Plutonium-244 dating

Re-examination of a vast amount of xenon isotope data which have been accumulated since the 1960s reveals that the so-called CCF (carbonaceous chondrite fission) xenon is a mixture of²⁴⁴Pu fission xenon and a severely mass-fractionated primordial xenon, whose isotopic composition has been further altered by neutron-capture and spallation reactions, which occurred in the vicinity of a supernova that most likely exploded sometime more than 4.8 billion years ago. The integrated flux of 10 KeV (stellar temperature) neutrons to which the xenon was exposed appears to have been in excess of 10²³ n/cm².     

Variation of the isotopic composition of xenon in the solar system

Re-examination of a vast amount of existing xenon isotope data, which have been accumulated in the literature since the 1960's, reveals that the variation of the isotopic composition of xenon in the solar system can be attributed to a combined effect of (a) mass-fractionation, (b) spallation and (c) stellar-temperature neutron-capture reactions plus the addition of (d) the beta-decay product of ¹²⁹I and of (e) the spontaneous fission products of ²⁴⁴Pu. The effect of each of the above-mentioned processes can be extremely large, due, primarily to the fact that these processes occurred in the interior of a supernova, which exploded about 5.1 billion years ago.     

Plutonium-244 fission xenon and primordial xenon in lunar samples and meteorites

Xenon found in lunar samples is a binary mixture of²⁴⁴Pu fission xenon and a trapped xenon, whose isotopic composition often shows a striking resemblance to that ofTakaoka's¹ primitive xenon. The decay product of¹²⁹I is conspicuously absent in lunar samples and this may be attributed to the facts that (a) the half-life of¹²⁹I is much shorter than that of²⁴⁴Pu, and (b) the separation of xenon from plutonium may take place easily, since the former is a gaseous element, while the latter is a refractory element. The separation of xenon from iodine may not take place easily, however, since the former is a gaseous element, while the latter is a volatile element. The isotopic compositions of the trapped xenon released from ordinary chondrites and achondrites resemble that ofTakaoka's primitive xenon, which has been mass-fractionated in such a manner that the heavier isotopes are systematically enriched relative to the lighter isotopes.     

Application of Nuclear Chemistry in the Study of the Universe

Isotopic compositions of the strange Xenon components-HL and the s-type xenon can be explained in a straightforward manner as due to the alteration of the isotopic composition of xenon caused by a combined effect of (a) mass-fractionation, (b) spallation and (c) stellar-temperature neutron-capture reactions. As much as 42.49% of total ¹³⁶Xe ( ¹³⁶Xe) found in the Allende diamond inclusions is ²⁴⁴Pu fission xenon (^136fXe) and the trapped xenon is severely mass-fractionated in such a manner that the lighter xenon isotopes are systematically depleted relative to the heavier isotopes. The relative abundances of ¹³⁰Xe and ¹³²Xe in the trapped xenon component are both markedly enhanced indicating that it was irradiated with a total flux of 1.2·10²³ n·cm^-2 of stellar-temperature (10 keV) neutrons. The xenon found in the s-type xenon, on the other hand, resemble that of the atmospheric xenon irradiated with a total flux of about 6.0·10²³ n·cm^-2 of 10 keV neutrons. These results indicate that we are seeing here the effects of nuclear processes occurring inside of a star, such as the exploding supernova.     

Plutonium-244 dating

Re-examination of all known xenon isotopic data for the carbonaceous chondrites Renazzo, Mokoia, and Groznaya reveals that these meteorites contain (26±7), (33±1), and (36±4)·10^–12 (ccSTP^136fXe/g) of²⁴⁴Pu fission xenon, respectively. These meteorites started to retain their xenon more than 4,800 million years ago at about the same time as did the carbonaceous chondrites Allende, Murray, and Murchison.     

Plutonium-244 dating VI. Initial ratios of plutonium to uranium in achondrites

Re-examination of all known xenon isotopic data for achondrites reveals that²⁴⁴Pu fission xenon can be resolved in about three-fourths of the meteorites of this class. The amounts of²⁴⁴Pu fission xenon found in these meteorites range from ca. 1–2 up to 20–40·10^–12 ccSTP/g. These meteorites started to retain their xenon some 200–500 million years later than did the carbonaceous chondrites Allende, Groznaya, Mokoia, Murchison, Murray, and Renazzo, which began to retain their xenon over 4800 million years ago.     

Plutonium-244 dating

Re-examination of all known xenon isotopic data for ordinary chondrites reveals that²⁴⁴Pu fission xenon can be resolved in about one-fourth of the meteorites of this class. The amounts of²⁴⁴Pu fission xenon found in these meteorites range from ca. 1–2 up to 6–8·10^?12 ccSTP/g. These meteorites started to retain their xenon some 200–500 million years later than did the carbonaceous chondrites Allende, Groznaya, Mokoia, Murchison, Murray, and Renazzo which began to retain their xenon over 4800 million years ago.     

Plutonium-244 dating I. Initial ratio of plutonium to uranium in the allende meteorite

Re-examination of all known xenon isotope data for the carbonaceous chondrite Allende reveals that this meteorite contains as much as (22±1)·10^{–1 2} csSTP per gram of fissogenic¹³⁶Xe (^136fXe) from the extinct nuclide²⁴⁴Pu and it appears to have started to retain its xenon more than 4800 million years ago, when the²⁴⁴Pu to²³⁸U ratio in the solar system was 0.113±0.006 (atom/atom).     

Environmental applications of stable xenon and radioxenon monitoring

Characterization of transuranic waste is needed for decisions about waste site remediation. Soil-gas sampling for xenon isotopes can be used to define the locations of spent fuel and transuranic waste. Radioxenon in the subsurface is characteristic of transuranic waste and can be measured with extreme sensitivity using large-volume soil-gas samples. Measurements at the Hanford Site showed ¹³³Xe and ¹³⁵Xe levels indicative of ²⁴⁰Pu spontaneous fission. Stable xenon isotopic ratios from fission are distinct from atmospheric xenon background. Neutron capture by ¹³⁵Xe produces an excess of ¹³⁶Xe in reactor-produced xenon, providing a means of distinguishing spent fuel from separated transuranic material.     

Plutonium-244 fission xenon in carbonaceous inclusions of primitive meteorites

A total of 13 samples of diamond separates studied so far, all contain excess ²⁴⁴Pu fission xenon. On the other hand, none of the SiC separates contains excess ²⁴⁴Pu fission xenon, while 5 out of 10 samples of graphite separates studied so far contain excess ²⁴⁴Pu fission xenon.     

Strange xenon in Jupiter

Jupiter's helium-rich atmosphere contains xenon with excess¹³⁶Xe and the ratio of r-products more closely resembles “strange” xenon (Xe-X, alias Xe-HL) seen in carbonaceous chondrites than xenon seen in the solar wind (SW-Xe). The linkage of primordial helium with Xe-X, as seen on a microscopic scale in meteorites, apparently extended across planetary distances in the solar nebula, This is expected if the solar system acquired its present chemical and isotopic diversity directly from debris of the star that produced our elements.     

Plutonium-244 and strange xenon components in the solar system

A number of strange xenon components have been reported in the literature during the past three decades; for example, AVCC (average carbonaceous chondrite), CCF (carbonaceous chondrite fission) xenon, xenon-X, xenon-H, xenon-L, xenon-S, xenon-U, SUCOR (surface correlated xenon), BEOC (Bern Oberflächen-Correliert) xenon, and so on. It is often assumed that they reprsent the isotopic compositions of more or less pure or primordial components of xenon. If one attempts to interpret the existing xenon isotope data for meteorites and lunar samples, assuming that they are pure or primordial, however, one encounters all sorts of problems and no coherent theory concerning the variation of the isotopic composition of xenon in the solar system emerges. We have therefore re-examined over 4,000 sets of existing xenon isotope data for meteorites and lunar samples. The results indicate that these strange xenon components are mixtures of²⁴⁴Pu fission xenon and atmospheric xenon, whose isotopic compositions have been altered by the processes of a) mass-fractionation, b) spallation and c) neutron-capture reactions.     

Quantitative and isotopic analysis of released and retained krypton and xenon fission gases from irradiated metallic fuels

We quantitatively measured the amounts and isotopic distributions of the released and retained fission gases (Kr and Xe) from two irradiated metallic fuels (U–10Zr and U–10Zr–5Ce) at approximately 2.9 at.% burnup, using a gas chromatography and a quadrupole mass spectrometer. The obtained Xe/Kr ratios indicate that the released and retained fission gases from the irradiated metallic fuels came primarily from the fission of ²³⁵U, instead of that of heavy isotopes such as ²³⁹Pu and ²⁴¹Pu. The calculated (⁸³Kr + ⁸⁴Kr)/⁸⁶Kr and (¹³¹Xe + ¹³²Xe)/¹³⁴Xe ratios suggest that no fuel rods became defective during the irradiation process.     

The pre-Fermi natural reactor: A note on the periodic mode of operation

The isotopic compositions of xenon released from the Oklo reactor at temperatures below 1000°C are such that the abundances of¹³¹Xe,¹³²Xe and¹³⁴Xe relative to¹³⁶Xe are markedly enhanced when compared to the relative fission yields from the thermal neutron-induced fission of²³⁵U. These anomalies can be attributed to the fact that¹³¹Xe,¹³²Xe and¹³⁴Xe have fairly long-lived precursors: 8.04-day¹³¹I, 78.2-hour¹³²Te and 42-minute¹³⁴Te, respectively. It is possible to determine the duration of the time when the reactor was turned off from the ratios of excess¹³²Xe to excess¹³⁴Xe in these anomalous xenon fractions released from the Oklo reactor. Calculations based on the available xenon isotope data that the time period during which the reactor was turned off was approximately 2 to 3 hours.     

Cumulative yields of short-lived xenon isotopes in the spontaneous fission of252Cf

Cumulative yields of short-lived xenon isotopes^137,138,139Xe have been determined in the spontaneous fission of²⁵²Cf, using a fast radiochemical separation method followed by gamma spectrometry. Xenon-137 yield is reported for the first time. The measured cumulative yields are converted to chain yields assuming normal charge distribution systematics for comparision with the literature data.     

Simulations of 129Xe NMR chemical shift of atomic xenon dissolved in liquid benzene

The isotropic ¹²⁹Xe NMR chemical shift of atomic Xe dissolved in liquid benzene was simulated by combining classical molecular dynamics and quantum chemical calculations of ¹²⁹Xe nuclear magnetic shielding. Snapshots from the molecular dynamics trajectory of xenon atom in a periodic box of benzene molecules were used for the quantum chemical calculations of isotropic ¹²⁹Xe chemical shift using nonrelativistic density functional theory as well as relativistic Breit?CPauli perturbation corrections. Thus, the correlation and relativistic effects as well as the temperature and dynamics effects could be included in the calculations. Theoretical results are in a very good agreement with the experimental data. The most of the experimentally observed isotropic ¹²⁹Xe shift was recovered in the nonrelativistic dynamical region, while the relativistic effects explain of about 8% of the total ¹²⁹Xe chemical shift.     

Non-destructive determination of spontaneously fissioning nuclides by neutron coincidence counting using multichannel time spectroscopy

A non-destructive method for determining the amount of actinoids has been developed. The method is based on thermal neutron coincidence counting and employs a selective detection of neutrons resulting from the spontaneous fission of actinoids. The detection system is described in detail and the measurement results of²⁴⁴Cm as an example are presented. The results show that the measured fission rate of²⁴⁴Cm is consistent with the fission rate calculated from ENDF/B-V data and that the amount of²⁴⁴Cm can be determined within about 5% accuracy even in the presence of a large amount of actinoids, for example, up to 2.6·10⁶, 3.6·10⁴, or 1.6·10³ times in the mass ratio of²³⁹Pu,²⁴¹Am, or²⁴⁰Pu to²⁴⁴Cm, respectively.     

Probing polymer colloids by Xe NMR

Model aqueous dispersions of polystyrene, poly(methyl methacrylate), poly(n-butyl acrylate) and a statistical copolymer poly(n-butyl acrylate-co-methyl methacrylate) were studied using xenon NMR spectroscopy. The ¹²⁹Xe NMR spectra of these various latexes reveal qualitative and quantitative differences in the number of peaks and in their line widths and chemical shifts. Above the glass transition temperature, exchange between xenon sorbed in the particle core and free xenon outside the particles is fast on the ¹²⁹Xe spectral time-scale and a single ¹²⁹Xe signal is observed. At temperatures below the glass transition temperature, the exchange between sorbed and free xenon is slow on the ¹²⁹Xe spectral time-scale and two ¹²⁹Xe NMR signals can be observed. If the signal of sorbed ¹²⁹Xe is observed, its chemical shift, line width and integral relative to the integral of free ¹²⁹Xe can be used for the characterization of the particle core. The line width of free ¹²⁹Xe provides the residence time of xenon outside the particles and can be used to determine the rate constant characterizing the kinetics of penetration of xenon in the particles. This rate constant emerges as promising parameter for the characterization of the polymer particle surface.     

Plutonium-244 dating VII. Initial abundances of uranium-235 and plutonium-244 in lunar samples

Re-examination of a vast amount of lead and xenon isotope data that have been accumulated since the Apollo 11 landing on the moon in July 1969 reveals that some of the lunar fines and breccia started to retain their radiogenic lead and fissiogenic xenon isotopes about 5 billion years ago when the ratios of²³⁵U and²⁴⁴Pu to²³⁸U in the early solar system were approximately 4 and 2 atoms per 10 atoms of²³⁸U, respectively.     

Underground sources of radioactive noble gas

It is well known that radon is present in relatively high concentrations below the surface of the Earth due to natural decay of uranium and thorium. However, less information is available on the background levels of other isotopes such as ¹³³Xe and ^131mXe produced via spontaneous fission of either manmade or naturally occurring elements. The background concentrations of radioxenon in the subsurface are important to understand because these isotopes potentially can be used to confirm violations of the comprehensive nuclear-test-ban treaty during an on-site inspection. Recently, Pacific Northwest National Laboratory measured radioxenon concentrations from the subsurface at the Nevada Nuclear Security Site (NNSS—formerly known as the Nevada Test Site) to determine whether xenon isotope background levels could be detected from spontaneous fission of naturally occurring uranium or legacy ²⁴⁰Pu as a result of historic nuclear testing. In this paper, we discuss the results of those measurements and review the sources of xenon background that must be taken into account during OSI noble gas measurements.