Kr and Xe isotopes from spontaneous fission of Cm-248 and Cf-250 - Comparison with noble gases in carbonaceous chondrites
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The principal mode of the nuclear decay of plutonium 238 is by alpha particle emission at a rate of 17 curies per gram. Gamma radiation also present in nuclear fuels arises primarily from the nuclear de-excitation of daughter nuclei as a result of the alpha decay of plutonium 238 and reactor-produced impurities. Plutonium 238 has a spontaneous fission half life of 4.8 x 10 to the 10th power years. Neutrons associated with this spontaneous fission are emitted at a rate of 28,000 neutrons per second per gram. Since the space fuel form of plutonium 238 is the oxide pressed into a cermet with molybdenum, a contribution to the neutron emission rate arises from (alpha, n) reactions with 0-17 and 0-18 which occur in natural oxygen.
The major sources of neutrons from plutonium dioxide nuclear fuel are considered in detail. These sources include spontaneous fission of several of the Pu isotopes, reactions with low Z impurities in the fuel, and reactions with O-18. For spontaneous fission neutrons a value of (1.95 plus or minus 0.07) X 1,000 n/s/q PuO2 is obtained. The neutron yield from (alpha, neutron) reactions with oxygen is calculated by integrating the reaction rate equation over all alpha particle energies and all center-of-mass angles. The results indicate a neutron emission rate of (1.42 plus or minus 0.32) X 10,000 n/s/q PuO2. The neutron yield from (alpha, neutron) reactions with low Z impurities in the fuel is presented in tabular form for one part per million of each impurity. The total neutron flux emitted from a particular fuel geometry is estimated by adding the neutron yield due to the induced fission to the other neutron sources.
The major sources of neutrons from plutonium dioxide nuclear fuel are considered in detail. These sources include spontaneous fission of several of the Pu isotopes, (alpha, n) reactions with low Z impurities in the fuel, and (alpha, n) reactions with O-18. For spontaneous fission neutrons a value of (1.95 + or - 0.07) X 1,000 n/s/g PuO2 is obtained. The neutron yield from (alpha, n) reactions with oxygen is calculated by integrating the reaction rate equation over all alpha-particle energies and all center-of-mass angles. The results indicate a neutron emission rate of (1.14 + or - 0.26) X 10,000 n/s/g PuO2. The neutron yield from (alpha, n) reactions with low Z impurities in the fuel is presented in tabular form for one part part per million of each impurity. The total neutron yield due to the combined effects of all the impurities depends upon the fractional weight concentration of each impurity. The total neutron flux emitted from a particular fuel geometry is estimated by adding the neutron yield due to the induced fission to the other neutron sources.
The lunar breccia 14318 is one of three Apollo-14 breccias containing substantial amounts of parentless xenon from the spontaneous fission of extinct Pu-244. The argon and xenon contained in this breccia were studied by stepwise heating of pristine and neutron-irradiated samples. The isotopic composition of xenon from fission, determined by an improved method, is shown to be from Pu-244. Concentrations of this fissiogenic xenon are in substantial excess (15-fold) of what could be produced by spontaneous fission of U-238. The breccia is found to contain abundant trapped argon with an Ar-40/Ar-36 ratio of roughly 14. Otherwise, the argon is radiogenic and gives a convincing K-Ar age of 3.69 plus or minus 0.09 b.y. by the stepwise Ar-40/Ar-39 method, nearly in agreement with ages for other Apollo-14 breccias.
When some nuclei are free from strong gravitational field, they are unstable and will become stable nuclei by competitions of following processes: (1) neutron-evaporation; (2) spontaneous fission; and (3) beta prime 3-decay. At the initial stage, (1) and (2) are important and (3) can be ignored. The qualitative results are as follows: (1) it seems that nuclei with A 100 come from the spontaneous fission and beta prime decay of neutron-evaporated nuclei with A similiar to 140-440, which can replace the r-process; (2) the super-heavy elements with Z=114--126 (A similiar to 330--360) can be formed. They can be observed in cosmic rage if they have the halftime T 10 to the 7th poweer years; (3) the peak in the rare-earth elements comes from the symmetric fission of super-heavy elements; (4) there are more neutron-rich nuclei in the fragments; and (5) the abundances of a 83 elements in cosmic rays are one order of magnitude higher than that in the solar system.
Fission threshold calculation for systematics of spontaneous fission rates and neutron-fission width ratio
Tracks attributed to the spontaneous fission of plutonium-244 and of uranium-238 were detected in a large whitlockite crystal in the lunar breccia 14321 from the Fra Mauro formation. For a track-retention age of 3.95 b.y., the number of plutonium tracks relative to the number of uranium tracks is 0.51 plus or minus 0.15, provided that the rock was not heavily neutron-irradiated 3.95 b.y. ago.
Whitlockite grains in two Apennine Front KREEP soil fragments contain extremely high densities of fission tracks. A new method is described in which particle tracks are examined in an actinide-poor phase bordering an actinide-rich whitlockite phase. This method clearly distinguishes the fission track contributions from other track sources; e.g., Fe-group cosmic rays, spallation recoils, and dislocations. Observed track excesses, when corrected for U- and Th-related fission sources, are 4-20 times greater than the contribution from spontaneous fission of U-238 (based on an age of 4 b.y.), and probably represent a large and variable contribution from the fission of Pu-244. These fragments may have pre-Imbrium ages, underscoring the importance of KREEP as a constituent of the pre-mare lunar crust. Track excesses are not correlated with the U or Th contents of the whitlockite grains. This behavior suggests that Pu fractionates differently from U and Th in lunar igneous KREEP.
Xenon extracted in step-wise heating of lunar breccia 14,301 contains a fission-like component in excess of that attributable to uranium decay during the age of the solar system. There seems to be no adequate source for this component other than Pu-244. Verification that this component is in fact due to the spontaneous fission of extinct Pu-244 comes from the derived spectrum which is similar to that observed from artificially produced Pu-244. It thus appears that Pu-244 was extant at the time lunar crustal material cooled sufficiently to arrest the thermal diffusion of xenon. Subsequent history has apparently maintained the isotopic integrity of plutonium fission xenon. Of major importance are details of the storage itself. Either the fission component is the result of in situ fission of Pu-244 and subsequent storage in 14,301 material, or the fission xenon was stored in an intermediate reservoir before incorporation into 14,301.
A space propulsion concept is proposed and analyzed which consists of a thin sheet coated on one side with fissionable material, so that nuclear power is converted directly into propulsive power. Thrust is available both from ejected fission fragments and from thermal radiation. Optimum thicknesses are determined for the active and substrate layers. This concept is shown to have potential mission capability (in terms of velocity increments) superior to that of all other advanced propulsion concepts for which performance estimates are available. A suitable spontaneously fissioning material such as Cf254 could provide an extremely high-performance first stage beyond earth orbit. In contrast with some other advanced nuclear propulsion concepts, there is no minimum size below which this concept is infeasible.
A space propulsion concept is proposed and analyzed which consists of a thin sheet coated on one side with fissionable material, so that nuclear power is converted directly into propulsive power. Thrust is available both from ejected fission fragments and from thermal radiation. Optimum thicknesses are determined for the active and substrate layers. This concept is shown to have potential mission capability (in terms of velocity increments) superior to that of all other advanced propulsion concepts for which performance estimates are available. A suitable spontaneously fissioning material such as Cf-254 could provide an extremely high-performance first stage beyond earth orbit. In contrast with some other advanced nuclear propulsion concepts, there is no minimum size below which this concept is infeasible.
Information about lunar surface history revealed by fossil particle tracks is summarized. Such tracks are the result of damage left in dielectric materials by highly ionizing charged particles including heavy solar and galactic cosmic ray nuclei, heavy nuclei recoiling from cosmic ray induced spallation reactions, and induced- and spontaneous-fission fragments. From the distribution of cosmic ray and spallation tracks in the lunar rock, surface residence times of 1 to 30 million years and rock erosion rates of 1 to 10 A/yr have been determined. Particle tracks also record surface orientation and depth history of the rocks and contain information about ancient solar activity.
Two Apollo 14 breccias have been found to contain xenon from the spontaneous fission of 82 my Pu-244. A third contains 60 times as much fission xenon as local uranium can account for and is probably of similar character. One of the breccias shows a Xe-129 excess most likely due to the decay of 17 my I-129. That these components can be separated and identified at all implies that complete isotopic homogenization has not occurred over a period which encompasses both extinction of these radionuclides and compaction of the breccias into their final form. In this sense isotope pre-history has been preserved in some lunar breccias providing information that pre-dates the formation of the rock itself (as determined by conventional techniques).
Particle track studies reveal an abundant record of fossil solar flare tracks in breccia components. Metamorphic events govern the degree to which this record is preserved, and studies of phases with different track retentivities allow limits to be placed on temperatures reached during a rock's history. The least affected breccias have never experienced temperatures as great as 300 C. Two breccias which contain xenon from spontaneous fission of Pu-244 (14301 and 14318) and Xe-129 (14301 only) have never been heated above about 700 C. This and evidence for a surface irradiation of some of the breccia components support a surface implantation model for the origin of the xenon in these breccias. Green glass spheres in 15086 have not been heated above about 300 C during or after breccia formation yet have retained fission tracks for less than 0.7 G.y. Argon ages of about 3.5 G.y. for similar green glass are at least five times as great and may indicate that the glass was not completely outgassed at is formation.
A description is presented for the isolation and characterization of the host phase from the Allende C3V chondrite and a mass spectrometric study of the five noble gases in this phase. It is though that the Xe component may have been produced by spontaneous fission of an extinct superheavy element. The fission Xe resides in a minor fraction comprising 0.5% of the meteorite. The fraction consists of chromite, an unknown Cr, Fe-mineral, and amorphous carbon. The gas components and the progenitor of the fission Xe may have been trapped in these minerals when they formed from the solar nebula.
Radiochemical neutron activation analysis of seven Allende samples for 26 trace elements were conducted. In addition, Cr and Fe were studied with the aid of instrumental neutron activation analysis. The investigation had the objective to identify the extinct superheavy element which was present in meteorites and decayed to Xe isotopes by spontaneous fission. The superheavy element was found to reside mainly in a rare mineral (probably a Fe, Ni, Cr, Al-sulfide), comprising only 0.04% of the meteorite. It is pointed out that of the nine volatile superheavy elements 111 to 119, only 115, 114, and 113 are expected to condense as sulfides in the temperature interval between 400 and 500 K corresponding to mineral formation conditions in the solar nebula.
We present a model of the steady-state transport assuming three reservoirs: a lower mantle (P) with a relatively undepleted inventory of U, Th, Pu, I, He, Ne, Xe, Ar; an upper mantle that has been extensively outgassed (D); and the atmosphere. There is mass transport at a rate M(sub PD) by plumes from the lower mantle, a fraction of which is outgassed directly into the atmosphere, while the remainder feeds matter and associated nuclei into D. D is well outgassed at spreading centers and has material containing atmospheric gases added to it by subduction. In the case of He, there is no subduction component. The approach follows the treatment of Kellogg and Wasserburg. A summary of the pertinent equations and constraints was reported earlier. The U, Th and Pu in P are estimated for Earth models from refractory element abundances in meteorites. In this model the inventory of rare gases in D is governed by the simple mixing of components from P (both radiogenic and original) with distinctive atmospheric components. In addition, alpha decay and spontaneous fission of U, and (alpha, n) reaction on oxygen from energetic alpha particles produce radiogenic/nuclear daughter products in D. These include (4)He, (136)Xe and (21)Ne. (40)K in D generates excess radiogenic (40)Ar.