The isotopic composition of meteorites reveals a fundamental dichotomy between non-carbonaceous (NC) and carbonaceous (CC) meteorites. However, the origin of this dichotomy—whether it results from processes within the solar protoplanetary disk or is an inherited heterogeneity from the solar system's parental molecular cloud—is not known. To evaluate the origin of the NC–CC dichotomy, we report Ni isotopic data for a comprehensive set of iron meteorites, with a special focus on groups that have not been analyzed before and belong to the CC group. The new Ni isotopic data demonstrate that the NC–CC dichotomy extends to Ni isotopes, and that CC meteorites are characterized by a ubiquitous 58Ni excess over NC meteorites. These data combined with prior observations reveal that, in general, the CC reservoir is characterized by an excess in nuclides produced in neutron-rich stellar environments, such as 50Ti, 54Cr, 58Ni, and r-process Mo isotopes. Because the NC–CC dichotomy exists for refractory (Ti, Mo) and non-refractory (Ni, Cr) elements, and is only evident for nuclides produced in specific, neutron-rich stellar environments, it neither reflects thermal processing of presolar carriers in the disk, nor the heterogeneous distribution of isotopically anomalous Ca–Al-rich inclusions (CAI). Instead, the NC–CC dichotomy reflects the distinct isotopic composition of later infalling material from the solar system's parental molecular cloud, which affected the inner and outer regions of the disk differently. Simple models of the infall process by themselves can support either infall of increasingly NC-like material onto an initially CC-like disk, or infall of increasingly CC-like material in the absence of disk evolution by spreading. However, provided that CAIs formed close to the Sun, followed by rapid outward transport, their isotopic composition likely reflects that of the earliest infalling material, implying that the composition of the inner disk (i.e., the NC reservoir) is dominated by later infalling material, whereas the outer disk (i.e., the CC reservoir) preserved a compositional signature of the earliest disk. The isotopic difference between the inner and outer disk was likely maintained through the rapid formation of Jupiter, which prevented complete homogenization between material from inside (NC reservoir) and outside (CC reservoir) its orbit.
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