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Consistent Nuclear Data Evaluations for Criticality Safety

Evaluations of nuclear data are based on statistical analysis of available experimental data and their uncertainties plus model calculations and their uncertainties. As the models are currently rather limited, the evaluations are heavily biassed toward experimental data, with the caveat that a thorough analysis is also required to understand possible discrepancies between data sets. Hence, as new experimental data become available, they are incorporated into the evaluation procedure. Recent measurements of the 233 U capture to fission cross section ratio at the Los Alamos Neutron Science Center have prompted a re-evaluation of the capture cross section in the resonance and fast regions up to 250 keV. We will discuss the challenges of including the new fast neutron experimental data in an evaluation that is consistent with the resonance region. We will also discuss our consistent evaluation procedure based on the Hauser-Feshbach statistical model for nuclear reactions and its application to the evaluations of 239 Pu and 139 La neutron-induced reactions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Volume 6: Experiment Facility Spectrum Tailoring (HFIR Futures – Enhanced Capabilities Series)

In-core irradiation experiment research, such as materials and fuels irradiation research and radioisotope production, is one of the primary missions of Oak Ridge National Laboratory’s (ORNL) versatile High Flux Isotope Reactor (HFIR). In support of the HFIR-Sustaining and Enhancing Neutron Science (SENSe) Initiative, a technically diverse group of ORNL irradiation research subject matter experts formed the Spectrum Tailoring Working Group, with the goal of developing a compendium of experiment facility concepts to enhance irradiation experiment conditions via neutron spectrum tailoring capabilities. The purpose of this report is to document the concepts developed in FY22 and the associated scientific justifications, identify potential facility sponsors, and estimate costs and schedules for each concept. This report documents the efforts performed in FY22, which may continue in FY23 or later pending the direction of the HFIR-SENSe Initiative and the interested sponsors.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

New capability for indirect neutron capture measurements: The DICER instrument at LANSCE

The Device for Indirect Capture on Radionuclides (DICER) implements a new indirect technique for (n,γ) studies in which the neutron capture rate is determined from analysis of resonance neutron transmission data. The DICER instrument and associated radionuclide production at the Isotope Production Facility (IPF), both at the Los Alamos Neutron Science Center (LANSCE), as well radioactive sample fabrication, have been under development in the last few years. First measurements on a radioactive sample ( 88 Zr, t ½ =83.4 days), which was recently reported to have an extremely large thermal neutron capture cross section and resonance integral, are planned for the winter of 2021. A performance overview, brief details on the 88Zr fabrication and proof of good operation results will be presented.

47 OTHER INSTRUMENTATION↗

Quasi-differential neutron induced neutron emissions from 235 U, and 239 Pu

Uncertainty in nuclear reaction cross sections, angular distributions, and other nuclear data directly impact how well simulations of nuclear systems represent physical observations. Here, to determine how well the nuclear data in ENDF/B-VIII.0, JEFF-3.3, and JENDL-4.0 evaluations describe the physical behaviour of 235 U, and 239 Pu when subjected to a neutron flux, the neutron emission spectrum was measured for carbon, 93.0% 235 U, and 93.9% 239 Pu samples, and compared against detailed MCNP6 simulations. The measurements were performed at the Los Alamos Neutron Science Center using a quasi-differential method previously developed at Rensselaer Polytechnic Institute. The measurement spanned 0.82–20 MeV and 30–150 degrees. The measurements show there are a significant number of discrepancies between library predictions of the neutron yield and physical observation. A few of the main discrepancies found are described in this paper. Based on these results a new evaluation utilizing these results for carbon, 235 U, and 239 Pu is recommended.

235U↗

Advancement of LANSCE accelerator facility as a 1-MW Fusion Prototypic Neutron Source

The Fusion Prototypic Neutron Source (FPNS) is considered to be a testbed for scientific understanding of material degradation in future nuclear fusion reactors (Zinkle and Moeslang, 2013; Summary Report on the FPNS Workshop, 2018; Pitcher et al., 2019). The primary mission of FPNS is to provide a damage rate in iron samples of 8-11 dpa/calendar year with He/dpa ratio of 10 appm in irradiation volume of 50 cm 3 or larger with irradiation temperature 300–1000 °C and flux gradient less than 20%/cm in the plane of the sample. The Los Alamos Neutron Science Center (LANSCE) is an attractive candidate for the FPNS project. The Accelerator Facility was designed and operated for an extended period as a 0.8-MW Meson Factory. The existing setup of the LANSCE accelerator complex can nearly fulfill requirements of the fusion neutron source station. The primary function of the upgraded accelerator systems is the safe and reliable delivery of a 1.25-mA continuous proton beam current at 800-MeV beam energy from the switchyard to the target assembly to create 1 MW power of proton beam interacting with a solid tungsten target. The present study describes existing accelerator setup and further development required to meet the needs of FPNS project.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Measurement of the free neutron lifetime in a magneto-gravitational trap with in situ detection

Here, in this study, we publish three years of data from the UCNτ experiment performed at the Los Alamos Ultracold Neutron Facility at the Los Alamos Neutron Science Center. These data are in addition to our previously published data. Our goals in this paper are to better understand and quantify systematic uncertainties and to improve the lifetime statistical precision. We previously reported a value from our 2017–2018 data for the neutron lifetime of 877.75 ± 0.28 (statistical) +0.22–0.16 (systematic) s. We have collected an additional three years of data reported here for the first time. When all the data from UCNτ are averaged for 2017, 2018, 2020, 2021, and 2022, we report an updated value for the lifetime of 877.83 ± 0.22 (statistical)+0.20–0.17 (systematic) s. We utilized improved monitor detectors, reduced our correction due to UCN upscattering on residual gas, and employed four different UCN detector geometries both to reduce the correction required for rate dependence and to explore potential contributions due to phase space evolution.

Cabibbo-Kobayashi-Maskawa matrix↗

Experimental realization of neutron helical waves

Methods of preparation and analysis of structured waves of light, electrons, and atoms have been advancing rapidly. Despite the proven power of neutrons for material characterization and studies of fundamental physics, neutron science has not been able to fully integrate these techniques because of small transverse coherence lengths, the relatively poor resolution of spatial detectors, and low fluence rates. Here, we demonstrate methods that are practical with the existing technologies and show the experimental achievement of neutron helical wavefronts that carry well-defined orbital angular momentum values. We discuss possible applications and extensions to spin-orbit correlations and material characterization techniques.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Data Science and Computation for Rapid and Dynamic Compression Experiment Workflows at Experimental Facilities, September 8-11, 2020. Workshop Report

The application of high pressure to materials has enabled discoveries in scientific fields such as planetary science, materials science, and materials synthesis. Recent advances in X-ray user light sources and other facilities, co-location and integration of user facilities with high-pressure drivers, availability of high-performance computing (HPC) platforms, and the development of new data science techniques have created opportunities for, and challenges in, advancing data analytics for rapid and dynamic compression experiments. To address these challenges, harness the emerging technology now available, and expedite scientific discovery, Los Alamos National Laboratory (LANL) hosted a virtual workshop entitled “Data Science and Computation for Rapid and Dynamic Compression Workflows at Experimental Facilities” from September 8 to 11, 2020. The workshop included 95 registered scientists and analytics experts from 15 universities, 9 United States (US) national laboratories, 5 US and European X-ray light sources, neutron sources such as the Los Alamos Neutron Science Center (LANSCE), other big science facilities such as the National Ignition Facility (NIF), and an industry representative. The workshop included 31 invited talks and 4 lightning talks by students and postdocs.

36 MATERIALS SCIENCE↗

Electrospraying deposition and characterization of potassium chloride targets for nuclear science measurements

Natural and isotopically enriched KCl targets were prepared using specially formulated KCl solutions, deposited by electrospraying on thin (1.5 μm) gold backings, followed by a short annealing in a preheated (350-450 °C) furnace. Various techniques, such as X-ray fluorescence (XRF), scanning electron microscopy (SEM) imaging, and energy-dispersive X-ray spectroscopy (EDS), were used to characterize the produced targets. A white neutron beam at the Los Alamos Neutron Science Center (LANSCE) facility was also used to verify the estimated atomic percentages of the enriched 40 KCl targets. KCl was deposited relatively uniformly as large particles rather than films on the gold surface. As a result, this method can be broadly extended to make stable targets that are difficult to produce with other methods and more exotic radioactive targets required for research in fundamental sciences and applications.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Briefing Book: Office of Experimental Sciences

Key to OES science is the advancement of experimental capabilities and vibrant partnerships with other elements of NNSA’s Defense Programs. OES fosters an experimental portfolio that spans the space from small scale studies utilizing tabletop instruments through complex and dynamic high energy density; hydrodynamic; and subcritical experiments on flagship national facilities like Los Alamos Neutron Science Center (LANSCE), National Ignition Facility (NIF), Z machine at Sandia National Laboratories, Dual Axis Radiographic Hydrodynamic Test (DARHT), and the U1a Complex in Nevada. Essential to meeting the deterrence challenges that drive OES is a functional strategy for integration of OES with Defense Programs pursuits in modeling and simulation, engineering and technology maturation, and stockpile and production modernization.

42 ENGINEERING↗

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↗

High-yield and high-angular-fluence neutron generation from deuterons accelerated by laser-driven collisionless shock

Since a bright collimated neutron source is an essential tool for global security missions and fundamental scientific research. In this paper, we study a compact high-yield and high-angular-fluence neutron source particularly suitable for high-energy neutron applications utilizing the breakup reaction of laser-driven deuterons in a 9 Be converter. The neutron generation scaling from such a reaction is used to guide the choice and optimization of the acceleration process for bulk ions in a low density CD 2 foam. In particular, the collisionless shock acceleration mechanism is exploited with proper choice in the laser and target parameter space to accelerate these ions toward energies above the temperature of the distribution. Particle-in-cell and Monte Carlo simulations are coupled here to investigate this concept and possible adverse effects as well as the contribution from the surface ions accelerated and the optimal converter design. The simulation results indicated that our design can be a practical approach to increase both the neutron yield and angular fluence of laser-driven neutron sources, reaching >10 11 neutron/pulse (or >10 8 neutron/J) and >10 11 neutron/sr (or >10 8 neutron/sr/J) with present-day kJ-class high-power lasers. Such developments will advance fundamental neutron science, high precision radiography, and other global security applications with laser-driven sources.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Remote Density Measurements of Molten Salts via Neutron Radiography

With an increased interest in the use of molten salts in both nuclear and non-nuclear systems, measuring important thermophysical properties of specific salt mixtures becomes critical in understanding salt performance and behavior. One of the more basic and significant thermophysical properties of a given salt system is density as a function of temperature. With this in mind, this work aims to present and layout a novel approach to measuring densities of molten salt systems using neutron radiography. This work was performed on Flight Path 5 at the Los Alamos Neutron Science Center at Los Alamos National Laboratory. In order to benchmark this initial work, three salt mixtures were measured, NaCl, LiCl (58.2 mol%) + KCl (41.8 mol%), and MgCl2 (32 mol%) + KCl (68 mol%). Resulting densities as a function of temperature for each sample from this work were then compared to previous works employing traditional techniques. Results from this work match well with previous literature values for all salt mixtures measured, establishing that neutron radiography is a viable technique to measure density as a function of temperature in molten salt systems. Finally, advantages of using neutron radiography over other methods are discussed and future work in improving this technique is covered.

Long, Alexander M. (ORCID:0000000343009454)↗

Investigation of Benchmark $k$ eff Sensitivity and Uncertainty for 239 Pu fission in Specific Energy Ranges

Nuclear data at intermediate energies (from 1 to 100s of keV) are evaluated based on scarce differential data and theory unable to capture physics’ expected structure. There is also a lack of integral data. This is a known deficiency and is challenging to address. Calculated effective multiplication factor, k eff , values for intermediate energy experiments are ~25× further from experiment than for fast energies and are often well outside the experimental uncertainties. The goal of the PARADIGM (PARallel Approach of Differential and InteGral Measurements) project is to significantly re duce the uncertainties of intermediate energy nuclear data for 239 Pu. To this end, PARADIGM simultaneously optimizes experiments at both the Los Alamos Neutron Science Center (LANSCE) and National Criticality Experiments Research Center (NCERC). The combined set of data will inform new intermediate-energy nuclear data. By execution of differential and integral experiments, establishment of new theory, and undertaking nuclear data evaluation in parallel, the timeline to deliver improved nuclear data to users will be reduced significantly that is to three years. For the PARADIGM project, it was decided to optimize an integral experiment for two neutron energy ranges, within the full intermediate energy range. The low energy range goes from 1 to 30 keV, while the higher energy range goes from 30 to 600 keV. This work focuses on nuclear data sensitivities and uncertainties for 239 Pu fission for existing experiments in the International Criticality Safety Benchmark Evaluation Project (ICSBEP). When designing new experiments, it is important to understand what benchmarks currently exist. For a more traditional experiment design (in which a specific application model(s) exists), comparisons would be made between the application model(s) and existing benchmarks. For PARADIGM, there is no specific application model, but instead the specific nuclear data reaction and energy ranges of interest can be explored for existing benchmarks.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Demonstration of neutron time-of-flight diffraction with an event-mode imaging detector

Neutron diffraction beamlines have traditionally relied on deploying large detector arrays of 3 He tubes or neutron-sensitive scintillators coupled with photomultipliers to efficiently probe crystallographic and microstructure information of a given material. Given the large upfront cost of custom-made data acquisition systems and the recent scarcity of 3 He, new diffraction beamlines or upgrades to existing ones demand innovative approaches. This paper introduces a novel Timepix3-based event-mode imaging neutron diffraction detector system as well as first results of a silicon powder diffraction measurement made at the HIPPO neutron powder diffractometer at the Los Alamos Neutron Science Center. Notably, these initial measurements were conducted simultaneously with the 3 He array on HIPPO, enabling direct comparison. Data reduction for this type of data was implemented in the MAUD code, enabling Rietveld analysis. Results from the Timepix3-based setup and HIPPO were benchmarked against McStas simulations, showing good agreement for peak resolution. With further development, systems such as the one presented here may substantially reduce the cost of detector systems for new neutron instrumentation as well as for upgrades of existing beamlines.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Neutron detector development for high-rate neutron reflectometry at the Second Target Station of Oak Ridge National Laboratory

The Second Target Station (STS) at the Oak Ridge National Laboratory Spallation Neutron Source (SNS) is expected to produce a neutron source that is the brightest in the world, having a significantly higher peak brightness compared to the First Target Station (FTS), where the reflectometry instruments already fall short of being able to handle the highest available flux by a factor of ~100. The neutron reflectometers at the SNS FTS are not suitable for the reflectometers planned for the SNS STS because of its unprecedentedly high peak brightness and the already limited capabilities of these instruments at high count rates. Furthermore, the high rate instruments that are now under development are expected to underperform with regard to gamma sensitivity, meaning that signal-to-noise will be reduced and they will be unable to measure weaker reflectance phenomena in the presence of the significant prompt gamma flash at SNS. To address these challenges, we conducted research to advances associated instruments, techniques, and capabilities for the SNS STS reflectometers. More specifically, we investigated the development of a scalable, 2-D positive-sensitive, pixelated, scintillator-based neutron detector module based on a newly developed scintillator. The work has potential for impact on future neutron reflectometry instruments and neutron science performed at the SNS STS. In particular, the improved background rejection capability of the developed detector could extend the available experimental dynamic Q range, allowing it to measure weak reflectance phenomena.

reflectometry, radiation instrumentation, neutron ↗

In-Situ Spatial Mapping of Hydrogen in Yttrium Hydrides at LANSCE

This report summarizes the neutron imaging techniques and experimental activities performed at the Los Alamos Neutron Science Center (LANSCE) with the main goal of measuring temperature driven hydrogen diffusion within bulk-yttrium hydride (YH x ) materials. The experimental results and technique developments reported herein support the US Department of Energy Office of Nuclear Energy’s (DOE-NE) Microreactor Program under Technology Maturation. In particular, the critical need to experimentally validate and verify hydrogen-diffusion models of metal hydrides used in hightemperature microreactor designs is addressed by means of high-spatial-resolution neutron imaging coupled with custom-built and application-specific furnaces. These capabilities were designed to apply large temperature gradients across centimeter-sized YH x pellets to simulate conditions faced in the microreactor environment. Neutron imaging, combined with in-situ sample heating, enables near real-time tracking of hydrogen diffusion in YH x on the sub-millimeter scale. In this report, an overview of neutron imaging methodology and technologies are given in the context of recent spatial measures of hydrogen concentrations in similar metals hydrides. Additionally, the commissioning and operation of a custom-built compact dual-zone furnace is given along with details on the first two in-situ heating measurements of YH x performed over the 2020 and 2021 LANSCE operation cycles. In parallel with in-situ heating measurements, neutron computed tomography scans were performed to visualize hydrogen aggregates in post-heated YH x samples. Analysis and results from these neutron imaging measurements are given along with outlooks and plans for improving future hydrogen diffusion measurements at LANSCE.

47 OTHER INSTRUMENTATION↗

Isotopically resolved neutron total cross sections at intermediate energies

The neutron total cross sections σ tot of 16,18 O, 58 64 Ni, 103 Rh, and 112,124 Sn have been measured at the Los Alamos Neutron Science Center from low to intermediate energies (3 ≤ E lab ≤ 450 MeV) by leveraging wave-form-digitizer technology. The σ tot relative differences between isotopes are presented, revealing additional information about the isovector components needed for an accurate optical-model description away from stability. Digitizer-enabled σ tot -measurement techniques are discussed and a series of uncertainty-quantified dispersive optical model (DOM) analyses using these new data is presented, validating the use of the DOM for modeling light systems ( 16,18 O) and systems with open neutron shells ( 58,64 Ni and 112,124 Sn). Here, the valence-nucleon spectroscopic factors extracted for each isotope reaffirm the usefulness of high-energy proton reaction cross sections for characterizing depletion from the mean-field expectation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗