Laser isotope separation of Gd-152 and Gd-160
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This report presents the progress achieved on our chlorine isotope separation efforts in the CRADA #667 agreement. We used a microchannel distillation (MCD) packing structure to enrich HCl isotopes (H35Cl, H37Cl) and an isotachophoresis (ITP) separation to enrich ionic chloride species (35Cl- and 37Cl-). A 2 m tall MCD column was constructed and achieved 264 separation stages over several days, which is well above the goal of 50 stages outlined in the CRADA. The resulting height equivalent to a theoretical plate (HETP) was 0.76 cm. ITP tests were run ~ 24 hours and achieved a single-stage separation factor of 1.559.
In a chloride molten salt fast reactor (Cl-MSFR), the fuel salt might be comprised of a specific eutectic composition of alkali and alkaline chlorides that solubilize major and minor actinide chlorides as the fertile component(s). Each of the chloride species contain the natural abundance ( 35 Cl ~76% and 37 Cl ~24%) of the two stable isotopes of chlorine 35 Cl and 37 Cl. There has been an ongoing controversy for the operation of the Cl-MSFRs concerning the potential of the 35 Cl(n,γ) 36 Cl, 35 Cl(n,p) 35 S, 35 Cl(n,α) 32 S reactions to produce 36 Cl, 32 S, and 32 P at relevant energies [Bulmer 1956]. The undesirable attributes of irradiated 35 Cl are enumerated further below.
Precipitation may form in humid containers undergoing rapid depressurization. This precipitation may be liquid, i.e. fog, if the dewpoint is crossed above the freezing point of water, or direct snow crystallization if the dewpoint is crossed below the freezing point. Accurate modeling of this effect is potentially important for rapidly ascending vented containers in aircraft, spacecraft, and launch vehicles, as well as rapidly depressurizing vacuum chambers. A transient thermodynamics model of precipitation formation during the rapid depressurization of a container was developed in python. The model is written for a generic container and includes an optional water pool and water vapor source. Details of the model and results from several example cases spanning the full capabilities of the model, including a validation case, will be presented. Although the model is not novel, in contrast to prior works, this one was treated as a case study of the assistance of AI Large Language Models (LLMs) to create physical models. Impressions, performance, time, and cost of using AI for this task will be discussed.
Temperature of discharging high-power-density primary battery maintained below specified level by evaporation of suitable liquid from jacket surrounding battery, according to proposal. Pressure-relief valve regulates pressure and boiling temperature of liquid. Less material needed in cooling by vaporization than in cooling by melting. Technique used to cool batteries in situations in which engineering constraints on volume, mass, and location prevent attachment of cooling fins, heat pipes, or like.
Vapor-liquid interfaces drive many important phenomena in cryogenic fluid management, including heat transfer, evaporation, and capillary flow. Design of cryogenic fluid systems, such as propellant storage, requires accurate predictions of fluid behavior, including evaporation rates. Many models have been proposed for heat and mass transfer at vapor liquid interfaces, but the accuracy of these models in the context of cryogenic fluids has not been performed. We use molecular dynamics simulations, which allow for nanometer scale resolution of fluid phenomena, to evaluate the accuracy of a variety of vapor-liquid boundary conditions at evaporating and condensing interfaces. We find that an anisotropic temperature distribution is a critical ingredient for accurate prediction of intensive evaporation and condensation.
A human spacecraft ATCS—especially one using single-phase coolant loops exposed to cabin atmospheric conditions—requires periodic degassing and refilling to support long-duration missions of 15 to 30 years. During initial fill operations, system maintenance, gas permeation, and quick-disconnect mating or de-mating, small amounts of gas can gradually enter the coolant system over time. This can lead to degraded heat transfer performance, pump cavitation, and potentially pump vapor lock if a significant gas volume accumulates over time. Additionally, system leaks and routine fluid sampling can gradually reduce accumulator volumes to unacceptable levels, requiring periodic refills. In more severe cases, catastrophic changes in fluid composition may necessitate emergency draining, refilling, and degassing to ensure continued system functionality. These risks were identified and mitigated on the ISS ITCS through the development of a dual-membrane degasser ORU and a Fluid Servicer System ORU for coolant refilling. These systems were developed for the fully water-based ISS ITCS Coolant[1]. The Gateway space station, the first permanent human habitat in lunar orbit, uses a propylene-glycol/water coolant mixture, which has significantly different fluid properties compared to pure water. Because microgravity degassing technologies are sensitive to fluid surface tension and viscosity, existing ISS hardware is not suitable for servicing a propylene-glycol-based TCS. Unlike the ISS, the Gateway will operate in a higher-radiation environment and must meet stricter mass constraints due to its location outside of low earth orbit. This Government Furnished Equipment (GFE) flight hardware project aims to develop a lightweight, radiation-resistant Coolant Servicer System (CSS) capable of degassing and refilling Gateway’s propylene-glycol water-based IATCS.
A human spacecraft ATCS—especially one using single-phase coolant loops exposed to cabin atmospheric conditions—requires periodic degassing and refilling to support long-duration missions of 15 to 30 years. During initial fill operations, system maintenance, gas permeation, and quick-disconnect mating or de-mating, small amounts of gas can gradually enter the coolant system over time. This can lead to degraded heat transfer performance, pump cavitation, and potentially pump vapor lock if a significant gas volume accumulates over time. Additionally, system leaks and routine fluid sampling can gradually reduce accumulator volumes to unacceptable levels, requiring periodic refills. In more severe cases, catastrophic changes in fluid composition may necessitate emergency draining, refilling, and degassing to ensure continued system functionality. These risks were identified and mitigated on the ISS ITCS through the development of a dual-membrane degasser ORU and a Fluid Servicer System ORU for coolant refilling. These systems were developed for the fully water-based ISS ITCS Coolant[1]. The Gateway space station, the first permanent human habitat in lunar orbit, uses a propylene-glycol/water coolant mixture, which has significantly different fluid properties compared to pure water. Because microgravity degassing technologies are sensitive to fluid surface tension and viscosity, existing ISS hardware is not suitable for servicing a propylene-glycol-based TCS. Unlike the ISS, the Gateway will operate in a higher-radiation environment and must meet stricter mass constraints due to its location outside of low earth orbit. This Government Furnished Equipment (GFE) flight hardware project aims to develop a lightweight, radiation-resistant Coolant Servicer System (CSS) capable of degassing and refilling Gateway’s propylene-glycol water-based IATCS.
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Two epitaxial growth experiments of Hg 1-x Cd x Te layers on (100) CdTe substrates in closed ampoules using HgI 2 as a transport agent have been performed during the USML-1 mission. The characterization results to date demonstrate a considerable improvement of the space-grown epitaxial layers relative to ground-control specimens in terms of morphology, compositional uniformity, and structural micro homogeneity. These results show the effects of microgravity and fluid dynamic disturbances on-ground on the deposition and growth processes. The continued analysis of this technologically important system is designed to further elucidate the observed crystallographic improvements and their relation to mass flow.
Abstract Spin defects in van der Waals materials offer a promising platform for advancing quantum technologies. Here, we propose and demonstrate a powerful technique based on isotope engineering of host materials to significantly enhance the coherence properties of embedded spin defects. Focusing on the recently-discovered negatively charged boron vacancy center ($${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − ) in hexagonal boron nitride (hBN), we grow isotopically purified h 10 B 15 N crystals. Compared to$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − in hBN with the natural distribution of isotopes, we observe substantially narrower and less crowded$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − spin transitions as well as extended coherence timeT 2 and relaxation timeT 1 . For quantum sensing,$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − centers in our h 10 B 15 N samples exhibit a factor of 4 (2) enhancement in DC (AC) magnetic field sensitivity. For additional quantum resources, the individual addressability of the$${{{{{{{{\rm{V}}}}}}}}}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$ V B − hyperfine levels enables the dynamical polarization and coherent control of the three nearest-neighbor 15 N nuclear spins. Our results demonstrate the power of isotope engineering for enhancing the properties of quantum spin defects in hBN, and can be readily extended to improving spin qubits in a broad family of van der Waals materials.
Hydrogen transfer is a critical component of many chemical and biological processes. The ratio of rate constants for hydrogen and deuterium transfer defines the H/D kinetic isotope effect (KIE), which is a powerful tool for elucidating hydrogen transfer mechanisms. Interpretation of experimental H/D KIEs relies on accurate and affordable computational methods. However, due to their light mass, hydrogen and deuterium can undergo tunneling, which is challenging to describe in multidimensional molecular systems. Herein, we introduce the nuclear–electronic orbital general rate theory (NEO-GRT), which enables the efficient prediction of H/D KIEs based on full-dimensional molecular quantum chemistry calculations. The NEO-GRT approach describes the hydrogen transfer rate constant with a general expression that spans the vibrationally adiabatic and nonadiabatic hydrogen tunneling regimes. The input quantities are computed using NEO density functional theory, which treats the transferring hydrogen or deuterium nucleus quantum mechanically on the same level as the electrons. We investigate two intramolecular proton transfer reactions in organic molecules at temperatures down to 50 K to evaluate the performance of NEO-GRT by comparison to transition state theory and ring-polymer instanton theory. The KIEs computed with NEO-GRT agree with those calculated using ring-polymer instanton theory for the full-dimensional molecular systems at the same level of electronic structure theory. This agreement indicates that NEO-GRT captures the deep hydrogen tunneling effects, in contrast to transition state theory, which neglects such effects. Given its relatively low computational cost, NEO-GRT is a promising approach for predicting H/D KIEs in large organic and organometallic systems.
Ivuna-type (CI) carbonaceous chondrites are primitive meteorites whose relative elemental abundances closely match the solar photosphere 1 , making them critical benchmarks for the bulk chemical and isotopic composition of the planet-forming disk. Recent sample-return missions to Ryugu 2 and Bennu 3 have enabled direct laboratory analysis of these rubble-pile CI-like asteroids 4 , formed from the reaccumulated fragments of once-larger parent bodies. As such, they may retain a broader spectrum of primordial nucleosynthetic components than is preserved in known meteorites. Here, we report the nucleosynthetic compositions of silicon (μ 30 Si), magnesium (μ 26 Mg*), and iron (μ 54 Fe), three of the four most abundant planet-building elements, in samples from Ryugu and Bennu, along with the newly discovered Oued Chebeika 002 CI chondrite 5 . In contrast to the isotopic homogeneity of CI chondrites, Ryugu and Bennu preserve resolvable μ 26 Mg* and μ 30 Si heterogeneity, revealing μ 26 Mg*- and μ 30 Si-rich nucleosynthetic components not sampled in meteorites. These components may reflect the preservation of previously unsampled primordial isotopic signals, prior to thermal processing 6,7 and late infall of primordial molecular cloud material to the outer disk 8,9 . Additionally, Ryugu particle C0002 exhibits a μ 26 Mg*-poor and μ 54 Cr-rich signature, consistent with incorporation of presolar material from massive supernovae 10,11 . Ryugu and Bennu samples define one end of a μ 54 Fe–μ 30 Si array among carbonaceous asteroid materials 9 , suggesting that the isotopic compositions of these asteroidal materials reflect mixing between early disk isotopic components identified in this study and material derived from the outermost disk 9 . This observation demonstrates that materials with solar chemical abundances can nonetheless exhibit markedly distinct nucleosynthetic signatures. Thus, Ryugu and Bennu samples are critical records of nucleosynthetic diversity among carbonaceous asteroids and underscore the value of sample-return missions in accessing primitive isotopic signatures absent from meteorite collections.
Tungsten monophosphide (WP) has been reported to superconduct below 0.8 K, and theoretical work has predicted an unconventional Cooper pairing mechanism. Here we present data for WP single crystals grown by means of chemical vapor transport (CVT) of WO3, P, and I2. In comparison to synthesis using WP powder as a starting material, this technique results in samples with substantially decreased low-temperature scattering and favors a more three-dimensional morphology. We also find that the resistive superconducting transitions in these samples begin above 1 K. Variation in Tc is often found in strongly correlated superconductors, and its presence in WP could be the result of influence from a competing order and/or a non-s-wave gap.
The method of salt-assisted vapor–liquid–solid (VLS) growth is introduced to synthesize 1D nanostructures of trichalcogenide van der Waals (vdW) materials, exemplified by niobium trisulfide (NbS 3 ). The method uses a unique catalyst consisting of an alloy of Au and an alkali metal halide (NaCl) to enable rapid and directional growth. High yields of two types of NbS 3 1D nanostructures, nanowires and nanoribbons, each with sub-ten nanometer diameter, tens of micrometers length, and distinct 1D morphology and growth orientation are demonstrated. Strategies to control the location, size, and morphology of growth, and extend the growth method to synthesize other transition metal trichalcogenides, NbSe 3 and TiS 3 , as nanowires are demonstrated. Finally, the role of the Au–NaCl alloy catalyst in guiding VLS synthesis is described and the growth mechanism based on the relationships measured between structure (growth orientation, morphology, and dimensions) and growth conditions (catalyst volume and growth time) is discussed. These results introduce opportunities to expand the library of emerging 1D vdW materials to make use of their unique properties through controlled growth at nanoscale dimensions.
The corrosion behavior of structural alloys SS304 and IN617 when exposed to vapors of MgCl 2 molten salt at 764 °C for 100 h in an argon atmosphere was investigated as a function of the level of oxidizing impurities (e.g., NaOH) present in the salt. Increasing the concentration of oxidizing impurities in the salt caused an increase in corrosion in both structural alloys, as measured by Cr depletion layers. A poorly adhered oxide scale layer containing Mg, Al, and Cr was observed on the surface of the metals, and local attack was observed as well. The Ni-based IN617 showed lower Cr depletion and less scale formation than the Fe-based SS304. These results demonstrate that oxidizing impurities in the molten salt will impact the vapor phase corrosion for structural members exposed to the molten salt headspace. This finding is highly relevant for understanding the effects of the vapor phase in molten salt applications, including molten salt thermal energy storage, molten salt nuclear reactors, and molten salt electrochemistry.
The opportunity to explore the properties of short-lived atomic nuclei—or rare isotopes—in laboratories has enabled discoveries across the sciences related to the nature of the nuclear force and the limits of nuclear existence, the origin of the elements in the Universe, the cosmic matter–antimatter asymmetry, and the application of rare isotopes for society and the nation. The newest-generation Facility for Rare Isotope Beams (FRIB) on the campus of Michigan State University commenced operations in May 2022 as a user facility for the US Department of Energy, Office of Science, Office of Nuclear Physics. FRIB provides fast, stopped, and reaccelerated beams of rare isotopes for measurements, serving a 1,800-member-strong community of scientists from around the world. Here, this article reviews some of the first results from FRIB, showcasing the breadth of the science discoveries that have already occurred while the facility is ramping up to full capability.
In the event of a leak of liquid hydrogen, a pool can form that vaporizes, disperses, and eventually dilutes to a non-flammable mixture. In this work, we describe fast-running models for the pooling and vaporization of liquid hydrogen in a steady cross-wind. Several pooling models from the literature are compared to solve for the flow and extent of the pool. The size of the pool can serve as the source for a separate dispersion model, which builds upon the existing one-dimensional Gaussian plume model in HyRAM+. Additional terms for the effects of a cross-wind on momentum and entrainment were added so that the model could handle the effects of a cross-wind on a low-speed flow. The models are compared to experimental data on pooling extent and downwind dispersion for steady flow rates of liquid hydrogen in a steady cross-wind. In the two compared experiments, liquid flow rates of 15 and 45 g/s were spilled onto concrete in cross-winds of approximately 1.8 m/s. The rate of growth of the pool and the downwind concentration boundaries are compared to the models, showing good agreement, although additional tuning is needed. These models can contribute to the advancement of codes and standards for liquid hydrogen systems.