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Buckner, M. Q.

Publications and source records attributed to Buckner, M. Q..

Measurement of the 239 Pu$(n, f$) prompt fission neutron spectrum from 10 keV to 10 MeV induced by neutrons of energy 1–20 MeV

Although the prompt fission neutron spectrum (PFNS) is an essential component of neutron-driven systems that has been measured for decades, there are still multiple glaring unknowns regarding the PFNS of major actinides in the fission neutron incident energy range, specifically with regard to multichance fission and pre-equilibrium neutron emission processes. The only impactful experimental 239 Pu PFNS measurements included in recent nuclear data evaluations were measured over a limited outgoing neutron energy range at thermal and 1.5-MeV average incident neutron energy, while other potentially impactful measurements have been shown to contain errors that resulted in either large uncertainty increases or in complete exclusion from nuclear data evaluation. Here, we report a measurement of the 239 Pu PFNS over a wide range of incident neutron energy (1–20 MeV) and three orders of magnitude in outgoing neutron energy (0.01–10 MeV) resulting from the Chi-Nu experiment at the Los Alamos Neutron Science Center. These results are the combination of separate PFNS measurements in the same experimental area, one using a Li-glass and the other a liquid scintillator detector array. Covariances between all PFNS data points from each detector and within each incident energy range were generated between all other data in both detector arrays and within all other incident neutron energy bins, yielding a single covariance matrix for all 1300 PFNS data points reported here. These covariances are based on a thorough assessment of systematic bias and uncertainties associated with the measurement, PFNS extraction technique, combination of data from each detector type, and other aspects of the analysis. The existence of covariances between PFNS data points in different incident neutron energy ranges yielded covariances between average PFNS energy values at each incident energy to be reported here as well, which allowed for firm statements to be made regarding a shape of a purely experimental mean PFNS energy trend for the first time. Although minor PFNS shape differences exist between the results reported here and recent nuclear data evaluations, the ENDF/B-VIII.0 and JEFF-3.3 PFNS evaluations agree reasonably well with the present results from 1-to 10-MeV incident neutron energy, which spans the well-measured 1.5-MeV incident neutron energy PFNS from Lestone and Shores as well as the onset of second-chance fission. However, while the pre-equilibrium component of the PFNS above 12-MeV incident neutron energy roughly agrees in position and magnitude with ENDF/B-VIII.0 and JEFF-3.3, clear differences relating to the relative magnitude of third-chance fission PFNS features are present in the PFNS shape and in the mean PFNS energy trends.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Preequilibrium Asymmetries in the Pu 239 ( n , f ) Prompt Fission Neutron Spectrum

The physical properties of neutrons emitted from neutron-induced fission are fundamental to our understanding of nuclear fission. However, while state-of-the-art fission models still incorporate isotropic fission neutron spectra, it is believed that the preequilibrium prefission component of these spectra is strongly anisotropic. The lack of experimental guidance on this feature has not motivated incorporation of anisotropic neutron spectra in fission models, though any significant anisotropy would impact descriptions of a fissioning system. In the present work, an excess of counts at high energies in the fission neutron spectrum of 239 Pu is clearly observed and identified as an excess of the preequilibrium prefission distribution above the postfission neutron spectrum. This excess is separated from the underlying postfission neutron spectrum, and its angular distribution is determined as a function in incident neutron energy and outgoing neutron detection angle. Comparison with neutron scattering models provides the first experimental evidence that the preequilibrium angular distribution is uncorrelated with the fission axis. The results presented here also impact the interpretation of several influential prompt fission neutron spectrum measurements.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Quantification of the systematic uncertainties associated with measuring a chance coincidence background at Chi-Nu

Modern advances in waveform digitizers allow coincidence experiments to be performed by recording singles data, and identifying coincidences in a later software analysis. It has been previously shown that for such data, the coincidence background can be obtained with unprecedented statistical precision. This method is especially attractive for experiments with complicated, time-varying backgrounds (i.e. not amenable to analytic or even a detailed Monte Carlo analysis). Many neutron detection experiments fall into this category, such as the Chi-Nu experiment to measure the prompt fission neutron spectra of the major actinides. While it is believed that use of this method will yield an improved systematic precision of the measured background, this has not previously been demonstrated. Presented here is the first analysis of the systematic uncertainties associated with this method

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Chi-Nu measurements of the prompt fission neutron spectrum of {sup 235}U and {sup 239}Pu - 25581

Knowledge of the prompt fission neutron spectrum is crucial for understanding the behavior of energetic nuclear systems. Although this energy spectrum has been measured for the major actinides {sup 235}U and {sup 239}Pu for decades, the majority of the available literature data lack the coverage of both incident and outgoing neutron energies and the precision required to accurately guide evaluations and fission models. The Chi-Nu experiment is designed to measure the prompt fission neutron spectrum for a wide range of incident and outgoing neutron energies with attention to uncertainty estimation and assessment of systematic errors in order to provide reliable guidance for evaluations and models of nuclear fission. Preliminary results of the prompt fission neutron spectrum from the neutron-induced fission of {sup 235}U and {sup 239}Pu are presented here, with a focus on the presence of spectral features near multi-chance fission thresholds, pre-equilibrium neutrons in the deduced spectrum, and also on trends of the mean fission neutron energy as a function of the incident neutron energy. While the mean energies of from ENDF/B-VIII.0 are in good agreement with those reported for {sup 235}U spectra, significant disagreements exist above an incident neutron energy of approximately 13 MeV for {sup 239}Pu. Furthermore, in general, the physics features regarding multi-chance fission and pre-equilibrium neutron emission newly-introduced into ENDF/B-VIII.0 appear provide an improved description of the data as compared to ENDF/B-VII.1. (authors)

61 RADIATION PROTECTION AND DOSIMETRY↗

Direct Measurement of Octupole Deformation in 146 Ba

The octupole strength present in the neutron-rich, radioactive nucleus 146 Ba has been experimentally determined for the first time using Coulomb excitation. To achieve this, A=146 fission fragments from CARIBU were post-accelerated by the Argonne Tandem Linac Accelerator System (ATLAS) and impinged on a thin 208 Pb target. Using the GRETINA gamma-ray spectrometer and the CHICO2 heavy-ion counter, the reduced transition probability B(E3; 3- ->0 + ) was determined as 48(+21/-29) W.u. The new result provides further experimental evidence for the presence of a region of octupole deformation surrounding the neutron-rich barium isotopes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The 235 U prompt fission neutron spectrum measured by the Chi-Nu project at LANSCE

The Chi-Nu experiment aims to accurately measure the prompt fission neutron spectrum for the major actinides. At the Los Alamos Neutron Science Center (LANSCE), fission can be induced with neutrons ranging from 0.7 MeV and above. Using a two arm time-of-flight (TOF) technique, the fission neutrons are measured in one of two arrays: a 22- 6 Li glass array for lower energies, or a 54-liquid scintillator array for outgoing energies of 0.5 MeV and greater. Presented here are the collaboration's preliminary efforts at measuring the 235 U PFNS.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Direct evidence for octupole deformation in Ba 146 and the origin of large E 1 moment variations in reflection-asymmetric nuclei

Despite the more than 1 order of magnitude difference between the measured dipole moments in 144 Ba and 146 Ba, the octupole correlations in 146Ba are found to be as strong as those in 144 Ba with a similarly large value of B(E3;3 – → 0 + ) determined as 48( +21 –29 ) W.u. Here, the new results not only establish unambiguously the presence of a region of octupole deformation centered on these neutron-rich Ba isotopes, but also manifest the dependence of the electric dipole moments on the occupancy of different neutron orbitals in nuclei with enhanced octupole strength, as revealed by fully microscopic calculations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Measurement of the Am 242 m neutron-induced reaction cross sections

The neutron-induced reaction cross sections of 242m Am were measured at the Los Alamos Neutron Science Center using the Detector for Advanced Neutron-Capture Experiments array along with a compact parallel-plate avalanche counter for fission-fragment detection. A new neutron-capture cross section was determined, and the absolute scale was set according to a concurrent measurement of the well-known 242m Am(n,f) cross section. The (n,γ) cross section was measured from thermal energy to an incident energy of 1 eV at which point the data quality was limited by the reaction yield in the laboratory. Our new 242m Am fission cross section was normalized to ENDF/B-VII.1 to set the absolute scale, and it agreed well with the (n,f) cross section from thermal energy to 1 keV. Lastly, the average absolute capture-to-fission ratio was determined from thermal energy to E n = 0.1 eV, and it was found to be 26(4)% as opposed to the ratio of 19% from the ENDF/B-VII.1 evaluation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Measurement of the E r c . m . = 259 keV resonance in the N 14 ( p , γ ) O 15 reaction

The N 14 ( p , γ ) O 15 reaction regulates the power generated by the CN cycle and thus impacts the structure and evolution of every star at some point in its life. The lowest positive-energy resonance in this reaction is located at E r c . m . = 259 keV, too high in energy to strongly influence quiescent stellar burning. Yet, the strength of this resonance is used as a cross-section normalization for lower-energy measurements of this reaction. We report on new measurements of the energy, strength, and γ -ray branching ratios for the 259-keV resonance, using different detection and data-analysis schemes. We have also reevaluated previous results, where possible. Our proposed recommended strength of ω γ = 12.6 ( 3 ) meV is in agreement with the previous value of 13.1(6) meV, but is more precise and thus provides a more reliable normalization for low-energy ( p , γ ) measurements.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

γ-Ray spectroscopy using a binned likelihood approach

The measurement of a reaction cross section from a pulse height spectrum is a ubiquitous problem in experimental nuclear physics. In γ-ray spectroscopy, this is accomplished frequently by measuring the intensity of full-energy primary transition peaks and correcting the intensities for experimental artifacts, such as detection efficiencies and angular correlations. Implicit in this procedure is the assumption that full-energy peaks do not overlap with any secondary peaks, escape peaks, or environmental back- grounds. However, for complex γ-ray cascades, this is often not the case. Furthermore, this technique is difficult to adapt for coincidence spectroscopy, where intensities depend not only on the detection efficiency, but also the detailed decay scheme. We present a method that incorporates the intensities of the entire spectrum (e.g., primary and secondary transition peaks, escape peaks, Compton continua, etc.) into a statistical model, where the transition intensities and branching ratios can be determined using Bayesian statistical inference. This new method provides an elegant solution to the difficulties associated with analyzing coincidence spectra. Finally, we describe it in detail and examine its efficacy in the analysis of 18 O(p,γ) 19 F and 25 Mg(p,γ) 26 Al resonance data. For the 18 O(p,γ) 19 F reaction, the measured branching ratios improve upon the literature values, with a factor of 3 reduction in the uncertainties.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Absolute measurement of the 242 Pu neutron-capture cross section

Here, the absolute neutron-capture cross section of 242 Pu was measured at the Los Alamos Neutron Science Center using the Detector for Advanced Neutron-Capture Experiments array along with a compact parallel-plate avalanche counter for fission-fragment detection. The first direct measurement of the 242 Pu(n,γ) cross section was made over the incident neutron energy range from thermal to ≈ 6 keV, and the absolute scale of the (n,γ) cross section was set according to the known 239 Pu(n,f) resonance at E n,R = 7.83 eV. This was accomplished by adding a small quantity of 239 Pu to the 242 Pu sample. The relative scale of the cross section, with a range of four orders of magnitude, was determined for incident neutron energies from thermal to ≈ 40 keV. Our data, in general, are in agreement with previous measurements and those reported in ENDF/B-VII.1; the 242 Pu(n,γ) cross section at the E n,R = 2.68 eV resonance is within 2.4% of the evaluated value. However, discrepancies exist at higher energies; our data are ≈30% lower than the evaluated data at E n ≈ 1 keV and are approximately 2σ away from the previous measurement at E n ≈ 20 keV.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗