The short-lived 26 Al radionuclide is thought to have been admixed into the initially 26 Al-poor protosolar molecular cloud before or contemporaneously with its collapse. Bulk inner Solar System reservoirs record positively correlated variability in mass-independent 54 Cr and 26 Mg*, the decay product of 26 Al. This correlation is interpreted as reflecting progressive thermal processing of infalling 26 Al-rich molecular cloud material in the inner Solar System. The thermally unprocessed molecular cloud matter reflecting the nucleosynthetic makeup of the molecular cloud before the last addition of stellar-derived 26 Al has not been identified yet but may be preserved in planetesimals that accreted in the outer Solar System. We show that metal-rich carbonaceous chondrites and their components have a unique isotopic signature extending from an inner Solar System composition toward a 26 Mg*-depleted and 54 Cr-enriched component. This composition is consistent with that expected for thermally unprocessed primordial molecular cloud material before its pollution by stellar-derived 26 Al. The 26 Mg* and 54 Cr compositions of bulk metal-rich chondrites require significant amounts (25-50%) of primordial molecular cloud matter in their precursor material. Given that such high fractions of primordial molecular cloud material are expected to survive only in the outer Solar System, we infer that, similarly to cometary bodies, metal-rich carbonaceous chondrites are samples of planetesimals that accreted beyond the orbits of the gas giants. The lack of evidence for this material in other chondrite groups requires isolation from the outer Solar System, possibly by the opening of disk gaps from the early formation of gas giants. molecular cloud | outer Solar System | metal-rich chondrites | isotopes | chondrite accretion regions L ow-mass stars like our Sun form by the gravitational collapse of the densest parts of molecular clouds comprising stellarderived dust and gas. Collapsing clouds swiftly evolve into deeply embedded protostars that rapidly accrete material from their surrounding envelopes via a protoplanetary disk (1), in which planetesimals and planetary embryos form over timescales of several million years (2). Chondritic meteorites (chondrites) are fragments of early-formed planetesimals that avoided melting and differentiation and, therefore, provide a record of the earliest evolutionary stages of the Sun and its protoplanetary disk. Most chondrites contain calcium−aluminum-rich inclusions (CAIs) and chondrules, which formed by high-temperature processes that included evaporation, condensation, and melting during short-lived heating events (3). CAIs represent the oldest dated solids and, thus, define the age of the Solar System at 4,567.3 ± 0.16 Ma (4). It is inferred that CAIs formed near the proto-Sun during a brief time interval (<0

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Mass spectrometry imaging is a field that promises to become a mainstream bioanalysis technology by allowing the combination of single-cell imaging and subcellular quantitative analysis. The frontier of single-cell imaging has advanced to the point where it is now possible to compare the chemical contents of individual organelles in terms of raw or normalized ion signal. However, to realize the full potential of this technology, it is necessary to move beyond this concept of relative quantification. Here we present a nanoSIMS imaging method that directly measures the absolute concentration of an organelle-associated, isotopically labeled, pro-drug directly from a mass spectrometry image. This is validated with a recently developed nanoelectrochemistry method for single organelles. We establish a limit of detection based on the number of isotopic labels used and the volume of the organelle of interest, also offering this calculation as a web application. This approach allows subcellular quantification of drugs and metabolites, an overarching and previously unmet goal in cell science and pharmaceutical development.

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We describe a procedure to determine precise and accurate elemental abundance by means of quantitative imaging using secondary ion mass spectrometry (on images covering $10 Â 10 mm 2 ) applied to natural Insoluble Organic Matter (IOM). Dynamic SIMS conditions are reached for a 16 keV Cs + fluence of >2.0 Â 10 17 Cs + cm À2 implanted at the surface of the IOM. Once the sample surface is saturated in cesium, steady-state implantation and sputtering yield are reached: constant secondary ion count rates are then observed. Two calibrations of the nitrogen abundance are presented. The nitrogen abundance is expressed either as [N] or N/C atomic ratio calibrated by means of 12 C 14 N À / 12 C À or 12 C 14 N À / 12 C 2 À ionic ratios respectively. The 12 C 14 N À / 12 C À uncertainty is always larger than the uncertainty of 12 C 14 N À / 12 C 2 À. At a smaller scale inside an image ($1 Â 1 mm 2 ), a little larger than the primary beam size, processes induced by topographic irregularity of the IOM powder result in a variation of the 12 C 14 N À , 12 C 2 À and 12 C À count rates and increase the variability of the ionic ratios. The chemical contrast produced by a rough sample surface exposed to the Cs + rastering is evaluated with a scratched epoxy resin for 12 C 14 N À / 12 C À and 12 C 14 N À / 12 C 2 À elemental ratios. Owing to similarities in emission parameters, the determination of the N/C ratio in rough organic surfaces is improved by using 12 C 14 N À / 12 C 2 À instead of 12 C 14 N À / 12 C À .