I-Xe systematics of the impact plume produced chondrules from the CB carbonaceous chondrites: Implications for the half-life value of 129I and absolute age normalization of 129I-129Xe chronometer.

It is inferred that magnesian non-porphyritic chondrules in the CB (Bencubbin-type) carbonaceous chondrites formed in an impact generated plume of gas and melt at 4562.49 ± 0.21 Ma (Bollard et al., 2015) and could be suitable for the absolute age normalization of relative chronometers. Here xenon isotopic compositions of neutron irradiated chondrules from the CB chondrites Gujba and Hammadah al Hamra (HH) 237 have been analyzed in an attempt to determine closure time of their I-Xe isotope systematics. One of the HH 237 chondrules, #1, yielded a well-defined I-Xe isochron that corresponds to a closure time of 0.29 ± 0.16 Ma after the Shallowater aubrite standard. Release profiles and diffusion properties of radiogenic 129*Xe and 128*Xe, extracted from this chondrule by step-wise pyrolysis, indicate presence of two iodine host phases with distinct activation energies of 73 and 120 kcal/mol. In spite of the activation energy differences, the I-Xe isotope systematics of these two phases closed simultaneously, suggesting rapid heating and cooling (possibly quenching) of the CB chondrules. The release profiles of U-fission Xe and I-derived Xe correlate in the high temperature host phase supporting simultaneous closure of 129I-129Xe and 207Pb-206Pb systematics. The absolute I-Xe age of Shallowater standard is derived from the observed correlation between I-Xe and Pb-Pb ages in a number of samples. It is re-evaluated here using Pb-Pb ages adjusted for an updated 238U/235U ratio of 137.794 and meteorite specific U-isotope ratios. With the addition of the new data for HH 237 chondrule #1, the re-evaluated absolute I-Xe age of Shallowater is 4562.4 ± 0.2 Ma. The absolute I-Xe age of the HH 237 chondrule #1 is 4562.1 ± 0.3 Ma, in good agreement with U-corrected Pb-Pb ages of the Gujba chondrules (Bollard et al., 2015) and HH 237 silicates (Krot et al., 2005). All I-Xe data used here, and in previous estimates of the absolute age of Shallowater, are calculated using 15.7 ± 0.6 Ma value for 129I half-life. The slopes of I-Xe - Pb-Pb correlation lines plotted for different sets of samples for Shallowater normalization are always ≤1. Assuming uranium half-life values are correct; this restricts the half-life of 129I to ≤15.7 Ma.

New evidence for chemical fractionation of radioactive xenon precursors in fission chains.

Mass-spectrometric analyses of Xe released from acid-treated U ore reveal that apparent Xe fission yields significantly deviate from the normal values. The anomalous Xe structure is attributed to chemically fractionated fission (CFF), previously observed only in materials experienced neutron bursts. The least retentive CFF-Xe isotopes, 136Xe and 134Xe, typically escape in 2:1 proportion. Xe retained in the sample is complimentarily depleted in these isotopes. This nucleochemical process allows understanding of unexplained Xe isotopic structures in several geophysical environments, which include well gasses, ancient anorthosite, some mantle rocks, as well as terrestrial atmosphere. CFF is likely responsible for the isotopic difference in Xe in the Earth's and Martian atmospheres and it is capable of explaining the relationship between two major solar system Xe carriers: the Sun and phase-Q, found in meteorites.

Record of cycling operation of the natural nuclear reactor in the Oklo/Okelobondo area in Gabon.

Using selective laser extraction technique combined with sensitive ion-counting mass spectrometry, we have analyzed the isotopic structure of fission noble gases in U-free La-Ce-Sr-Ca aluminous hydroxy phosphate associated with the 2 billion yr old Oklo natural nuclear reactor. In addition to elevated abundances of fission-produced Zr, Ce, and Sr, we discovered high (up to 0.03 cm(3) STP/g) concentrations of fission Xe and Kr, the largest ever observed in any natural material. The specific isotopic structure of xenon in this mineral defines a cycling operation for the reactor with 30-min active pulses separated by 2.5 h dormant periods. Thus, nature not only created conditions for self-sustained nuclear chain reactions, but also provided clues on how to retain nuclear wastes, including fission Xe and Kr, and prevent uncontrolled runaway chain reaction.

Noble gases in stratospheric dust particles: confirmation of extraterrestrial origin.

Noble gas elemental and isotopic ratios were measured in a group of 13 "chondritic" stratospheric dust particles. Neon and argon are present in "solar" proportions; xenon appears to be dominated by contributions from "planetary" sources. The apparent xenon concentration is higher than that measured in any bulk meteorite, approaching the concentration found in the noble gas-rich, acid-insoluble residues from carbonaceous chondrites.

Isotopic analysis of rare gases from stepwise heating of lunar fines and rocks.

Highlights of a first effort in sorting out rare gases in lunar material are solar wind rare gases in abundance; variable (20)Ne/(22)Ne but constant (21)Ne/ (22)Ne ratios in fractions of the trapped neon; cosmogenic rare gases similar to those found in meteorites, except for copious (131)Xe in one rock but not in another; at Tranquillity Base a rock 4.1 x 10(9) years old which reached the surface 35 to 65 million years ago, amid soil whose particles have typically been within a meter of the surface for 10(9) years or more.

Radioisotopes and the history of nucleosynthesis in the galaxy.

Nearly all of the heavier elements seem to have been assembled by successive neutron captures occurring in two distinct processes: the s (slow) process refers to neutron capture at a rate which is slow compared to the intervening beta-decay; the r (rapid) process refers to neutron capture at a rate which is rapid compared to the beta process. It is becoming increasingly apparent that simple models for galactic r-process nucleosynthesis are inadequate. Modern astronomical observations, which indicate that the bulk of r-process synthesis may have occurred early in the life of the galaxy, cannot be ignored. Recent data on the fissiogenic xenon in whitlockite from the St. Severin meteorite also place stringent conditions on permissible models for element synthesis. It appears that neither sudden nor continuous models for element formation are consistent with isotopic data now available. I propose a more complex model for the synthesis of solar system material in which the r-process is allowed to occur in three distinct modes: a "prompt" synthesis early in the history of the galaxy, a "continuous" synthesis whereby r-process products are continuously added to the galactic mix, and a "last-minute" synthesis which enriches the solar nebula with r-process material shortly before the formation of the solar system. Calculations based on the present abundances of uranium-235, uranium-238, and thorium-232 and the measured abundances of iodine-129 and plutonium-244 present when meteorites began to retain xenon indicate that the galactic age is between 8.0 and 8.8 billion years, with the initial "prompt" synthesis accounting for 81 to 89 percent of the total r-process material ever produced, the "last-minute" synthesis contributing between 11 and 13 percent, and 0 to 8 percent occurring in the continuous mode. The time interval between the isolation of the solar nebula from galactic r-process and the onset of xenon retention in meteorites lies between 176 and 179 million years.

Xenon-iodine dating: sharp isochronism in chondrites.

Measurements of the accumulation of Xe(l29) from radioactive decay of extinct 1(129) in meteorites show that the 1(129)/ 1(127) ratio in high-temperature minerals in diverse chondrites was 10(-4) at the time of cooling. The uniformity in the ratio indicates that the minerals cooled simultaneously within 1 or 2 million years.