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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Synthetic diversity in the preparation of metallic uranium

Uranium metal is associated with several aspects of nuclear technology; it is used as fuel for research and power reactors, targets for medical isotope productions, explosive for nuclear weapons and precursors in synthetic chemistry. The study of uranium metal at the laboratory scale presents the opportunity to evaluate metallic nuclear fuels, develop new methods for metallic spent fuel reprocessing and advance the science relevant to nuclear forensics and medical isotope production. Since its first isolation in 1841, from the reaction of uranium chloride and potassium metal, uranium metal has been prepared by solid-state reactions and in solution by electrochemical, chemical and radiochemical methods. The present review summarizes the methods outlined above and describes the chemistry associated with each preparation.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Measurement of the 73 As ⁢(𝑛,𝛾) cross section at thermal neutron energies

A measurement of the thermal neutron capture cross section of 73 As (t 1/2 = 80.3 d) was performed utilizing the University of Missouri Research Reactor. Two sealed quartz tubes containing 73 As were prepared and characterized before being irradiated for ≈1 week. The resulting production of 74 As was quantified with γ-ray spectroscopy. Monitor foils of Fe, Zr, and Mo were irradiated alongside the 73 As samples to assess the thermal and resonance region neutron fluxes. In conclusion, the thermal 73 As ⁢(𝑛,𝛾) cross section was determined to be 56.1 ± 8.9 b based on the average of the two 73 As samples and represents the first neutron-induced reaction cross section measured on 73 As.

and nuclear chemistry↗
DOE OSTI2026

Measurement of the 75 As ⁢(𝑛, 2⁢𝑛) cross section at 14.1 MeV at the National Ignition Facility

Here, a new measurement of the 75 As (𝑛, 2⁢𝑛) measurement was performed using the 14.1 MeV neutron pulse produced by fusion experiments at the National Ignition Facility (NIF). The target material consisted of GaAs foils encapsulated in aluminum irradiation containers, along with Au monitor foils, and positioned in the NIF chamber during high neutron yield shots. After irradiation, the GaAs and Au foils were counted with high purity germanium detectors to assess the production of (𝑛, 2⁢𝑛) activation products to determine the flux and the cross section of interest. The measured cross section was 966 ± 71 mb at 14.1 ± 0.37 MeV. This work provides a proof of concept for a platform for performing “ride-along” cross section measurements at NIF to contribute to existing nuclear data as well as measure new cross sections in the future.

and nuclear chemistry↗
DOE OSTI2020

12 C(p,p') 12 C Reaction ( E p =19.5–30 MeV) for Active Interrogation of Special Nuclear Material

Passive detection of special nuclear material (SNM) is challenging due to its inherently low rate of spontaneous emission of penetrating radiation, the relative ease of shielding, and the fluctuating and frequently overwhelming background. Active interrogation, the use of external radiation to increase the emission rate of characteristic radiation from SNM, has long been considered to be a promising method to overcome those challenges. Current active-interrogation systems that incorporate radiography tend to use bremsstrahlung beams, which can deliver high radiation doses. Low-energy ion-driven nuclear reactions that produce multiple monoenergetic photons may be used as an alternative. The 12 C ( p , p ' ) 12 C reaction is one such reaction that could produce large yields of highly penetrating 4.4- and 15.1-MeV gamma rays. This reaction does not directly produce neutrons below the approximately 19.7 MeV threshold, and the 15.1-MeV gamma-ray line is well matched to the photofission cross section of 235 U and 238 U . In this article, we report the measurements of thick-target gamma-ray yields at 4.4 and 15.1 MeV from the 12 C ( p , p ' ) 12 C reaction at proton energies of 19.5, 25, and 30 MeV. Measurements are made with two 3 -in. EJ-309 cylindrical liquid scintillation detectors and thermoluminescent dosimeters placed at 0 ° and 90 ° , with an additional 1.5 -in. Na I ( Tl ) cylindrical scintillation detector at 0 ° . We estimate the highest yields of the 4.4- and 15.1-MeV gamma rays of 1.65 × 10 10 and 4.47 × 10 8 sr - 1 μ C - 1 at a proton energy of 30 MeV, respectively. The yields in all experimental configurations are greater than in a comparable deuteron-driven reaction that produces the same gamma-ray energies— 11 B ( d , n γ ) 12 C . However, a significant increase of the neutron radiation dose accompanies the proton energy increase from 19.5 to 30 MeV.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Mass-asymmetric fission of 205,207,209 Bi at energies close to the fission barrier using proton bombardment of 204,206,208 Pb

Background: Recent observation of mass-asymmetric fission in neutron-deficient Hg and Pt nuclei has reignited interest in fission fragment mass distributions close to Pb. Investigations at energies close to the fission barrier, where mass-asymmetric fission is expected to be most obvious and the sensitivity to shell effects is maximized, are limited in this mass region. Purpose: To measure fission mass distributions for 205,207,209 Bi nuclei at the lowest possible excitation energies to determine how the mass distributions change with excitation energy and the neutron number of the compound nucleus. Method: Proton beams bombarding targets of 204,206,208 Pb were used to study the fission of 205,207,209 Bi at energies from just above to 10 MeV above their fission barriers. Fission fragments were measured using the CUBE fission spectrometer. Fission fragment mass distributions were determined using a newly developed time difference analysis method. Mass distributions were characterized by triple-Gaussian fits to determine the systematic trends across each isotope with excitation energy. Results: Measured mass distributions of all three Bi isotopes exhibit a component of mass-asymmetric fission at all energies studied. The probability of mass-asymmetric fission decreases significantly with increasing excitation energy, from ≈70 to ≈40% over a 10-MeV range. Comparisons between the three Bi isotopes hint at an increase in the mass-symmetric fission yield with increasing neutron number, which could be due to a decrease in the difference between the symmetric and asymmetric fission barriers. The centroids of the mass-asymmetric peaks suggest that several deformed shell gaps in the fission fragments could be contributing to the presence of the mass-asymmetric fission mode with Z light ≃ 38, Z heavy ≃ 45, and N light ≃ 56 all present in the fission fragments. Conclusions: Measurements of fission mass distributions at the lowest possible excitation energies above the fission barrier provide an excellent platform to investigate the origins of the mass-asymmetric fission mode. Finally, further systematic measurements at these energies offer an opportunity to rigorously test new models of fission in this mass region.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Search for elements 119 and 120

In this work, a search for production of the superheavy elements with atomic numbers 119 and 120 was performed in the 50 Ti + 249 Bk and 50 Ti + 249 Cf fusion-evaporation reactions, respectively, at the gas-filled recoil separator TASCA at GSI Darmstadt, Germany. Over four months of irradiation, the 249 Bk target partially decayed into 249 Cf, which allowed for a simultaneous search for both elements. Neither was detected at cross-section sensitivity levels of 65 and 200 fb for the 50 Ti + 249 Bk and 50 Ti + 249 Cf reactions, respectively, at a midtarget beam energy of E lab = 281.5 MeV. The nonobservation of elements 119 and 120 is discussed within the concept of fusion-evaporation reactions including various theoretical predictions on the fission-barrier heights of superheavy nuclei in the region of the island of stability.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

Aqueous harvesting of 88 Zr at a radioactive-ion-beam facility for cross-section measurements

Isotope harvesting is a method of collecting the long-lived radioisotopes that build up during the operation of ion-beam facilities in a way that is useful for subsequent research. As a demonstration of this method for the collection of a group IV metal at a fragmentation facility, the high-energy Zr 88 secondary beam produced from a 140-MeV/u Mo 92 primary beam at the National Superconducting Cyclotron Laboratory (NSCL) was stopped in a water target. The setup aimed to mimic the aqueous beam dump that will be implemented at the Facility for Rare Isotope Beams (FRIB). The collected Zr 88 and accompanying Y 88 decay daughter were radiochemically extracted from the solution and made into target samples suitable for neutron-capture cross-section measurements. These samples were then irradiated at two reactor facilities, and the Zr 88 average thermal-neutron-capture cross section ( σ T ) and resonance integral ( I ) were determined to be σ T = ( 8.04 ± 0.63 ) × 10 5 b and I = ( 2.53 ± 0.28 ) × 10 6 b. The σ T value agrees well with previous results and I , determined for the first time here, was found to be the largest measured resonance integral by two orders of magnitude. The Y 88 thermal-neutron-capture cross section was determined to be less than 1.8 × 10 4 b. This work demonstrates the steps needed to make cross-section measurements with samples produced via aqueous isotope harvesting.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

Measurement of the 230 Th( p ,2n)Pa229 and 230 Th( p ,3n)Pa228 reaction cross sections from 14.1 to 16.9 MeV

Actinium-225 is of interest for medical isotope production and there is on-going research into methods of producing Ac 225 , either directly or via the decay of its parent isotopes ( Th 229 , Pa 229 , and Ra 225 ). One method that has been suggested is the Th 230 ( p , 2 n ) Pa 229 reaction. However, there is no available cross-section data for this reaction in the literature. Purpose: Measure the Th 230 ( p , 2 n ) and Th 230 ( p , 3 n ) reaction cross sections in the energy range where the ( p , 2 n ) reaction is predicted to peak to determine the feasibility of Ac 225 production via the Th 230 ( p , 2 n ) reaction. Methods: Targets naturally enriched in Th 230 were irradiated at the Center for Accelerator Mass Spectrometry at Lawrence Livermore National Laboratory with energies ranging from 14.1 to 16.9 MeV. Furthermore, chemical processing was used to separate the protactinium activation products, followed by γ -ray spectroscopy to measure the activities of Pa 228 , 229 , 230 , 232 produced in the irradiation. Results: We find that excitation functions are reported for the first time in the literature for the Th 230 ( p , 2 n ) and Th 230 ( p , 3 n ) reactions in this energy range. The peak measured value of the Th 230 ( p , 2 n ) reaction was found to be 182 ± 12 mb at 14.4 ± 0.1 MeV. The Th 232 ( p , n ) Pa 232 reaction was used to verify the experimental conditions, the measured values are reported and are comparable to the existing literature values. From the γ -ray spectrometry data, the half-life of Pa 229 was measured as 1.5 ± 0.1 days, which is within the error of the half-life reported in the evaluated nuclear data as well as in the recent measurements, and the half-life of Pa 228 was measured as 19.5 ± 0.4 hours. Conclusions: Overall, the Th 230 ( p , 2 n ) Pa 229 reaction could reasonably be used for Ac 225 isotope production, although significant amounts of relatively isotopically pure Th 230 would be needed for significant production because the low alpha-decay branching ratio of Pa 229 and long half-life of Th 229 inhibit the in-growth of significant amounts of Ac 225 .

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

169 Tm(n,2n) 168 Tm and 169 Tm(n,3n) 167 Tm cross-section measurements from 15 to 21 MeV

The 169 Tm(n,2n) 168 Tm and 169 Tm(n,3n) 167 Tm cross sections have been measured in the neutron energy range between 15 and 21 MeV using the 3 H(d,n) 4 He neutron source reaction. The 169 Tm(n,3n) 167 Tm data are intended to provide an accurate database for interpreting so-called reaction-in-flight neutron yields, which provide a sensitive tool for studying properties of the deuterium-tritium plasma created in inertial confinement fusion laser shots at the National Ignition Facility at Lawrence Livermore National Laboratory. The data are compared to previous data and evaluations for the reaction studied and are found to be in good agreement with the ENDF/B-VIII.0 evaluation, although small adjustments are necessary for the 169 Tm(n,3n) 167 Tm reaction. Here, for the first time in any (n,2n) cross-section measurements to date, a comprehensive data set ranging from threshold to 21 MeV has been obtained by the same group.

150 ≤ A ≤ 189↗
DOE OSTI2022

Measurements of the 96 Zr(α,n) cross section for astrophysics and applications

The reaction 96 Zr(α,n) plays an important role in ν-driven wind nucleosynthesis in core-collapse supernovae and is a possible avenue for medical isotope production. Here, cross section measurements were performed using the activation technique at the Edwards Accelerator Laboratory. Results were analyzed along with world data on the 96 Zr(α, n) cross section and 96 Zr(α, α) differential cross section using large-scale Hauser-Feshbach calculations. We find general agreement between our data, previous measurements, and a statistical description of the reaction. However, we find a larger cross section at low energies compared to prior experimental results, allowing for a larger astrophysical reaction rate. This may impact results of core-collapse supernova ν-driven wind nucleosynthesis calculations, but does not significantly alter prior conclusions about 99 Mo production for medical physics applications. The results from our large-scale Hauser-Feshbach calculations demonstrate that phenomenological optical potentials may yet be adequate to describe (α, n) reactions of interest for ν-driven wind nucleosynthesis, albeit with regionally-adjusted model parameters.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

Determining the 9 $\mathrm{Be}$($n, γ$) 10 $\mathrm{Be}$ integral cross section at fission neutron energies

The 9 B neutron capture cross section has significant implications for Be materials in the nuclear industry as well as the α process in stellar nucleosynthesis. While the cross section is well constrained at thermal neutron energies, there is a lack of experimental data at higher neutron energies, and the evaluated nuclear data libraries can differ by up to two orders of magnitude. We calculate the 9 Be(n, γ) 10 Be integral cross section at fission neutron energies in an effort to resolve disagreements amongst the nuclear data libraries. Foil irradiation experiments were performed using the Flattop critical assembly at the National Criticality Experiments Research Center with either the highly enriched U or Pu cores, with target foil stacks placed at multiple locations to exploit different neutron energy profiles. Accelerator mass spectrometry was used to measure the 10 Be/ 9 Be ratio in irradiated Be foils, while all other activation products were quantified through gamma spectrometry. The experiments were simulated using the Monte Carlo N-Particle radiation transport code and combined with experimental results to determine the total neutron fluence, while the staysl-pnnl suite and fispact-ii code were used to validate the model and assess the systematic uncertainty. The new 9 Be(n, γ) 10 Be integral cross sections calculated in this work are 26.5 ± 2.2µb at 0.59 ± 0.07 MeV, 24 ± 3 µb at 0.98 ± 0.14 MeV, 21.7 ± 1.3 µb at 1.26 ± 0.11 MeV, 21.8 ± 1.4 µb at 1.32 ± 0.11 MeV, and 18.6 ± 1.1 µb at 1.46 ± 0.13 MeV. These results do not agree with integral cross sections from any of the nuclear data library evaluations. Discrepancies between the new integral cross sections reported here and the nuclear data libraries suggest a more complex cross-section structure in the MeV range which allows for more resonance contributions, and more work is needed to further constrain the evaluated cross sections.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

Energy dependence of fission product yields in the second-chance fission region

An extensive dataset of cumulative fission product yields has been generated under a joint collaboration between Los Alamos National Laboratory (LANL), Lawrence Livermore National Laboratory (LLNL), and the Triangle Universities Nuclear Laboratory (TUNL). The energy dependence of the cumulative yield for a select number of high-yield fission products has been measured using quasimonoenergetic neutrons with energies between 5.5 and 11.0 MeV. This is in addition to previously published data covering 0.5–4.5 and 14.8 MeV. The absolute number of fissions was determined during the irradiation period using dual-fission ionization chambers, and the fission products were measured postactivation by whole target γ-ray spectroscopy. Here this paper presents the absolute cumulative fission product yields as a function of incident neutron energy from the neutron-induced fission of 235 U, 238 U, and 239 Pu isotopes at four incident energies in the second-chance fission region and compares them with existing literature values. Corrections relevant to this collaboration's previously published data are also discussed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Measurement of the 175 Hf half-life

Hafnium-175 is a useful radioisotope for numerous applications; however, its evaluated half-life (70 ± 2 days) has a large uncertainty. To enable a new measurement of the half-life, 175 Hf was produced via proton irradiation of natural lutetium and chemically purified. The 175 Hf sample was counted approximately once a month with three high-purity germanium detectors for 13 months (~5.5 half-lives). A 133 Ba standard was counted in an identical manner to quantify systematic uncertainties over the measurement period. In conclusion, the measured 175 Hf half-life is 69.90 ± 0.07 days, in agreement with the evaluated value, but with significantly reduced uncertainty.

150 ≤ A ≤ 189↗
DOE OSTI2020

Identification of the New Isotope 244 Md

In an experiment performed at Lawrence Berkeley National Laboratory’s 88-inch cyclotron, the isotope Md 244 was produced in the Bi 209 ( Ar 40 , 5 n ) reaction. Decay properties of Md 244 were measured at the focal plane of the Berkeley Gas-filled Separator, and the mass number assignment of A = 244 was confirmed with the apparatus for the identification of nuclide A . The isotope Md 244 is reported to have one, possibly two, α -decaying states with α energies of 8.66(2) and 8.31(2) MeV and half-lives of 0.4 – 0.1 + 0.4 and ~ 6 s , respectively. Furtermore, first evidence of the α decay of Bk 236 was observed and is reported.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Two-stage reflective self-seeding scheme for high-repetition-rate X-ray free-electron lasers

X-ray free-electron lasers (XFELs) open a new era of X-ray based research by generating extremely intense X-ray flashes. To further improve the spectrum brightness, a self-seeding FEL scheme has been developed and demonstrated experimentally. As the next step, new-generation FELs with high repetition rates are being designed, built and commissioned around the world. A high repetition rate would significantly speed up the scientific research; however, alongside this improvement comes new challenges surrounding thermal management of the self-seeding monochromator. Here, a new configuration for self-seeding FELs is proposed, operated under a high repetition rate which can strongly suppress the thermal effects on the monochromator and provides a narrow-bandwidth FEL pulse. Three-dimension time-dependent simulations have been performed to demonstrate this idea. Finally, with this proposed configuration, high-repetition-rate XFEL facilities are able to generate narrow-bandwidth X-ray pulses without obvious thermal concern on the monochromators.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

New high-throughput endstation to accelerate the experimental optimization pipeline for synchrotron X-ray footprinting

Synchrotron X-ray footprinting (XF) is a growing structural biology technique that leverages radiation-induced chemical modifications via X-ray radiolysis of water to produce hydroxyl radicals that probe changes in macromolecular structure and dynamics in solution states of interest. The X-ray Footprinting of Biological Materials (XFP) beamline at the National Synchrotron Light Source II provides the structural biology community with access to instrumentation and expert support in the XF method, and is also a platform for development of new technological capabilities in this field. Hee, the design and implementation of a new high-throughput endstation device based around use of a 96-well PCR plate form factor and supporting diagnostic instrumentation for synchrotron XF is described. This development enables a pipeline for rapid comprehensive screening of the influence of sample chemistry on hydroxyl radical dose using a convenient fluorescent assay, illustrated here with a study of 26 organic compounds. The new high-throughput endstation device and sample evaluation pipeline now available at the XFP beamline provide the worldwide structural biology community with a robust resource for carrying out well optimized synchrotron XF studies of challenging biological systems with complex sample compositions.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

Ground electronic state description of thiourea coordination in homoleptic Zn 2+ , Ni 2+ and Co 2+ complexes using sulfur K -edge X-ray absorption spectroscopy

Sulfur K-edge X-ray absorption spectroscopy (XAS) was employed to experimentally characterize the coordinative bond between the thiourea (TU) or thiocarbamide ligand and transition metal (TM) ions Zn 2+ , Co 2+ and Ni 2+ in distorted tetrahedral and octahedral homoleptic coordination environments. Comparisons of XAS spectra of the free TU ligand and [Zn(TU) 4 ] 2+ , [Co(TU) 4 ] 2+ and [Ni(TU) 6 ] 2+ complexes clearly identify spectral features unique to TM 2+ –S(TU) bonding. Quantitative analysis of pre-edge intensities describes the covalency of Ni 2+ —S(TU) and Co 2+ —S(TU) bonding to be at most 21% and 9% as expressed by the S 3p contributions per TM 3d electron hole. Using relevant Ni 2+ complexes with dithiocarbamate and thioether ligands, we evaluated the empirical S 1s → 3p transition dipole integrals developed for S-donor ligands and their dependence on heteroatom substitutions. With the aid of density functional theory-based ground electronic state calculations, we found evidence for the need of using a transition dipole that is dependent on the presence of conjugated heteroatom (N) substitution in these S-donor ligands.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗