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At least 19 records

Investigating rapid alpha-decay induced aging of 238 PuO 2 by Raman Spectroscopy

Investigating alpha-decay induced aging in PuO 2 is useful in nuclear forensics; helping to determine the time since last calcination. This was previously investigate by monitoring the damage to 240 PuO 2 over the course of a few years. The rate of alpha-decay induced aging has long been assumed to scale only with the decay rate of other isotopes without direct verification. This article reports the first alpha-decay aging study of 238 PuO 2 by Raman spectroscopy. Contrary to the expected 10 days for 238 PuO 2 to reach steady state based on 240 PuO 2 studies, the alpha aging curve reached an approximate steady state ∼24–30 h after laser annealing. While the cause of the order of magnitude decrease is unknown, it is speculated that dynamic annealing could contribute to the differences in rate of induced aging. The Raman spectra of annealed and aged 238 PuO 2 matched the expected features in 239 PuO 2 and 240 PuO 2 spectra; showing no formation of new stable chemical species in the material such as secondary Pu oxide phases (e.g., Pu 4 O 9 ). In conclusion, results indicate that 238 Pu could be leveraged for rapid alpha-decay aging studies to characterize alpha-decay induced features and better understand matrix temperatures and the annealing of Frankel pair defects.

Actinide↗

A New Approach for Calculating the Alpha-Decay Half-Life for the Heavy and Super-heavy Elements and an Exact A Priori Result for Beyllium-8

A new general method for calculating the alpha decay half-life is presented. The method predicts an a priori exact value for the beryllium-8 half-life. Beryllium-8 is an exception to the current alpha decay theory captured in the Geiger-Nuttal law. The new method predicts the beryllium-8 alpha half-life using only constants and measured isotopic mass. The method also reliably predicts all the heavier isotope alpha decay half-lives consistent with the Geiger-Nuttal law. With respect to current theory, the inability of the Geiger-Nuttal Law to predict the alpha-decay half-life in the case of beryllium-8 has led to consideration of other decay mechanisms for this isotope, such as fission for example. One result is that given the consistency of the new method presented here for all isotopes including an exact a priori result for beryllium-8, the evidence strongly suggests that the beryllium-8 decay is in fact an alpha decay. A second result is that the method definitively demonstrates that the entire rest mass of the two helium-4 electrons is converted to energy in the decay process and this energy becomes part of the emitted alpha particle kinetic energy.

07 ISOTOPE AND RADIATION SOURCES↗

Alpha-decay induced shortening of fission tracks simulated by in situ ion irradiation

The diffusion of defects (e.g., vacancies and interstitials) and elements used for dating (e.g., He and Pb) in a mineral structure is a thermal process: This is the primary assumption used to determine the age and thermal history of minerals. For instance, thermal history reconstruction, through the number and length distribution of tracks produced by spontaneous fission of 238 U, is obtained by assuming a thermal event to be the only energy source for shortening of fission tracks. Here, we report a new, non-thermal energy source that induces additional shortening of fission tracks by the irradiation of alpha-recoils from the alpha-decay of 238 U and 232 Th. We simulate alpha-decay induced track-shortening by combining ion accelerator irradiations with transmission electron microscopy. This allows for the first observation of track-shrinkage during in situ ion irradiation. We show that rather than alpha-particles, alpha-recoils induce a significant shortening of fission tracks by nuclear-collisions. The shortening of track-length can be quantified as a function of alpha-decay event dose. However, apatite is less sensitive than zircon to this non-thermal process. Furthermore, the findings exemplify the interactions among different types of self-irradiation from alpha-particles, alpha-recoils and fission-fragment nuclei in single mineral grains and have important implications for the use of zircon and apatite for radiometric dating and thermochronology.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Alpha-decay-induced fracturing in zircon - The transition from the crystalline to the metamict state

Zonation due to alpha-decay damage in a natural single crystal of zircon from Sri Lanka is discussed. The zones vary in thickness on a scale from one to hundreds of microns. The uranium and thorium concentrations vary from zone to zone such that the alpha decay dose is between 0.2 x 10 to the 16th and 0.8 x 10 to the 16th alpha-events per milligram. The transition from the crystalline to the aperiodic metamict state occurs over this dose range. At doses greater than 0.8 x 10 to the 16th alpha events/mg there is no evidence for long-range order. This type of damage will accumulate in actinide-bearing, ceramic nuclear waste forms. The systematic pattern of fractures would occur in crystalline phases that are zoned with respect to actinide radionuclides.

Chakoumakos, Bryan C.↗

Alpha-decay width of a near proton-threshold resonance in the 7 Li( α, α ) channel

We investigate the alpha-decay width of a near proton-threshold resonance in 11 B by the excitation functions of 7 Li(α, α) and 7 Li(α, α’) reactions. This resonance is an example of loosely bound atomic nuclei, understood as small open quantum systems, that exhibit properties significantly influenced by their coupling to the continuum. The present experiment focuses on the formation of a specific state in 11 B at excitation energy in the region near 11.4 MeV by bombarding a 7 Li target with a 4 He beam at energies ranging from 3.92 to 4.56 MeV in the laboratory frame. The study provides data complementary to previous observations of the proton emission in the β-decay of the neutron-rich halo nucleus 11 Be. An R-matrix fit to the data provides resonance energy and partial widths consistent with J π =1/2 + for a narrow near-threshold state in 11 B at 11.400(20) MeV, that is 171(20) keV above the proton emission threshold, with partial α-decay width Γ α =2.5$^{+3.5}_{–1.5}$ keV in elastic scattering and Γ α' =15.8$^{+1.9}_{–0.4}$ keV in inelastic scattering. These findings contribute to the understanding of the structure of this open quantum system resonance.

11B↗

Alpha Decay Chains as Thermal Power Sources: Analysis and Applications for RTGs

Radioactive sources can provide power in remote and environmentally harsh locations such as the arctic or space. The generators powered by such sources are rugged and can withstand extreme temperatures, lack of sunlight, and require no human intervention for multiple years. Radioisotopes are used in thermoelectric generators to provide power at remote sites and deep in space. Isotopes like Pu-238, Cm-244, and Am-241 are used in these generators by NASA for power in space probes and spacecrafts. These power sources deliver a steady supply of energy over extended periods of time. Alpha particles created during decay do not travel far in a material. Their kinetic energy is transferred to heat that we can then convert into energy. Unlike beta and gamma decay, the slower-moving alpha particles stop in the material, making their energy available for use. Energy from these natural decay processes provides a reliable source of power. Spontaneous fission is rare and unreliable, and unlike induced fission processes, alpha decay occurs naturally and does not require external management or ignition. The ideal properties of an isotope for use as a power source depend upon the intended use. For use in an Arctic research base over a period of several years, but less than a decade, an isotope that provides high power output over a shorter lifespan may be the most suitable option. Whereas, for deep space missions where a consistent power source for decades or perhaps more than 100 years is needed that would require a very different isotope. One with a much longer half-life that would provide consistent power throughout that time and survive in that state in for these extended periods of time. These examples represent two extreme sides in terms of time frames. By analyzing the power produced by different radioactive decay processes over time, we can evaluate the suitability of various isotope decay chains for specific uses. Some unstable isotopes undergo a series of radioactive decays, transforming into different isotopes at each step and resulting in a stable isotope. The lists of isotopes in these decay processes are known as decay chains. Some of these chains, illustrated in the figures below, are currently being investigated for use in radioisotope thermoelectric generators (RTGs) designed for a range of operational durations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Simulation of radiation damage via alpha decay in BFS:PC grouts using 4 He 2+ ion acceleration

The impact of alpha radiation on cements used to encapsulate intermediate-level waste (ILW) is not well understood. ILW wastes can contain high levels of alpha-emitting radionuclides, meaning that the grouts used to encapsulate them are exposed to significant ionising radiation. Thus, a damaged region could develop in the grout adjacent to the alpha-emitting species. This work attempted to recreate this behaviour through nonradioactive 4 He 2+ ion-accelerator experiments, which have not previously been applied to common encapsulation grouts. The influence of this irradiation on a slag-Portland cement was investigated at different ages via transmission electron microscopy energy-dispersive x-ray spectroscopy (TEM-EDX) and supporting techniques, to assess whether 4 He 2+ irradiation caused textural or chemical zonation. No significant changes in hydrate phases or textures were observed, other than minor variations associated with carbonation. This paper provides a proof of concept for using ion acceleration techniques on cements and furthers knowledge on their radiation response.

36 MATERIALS SCIENCE↗

Statistical aspects of the 1980 solar flares. Part 3: Parametric comparison and final comments

The 1349 study flares are considered addressing relationships between pairs of specific study paremeters; namely, H alpha rise time versus H alpha importance, X-ray class and H alpha decay time; H alpha decay time versus H alpha importance and X-ray class; and H alpha importance versus X-ray class. Mean H alpha rise time and decay time versus X-ray class and H alpha importance will also be discussed, and some final comments regarding the study flares are given.

Wilson, R. M.↗

Scintillation of liquid nitrogen

Liquid nitrogen is commonly used in cryogenic applications and is a promising medium for the direct immersion cooling of sensors used for nuclear and particle physics experiments. The scintillation properties of gaseous nitrogen are well-documented, but little is known about the scintillation of liquid nitrogen. If present, scintillation light from interactions of ambient radioactivity could produce backgrounds for rare event searches such as the direct detection of dark matter. Using a coincidence-tagged alpha decay, we demonstrate that liquid nitrogen exhibits measurable, albeit very faint, scintillation. Assuming the same scintillation wavelengths as gaseous nitrogen, we estimate a relative scintillation yield of $Y_{\liquidn}/Y^{\STP}_{\gasn} =$ \num[uncertainty-descriptors={stat,sys}]{0.0142(0.0005)(0.0030)} with respect to gaseous nitrogen at standard temperature and pressure. Considering the average scintillation yield from alpha decays in gaseous nitrogen, this implies a scintillation yield for alpha decays in liquid nitrogen of $Y_{\liquidn} = \qty[]{2.39(0.56)}{photons~per~MeV}$. To our knowledge this is the first measurement of scintillation in liquid nitrogen.

Pagani, Luca (ORCID:0000000234692581)↗

Raman signatures from age-dating PuO 2 since last calcination

The self-irradiation of PuO 2 has been shown to affect the attributes of fifteen vibrational bands in the Raman spectrum. The vibrational bands correspond to the Raman allowed vibrational mode T 2g , overtones, defects, and bands from electronic origin. Defects in the crystal lattice from low-calcination temperature and alpha decay origins are responsible for the changes in the band attributes (band position, full-width half maximum (FWHM), intensity). Crystal lattice defects are also responsible for the growth of the defect bands. The temporal behavior of the vibrational bands can be used to estimate the age of the material since last calcination. Laser annealing was used to reset the material to full crystallinity prior to the aging study. 240 PuO 2 , with an alpha decay rate of 3.67 greater than the decay rate of 239 PuO 2 , was primarily used to assess the alpha decay-induced damage within 3 years. The aging study focused on the time-dependent properties of the T 2g band and the growth of defect bands. The FWHM of the T 2g band and the ratio of the areas of the defect bands/T 2g band were measured through a time period in excess of 3 years. The data from this study were found very close to the data describing the temporal evolution of the lattice constant measured with the X-ray diffraction (XRD) technique. The local physical properties of the material measured with Raman spectroscopy and the lattice parameter constant measured with XRD indicates a strong correlation between the two techniques. Although both techniques provide similar age-dating information, in contrast to the few milligram quantities required for XRD, Raman spectroscopy requires a 10 µm diameter PuO 2 particle to provide an estimate of the material age since last calcination.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

α decay of the neutron-deficient isotope At 190

The alpha decay of the neutron-deficient 190 At isotope was observed following the 103 Rh( 90 Zr, 3n) 190 At reaction at Argonne National Laboratory. The reaction products were separated from the beam using the Argonne Gas-Filled Analyzer and implanted into a double-sided Si strip detector. The spatial and temporal correlations between implanted nuclei and subsequent α decays towards the known daughter isotope 186 Bi were used to identify and characterize 190 At nuclei. In this paper, two possible decay scenarios are proposed for the 190 At → 186 Bi decay.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

$\mathrm{α}$ decay of the longest-lived Cm isotope: $^{247}_{96}\mathrm{Cm}$

We report alpha decay of 247 Cm was studied fifty years ago using a 1.6 Bq source containing 99.4 % 247 Cm and levels in 243 Pu were deduced. Using the same source, γ-ray spectra were measured with a more efficient Ge detector. A γ-ray spectrum was also measured in coincidence with α particles for a period of two months and has 80 times more counts than the previously published spectrum. Gamma-ray energies were determined with higher precision and four new γ rays were identified. A new high-energy γ ray of 564.5 keV was observed, which is interpreted as a transition between a level at 564.5 keV and the ground state of 243 Pu. The 564.5-keV level has been tentatively assigned to the 7/2 - [743] Nilsson state.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Effects of He Ion Irradiation in Simple Borosilicate Glasses for HLW Immobilisation - 20324

High-level radioactive waste (HLW) consists of fission products and minor actinides. Borosilicate glass is the host material of choice in most countries to safely immobilize HLW, followed by eventual geological disposal. HLW glasses will experience both self-heating and self-irradiation effects due to the decay of fission products and minor actinides present therein. During the first 500 years of geological disposal, beta-gamma decay will be the main source of radiation due to short half-lives of fission products, as compared to very long-lived actinides which will be responsible for irradiation over much longer timescales. High-energy alpha particles and alpha recoil nuclei can potentially have significant impact (stored energy, volume change, accumulated dose, chemical durability) on the performance of the wasteform over longer timescales. Thus, to ensure safe and economic disposal over geological periods (10{sup 4} - 10{sup 6} years), the assessment of performance and properties in terms of radiation effects becomes indispensable. This work aims to simulate the effects of alpha decay in radioactive waste glasses. Two international glasses, namely UK 'MW' lithium-sodium borosilicate and Indian sodium-barium borosilicate, which are being used as HLW immobilization matrices by the UK and India respectively, were prepared by a melt-quench method and annealed below their glass transition temperatures. Both glasses were irradiated with 650 KeV He{sup 2+} ions with doses ranging from 10{sup 15} to 10{sup 17} ions/cm{sup 2}. Structural analysis was carried out using electron paramagnetic resonance (EPR) and Raman spectroscopies. First derivative continuous wave EPR spectra were recorded for all pristine and irradiated glass monoliths at room temperature using an X-band (frequency 9.6 GHz) EPR Bruker spectrometer. Results from EPR analyses showed the formation of irradiation induced paramagnetic centers at g ∼ 2.00 in all irradiated glasses. Raman spectra of pristine and irradiated samples were acquired, and showed notable changes in glass structure post-irradiation, with the emergence of a broad Raman band at 1560 cm{sup -1} upon irradiation with high fluences. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Absorber Clamp for Microcalorimeter Decay Energy Spectrometry

Microcalorimeter Decay Energy Spectrometry (DES) is of interest to nuclear safeguards due to its ability to provide high precision isotopic compositions of nanogram-to microgram-scale samples of Pu and U and related daughter products. The DES method is able to record decay energy of each alpha-decay event in a sample that is embedded in a metal matrix (absorber) and thermally linked to a microcalorimeter detector. This work optimizes the DES technique used to thermally link the absorber and microcalorimeter detector element to allow for more rapid assembly and to increase detector performance and operating life. Optimized attachment methods are crucial for enhancing the viability of DES in high-sample-throughput facilities, such as those that support international nuclear safeguards measurements. Here, in this study, we designed and implemented a pressure-based absorber clamp and evaluated the performance of this new attachment method relative to pressed indium bond attachment. Results using the absorber clamp demonstrate a streamlined detector assembly procedure that minimizes accidental damage to detectors, as well as increasing detector pulse speeds by 57%. Spectral comparison shows the clamp preserves detector performance relative to indium attachment.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Mechanical Detection of Nuclear Decays

We report the detection of individual nuclear alpha decays through the mechanical recoil of the entire micron-sized particle in which the decaying nuclei are embedded. Momentum conservation ensures that such measurements are sensitive to any particles emitted in the decay, including neutral particles that may otherwise evade detection with existing techniques. Detection of the minuscule recoil of an object more than 10^12 times more massive than the emitted particles is made possible by recently developed techniques in levitated optomechanics, which enable high-precision optical control and measurement of the mechanical motion of optically trapped particles. Observation of a change in the net charge of the particle coincident with the recoil allows decays to be identified with background levels at the micro-Becquerel level. Here, the techniques developed here may find use in fields ranging from nuclear forensics to dark matter and neutrino physics.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Radiation from plutonium 238 used in space applications

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.

Keenan, T. K.↗

He, Xe and Ne isotopes in a steady-state mass transport model and implications about terrestrial volatiles

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.

Wasserburg, G. J.↗

Uranium series dating of Allan Hills ice

Uranium-238 decay series nuclides dissolved in Antarctic ice samples were measured in areas of both high and low concentrations of volcanic glass shards. Ice from the Allan Hills site (high shard content) had high Ra-226, Th-230 and U-234 activities but similarly low U-238 activities in comparison with Antarctic ice samples without shards. The Ra-226, Th-230 and U-234 excesses were found to be proportional to the shard content, while the U-238 decay series results were consistent with the assumption that alpha decay products recoiled into the ice from the shards. Through this method of uranium series dating, it was learned that the Allen Hills Cul de Sac ice is approximately 325,000 years old.

Fireman, E. L.↗