Extreme deuterium enrichment of organic radicals in the Orgueil meteorite: Revisiting the interstellar interpretation?

The insoluble organic matter of the carbonaceous meteorites contains radicals having a polyaromatic structure and a heterogeneous distribution. By using Hyperfine Sublevel Correlation spectroscopy (HYSCORE) in pulsed Electron Paramagnetic Resonance (pulsed-EPR), whereby nuclear frequencies of magnetic nuclei and their hyperfine interaction with electron spin of radicals are detected with high resolution, the radicals are shown to be considerably enriched in deuterium in the Orgueil meteorite, with a D/H ratio of 1.5 +/- 0.5 x 10(-2). These radicals hold 3.6 +/- 1.2 x 10(-3) H relative to total organic H. Analysis of hydrogen and deuterium hyperfine interactions indicates that the deuterium atoms are localized in the benzylic position, on aliphatic carbons bonded to aromatic radical moieties. This type of C-H bond exhibits one of the smallest bond energy, reinforcing the recent finding that the lower the C-H bond energy the higher the deuterium-enrichment (Remusat L., Palhol F., Robert F., Derenne S. and France-Lanord C. (2006) Enrichment of deuterium in insoluble organic matter from primitive meteorites: a solar system origin? Earth Planet. Sci. Lett. 243, 15-25). Such a behavior is difficult to reconcile with the usual interpretation according to which high D/H ratios represent survivals of interstellar grains. More likely, the deuterium-enrichment process took place after the formation of organic grains whose initial isotopic compositions was close to the protosolar D/H ratio. These grains were possibly loaded at the surface of the protosolar disk where they exposed to the intense solar UV irradiation, triggering an isotopic exchange with deuterium-rich highly reactive ions. (C) 2008 Elsevier Ltd. All rights reserved.