></tr><tr><td>-0.16</td><td></td><td>-0.18</td><td></td><td>-0.35</td><td></td></tr><tr><td>-0.15</td><td></td><td>-0.23</td><td></td><td>-0.33</td><td></td></tr><tr><td>-0.17</td><td></td><td>-0.24</td><td></td><td>-0.35</td><td></td></tr><tr><td rowspan="6">April-2018</td><td>-0.19</td><td></td><td>-0.27</td><td></td><td>-0.39</td><td></td></tr><tr><td>-0.13</td><td></td><td>-0.16</td><td></td><td>-0.32</td><td></td></tr><tr><td>-0.2</td><td></td><td>-0.34</td><td></td><td>-0.4</td><td></td></tr><tr><td>-0.08</td><td></td><td>-0.14</td><td></td><td>-0.23</td><td></td></tr><tr><td>-0.17</td><td></td><td>-0.21</td><td></td><td>-0.38</td><td></td></tr><tr><td>-0.13</td><td></td><td>-0.13</td><td></td><td>-0.27</td><td></td></tr><tr><td rowspan="6">September-2018</td><td>-0.2</td><td></td><td>-0.28</td><td></td><td>-0.41</td><td></td></tr><tr><td>-0.11</td><td></td><td>-0.15</td><td></td><td>-0.24</td><td></td></tr><tr><td>-0.16</td><td></td><td>-0.22</td><td></td><td>-0.28</td><td></td></tr><tr><td>-0.14</td><td></td><td>-0.17</td><td></td><td>-0.32</td><td></td></tr><tr><td>-0.17</td><td></td><td>-0.17</td><td></td><td>-0.3</td><td></td></tr><tr><td>-0.17</td><td></td><td>-0.25</td><td></td><td>-0.35</td><td></td></tr><tr><td rowspan="10">October-2018</td><td>-0.17</td><td></td><td>-0.24</td><td></td><td>-0.34</td><td></td></tr><tr><td>-0.12</td><td></td><td>-0.18</td><td></td><td>-0.27</td><td></td></tr><tr><td>-0.12</td><td></td><td>-0.23</td><td></td><td>-0.32</td><td></td></tr><tr><td>-0.12</td><td></td><td>-0.12</td><td></td><td>-0.25</td><td></td></tr><tr><td>-0.15</td><td></td><td>-0.19</td><td></td><td>-0.27</td><td></td></tr><tr><td>-0.15</td><td></td><td>-0.21</td><td></td><td>-0.31</td><td></td></tr><tr><td>-0.13</td><td></td><td>-0.15</td><td></td><td>-0.26</td><td></td></tr><tr><td>-0.17</td><td></td><td>-0.22</td><td></td><td>-0.33</td><td></td></tr><tr><td>-0.15</td><td></td><td>-0.18</td><td></td><td>-0.28</td><td></td></tr><tr><td>-0.14</td><td></td><td>-0.18</td><td></td><td>-0.33</td><td></td></tr><tr><td rowspan="6">January-2019</td><td>-0.14</td><td></td><td>-0.25</td><td></td><td>-0.31</td><td></td></tr><tr><td>-0.14</td><td></td><td>-0.22</td><td></td><td>-0.32</td><td></td></tr><tr><td>-0.11</td><td></td><td>-0.14</td><td></td><td>-0.21</td><td></td></tr><tr><td>-0.11</td><td></td><td>-0.18</td><td></td><td>-0.23</td><td></td></tr><tr><td>-0.15</td><td></td><td>-0.29</td><td></td><td>-0.31</td><td></td></tr><tr><td>-0.21</td><td></td><td>-0.28</td><td></td><td>-0.37</td><td></td></tr><tr><td rowspan="6">September-2020</td><td>-0.2</td><td></td><td>-0.21</td><td></td><td>-0.36</td><td></td></tr><tr><td>-0.14</td><td></td><td>-0.21</td><td></td><td>-0.34</td><td></td></tr><tr><td>-0.16</td><td></td><td>-0.16</td><td></td><td>-0.34</td><td></td></tr><tr><td>-0.17</td><td></td><td></td><td></td><td>-0.3</td><td></td></tr><tr><td>-0.15</td><td></td><td>-0.23</td><td></td><td>-0.3</td><td></td></tr><tr><td>-0.16</td><td></td><td>-0.21</td><td></td><td>-0.31</td><td></td></tr><tr><td rowspan="4">January-2019</td><td>-0.19</td><td></td><td>-0.26</td><td></td><td>-0.42</td><td></td></tr><tr><td>-0.08</td><td></td><td>-0.17</td><td></td><td>-0.26</td><td></td></tr><tr><td>-0.14</td><td></td><td>-0.15</td><td></td><td>-0.31</td><td></td></tr><tr><td>-0.15</td><td></td><td>-0.23</td><td></td><td>-0.3</td><td></td></tr></tbody></table>
<table><thead><tr><th>Standard name</th><th>Date</th><th>δ<sup>72/70</sup>Ge<sub>NIST3120a</sub><br>‰</th><th>±2σ SD</th><th>δ<sup>73/70</sup>Ge<sub>NIST3120a</sub><br>‰</th><th>±2σ SD</th><th>δ<sup>74/70</sup>Ge<sub>NIST3120a</sub><br>‰</th><th>±2σ SD</th></tr></thead><tbody><tr><td rowspan="4">JMC</td><td></td><td>-0.16</td><td></td><td>-0.19</td><td></td><td>-0.33</td><td></td></tr><tr><td></td><td>-0.12</td><td></td><td>-0.13</td><td></td><td>-0.25</td><td></td></tr><tr><td></td><td>-0.13</td><td></td><td>-0.15</td><td></td><td>-0.26</td><td></td></tr><tr><td></td><td>-0.16</td><td></td><td>-0.23</td><td></td><td>-0.32</td><td></td></tr><tr><td>Average</td><td></td><td><strong>-0.15</strong></td><td><strong>0.06</strong></td><td><strong>-0.2</strong></td><td><strong>0.1</strong></td><td><strong>-0.31</strong></td><td><strong>0.09</strong></td></tr></tbody></table>

## 2. Linear Regression and Mixing Model

All parameters needed to perform mixing models presented herein are reported in Tables S3 and S4.

We performed our chondrule-matrix mixing model in several steps. The initial step was to estimate the Ge elemental and isotopic composition of the non-matrix component. In the [Ge] vs. matrix and δ<sup>74/70</sup>Ge vs. matrix diagrams (Fig. 4b, c), we first calculate the linear regression through the averaged chondrite groups, regardless of NCC or CC affiliation. In such orthogonal, logarithmic-free diagrams these two linear regressions do not imply mixing and produce *straight lines* expressed simply as:

$$y = ax + b$$

where *a* is the slope, *b* is the y-intercept, *y* represents either [Ge] or δ<sup>74/70</sup>Ge, and *x* is the percentage of matrix. Thus, by assuming *x* = 0 wt.% matrix, we determined the elemental and isotopic composition of the matrix-free component: [Ge] = 10.74 µg/g (Fig. 2b) and δ<sup>74/70</sup>Ge = -0.51 ‰ (Fig. 2c). Our results are in good agreement with H-type OC chondrule composition previously measured by Florin et al. (2020). However, we have no measurements for CC chondrules. Therefore, in the following we use calculated values of chondrules, because we assume that they better represent the average composition of NCC and CC chondrules compared to the chondrule pools measured exclusively for H-type ordinary chondrites.

Secondly, we calculated three mixing models in the [Ge] vs matrix, δ<sup>74/70</sup>Ge vs matrix, and δ<sup>74/70</sup>Ge vs [Ge] diagrams. In the [Ge] vs. matrix diagram (Fig. 4b), the Ge content can be calculated for any chondrules + matrix assembly following:

$$[Ge]_{i} = f \times [Ge]_{matrix} + (1 - f) \times [Ge]_{non-matrix}$$

where [Ge]<sub>i</sub> is the germanium content for a given matrix fraction *f* and non-matrix fraction (1 - *f*). In this diagram the mixing model is a straight line. In the δ<sup>74/70</sup>Ge vs matrix diagram (Fig. 4c), the Ge isotopic composition can be calculated for any chondrules +matrix assembly following:
$$ \delta^{74/70}\text{Ge}_i = \frac{f \times [\text{Ge}]_{\text{matrix}} \times \delta^{74/70}\text{Ge}_{\text{matrix}} + (1-f) \times [\text{Ge}]_{\text{non-matrix}} \times \delta^{74/70}\text{Ge}_{\text{non-matrix}}}{f \times [\text{Ge}]_{\text{matrix}} + (1-f) \times [\text{Ge}]_{\text{non-matrix}}} $$

where $\delta^{74/70}\text{Ge}_i$ is the germanium isotopic composition for a given matrix fraction $f$ of composition $\delta^{74/70}\text{Ge}_{\text{matrix}}$ and a non-matrix fraction $(1-f)$ of a composition $\delta^{74/70}\text{Ge}_{\text{non-matrix}}$. In contrast with, to the [Ge] vs matrix mixing line, the mixing curve in the $\delta^{74/70}\text{Ge}$ vs. matrix diagram is a hyperbola because the calculation involves ratios. Then, by combining the two calculations we can model mixing in the $\delta^{74/70}\text{Ge}$ vs [Ge] diagram (Fig. 4a). Similar equations were used to calculate the mixing model presented in Figures 5.
<table><caption>**Table S3.** Matrix parameters and mean elemental, mass-dependent and nucleosynthetic isotopic compositions for chondrite groups, winonaites, main-group pallasites, Earth and Mars.</caption><thead><tr><th></th><th>CI</th><th>Ti</th><th>CV</th><th>CM</th><th>CO</th><th>CBa</th><th>CBb</th><th>H</th><th>L</th><th>LL</th><th>Earth</th><th>Mars</th><th>Winonaites</th><th>MGP</th><th>References</th></tr></thead><tbody><tr><td>Matrix (wt.%)</td><td>97</td><td>64</td><td>30</td><td>50</td><td>20</td><td>1</td><td>1</td><td>9</td><td>11</td><td>11</td><td></td><td></td><td></td><td></td><td>1,2</td></tr><tr><td>δ<sup>128</sup>Te (‰)</td><td>0.15</td><td>0.11</td><td>0.01</td><td>0.08</td><td>-0.03</td><td></td><td></td><td>0.09</td><td>0.44</td><td>0.17</td><td>0.07</td><td></td><td></td><td></td><td>1, 2</td></tr><tr><td>95% 2sd</td><td>0.04</td><td>0.01</td><td>0.02</td><td>0.02</td><td>0.03</td><td></td><td></td><td>0.05</td><td>0.34</td><td>0.08</td><td>0.02</td><td></td><td></td><td></td><td></td></tr><tr><td>δ<sup>66</sup>Zn (‰)</td><td>0.49</td><td>0.45</td><td>0.31</td><td>0.37</td><td>0.22</td><td>0.20</td><td></td><td>0.28</td><td>0.12</td><td>-0.14</td><td>0.24</td><td></td><td></td><td></td><td>3-5</td></tr><tr><td>95% 2sd</td><td>0.00</td><td>0.00</td><td>0.06</td><td>0.03</td><td>0.01</td><td></td><td></td><td>0.10</td><td>0.06</td><td>0.15</td><td>0.43</td><td></td><td></td><td></td><td></td></tr><tr><td>δ<sup>80</sup>Rb (‰)</td><td>0.17</td><td></td><td>0.03</td><td>0.06</td><td>0.01</td><td></td><td></td><td>-0.49</td><td>-0.19</td><td>-0.35</td><td>-0.17</td><td></td><td></td><td></td><td>6, 7</td></tr><tr><td>95% 2sd</td><td>0.06</td><td></td><td>0.06</td><td>0.05</td><td>0.04</td><td></td><td></td><td>0.03</td><td>0.03</td><td>0.03</td><td>0.01</td><td></td><td></td><td></td><td></td></tr><tr><td>δ<sup>40</sup>K (‰)</td><td>-0.16</td><td></td><td>-0.24</td><td>-0.19</td><td>-0.18</td><td></td><td></td><td>-0.63</td><td>-0.71</td><td>-0.58</td><td>-0.43</td><td></td><td></td><td></td><td>6, 9</td></tr><tr><td>95% 2sd</td><td>0.09</td><td></td><td>0.06</td><td>0.05</td><td>0.04</td><td></td><td></td><td>0.03</td><td>0.04</td><td>0.05</td><td>0.05</td><td></td><td></td><td></td><td></td></tr><tr><td>δ<sup>71</sup>Ga (‰)</td><td>-0.07</td><td></td><td>-0.43</td><td>-0.05</td><td>-0.18</td><td></td><td></td><td>-0.63</td><td>-0.66</td><td>-0.44</td><td>0.00</td><td></td><td></td><td></td><td>10, 11</td></tr><tr><td>95% 2sd</td><td>0.09</td><td></td><td>0.01</td><td>0.12</td><td>0.08</td><td></td><td></td><td>0.70</td><td>0.49</td><td>0.24</td><td>0.03</td><td></td><td></td><td></td><td></td></tr><tr><td>δ<sup>65</sup>Cu (‰)</td><td>0.05</td><td>-0.25</td><td>-1.49</td><td>-0.50</td><td>-0.86</td><td>-0.82</td><td>-2.04</td><td>-0.46</td><td>-0.08</td><td>0.08</td><td>0.03</td><td></td><td></td><td></td><td>12-14</td></tr><tr><td>95% 2sd</td><td>0.16</td><td>0.10</td><td>0.14</td><td>0.06</td><td>0.01</td><td>0.10</td><td>0.10</td><td>0.08</td><td>0.15</td><td>0.07</td><td>0.06</td><td></td><td></td><td></td><td></td></tr><tr><td>δ<sup>51</sup>V (‰)</td><td>-0.95</td><td></td><td>-1.15</td><td>-1.07</td><td>-1.22</td><td></td><td></td><td>-1.37</td><td>-1.25</td><td>-1.09</td><td></td><td></td><td></td><td></td><td>56</td></tr><tr><td>95% 2sd</td><td></td><td></td><td>0.16</td><td>0.06</td><td>0.03</td><td></td><td></td><td>0.04</td><td>0.03</td><td>0.11</td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Δ<sup>17</sup>O (‰)</td><td>0.31</td><td>-0.96</td><td>-3.52</td><td>-2.71</td><td>-4.44</td><td>-1.98</td><td>-2.19</td><td>0.69</td><td>1.04</td><td>1.08</td><td>0</td><td>0.32</td><td>-0.51</td><td>-0.20</td><td>15-18</td></tr><tr><td>95% 2sd</td><td>0.00</td><td>0.00</td><td>0.00</td><td>1.01</td><td>0.00</td><td>0.54</td><td>0.00</td><td>0.12</td><td>0.10</td><td>0.10</td><td>0</td><td>0.03</td><td>0.08</td><td>0.06</td><td></td></tr><tr><td>ε<sup>50</sup>Ti</td><td>1.85</td><td>2.76</td><td>3.49</td><td>3.01</td><td>3.77</td><td>2.04</td><td>0.00</td><td>-0.64</td><td>-0.63</td><td>-0.66</td><td>0</td><td>-0.45</td><td>-0.30</td><td>-1.37</td><td>19-25</td></tr><tr><td>95% 2sd</td><td>0.12</td><td>0.00</td><td>0.20</td><td>0.10</td><td>0.50</td><td>0.07</td><td>0.00</td><td>0.17</td><td>0.08</td><td>0.14</td><td>0</td><td>0.05</td><td>0.23</td><td>0.08</td><td></td></tr><tr><td>ε<sup>54</sup>Cr</td><td>1.56</td><td>1.29</td><td>0.87</td><td>1.02</td><td>0.62</td><td>1.09</td><td>0.87</td><td>-0.36</td><td>-0.40</td><td>-0.42</td><td>0</td><td>-0.16</td><td>-0.52</td><td>-0.34</td><td>19, 20, 24, 26-34</td></tr><tr><td>95% 2sd</td><td>0.06</td><td>0.19</td><td>0.07</td><td>0.08</td><td>0.10</td><td>0.06</td><td>0.00</td><td>0.08</td><td>0.10</td><td>0.07</td><td>0</td><td>0.03</td><td>0.06</td><td>0.04</td><td></td></tr><tr><td>ε<sup>64</sup>Ni</td><td>0.55</td><td></td><td>0.30</td><td>0.36</td><td>0.26</td><td>0.00</td><td>0.00</td><td>-0.18</td><td>-0.11</td><td>-0.19</td><td>0</td><td></td><td></td><td>-0.13</td><td>20, 23, 30, 35-37</td></tr><tr><td>95% 2sd</td><td>0.05</td><td></td><td>0.09</td><td>0.13</td><td>0.00</td><td>0.00</td><td>0.00</td><td>0.05</td><td>0.01</td><td>0.04</td><td>0</td><td></td><td></td><td>0.19</td><td></td></tr><tr><td>ε<sup>48</sup>Ca</td><td>2.11</td><td>2.91</td><td>3.53</td><td>2.90</td><td>3.87</td><td></td><td></td><td>-0.05</td><td>-0.33</td><td>-0.15</td><td>0</td><td>-0.11</td><td>-0.21</td><td></td><td>20, 21, 30, 35, 38-41</td></tr><tr><td>95% 2sd</td><td>0.13</td><td>0.05</td><td>0.55</td><td>0.77</td><td>0.56</td><td></td><td></td><td>0.39</td><td>0.65</td><td>0.39</td><td>0</td><td>0.16</td><td>0.09</td><td></td><td></td></tr><tr><td>ε<sup>92</sup>Mo</td><td>1.12</td><td></td><td>1.41</td><td>6.44</td><td>3.00</td><td>1.53</td><td></td><td>0.82</td><td>0.76</td><td>0.68</td><td>0.11</td><td>0.20</td><td>0.30</td><td>0.99</td><td>32, 35, 42-46</td></tr><tr><td>95% 2sd</td><td>0.59</td><td></td><td>0.27</td><td>0.39</td><td>1.17</td><td>0.08</td><td></td><td>0.63</td><td>0.51</td><td>0.52</td><td>0.52</td><td>0.53</td><td>0.28</td><td>0.32</td><td></td></tr><tr><td>μ<sup>96</sup>Zr</td><td>89</td><td></td><td>126</td><td>120</td><td>114</td><td>121</td><td>0</td><td>35</td><td>28</td><td>31</td><td>1</td><td></td><td>2</td><td></td><td>31</td></tr><tr><td>95% 2sd</td><td>18</td><td></td><td>8</td><td>6</td><td>8</td><td>18</td><td>0</td><td>3</td><td>5</td><td>7</td><td>2</td><td></td><td>9</td><td></td><td></td></tr><tr><td>ε<sup>100</sup>Ru</td><td>-0.24</td><td>-1.03</td><td>-0.93</td><td>-0.69</td><td>-0.92</td><td>-1.05</td><td></td><td>-0.26</td><td>-0.28</td><td>-0.29</td><td>0.05</td><td>-0.06</td><td>-0.47</td><td></td><td>30, 35, 47, 48</td></tr><tr><td>95% 2sd</td><td>0.13</td><td>0.13</td><td>0.12</td><td>0.13</td><td>0.13</td><td>0.13</td><td></td><td>0.14</td><td>0.13</td><td>0.03</td><td>0.01</td><td>0.01</td><td>0.16</td><td></td><td></td></tr><tr><td>μ<sup>66</sup>Zn</td><td>18</td><td>34</td><td>30</td><td>23</td><td>26</td><td></td><td></td><td>-18</td><td>-23</td><td>-17</td><td>-5</td><td></td><td></td><td></td><td>36, 49</td></tr><tr><td>95% 2sd</td><td>18</td><td>0</td><td>3</td><td>5</td><td>4</td><td></td><td></td><td>5</td><td>24</td><td>34</td><td>2</td><td></td><td></td><td></td><td></td></tr><tr><td>ε<sup>40</sup>K</td><td>2.37</td><td></td><td>1.65</td><td>1.03</td><td>0.85</td><td></td><td></td><td>-0.05</td><td>0.56</td><td>0.60</td><td>0.10</td><td>2.40</td><td></td><td></td><td>6-9</td></tr><tr><td>95% 2sd</td><td>0.30</td><td></td><td>0.50</td><td>0.45</td><td>0.85</td><td></td><td></td><td>0.65</td><td>0.38</td><td>0.43</td><td>0.30</td><td>0.90</td><td></td><td></td><td></td></tr><tr><td>μ<sup>30</sup>Si</td><td>30.2</td><td>27.0</td><td>11.5</td><td>16.3</td><td>19.3</td><td></td><td></td><td></td><td>7.4</td><td>7.6</td><td>0.19</td><td>-6.8</td><td></td><td></td><td>57</td></tr><tr><td>95% 2sd</td><td>3.8</td><td>7.4</td><td>3.1</td><td>1.1</td><td>1.4</td><td></td><td></td><td></td><td>4.3</td><td>3.0</td><td>0.73</td><td>1.8</td><td></td><td></td><td></td></tr></tbody></table>
<table><thead><tr><th></th><th>CI</th><th>Tl</th><th>CV</th><th>CM</th><th>CO</th><th>CBa</th><th>CBb</th><th>H</th><th>L</th><th>LL</th><th>Earth</th><th>Mars</th><th>Winonaites</th><th>MGP</th><th>References</th></tr></thead><tbody><tr><td>Mg (mg/g)</td><td>95.4</td><td>109</td><td>148</td><td>117</td><td>144</td><td></td><td></td><td>140</td><td>149</td><td>153</td><td></td><td></td><td></td><td></td><td></td><td>50-55</td></tr><tr><td>Al (mg/g)</td><td>8.4</td><td>10.1</td><td>17.2</td><td>11.6</td><td>14.3</td><td></td><td></td><td>11.3</td><td>12.2</td><td>11.9</td><td></td><td></td><td></td><td></td><td></td><td>50-54</td></tr><tr><td>Si (mg/g)</td><td>107</td><td>116</td><td>160</td><td>130</td><td>160</td><td></td><td></td><td>169</td><td>185</td><td>189</td><td></td><td></td><td></td><td></td><td></td><td>50-55</td></tr><tr><td>Fe (mg/g)</td><td>185</td><td>189</td><td>236</td><td>212</td><td>247</td><td></td><td></td><td>275</td><td>215</td><td>185</td><td></td><td></td><td></td><td></td><td></td><td>50-55</td></tr><tr><td>V (µg/g)</td><td>54.6</td><td>57</td><td>98</td><td>74</td><td>92</td><td></td><td></td><td>74</td><td>77</td><td>75</td><td></td><td></td><td></td><td></td><td></td><td>50-54</td></tr><tr><td>Zn (µg/g)</td><td>309</td><td>216</td><td>107</td><td>180</td><td>100</td><td></td><td></td><td>47</td><td>50</td><td>46</td><td></td><td></td><td></td><td></td><td></td><td>50-54</td></tr><tr><td>Ga (µg/g)</td><td>9.62</td><td>8</td><td>5.9</td><td>7.5</td><td>7.1</td><td></td><td></td><td>6</td><td>5.7</td><td>5</td><td></td><td></td><td></td><td></td><td></td><td>50-54</td></tr><tr><td>Ge (µg/g)</td><td>32.6</td><td>25</td><td>17</td><td>23</td><td>21</td><td></td><td></td><td>13</td><td>10</td><td>9</td><td></td><td></td><td></td><td></td><td></td><td>50-54</td></tr><tr><td>Mg/Si</td><td>0.89</td><td>0.94</td><td>0.93</td><td>0.90</td><td>0.90</td><td></td><td></td><td>0.83</td><td>0.81</td><td>0.81</td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Al/Si</td><td>0.079</td><td>0.087</td><td>0.108</td><td>0.089</td><td>0.089</td><td></td><td></td><td>0.067</td><td>0.066</td><td>0.063</td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Fe/Si</td><td>1.73</td><td>1.63</td><td>1.48</td><td>1.63</td><td>1.54</td><td></td><td></td><td>1.63</td><td>1.16</td><td>0.98</td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Zn/Si *10<sup>4</sup></td><td>2.89</td><td>1.86</td><td>0.67</td><td>1.38</td><td>0.63</td><td></td><td></td><td>0.28</td><td>0.27</td><td>0.24</td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Te/Si *10<sup>4</sup></td><td>0.021</td><td>0.012</td><td>0.006</td><td>0.011</td><td>0.006</td><td></td><td></td><td>0.003</td><td>0.003</td><td>0.003</td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Al/Ge</td><td>257</td><td>404</td><td>1011</td><td>504</td><td>680</td><td></td><td></td><td>869</td><td>1220</td><td>1322</td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>V/Ge</td><td>1.67</td><td>2.28</td><td>5.76</td><td>3.22</td><td>4.38</td><td></td><td></td><td>5.69</td><td>7.70</td><td>8.33</td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Fe/Ge</td><td>5675</td><td>7560</td><td>16714</td><td>9217</td><td>11762</td><td></td><td></td><td>21154</td><td>21500</td><td>20556</td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Ga/Ge</td><td>0.29</td><td>0.32</td><td>0.338</td><td>0.326</td><td>0.338</td><td></td><td></td><td>0.462</td><td>0.570</td><td>0.556</td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Zn/Ge</td><td>9.48</td><td>8.64</td><td>6.29</td><td>7.83</td><td>4.76</td><td></td><td></td><td>3.62</td><td>5.00</td><td>5.11</td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Te/Ge</td><td>0.070</td><td>0.054</td><td>0.060</td><td>0.061</td><td>0.043</td><td></td><td></td><td>0.040</td><td>0.048</td><td>0.054</td><td></td><td></td><td></td><td></td><td></td><td></td></tr></tbody></table>

**References:** (1) Hellmann et al. (2021), (2) Hellmann et al. (2020), (3) Luck et al. (2005), (4) Moynier et al. (2007), (5) Pringle et al. (2017), (6) Nie et al. (2021), (7) Nie et al. (2023), (8) Koefoed et al. (2023), (9) Ku and Jacobsen (2020), (10) Kato and Moynier (2017), (11) Kato et al. (2017), (12) Barrat et al. (2012), (13) Luck et al. (2003), (14) Sossi et al. (2015), (15) Clayton and Mayeda (1999), (16) Clayton et al. 1991), (17) Greenwood et al. (2020), (18) Greenwood et al. (2017), (19) Burkhardt et al. (2019), (20) Burkhardt et al. (2017), (21) Dauphas et al. (2014), (22) Rüfenacht et al. (2023), (23) Trinquier et al. (2007), (24) Wang et al. (2021), (25) Yokoyama et al. (2019), (26) Göpel et al. (2015), (27) Kruijer et al. (2020), (28) Petitat et al. (2011), (29) Qin et al. (2010), (30) Qin and Carlson (2016), (31) Render et al. (2022), (32) Render et al. (2017), (33) Tang et al. (2014), (34) Trinquier et al. (2009), (35) Dauphas (2017), (36) Steele et al. (2011), (37) Righter (2019), (38) Burkhardt et al. (2021), (39) Chen et al. (2011), (40) Schiller et al. (2018), (41) Schiller et al. (2015), (42) Budde et al. (2016), (43) Budde et al. (2019), (44) Burkhardt et al. (2014), (45) Burkhardt et al. (2011), (46) Warren (2011), (47) Fischer-Gödde et al. (2015), (48) Fischer-Gödde and Kleine (2017), (49) Martins et al. (2023), (50) Alexander (2019a), (51) Alexander (2019b), (52) Braukmüller et al. (2019), (53) Braukmüller et al. (2018), (54) Lodders et al. (2009), (55) Palme et al. (2015), (56) Nielsen et al. (2019), (57) Onyett et al. (2023).
<table><caption>**Table S4.** Elemental contents and nucleosynthetic anomalies in CC and NC chondrules, in CC and NC matrices used to model mixing lines. Estimated matrix fractions in NC are given as ranges according to Figure 4 (see text for details). Elemental composition in matrix fraction is supposed to be similar to CI chondrites.</caption><thead><tr><th></th><th>Chondrule CC</th><th>Chondrule NC</th><th>Matrix CC (CI)</th><th>Matrix NCC</th><th>References</th><th>Comments</th></tr></thead><tbody><tr><td>Ti (ppm)</td><td>1435</td><td>1326</td><td>420</td><td></td><td>53, 58, 59</td><td>Mean from the chondrule database (56, 57) and CI composition from (58)</td></tr><tr><td>95% 2SD</td><td>104</td><td>197</td><td>13</td><td></td><td></td><td></td></tr><tr><td>ε<sup>50</sup>Ti</td><td>4.15</td><td>-0.81</td><td>1.88</td><td>-3 to +1</td><td>34, 60</td><td>CC: Weighted average of sequentially digested fractions 3d, 3e, 3f, and 4 from Orgueil. This represents the chondrules plus the refractory inclusions, pure chondrules have a ε50Ti=2.5. NC: chondrules from (34)</td></tr><tr><td>95% 2SD</td><td>0.14</td><td>0.12</td><td>0.12</td><td></td><td></td><td></td></tr><tr><td>Cr (ppm)</td><td>3200</td><td>3811</td><td>2620</td><td></td><td>34, 58-60</td><td>NC compositions are averages from the chondrule database (56, 57)</td></tr><tr><td>95% 2SD</td><td>129</td><td>127</td><td>100</td><td></td><td></td><td></td></tr><tr><td>ε<sup>54</sup>Cr</td><td>0.57</td><td>-0.45</td><td>1.56</td><td>0 to +2</td><td>23, 60</td><td>CC: Table A2 from (58) and after the compilation of (35)<br>NC: average composition of separated chondrules from (23)</td></tr><tr><td>95% 2SD</td><td>0.14</td><td>0.13</td><td>0.06</td><td></td><td></td><td></td></tr><tr><td>Ni (ppm)</td><td>6091</td><td>3463</td><td>11665</td><td></td><td>53, 58, 59</td><td>Mean from the chondrule database (56, 57).</td></tr><tr><td>95% 2SD</td><td>642</td><td>454</td><td>460</td><td></td><td></td><td></td></tr><tr><td>ε<sup>64</sup>Ni</td><td>0.14</td><td>-0.22</td><td>0.55</td><td>-0.22 to +0.2</td><td></td><td>Matrix (CI,) (33). Chondrule compositions obtained by linear regression to 0% matrix in the NC and CC groups individually.</td></tr><tr><td>95% 2SD</td><td>0.1</td><td>0.1</td><td>0.05</td><td></td><td></td><td></td></tr><tr><td>Ca (ppm)</td><td>10000</td><td>9800</td><td>8976</td><td></td><td>53, 58, 59</td><td>Mean from the chondrule database (56, 57).</td></tr><tr><td>95% 2SD</td><td>2500</td><td>2500</td><td>200</td><td></td><td></td><td></td></tr><tr><td>ε<sup>48</sup>Ca</td><td>4.49</td><td>0.01</td><td>2.11</td><td>-2 to +0.3</td><td>39</td><td>Matrix (CI), (39). Chondrule compositions obtained by linear regression to 0% matrix in the NC and CC groups individually.</td></tr><tr><td>95% 2SD</td><td>0.3</td><td>0.3</td><td>0.05</td><td></td><td></td><td></td></tr></tbody></table>

**References.** As in Table S3, and (58) Hezel, et al., (2018a), (59) Hezel, et al. (2018b), (60) Hellmann et al., (2023).
3. Supplementary Figures

<figure><img src="image_6.png" /><figcaption>Figure S1</figcaption></figure>

**Figure S1** - Variations of Ge contents among CC and OC chondrites versus refractory major (Al, Mg, Fe) and trace (V) elements, and volatile trace elements (Te, Zn) normalized to Si and Cl chondrites, extending the trend of Alexander (2019a) to both OC and CC chondrites. Ge behaves independently from lithophile refractory elements (Al, Mg, V). The Ge-Fe negative trend in CC is below the 1:1 line, similar to lithophile volatiles (e.g., Na) (Alexander 2019a), reflecting Ge and Fe-Ni metal loss from the “chondrule component” (Alexander 2019a). However, Ge variations in both chondrite groups show parallel volatile Te and Zn variations, slightly above the 1:1 line for Ge-Te and Ge-Zn, illustrating that Ge variations are primarily controlled by volatility, and that the volatility of Ge approaches that of Te or Zn (Alexander 2019a).
<figure><img src="image_7.png" /><figcaption>Figure S2</figcaption></figure>

**Figure S2** - Variations of δ<sup>74</sup>Ge values CC and OC chondrites versus refractory major (Al, Fe) and trace elements (V), a moderately volatile trace element (Ga), and volatile trace elements (Zn, Te) normalized to Ge. δ<sup>74</sup>Ge values are negatively correlated with refractory elements, whether they are lithophile or siderophile, are indicative of δ<sup>74</sup>Ge-[Ge] correlation (see Figure 2 main text). The δ<sup>74</sup>Ge is positively correlated with Z, Te volatile elements. The intermediately volatile element Ga shows a vertical trend that is similar to Cu (not reported here). This behavior from refractory to volatile elements highlights the effect of volatility on Ge.
<figure><img src="image_8.png" /><figcaption>Figure S3</figcaption></figure>

**Figure S3.** Variations of the nucleosynthetic anomalies of ε⁴⁰K, ε⁶⁶Zn, ε⁹²Mo, ε¹⁰⁰Ru, and ε⁹⁶Zr vs. δ⁷⁴/⁷⁰Ge, and Δ¹⁷O vs. δ⁷⁴/⁷⁰Ge. Symbols are as in Figures 1 to 3. Data and references for nucleosynthetic anomalies are reported in Table S4.
4 - SI - References

Alexander, C. M. D., 2019a. Quantitative models for the elemental and isotopic fractionations in chondrites: The carbonaceous chondrites. Geochim. Cosmochim. Acta 254, 277-309.

Alexander, C. M. D., 2019b. Quantitative models for the elemental and isotopic fractionations in the chondrites: The non-carbonaceous chondrites. Geochim. Cosmochim. Acta 254, 246-276.

Barrat, J. A., Zanda, B., Moynier, F., Bollinger, C., Liorzou, C., Bayon, G., 2012. Geochemistry of CI chondrites: Major and trace elements, and Cu and Zn isotopes. Geochim. Cosmochim. Acta 83, 79-92.

Braukmüller, N., Wombacher, F., Funk, C., Münker, C., 2019. Earth's volatile element depletion pattern inherited from a carbonaceous chondrite-like source. Nature Geosci. 12(7), 564-568.

Braukmüller, N., Wombacher, F., Hezel, D. C., Escoube, R., Münker, C., 2018. The chemical composition of carbonaceous chondrites: Implications for volatile element depletion, complementarity and alteration. Geochim. Cosmochim. Acta 239, 17-48.

Budde, G., Burkhardt, C., Kleine, T., 2019. Molybdenum isotopic evidence for the late accretion of outer Solar System material to Earth. Nature Astron. 3(8), 736-741.

Budde, G., Burkhardt, C., Brennecka, G. A., Fischer-Gödde, M., Kruijer, T. S., Kleine, T., 2016. Molybdenum isotopic evidence for the origin of chondrules and a distinct genetic heritage of carbonaceous and non-carbonaceous meteorites. Earth Planet. Sci. Lett. 454, 293-303.

Burkhardt, C., Dauphas, N., Hans, U., Bourdon, B., Kleine, T., 2019. Elemental and isotopic variability in solar system materials by mixing and processing of primordial disk reservoirs. Geochim. Cosmochim. Acta 261, 145-170.

Burkhardt, C., Dauphas, N., Tang, H., Fischer-Gödde, M., Qin, L., Chen, J. H., ... Papanastassiou, D. A., 2017. In search of the Earth-forming reservoir: Mineralogical, chemical, and isotopic characterizations of the ungrouped achondrite NWA 5363/NWA 5400 and selected chondrites. Meteorit. Planet. Sci. 52(5), 807-826.

Burkhardt, C., Hin, R. C., Kleine, T., Bourdon, B., 2014. Evidence for Mo isotope fractionation in the solar nebula and during planetary differentiation. Earth Planet. Sci. Lett. 391, 201-211.

Burkhardt, C., Kleine, T., Oberli, F., Pack, A., Bourdon, B., Wieler, R., 2011. Molybdenum isotope anomalies in meteorites: Constraints on solar nebula evolution and origin of the Earth. Earth Planet. Sci. Lett. 312 (3-4), 390-400.

Burkhardt, C., Spitzer, F., Morbidelli, A., Budde, G., Render, J. H., Kruijer, T. S., Kleine, T., 2021. Terrestrial planet formation from lost inner solar system material. Science Adv. 7(52), eabj7601.

Carignan, J., Hild, P., Mevelle, G., Morel, J., Yeghicheyan, D., 2001. Routine Analyses of Trace Elements in Geological Samples using Flow Injection and Low Pressure On-Line Liquid Chromatography Coupled to ICP-MS: A Study of Geochemical Reference Materials BR, DR-N, UB-N, AN-G and GH. Geostand. Newslett. 25, 187-198.

Chen, H. W., Lee, T., Lee, D. C., J-S. Shen, J., Chen, J. C., 2011. 48Ca heterogeneity in differentiated meteorites. The Astrophys. Journ. Lett. 743(1), L23.

Clayton, R. N., Mayeda, T. K., 1999. Oxygen isotope studies of carbonaceous chondrites. Geochim. Cosmochim. Acta 63(13-14), 2089-2104.

Clayton, R. N., Mayeda, T. K., Goswami, J. N., Olsen, E. J., 1991. Oxygen isotope studies of ordinary chondrites. Geochimica et Cosmochimica Acta 55(8), 2317-2337.

Dauphas, N., 2017. The isotopic nature of the Earth's accreting material through time. Nature 541(7638), 521-524.

Dauphas, N., Chen, J. H., Zhang, J., Papanastassiou, D. A., Davis, A. M., Travaglio, C., 2014. Calcium-48 isotopic anomalies in bulk chondrites and achondrites: Evidence for a uniform isotopic reservoir in the inner protoplanetary disk. Earth Planet. Sci. Lett. 407, 96-108.

Escoube, R., Rouxel, O. J., Luais, B., Ponzevera, E., Donard, O. F. X., 2012. An Intercomparison Study
of the Germanium Isotope Composition of Geological Reference Materials. Geost. Geoanal. Res. 36, 149-159.

Florin, G., Luais, B., Rushmer, T., Alard, O., 2020. Influence of redox processes on the germanium isotopic composition of ordinary chondrites. Geochim. Cosmochim. Acta 269, 270-291.

Fischer-Gödde, M., Kleine, T., 2017. Ruthenium isotopic evidence for an inner Solar System origin of the late veneer. Nature 541(7638), 525-527.

Fischer-Gödde, M., Burkhardt, C., Kruijer, T. S., Kleine, T., 2015. Ru isotope heterogeneity in the solar protoplanetary disk. Geochim. Cosmochim. Acta 168, 151-171.

Göpel, C., Birck, J. L., Galy, A., Barrat, J. A., Zanda, B., 2015. Mn–Cr systematics in primitive meteorites: Insights from mineral separation and partial dissolution. Geochim. Cosmochim. Acta 156, 1-24.

Greenwood, R. C., Burbine, T. H., Franchi, I. A., 2020. Linking asteroids and meteorites to the primordial planetesimal population. Geochim. Cosmochim. Acta 277, 377-406.

Greenwood, R. C., Burbine, T. H., Miller, M. F., Franchi, I. A., 2017. Melting and differentiation of early-formed asteroids: The perspective from high precision oxygen isotope studies. Geochemistry 77(1), 1-43.

Hellmann, J.L., Hopp, T., Burkhardt, C., Becker, H., Fischer-Gödde, M., Kleine, T., 2021. Tellurium isotope cosmochemistry: Implications for volatile fractionation in chondrite parent bodies and origin of the late veneer. Geochim. Cosmochim. Acta 309, 313-328.

Hellmann, J.L., Hopp, T., Burkhardt, C., Kleine, T., 2020. Origin of volatile element depletion among carbonaceous chondrites. Earth Planet. Sci. Lett. 549, 116508.

Hellmann, J. L., Schneider, J. M., Wölfer, E., Drążkowska, J., Jansen, C. A., Hopp, T., ... Kleine, T., 2023. Origin of isotopic diversity among carbonaceous chondrites. The Astrophys. Journ. Lett. 946(2), L34.

Hezel, D.C., Bland, P.A., Palme, H., Jacquet, E., Bigolski, J., 2018a. Composition of chondrules and matrix and their complementary relationship in chondrites, Chondrules. pp. 91-121.

Hezel, D.C., Harak, M., Libourel, G., 2018b. What we know about elemental bulk chondrule and matrix compositions: Presenting the ChondriteDB Database. Geochem. 78(1), 1-14.

Kato, C., Moynier, F., 2017. Gallium isotopic evidence for extensive volatile loss from the Moon during its formation. Science Adv. 3(7), e1700571

Kato, C., Moynier, F., Foriel, J., Teng, F. Z., Puchtel, I. S., 2017. The gallium isotopic composition of the bulk silicate Earth. Chem. Geol. 448, 164-172.

Koefoed, P., Barrat, J. A., Pravdivtseva, O., Alexander, C. M. D., Lodders, K., Ogliore, R., Wang, K., 2023. The potassium isotopic composition of CI chondrites and the origin of isotopic variations among primitive planetary bodies. Geochim. Cosmochim. Acta 358, 49-60.

Kruijer, T. S., Borg, L. E., Wimpenny, J., Sio, C. K., 2020. Onset of magma ocean solidification on Mars inferred from Mn-Cr chronometry. Earth Planet. Sci. Lett. 542, 116315.

Ku, Y., & Jacobsen, S. B., 2020. Potassium isotope anomalies in meteorites inherited from the protosolar molecular cloud. Science Adv. 6(41), eabd0511.

Lodders, K., Palme, H., Gail, H. P., 2009. 4.4 Abundances of the elements in the Solar System. In Solar System, J. E. Trümper, Ed. (Springer-Verlag Berlin Heidelberg), 712-770.

Luais, B., 2007. Isotopic fractionation of germanium in iron meteorites: Significance for nebular condensation, core formation and impact processes. Earth Planet. Sci. Lett. 262(1), 21-36.

Luais, B., 2012. Germanium chemistry and MC-ICPMS isotopic measurements of Fe–Ni, Zn alloys and silicate matrices: Insights into deep Earth processes. Chem. Geol. 334, 295-311.

Luais B., Le Carlier de Veslud C., Géraud Y., Gauthier-Lafaye F., 2009. Comparative behavior of Sr, Nd and Hf isotopic systems during fluid-related deformation at middle crust levels. Geochim. Cosmochim. Acta 73, 2961-2977.

Luck, J. M., Othman, D. B., Barrat, J. A., Albarède, F., 2003. Coupled 63Cu and 16O excesses in chondrites. Geochim. Cosmochim. Acta 67(1), 143-151.

Martins, R., Kuthning, S., Coles, B. J., Kreissig, K., Rehkämper, M., 2023. Nucleosynthetic isotope
anomalies of zinc in meteorites constrain the origin of Earth's volatiles. Science 379(6630), 369-372.

Moynier, F., Blichert-Toft, J., Telouk, P., Luck, J. M., Albarède, F., 2007. Comparative stable isotope geochemistry of Ni, Cu, Zn, and Fe in chondrites and iron meteorites. Geochim. Cosmochim. Acta 71(17), 4365-4379.

Nie, N. X., Chen, X. Y., Hopp, T., Hu, J. Y., Zhang, Z. J., Teng, F. Z., ... Dauphas, N., 2021. Imprint of chondrule formation on the K and Rb isotopic compositions of carbonaceous meteorites. Science Adv. 7(49), eabl3929.

Nie, N. X., Chen, X. Y., Zhang, Z. J., Hu, J. Y., Liu, W., Tissot, F. L., ... Dauphas, N., 2023. Rubidium and potassium isotopic variations in chondrites and Mars: Accretion signatures and planetary overprints. Geochim. Cosmochim. Acta 344, 207-229.78.

Nielsen, S.G., Auro, M., Righter, K., Davis, D., Prytulak, J., Wu, F., Owens, J.D., 2019. Nucleosynthetic vanadium isotope heterogeneity of the early solar system recorded in chondritic meteorites. Earth Planet. Sci. Lett. 505, 131-140.

Onyett, I.J., Schiller, M., Makhatadze, G.V., Deng, Z., Johansen, A., Bizzarro, M., 2023. Silicon isotope constraints on terrestrial planet accretion. Nature 619(7970), 539-544.

Palme, H., Hezel, D. C., Ebel, D. S., 2015. The origin of chondrules: Constraints from matrix composition and matrix-chondrule complementarity. Earth Planet. Sci. Lett. 411, 11-19.

Petitat, M., Birck, J. L., Luu, T. H., Gounelle, M., 2011. The chromium isotopic composition of the ungrouped carbonaceous chondrite Tagish Lake. The Astrophys. Journ. 736(1), 23.

Pringle, E. A., Moynier, F., Beck, P., Paniello, R., Hezel, D. C., 2017. The origin of volatile element depletion in early solar system material: Clues from Zn isotopes in chondrules. Earth Planet. Sci. Lett. 468, 62-71.

Qi, H.-W., Rouxel, O., Hu, R.-Z., Bi, X.-W., Wen, H.-J., 2011. Germanium isotopic systematics in Ger- rich coal from the Lincang Ge deposit, Yunnan, Southwestern China. Chem. Geol.

Qin, L., Carlson, R. W., 2016. Nucleosynthetic isotope anomalies and their cosmochemical significance. Geochem. J. 50(1), 43-65.

Qin, L., Alexander, C. M. D., Carlson, R. W., Horan, M. F., Yokoyama, T., 2010. Contributors to chromium isotope variation of meteorites. Geochim. Cosmochim. Acta 74(3), 1122-1145.

Render, J., Brennecka, G. A., Burkhardt, C., Kleine, T., 2022. Solar System evolution and terrestrial planet accretion determined by Zr isotopic signatures of meteorites. Earth Planet. Sci. Lett. 595, 1177-1189.

Render, J., Fischer-Gödde, M., Burkhardt, C., Kleine, T., 2017. The cosmic molybdenum-neodymium isotope correlation and the building material of the Earth. Geochem. Perspect. Lett. 3, 170-178.

Righter, K., 2019. Volatile element depletion of the Moon—The roles of precursors, post-impact disk dynamics, and core formation. Science Adv. 5(1), eaau7658.

Rüfenacht, M., Morino, P., Lai, Y. J., Fehr, M. A., Haba, M. K., Schönbächler, M., 2023. Genetic relationships of solar system bodies based on their nucleosynthetic Ti isotope compositions and sub-structures of the solar protoplanetary disk. Geochim. Cosmochim. Acta 355, 110-125.

Schiller, M., Bizzarro, M., Fernandes, V. A., 2018. Isotopic evolution of the protoplanetary disk and the building blocks of Earth and the Moon. Nature 555(7697), 507-510.

Schiller, M., Paton, C., Bizzarro, M., 2015. Evidence for nucleosynthetic enrichment of the protosolar molecular cloud core by multiple supernova events. Geochim. Cosmochim. Acta 149, 88-102.

Sossi, P. A., Halverson, G. P., Nebel, O., Eggins, S. M., 2015. Combined separation of Cu, Fe and Zn from rock matrices and improved analytical protocols for stable isotope determination. Geostand. Geoanal. Res. 39(2), 129-149.

Steele, R. C., Elliott, T., Coath, C. D., Regelous, M., 2011. Confirmation of mass-independent Ni isotopic variability in iron meteorites. Geochim. Cosmochim. Acta 75(24), 7906-7925.
Tang, H., Dauphas, N., 2014. 60Fe-60Ni chronology of core formation in Mars. Earth Planet. Sci. Lett. 390, 264-274.

Trinquier, A., Birck, J. L., Allegre, C. J., 2007. Widespread 54Cr heterogeneity in the inner solar system. The Astrophys. Journ. 655(2), 1179.

Trinquier, A., Elliott, T., Ulfbeck, D., Coath, C., Krot, A. N., Bizzarro, M., 2009. Origin of nucleosynthetic isotope heterogeneity in the solar protoplanetary disk. Science 324(5925), 374-376.

Wang, S. J., Wang, W., Zhu, J. M., Wu, Z., Liu, J., Han, G., ... Li, W., 2021. Nickel isotopic evidence for late-stage accretion of Mercury-like differentiated planetary embryos. Nat. Commun. 12(1), 294.

Warren, P. H., 2011. Stable-isotopic anomalies and the accretionary assemblage of the Earth and Mars: A subordinate role for carbonaceous chondrites. Earth Planet. Sci. Lett. 311(1-2), 93-100.

Yokoyama, T., Nagai, Y., Fukai, R., Hirata, T., 2019. Origin and evolution of distinct molybdenum isotopic variabilities within carbonaceous and noncarbonaceous reservoirs. The Astrophys. Journ. 883(1), 62