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At least 163 records · Page 9

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DOE OSTI2024

Revisiting the Optical Spectrum of the Plutonyl Ion (PuO 2 ) 2+ in 1 M HClO 4

The analysis of the solution absorption spectrum of the plutonyl ion in an aqueous environment was given by Eisenstein and Pryce (E&P) in 1968. In 2011 a new spectrum was published of the (PuO 2 ) 2+ ion in 1 M HClO 4 . We have been provided with the original data of this spectrum and have found in the data a previously unreported low-lying transition at 7385 cm –1 which we have assigned as a magnetic dipole transition. We have fit most of the near-infrared and optical transitions with Gaussian fits and tabulated a new energy level list up to 22,000 cm –1 which mostly agrees with the data of E&P. We assumed a crystal field of D ∞h (only axial symmetry) and utilized the intensity calculations published for the isoelectronic (NpO 2 ) 1+ ion using a complete basis set for the 5f 2 problem including the Coulombic, spin–orbit as well as the crystal field Hamiltonian. Our results differ substantially from those of E&P. Subsequently, we used a truncated Hamiltonian to try to establish the effects of assuming the σ antibonding orbitals are at such high energies that we can ignore their contributions to the lower lying φ and δ orbitals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Transuranium Sulfide via the Boron Chalcogen Mixture Method and Reversible Water Uptake in the NaCu T S 3 Family

The behavior of 5f electrons in soft ligand environments makes actinides, and especially transuranium chalcogenides, an intriguing class of materials for fundamental studies. Due to the affinity of actinides for oxygen, however, it is a challenge to synthesize actinide chalcogenides using non-metallic reagents. Using the Boron Chalcogen Mixture (BCM) method, we achieved the synthesis of the transuranium sulfide NaCuNpS 3 starting from the oxide reagent, NpO 2 . Via the same synthetic route, the isostructural composition of NaCuUS 3 was synthesized and the material contrasted with NaCuNpS 3 . Single crystals of the U-analog, NaCuUS 3 , were found to undergo an unexpected reversible hydration process to form NaCuUS 3 ·xH 2 O (x ≈ 1.5). Here, a large combination of techniques was used to fully characterize the structure, hydration process, and electronic structures, specifically a combination of single crystal, powder, high temperature powder X-ray diffraction, extended X-ray ab-sorption fine structure, infrared, and inductively coupled plasma spectroscopies, thermogravimetric analysis, and density functional theory calculations. The outcome of these analyses enabled us to determine the composition of NaCuUS 3 ·xH 2 O and obtain a structural model that demonstrated the retention of the local structure within the [CuUS 3 ] – layers throughout the hydration-dehydration process. Band structure, density of states, and Bader charge calculations for NaCuUS 3 , NaCu-US 3 ·xH 2 O, and NaCuNpS 3 along with X-ray absorption near edge structure, UV-vis-NIR and work function measurements on ACuUS 3 (A = Na, K, and Rb) and NaCuUS 3 ·xH 2 O samples were carried out to demonstrate that electronic properties arise from the [CuTS 3 ] – layers and show surprisingly little dependence on the interlayer distance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Preparation of Neptunyl and Plutonyl Acetates To Access Nonaqueous Transuranium Coordination Chemistry

Uranyl diacetate dihydrate is a useful reagent for the preparation of uranyl (UO 2 2+ ) coordination complexes, as it is a well-defined stoichiometric compound featuring moderately basic acetates that can facilitate protonolysis reactivity, unlike other anions commonly used in synthetic actinide chemistry such as halides or nitrate. Despite these attractive features, analogous neptunium (Np) and plutonium (Pu) compounds are unknown to date. Here, in this study, a modular synthetic route is reported for accessing stoichiometric neptunyl(VI) and plutonyl(VI) diacetate compounds that can serve as starting materials for transuranic coordination chemistry. The new NpO 2 2+ and PuO 2 2+ complexes, as well as a corresponding molecular UO 2 2+ complex, are isomorphous in the solid state, and in solution show similar solubility properties that facilitate their use in synthesis. In both solid and solution state, the +VI oxidation state (O.S.) is maintained, as demonstrated by vibrational and optical spectroscopy, confirming that acetate anions stabilize the oxidizing, high-valent +VI states of Np and Pu as they do for the more stable U(VI). All three acetate salts readily react with a model diprotic ligand, affording incorporation of U(VI), Np(VI), and Pu(VI) cores into molecular coordination compounds that occurs concomitantly with elimination of acetic acid; the new complexes are high-valent, yet overall charge neutral, facilitating entry into nonaqueous chemistry by rational synthesis. Computational studies reveal that the dianionic ligand framework assists in stabilizing the +VI O.S. via donation to the 5f shells of the actinides, highlighting the potential usefulness of protonolysis reactivity toward preparation of stabilized high-valent transuranic species.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Benchmarking performance changes in the simulation of extratropical modes of variability across CMIP generations

In this work, we evaluate extratropical modes of variability in the three most recent phases of the Coupled Model Intercomparison Project (CMIP3, 5, and 6) to gauge improvement of climate models over time. A suite of high-level metrics is employed to objectively evaluate how well climate models simulate the qobserved Northern Annular Mode (NAM), North Atlantic Oscillation (NAO), Pacific North America pattern (PNA), Southern Annular Mode (SAM), Pacific Decadal Oscillation (PDO), North Pacific Oscillation (NPO), and North Pacific Gyre Oscillation (NPGO). We apply a Common Basis Function (CBF) approach that projects model anomalies onto observed empirical orthogonal functions (EOFs), together with the traditional EOF approach, to CMIP Historical and AMIP models. We find simulated spatial patterns of those modes have been significantly improved in the newer models, although the skill improvement is sensitive to the mode and season considered. We identify some potential contributions to the pattern improvement of certain modes (e.g., the Southern Hemisphere jet and High-top vertical coordinate), however the performance changes are likely attributed to gradual improvement of the base climate and multiple relevant processes. Less performance improvement is evident in the mode amplitude of these modes and systematic overestimation of the mode amplitude in spring remains in the newer climate models. We find that the post-dominant season amplitude errors in atmospheric modes are not limited to coupled runs but are often already evident in AMIP simulations. This suggests that rectifying the egregious post-dominant season amplitude errors found in many models can be addressed in an atmospheric-only framework making it more tractable to address in the model development process.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Report on the Analysis of Plutonium-238 Oxide, Campaign #P5PO

Oak Ridge National Laboratory (ORNL) is currently producing Plutonium-238 oxide for NASA space programs. Through the irradiation of NpO 2 pellets in the High Flux Isotope Reactor (HFIR), the production of Pu-238 oxide will be used for electrical power and heat on NASA spacecraft such as the Curiosity Mars Rover and the Voyager 1 and 2. The Transuranium Analytical Laboratory (TAL) leads the analytical effort for this project, which includes the dissolution of plutonium product oxide (PUP) and the analysis of the dissolved product solution using both radiological and inductively coupled plasma mass spectrometry (ICP-MS) techniques that are required to meet product specifications. The Transuranic Analytical Laboratory received three samples of Pu-238 oxide for analysis in January of 2022. This report documents the analytical protocols performed by the TAL along with the results produced from said analytical protocols. This report also includes a comparison with the general-purpose heat source (GPHS) specifications.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2022

Neptunium mononitride as a target material for Pu-238 production

Deep space exploration requires specialized sources for both thermal and power applications. Radioactive decay heat of plutonium-238 (238Pu) provides these sources in the form of radioisotope thermoelectric generators (RTGs). The 238 Pu is produced via neutron capture reaction involving neptunium-237 ( 237 Np) target material. Continual optimization of 237 Np target materials and evaluation of potential alternative targets for production of 238 Pu RTGs are advantageous for meeting ongoing space power system resource requirements. Current production of 238 Pu for RTGs for the United States space program utilizes neptunium dioxide ( 237 NpO 2 ) targets; however, the use of neptunium mononitride ( 237 NpN) presents an opportunity to increase the mass of 237 Np per target compared to the dioxide form, as well as increase the thermal conductivity of the target. To assess the viability of a 237 NpN target material, the material chemistry must be thoroughly evaluated, including synthesis methods and dissolution and reprocessing schemes. This review presents a summary of synthesis pathways for 237 NpN based on published literature on actinide mononitrides. Specific literature on 237 NpN is limited, necessitating evaluation of other actinide systems to gather parallels. This suggests a need for additional experimental studies on 237 NpN. A particular limitation in the existing literature is a lack of information on the differences in material characteristics, such as morphology, particle size, and trace chemical impurities, as a function of synthesis method. These parameters may affect subsequent reactor performance or dissolution of irradiated targets. The evaluation of existing literature is presented with a focus on the efficacy of 237 NpN targets for 238 Pu production.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

NASA NTRS1987

Electrically Conductive, Heat-Resistant Paint

Improved, sprayable, thermal- and electrostatic-discharge-control coating for titanium possesses excellent adhesion and high resistance to both vibration and thermal shock. Coating is improved formulation of one described in "High-Temperature Coatings for Titanium" (NPO-16222).

Hribar, V. F.↗

NASA NTRS1988

Calculating Atmospheric Effects In Satellite Imagery: Part 2

Practical computational techniques developed. Report discusses practical considerations of calculation of three-dimensional radiative transfer. Extension of earlier theoretical developments described in "Calculating Atmospheric Effects in Satellite Imagery" NPO-16373.

Diner, David J.↗

NASA NTRS1988

Phase-Locked Semiconductor Lasers With Separate Contacts

Individual current feeds enable better uniformity and flexible control. Separate contacts for lasers in array enable control of output radiation pattern and compensation of manufacturing nonuniformities among lasers. Concept of separate current control described for two-laser array in "Semiconductor Laser Phased Array" (NPO-15963).

Katz, Joseph↗

NASA NTRS1988

Substrates For High-Temperature Superconductors

Proposed hot-dipping process prepares materials well suited to serve as substrates for high-temperature superconductors. Makes it possible to produce substrates combining properties needed for given application, such as flexibility, strength, long grains, and <001> crystal orientation. Properties favor growth of superconductive films carrying high current and fabricated in variety of useful shapes. Used in making solar cells, described in "Hot-Dipped Metal Films as Epitaxial Substrates" (NPO-15904).

Shlichta, Paul J.↗

NASA NTRS1989

Automatic Frequency Control For DMSK Receiver

Report discusses performance of automatic frequency-control (AFC) subsystem of differential minimum-shift-keying receiver described in "DMSK Receiver for Moblile/Satellite Service," NPO-16659. Describes efforts to quantify behavior of system during acquisition of carrier signal; including theoretical analysis leading to numerical simulation, and measurements of performance of receiving equipment.

Davarian, Faramaz↗

NASA NTRS1989

Improved Algorithm For Finite-Field Normal-Basis Multipliers

Improved algorithm reduces complexity of calculations that must precede design of Massey-Omura finite-field normal-basis multipliers, used in error-correcting-code equipment and cryptographic devices. Algorithm represents an extension of development reported in "Algorithm To Design Finite-Field Normal-Basis Multipliers" (NPO-17109), NASA Tech Briefs, Vol. 12, No. 5, page 82.

Wang, C. C.↗

NASA NTRS1989

Photovoltaic-Driven Multiple-Quantum-Well Modulator

Proposed high-performance spatial light modulator consists of multiple-quantum-well, strain-layer superlattice similar to one described in accompanying article, "Strain-Layer-Superlattice Light Modulator" (NPO-16915). Device differs from other one, operates in transmission rather than in resonant reflection and therefore includes only one stack of GaAs/InAs layers having total thickness less than penetration depth (1 to 2 micrometer) of optical modulating signal. Alternating, semitransparent semiconductor layers contain space-charge barriers forming quantum wells. Modulating light (with photon energy greater than semiconductor band gap) induces photovoltaic action, which affects transmission of modulated light (having photon energy less than band gap).

Maserjian, Joseph↗

NASA NTRS1989

Improved Flow-Controlling Vortex Generator

Symmetrical tangential streams control flow of radial primary streams. Vortex generator uses small secondary stream of fluid to control normally-larger primary stream. Improved version of vortex generator described in "Variable Control Port for Fluidic Control Device," (NPO-16603). Secondary, or control, flows entering tangentially through diametrically opposite ports set up swirling motion restraining primary flow. Pressure of secondary fluid in relation to primary fluid controlling factor. Like valve, vortex generator varies rate of flow of primary fluid from maximum value down to zero. When properly designed, requires low pressure differential between primary and secondary streams and expends relatively small amount of secondary fluid.

Collins, Earl R., Jr.↗

NASA NTRS1989

Twisted Pair Of Insulated Wires Senses Moisture

Sensitivity of electronic moisture sensor to low levels of moisture increased by new electrode configuration. Moisture-sensing circuit described in "Low-Cost Humidity Sensor" (NPO-16544). New twisted pair of wires takes place of flat-plate capacitor in circuit. Configuration allows for thermal expansion and contraction of polymer while maintaining nearly constant area of contact between polymer and wires.

Laue, Eric G.↗

NASA NTRS1989

Effects Of Turbulence On Ignition

Report presents theoretical study of effects of turbulence on ignition of drops of single-component liquid fuel. Closely related to article, "Turbulence and Evaporation in Clusters of Drops" (NPO-17323). Uses theoretical model for evaporation and model for ignition developed previously. Radial velocity, va, of gas at surface of sphere of influence taken as algebraic combination of rate of evaporation and speed with which radius changes. Weighting factors of algebraic combination are such that in dilute spray, all new vapor coming from drops trapped in cluster, whereas in dense spray where evaporation strong, maximum new vapor escapes to ambient.

Bellan, Josette↗

NASA NTRS1989

Insulated Honeycomb

Proposed insulated honeycomb structure similar to reinforced honeycomb structure described in NPO-17538. Panels of insulated honeycomb used to make supports for solar-energy collectors and radar antennas.

Bhat, Balakrishna T.↗

NASA NTRS1990

Convective Evaporation Of Clusters Of Drops

Report presents results of continuing theoretical research in behaviors of sprayed liquid fuels at temperatures characteristic of furnaces. Two earlier papers arising from this investigation described in "Evaporation of Dense Fuel Sprays" (NPO-16954).

Bellan, Josette↗