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NASA NTRS1990

Climate and atmospheric modeling studies. Climate applications of Earth and planetary observations. Chemistry of Earth and environment

The research conducted during the past year in the climate and atmospheric modeling programs concentrated on the development of appropriate atmospheric and upper ocean models, and preliminary applications of these models. Principal models are a one-dimensional radiative-convective model, a three-dimensional global climate model, and an upper ocean model. Principal applications have been the study of the impact of CO2, aerosols and the solar 'constant' on climate. Progress was made in the 3-D model development towards physically realistic treatment of these processes. In particular, a map of soil classifications on 1 degree x 1 degree resolution has been digitized, and soil properties have been assigned to each soil type. Using this information about soil properties, a method was developed to simulate the hydraulic behavior of soils of the world. This improved treatment of soil hydrology, together with the seasonally varying vegetation cover, will provide a more realistic study of the role of the terrestrial biota in climate change. A new version of the climate model was created which follows the isotopes of water and sources of water (or colored water) throughout the planet. Each isotope or colored water source is a fraction of the climate model's water. It participates in condensation and surface evaporation at different fractionation rates and is transported by the dynamics. A major benefit of this project has been to improve the programming techniques and physical simulation of the water vapor budget of the climate model.

Source record↗

NASA NTRS2008

Radioisotope Power: A Key Technology for Deep Space Exploration

A Radioisotope Power System (RPS) generates power by converting the heat released from the nuclear decay of radioactive isotopes, such as Plutonium-238 (Pu-238), into electricity. First used in space by the U.S. in 1961, these devices have enabled some of the most challenging and exciting space missions in history, including the Pioneer and Voyager probes to the outer solar system; the Apollo lunar surface experiments; the Viking landers; the Ulysses polar orbital mission about the Sun; the Galileo mission to Jupiter; the Cassini mission orbiting Saturn; and the recently launched New Horizons mission to Pluto. Radioisotopes have also served as a versatile heat source for moderating equipment thermal environments on these and many other missions, including the Mars exploration rovers, Spirit and Opportunity. The key advantage of RPS is its ability to operate continuously, independent of orientation and distance relative to the Sun. Radioisotope systems are long-lived, rugged, compact, highly reliable, and relatively insensitive to radiation and other environmental effects. As such, they are ideally suited for missions involving long-lived, autonomous operations in the extreme conditions of space and other planetary bodies. This paper reviews the history of RPS for the U.S. space program. It also describes current development of a new Stirling cycle-based generator that will greatly expand the application of nuclear-powered missions in the future.

Schmidt, George↗

NASA NTRS2009

Radioisotope Power: A Key Technology for Deep Space Explorations

Schmidt, George R.↗

DOE OSTI2026

Stable and tunable MeV $$\gamma$$-ray generation via dual-laser inverse Thomson scattering from a laser-plasma accelerator

Abstract Inverse Thomson scattering from laser-plasma accelerators offers a pathway to compact, tunable MeV $$\gamma$$ -ray sources for reduced-dose radiography and enhanced performance in nuclear resonance fluorescence (NRF)-based isotope identification. However, photon yield and spectral quality are often limited by constraints on interaction geometry and scatter-laser tunability. Here we demonstrate a MeV $$\gamma$$ -ray source based on a dual-laser inverse Thomson scattering configuration driven by a 100-TW laser-plasma accelerator. Electron beams tunable from 122 to 204 MeV with $$<5$$ mrad divergence and $$<1$$ mrad pointing stability generate $$\gamma$$ rays with peak energies from 276 keV to 1.2 MeV and yields up to $$2\times 10^{7}$$ photons per shot. By independently controlling the interaction position and the scatter-pulse duration, we experimentally match the scatter pulse to the walk-off-limited interaction length. Extending the scatter pulse to 200 fs increases photon production by approximately $$15\%$$ while maintaining operation in the linear Thomson regime, thereby preserving narrow spectral bandwidth and controlled radiation divergence. Radiographic characterization demonstrates MeV-level penetration and $$\approx 0.1$$ mm spatial resolution, while stable operation is sustained over multi-hour timescales across multiple days. These results show that interaction-length optimization provides a scalable strategy for improving photon yield, spectral control, and operational stability in compact laser-plasma-accelerator-driven $$\gamma$$ -ray sources.

Tsai, Hai-En↗

DOE OSTI2021

Experience with Inner Reflector Plug exchange in SNS

The Inner Reflector Plug (IRP) is a central component of the Spallation Neutron Source target monolith, which houses the mercury target and four liter-sized neutron moderator units. It is exposed to high-level radiation fields during routine operation and builds up significant activity. The IRP needs to be replaced due to moderator neutron poison and decoupler burn-out, which is used for shaping neutron pulses. The first IRP exchange took place in March 2018. The old IRP was extracted from the target monolith, providing space for the new one. It was split into three segments, each of which was handled separately. The lowest section of the IRP is the largest segment in size and in activity and is temporarily stored on-site for cool down before conduction post irradiation examination. In support of planning the replacement activities, a wide range of activation and transport analyses were performed. This included calculating isotope inventories and the radiation fields for each segment as it is extracted in storage casks, and the radiation field from the empty IRP pit in the target monolith. While the replacement was taking place, measurements were performed and later on compared to the calculations. During these studies, it was discovered that a significant contributor to the radiation field from the lower IRP segment is from photo-neutrons. Photo-nuclear physics was added to the analyses and calculated results compared well with measured dose rates.

Popova, Irina I.↗

NASA NTRS1991

Semiannual progress report, April - September 1991

Research conducted during the past year in the climate and modeling programs has concentrated on the development of appropriate atmospheric and upper ocean models, and preliminary applications of these models. Principal models are a one-dimensional radiative-convective model, a three dimensional global climate model, and an upper ocean model. Principal applications have been the study of the impact of CO2, aerosols, and the solar constant on climate. Progress was made in the 3-D model development towards physically realistic treatment of these processes. In particular, a map of soil classifications on 1 degree by 1 degree resolution has now been digitized, and soil properties have been assigned to each soil type. Using this information about soil properties, a method has been developed to simulate the hydraulic behavior of the soils of the world. This improved treatment of soil hydrology, together with the seasonally varying vegetation cover, will provide a more realistic study of the role of the terrestrial biota in climate change. A new version of the climate model was created which follows the isotopes of water and sources of water throughout the planet.

Source record↗

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 OSTI2023

New NBL Pu Isotopic Standards C137A and C136A as Working Reference Materials for Radiochronometry in Nuclear Forensics

Lawrence Livermore National Laboratory (LLNL) and the NBL Program Office (NBL PO) are collaborating on production of purified sub-units of the former NBS 936, 937 and 938 plutonium isotopic reference materials, which will be certified for plutonium isotopic composition and sold as certified reference materials (CRMs) C136A, C137A, and C138A, respectively. These reference materials are used throughout the United States and international community as standards for isotopic measurement method calibration and quality control and were first produced over 50 years ago. To reduce quantities of in-grown daughter products and potentially enable their use as Pu radiochronometry reference materials, the materials undergo a two-stage anion exchange purification to significantly reduce the quantities of U, Am, and Np in the source material. The purified Pu is aliquoted into ~1 mg units in the nitrate form, which will facilitate easier shipping and use compared to the 0.25 g parent units. The production process has been completed for the high- and medium- burnup isotopic standards C137A and C136A and will soon be performed for the weapons-grade Pu standard C138A. This report describes the measurement of trace actinide progeny of the Pu isotopes ( 234 U, 235 U, 236U, 241 Am and 237 Np) in purified C137A and 136A isotopic standards to provide informational values and assess the possibility of their use as working reference materials for radiochronometry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Angular Correlations of Gamma Rays from Fission Product Solution

Fission products from photon-induced fission are routinely used at Idaho National Laboratory as part of nuclear forensics activities. Typically, the focus is on fission products with relatively large fission yields (Ba-140, Mo-99, etc.). The nuclear data associated with the well-known isotopes have small uncertainties, and many have well-known angular correlations between emitted gamma-rays, if applicable. However, for isotopes with smaller fission yields or less intense gamma-ray emission intensities, the nuclear decay schemes and gamma-ray emission intensities may be less well-known. The Germanium Rotational Measurements for Angular Correlation (GeRMAC) system was designed to use two high-purity germanium (HPGe) detectors in a coincidence counting set-up but allows one of the HPGe detectors to rotate at a constant distance from a radioactive source, changing the relative angle between the two HPGe detectors. Angular correlations can then be determined from the relative photopeak areas between two gamma-rays emitted as part of the same nuclear decay. By recording the HPGe spectra in list mode, the angular correlations of gamma-rays emitted from complex sources, consisting of multiple isotopes, can be measured simultaneously and the individual isotope emissions can be isolated. Using the GeRMAC system, a multi-isotope fission product source, produced with photon-induced fission of U-238, was measured using a single rotational arc (180 degrees) to obtain the angular correlation between gamma-rays emitted by the large number of fission products contained in the solution with an angular accuracy of 1 degree. In particular, La-140 (38 gamma rays) and Nd-147 (26 gamma rays) are of interest to the nuclear forensics community.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

NASA NTRS1991

A dynamic isotope power system portable generator for the moon or Mars

The dynamic isotope power systems (DIPS) demonstration program is focused on a standardized 2.5 kWe portable generator for multiple uses on the lunar or Martian surface. A variety of potential remote or mobile applications has been identified by NASA. These applications include remote power to science packages, surface rovers for both short and extended duration missions, and backup to central base power. Reviews conducted on alternative power sources for these applications are described. These include the comparison of DIPS to regenerative fuel cells (RFCs). Recent work is presented refining the 2.5 kWe design to assure compatibility with the Martian environment while imposing only a minor mass penalty on lunar operations. This was accomplished by limiting temperatures, except in the heat source unit (HSU), to the nonrefractory materials regime and protecting the necessary refractories in the HSU from the environment. Design changes to the HSU are described. Work related to recent concerns regarding astronaut radiation doses is described. This work includes the bases for the calculations to determine the necessary shielding or operational limitations.

Johnson, Richard A.↗

DOE OSTI2020

Tracking Radioactive Isotopes in HVAC and Application for Hot Cell Analyses - 20155

In recent years, the surge in the number of isotope production facilities under design has increased the need to analyze isotope migration in facility Heating, Ventilation, and Air Conditioning (HVAC) during normal operations and accident scenarios. These facilities are used to produce isotopes for medical, security, and industrial applications and as such are subject to license and regulatory requirements 10CFR20, 10CFR30, 10CFR50, and 10CFR70. GOTHIC, a general-purpose thermal-hydraulics software package, includes the ability to model isotopic tracers, radioactive decay and isotope migration as well as HEPA and charcoal filters for isotope retention. A GOTHIC model was developed by Zachry Nuclear Engineering (ZNE) to examine the effect of negative room pressure, HEPA filtration, and HVAC fluctuations on radiation areas, hot cells and gloveboxes. Radioactive tracers were used to simulate the concentration of spills within contaminated areas, track the migration of isotopes of interest, and determine the isotopic retention and buildup on facility HEPA filters. A variety of isotopes with concern to dose (e.g., Kr-85, Sr-90, I-131, etc.), including their decay and progeny, are included in the analysis. Negative pressures are maintained in the regions of interest by a representative central HVAC system equipped with a volumetric fan that exhausts to the environment after a series of isolation valves and HEPA filters. GOTHIC is an industry trusted tool for providing engineering solutions for a variety of applications, including fission product tracking, aerosol and particulate transport and ventilation assessments. The software provides an integrated analysis environment that includes a graphical user interface (GUI) for constructing analysis models, a numerical solver that includes parallel processing capabilities and a post-processor for evaluating simulation results. It solves the conservation equations for mass, momentum and energy for multicomponent, multi-phase flow in lumped parameter and multi-dimensional geometries (1, 2, or full 3D), including the effects of turbulence, diffusion and buoyancy. It has been developed and maintained under a Quality Assurance program in compliance with the requirements of 10CFR50 Appendix B and applicable portions of ASME NQA-1 since 1995. GOTHIC has been used for assessing both forced and natural convection conditions for a wide range of applications, including: - Tracking concentration of hazardous gases and chemicals for habitability and safety assessments - Determining ventilation and filtration requirements and optimizing location and arrangement of these systems - Room heat-up, including diverse and Flexible coping strategies for Extended Loss of AC Power (FLEX/ELAP) - Equipment Qualification (EQ) A distinctive feature of GOTHIC is the ability to track many different fields/substances in a simulation, including user defined tracer elements, in the liquid, vapor and droplet fields as well as surfaces and filters. This capability allows GOTHIC to model fission product transport and release or the removal of particulates or harmful toxins from exhaust gases using a spray scrubber or other types of filtration systems. GOTHIC also includes models for engineered equipment, such as fans, filters, charcoal filters, dryers/demisters, dampers, etc. The aerosols and other filtered material are removed or accumulated in these components. The range of aerosol and radiological applications that GOTHIC has been used for includes: - Source Term: Primary Coolant (Equilibrium) Activity; Non-Water Coolant Source/Leakage. - Conditions for Iodine Re-evolution: Sump/Suppression Pool Conditions and pH; - RWST Conditions and pH. - Isotope Removal Mechanisms: Containment Sprayed and Unsprayed Region Mixing; Charcoal Filter Heating due to Iodine decay. - Radionuclide Transport and Decay: Post-LOCA Release in containment; Transport between connected Compartments and vent systems; Groundwater transport of radionuclides. - Non-Newtonian Fluid modeling for sludge, waste tanks, etc. ADAMS ML071581053 (titled 'Best Practice Guidelines for the use of CFD in Nuclear Reactor Safety Applications') poses guidelines for applying single phase CFD codes in nuclear reactor safety problems and GOTHIC is listed as a 'tool for 3D flows' and 'dispersal and deposition of radionuclides.' The Nuclear Quality Assurance (NQA) pedigree of GOTHIC is an important aspect for applications in the nuclear industry. The fundamental tracer models (convective transport, molecular and turbulent diffusion, removal mechanisms, etc.) have been verified using analytical solutions and validated against applicable separate effects tests. Also, GOTHIC has been benchmarked to many integrated effects tests, including Phebus FP (Fission Product). GOTHIC gives good agreement for the buildup and decay of fission products in Phebus Test 3. The model developed by ZNE demonstrates GOTHIC's applicability and acceptability for use in analyzing the migration and retention of radioactive isotopes and their progeny in normal operation and accident scenario analyses for isotope production facilities, hot cells, and gloveboxes. The tracer activities calculated by GOTHIC can then be used in downstream radiation transport and shielding codes like RADTRAD-NAI{sup C}, MCNP{sup R}, and MicroShield{sup R} to determine on-site and of-site doses. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Status of CHIP-TRAP: The Central Michigan University High-Precision Penning Trap

Precise and accurate atomic mass data provide crucial information for applications in a wide range of fields in physics and beyond, including astrophysics, nuclear structure, particle and neutrino physics, fundamental symmetries, chemistry, and metrology. The most precise atomic mass measurements are performed on charged particles confined in a Penning trap. Here, we describe the development, status, and outlook of CHIP-TRAP: the Central Michigan University high-precision Penning trap. CHIP-TRAP aims to perform ultra-high precision (~1 part in 10 11 fractional precision) mass measurements on stable and long-lived isotopes produced with external ion sources and transported to the Penning traps. Along the way, ions of a particular m/q are selected with a multi-reflection time-of-flight mass separator (MR-TOF-MS), with further filtering performed in a cylindrical capture trap before the ions are transported to a pair of hyperbolic measurement traps. In this paper, we report on the design and status of CHIP-TRAP and present results from the commissioning of the ion sources, MR-TOF-MS, and capture trap. We also provide an outlook on the continued development and commissioning of CHIP-TRAP.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2022

An Ensemble Approach to Computationally Efficient Radiological Anomaly Detection and Isotope Identification

Radiological source search is a challenging task involving detection and identification of weak sources in a constantly changing radiological background. As of now, many radiological source detection algorithms have been proposed; however, their computational complexity, and hence reliance on power intensive processing units inhibit low-power applications of radiological source search systems. In this work, we introduce the anomaly filter (AF) algorithm; a computationally light, yet effective time-series source detection algorithm based on exponential weighted moving average (EWMA) and Poisson deviance statistics. Then, we demonstrate that the proposed algorithm can be used in ensemble with other more computationally intensive source detection and identification algorithms to achieve both increased detection performance and reduced power consumption. The proposed AF algorithm and the ensemble algorithms were thoroughly benchmarked against several existing source detection and identification algorithms. The results show that the AF algorithm outperforms existing conventional source detection algorithms, and the ensemble approach improves the overall performance of existing source detection and isotope identification algorithms. Furthermore, the AF algorithm and the Non-negative Matrix Factorization approach based source identification (NMF-ID) algorithm were combined and implemented on a singleboard microcontroller and the power consumption was measured. This ensemble algorithm reduced the power consumption of the NMF-ID algorithm almost by a factor of 100, while improving the detection performance of the overall system.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2022

Variability in observed stable water isotopes in snowpack across a mountainous watershed in Colorado

In this study, isotopic information from 81 snowpits was collected over a 5-year period in a large, Colorado watershed. Data spans gradients in elevation, aspect, vegetation, and seasonal climate. They are combined with overlapping campaigns for water isotopes in precipitation and snowmelt, and a land-surface model for detailed estimates of snowfall and climate at sample locations. Snowfall isotopic inputs, describe the majority of δ18O snowpack variability. Aspect is a secondary control, with slightly more enriched conditions on east and north facing slopes. This is attributed to preservation of seasonally enriched snowfall and vapour loss in the early winter. Sublimation, expressed by decreases in snowpack d-excess in comparison to snowfall contributions, increases at low elevation and when seasonal temperature and solar radiation are high. At peak snow accumulation, post-depositional fractionation appears to occur in the top 25 ± 14% of the snowpack due to melt-freeze redistribution of lighter isotopes deeper into the snowpack and vapour loss to the atmosphere during intermittent periods of low relative humidity and high windspeed. Relative depth of fractionation increases when winter daytime temperatures are high and winter precipitation is low. Once isothermal, snowpack isotopic homogenization and enrichment was observed with initial snowmelt isotopically depleted in comparison to snowpack and enriching over time. The rate of δ18O increase (d-excess decrease) in snowmelt was 0.02‰ per day per 100-m elevation loss. Isotopic data suggests elevation dictates snowpack and snowmelt evolution by controlling early snow persistence (or absence), isotopic lapse rates in precipitation and the ratio of energy to snow availability. Hydrologic tracer studies using stable water isotopes in basins of large topographic relief will require adjustment for these elevational controls to properly constrain stream water sourcing from snowmelt.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Review of capture cross sections relevant for intentional nuclear forensics

The NA-22 Intentional Forensics Venture is developing a system for tagging nuclear fuel using various methods of information encoding. One of the main methods under development is the insertion of isotopically enriched tracers into the fuel. In order to aid in the understanding of the neutronic performance of these taggants, we assess the quality of the nuclear data underpinning simulations, which are driven by the neutron-capture cross sections. We present these cross sections of naturally occurring isotopes of the elements provided in the neutron sublibrary of the planned ENDF/B-VIII.1 Feb. 2023 library release. We make this assessment using a rubric designed for this effort, which quantifies orthogonal features related to the overall quality. The quality metric highlights 6 aspects: experimental data, resonance evaluations, integral metrics, covariances, fission products, and documentation. We focus on energy ranges relevant for reactor applications. We also discuss additional sources for new, high-quality cross-section data that may be utilized on the time scale of the venture, including existing global data, new experiments, and computational methods. Finally, overall outlook is presented with conclusions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2021

High efficiency laser resonance ionization of plutonium

Three-step resonance photoionization spectra of plutonium have been studied with Ti:Sapphire lasers for the development of efficient laser ionization schemes for ultra-trace analysis of Pu isotopes by resonance ionization mass spectrometry. We observed eighteen intermediate excited states of even parity in the energy range 35568–36701 cm -1 , thirteen of them have not been previously documented, and a larger number of high-lying excited states and autoionizing states of odd-parity between 48238 and 49510 cm -1 . Three-color, three-photon ionization schemes via six intermediate states were evaluated under similar ion source operating conditions. This led to a highly efficient three-step scheme with an overall ionization efficiency of 51.1±1.3%, which is an order of magnitude improvement over the previously reported ionization efficiency for Pu.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2021

Impact of Spontaneous Fission Neutron Emission Energy on Neutron Detector Response

A parametric study was simulated in MCNP to investigate the impact of spontaneous fission neutron energy on neutron detector response. A total of 880 configurations were simulated by varying 3 He pressure and polyethylene reflector thickness for 8 different isotopes. Results showed that deviations between the simulated isotopes become more prevalent at higher energies with 238 U showing the greatest deviation. It was also observed that configurations comparable to most detection setups, 10 atm and 6 - 8 cm polyethylene, were closer to the upper bound of deviations from a 252 Cf. 240 Pu, a common spontaneous fission source of interest, ranged from 2% - 3% within this space. This suggests that further investigation is required to determine exact correction factors when calibrating neutron detectors with a 252 Cf. Although demonstrated here for a 4π-detection system, future plans include simulating a more detailed model of the MC-15 detection setup to determine exact correction factors for future experiments.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

State-of-the-art γ-ray assay of 86 Y for medical imaging

An emerging direction in nuclear medicine is the coupling of a therapeutic isotope with an imaging isotope to form a so-called theranostic pair, which allows one to quantitatively track and image the delivery of the therapeutic isotope. 90 Y is used in several therapy applications and a convenient candidate imaging partner is the positron emitter 86 Y. A 27.6 MBq source of 86 Y was produced at the University of Wisconsin and assayed with the Gammasphere array at Argonne National Laboratory. Over 200 γ-ray transitions were identified, more than double that which was previously known. In conclusion, the positron emission probability inferred from the present level scheme leads to 27.9(12)%, an important (≈14%) reduction with respect to the previously recommended value.

59 ≤ A ≤ 89↗