Journal
GEOCHIMICA ET COSMOCHIMICA ACTA
Volume 64, Issue 9, Pages 1651-1661Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/S0016-7037(00)00334-3
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In situ laser extraction techniques were applied for the study of heavy noble gases in a polished section of Zone 13 from the natural nuclear reactor in Okelobondo. Three main mineral phases were identified in this polished section using SEM-EDX. The Xe and Kr isotopic structures were determined by multiple measurements in each of these phases. Twenty-four isotopic analyses of the gases extracted from two different U-rich phases revealed nearly normal fission spectra. All 9 analyses of a U-free phase, consisting mainly of alumophosphates, demonstrated an unusual isotopic composition (Xe-136/Xe-134/Xe-132/Xe-131/Xe-130/Xe-129/ Xe-128 = 1/1.25/1.73/0.89/0.0045/0.274/0) with concentrations ranging up to 10(-2) cm(3) STP/g. This is the highest Xe concentration ever measured in a natural material. Kr was also anomalous, although to a lesser extent. These results confirm the presence of Chemical Fractionation of Fission Xe (CFF-Xe) in the Okelobondo alumophosphates. CFF-Xe is a decay product of intermediate fission fragments that have migrated out of the U-rich host phases into adjacent U-free minerals. The CFF-Xe spectra in the alumophosphates are also accompanied by Xe-130 excesses, which are attributed to neutron capture on fissiogenic I-129 that apparently migrated out of the nearby U-rich minerals. The Xe-130/Xe-129 ratio allows us to estimate the thermal equivalent neutron dose of 1.1 x 10(21) n/cm(2). The presence of an unknown fission component remarkably similar in composition to CFF-Xe can be inferred from the atmospheric and terrestrial data. This leads us to the hypothesis that the CFF process has operated on a global scale on the Earth. Copyright (C) 2000 Elsevier Science Ltd.
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