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At least 973 records · Page 54

First-of-a-Kind Fuel-bearing Molten Chloride Irradiation Experiment

As a dozen MSR developers in the U.S. work toward an aggressive commercialization timeline, many of their fueled-salts—notably, chloride-based compositions—have never been irradiated. Licensing and operating these reactors requires an understanding of (1) the source term, radiation chemistry, and gas generation; (2) unanticipated irradiation-induced corrosion effects; and (3) the impact of burnup on thermophysical properties, all of which can be deduced through irradiation testing. Idaho National Laboratory (INL) is ideally suited to leverage its expertise in chloride salt chemistry, as well as its Neutron Radiography Reactor (NRAD) facility in the Hot Fuels Examination Facility (HFEF) at the Materials and Fuels Complex (MFC), to conduct the world’s first fuel-bearing chloride salt irradiation and fill in the knowledge gaps pertaining to salt chemistry under irradiation. Molten-salt Research Temperature-controlled Irradiation (MRTI) consists of a salt-containing capsule that is internally heated inside of a secondary containment. The experiment must rely on resistive heating to melt the salt before irradiation (to avoid the impact of radiolysis) and once the reactor is turned on and fission reactions commence in the salt, the resistive power can then be reduced. Salt-immersed thermocouples coupled to a controller allow for the heater power to be adjusted as needed to meet experimental objectives. The bulk of the experimental results will be achieved through Post-Irradiation Examination (PIE). At which point a range of different measurements are anticipated to assess the salt/plenum/wall composition, the capsule corrosion rate, and the evolution of salt properties.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

An Optothermal Raman Model Accounting for Convection, Radiation, and Substrate Effects for Evaluation of the Thermal Conductivity of Two‐Dimensional Coatings

Thermal conductivity of two‐dimensional (2D) materials is important to characterize as this will govern thermal transport physics in the various thermal and energy applications benefitting from the unique properties of these materials. Here, analytical and numerical techniques are presented to determine the thermal conductivity and interfacial conductance of a 2D material coating using confocal micro‐Raman spectroscopy as a noncontact diagnostic. While several methods have been proposed for calculating the values of thermal conductivity, interfacial conductance, and spatial temperature profile, these models often do not consider effects of radiation, convection, and substrate resistance on the temperature and heat flux profiles. We present a model to calculate the thermal conductivity and interfacial conductance which accounts for convection, radiation, and substrate effects to characterize a variety of 2D material coatings, which is demonstrated using large area graphene transferred onto copper and nickel substrates. Convection and radiation effects are found to have a negligible effect on the temperature profile of supported coatings, while the substrate effects have a considerable effect and therefore impact the quantification of thermal conductivity and interfacial conductance in addition to limiting the spatial resolution of the technique. These findings will allow for more accurate and reproducible extraction of the thermal conductivity of graphene and other 2D material coatings when employing noncontact optothermal Raman spectroscopy methods.

2D coatings↗

Predicting Radiation-Induced Plutonium Redox Chemistry using Multiscale Modeling Methods

Over the the last 70 years plutonium (Pu) has been integral in the development of several technologies that have changed the world, yet our fundamental understanding of its chemistry is still far from complete. This is a testament to this element?s unique and complex properties, such as its ability to coexist as multiple oxidation states in aqueous solution. Careful manipulation of plutonium oxidation states is essential in the study and utilization of its rich chemistry. To achieve this level of control, a comprehensive mechanistic understanding of radiation-induced plutonium redox chemistry is critical due to the unavoidable exposure of plutonium to ionizing radiation fields, both inherent and from in-process applications. For this reason, we have developed an experimentally evaluated multi-scale computer model for the prediction of gamma radiation-induced Pu(IV) redox chemistry in concentrated nitric acid solutions (1.0, 3.0, and 6.0 M).

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Lithium indium diselenide — An advanced material for neutron detection

Here, this paper describes the synthesis, crystal growth, detector fabrication, radiation hardening studies, MCNP modeling, and characterization of lithium indium diselenide or LiInSe 2 . This newly-developed room temperature thermal neutron detector has semiconducting and scintillating properties and it is suitable for neutron detection application. LiInSe 2 was synthesized starting from elemental Li, In, Se in two steps due to high reactivity of Li. A single crystal of LiInSe 2 was grown using the Vertical Bridgman method. The room temperature band gap was found to be 2.8 eV using optical absorption measurements. Bulk resistivity was measured at ∼5 × 10 11 Ωcm. Photoconductivity measurements of LiInSe 2 wafers identified a peak in the photocurrent around 445 nm. Nuclear radiation detectors were fabricated from single crystal wafer and the responses to alpha particles at various biases were measured. The mobility-lifetime product was estimated. Gamma irradiation studies were performed with calculated absorbed doses ranging from 0.2126 to 21,262 Gy. The characterization of the two wafers for their scintillator performance was conducted after each irradiation. The gamma irradiation produced a reduction of the light yield that translated to a lower channel number for the centroid of alpha detection spectra. It also showed a considerable reduction of the decay time after the first irradiation. These are the first studies on gamma radiation hardening with this material.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Characterization of retroreflective tape optical properties for use with position-sensitive scintillator detectors

Reflective materials such as Teflon and Enhanced Specular Reflector are commonly used to maximize light collection in scintillator-based radiation detection systems. While effective, in most cases, the spatial information carried by the light is diminished or lost entirely. Retroreflectors, in contrast, better preserve the spatial information and have been shown to improve the localization performance of such systems. In this work, the relative retroreflectivity of a selection of commercial retroreflective tapes and their performance impact when coupled to a plastic scintillator are reported. Finally, we demonstrate improved localization performance with some tapes compared to Teflon and black paint.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Report on Evolution of Inconel 718 Following HFIR Irradiation

The report presents the microstructure and mechanical properties of 3D printed Inconel 718 after irradiation in the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory (ORNL) to assess its potential use as a structural material. The structural components near the outlets of several proposed reactor cores will experience significant neutron fluxes and outlet coolant temperatures ranging from the hot standby temperature of 300 °C to nearly 550 °C at the center of the part. These components must support the core in appropriate loading conditions and require structural analysis at relevant temperatures. In FY21, three heat treatments were designed and conducted to simplify the microstructure and to determine how each precipitating phase contributed to the overall strength. In FY21, baseline mechanical properties were measured from uniaxial tensile tests on subsize SS-J2 specimens at room temperature and at elevated temperatures of 300, 450, and 600 °C to serve a comparison to the irradiated properties. Four capsules containing 3D printed Inconel 718 were inserted into HFIR in FY21 for a matrix of two temperatures and two doses. The lower of the two doses was available for characterization in FY22. Multiple heat treatments of Inconel 718 irradiated to nominal conditions of 2 displacements per atom (dpa) at either 300 or 600 °C were strained with uniaxial tensile tests at the Irradiated Material Examination and Testing (IMET) Facility to discern the mechanical properties. Transmission electron microscopy was performed to correlate the observed mechanical properties with nanoscale features. The initially homogenous AM718-HM increased in strength at both irradiation temperatures based on a high density of nanometer-scale radiation-induced cavities at lower temperature and nucleation and growth of γ" precipitates at higher temperatures. The precipitate-hardened AM718-HT2 showed very small differences in strength before and after irradiation: the contribution to strength from γ" precipitates was replaced with dislocation loops. Because the radioactivity of the nickel superalloys from neutron activation limited the scope of the analysis, a feasibility study examined the possibility of an ultra-miniature specimen geometry, colloquially SS-Tiny (SS-T), for mechanical property determination using the nonirradiated Inconel 718. This study found an overestimation of ductility from the SS-T geometry with yield strength and ultimate tensile strength slightly above the SS-J2 geometry: this could be contributed to a reduction in specimen thickness.

36 MATERIALS SCIENCE↗

Establishing robust correction schemes for improved and reliable ARM-AOS aerosol optical data products

Aerosol light absorption and scattering of solar radiation play an important role in the earth’s atmosphere in terms of direct and semi-direct radiative forcing. Optical parameters of importance to the US Department of Energy (DOE) climate models include absorption and scattering coefficients, single scattering albedo (SSA), absorption Angstrom exponents (AAE), and the asymmetry parameter (g). These parameters depend on aerosol size, shape and composition (refractive index), and are spectrally sensitive in the shortwave region. Additionally, these parameters have a complex dependency on the emission source, especially for carbonaceous aerosols. The DOE Atmospheric Radiation Measurement (ARM) user facility has deployed aerosol observing systems (AOS) containing several filter-based instruments to measure and constrain aerosol optical properties and related parameters at multiple sites worldwide. For measurement of aerosol light absorption, the AOS includes filter-based instruments (particle soot absorption photometer and tricolor absorption photometer) that infer particle-phase aerosol absorption coefficients at nominal red, green, and blue wavelength bands from the attenuation (ATN) of light passing through a particulate filter on which aerosols are deposited. Measurement of aerosol scattering is done in situ using nephelometers. By combining inferred absorption coefficients from filter-based ATN measurements and in situ scattering coefficients, value-added products (VAPs) such as SSA, AAE, and g are derived.

54 ENVIRONMENTAL SCIENCES↗

A nanoscale photonic thermal transistor for sub-second heat flow switching

Abstract Control of heat flow is critical for thermal logic devices and thermal management and has been explored theoretically. However, experimental progress on active control of heat flow has been limited. Here, we describe a nanoscale radiative thermal transistor that comprises of a hot source and a cold drain (both are ~250 nm-thick silicon nitride membranes), which are analogous to the source and drain electrodes of a transistor. The source and drain are in close proximity to a vanadium oxide (VO x )-based planar gate electrode, whose dielectric properties can be adjusted by changing its temperature. We demonstrate that when the gate is located close ( < ~1 µm) to the source-drain device and undergoes a metal-insulator transition, the radiative heat transfer between the source and drain can be changed by a factor of three. More importantly, our nanomembrane-based thermal transistor features fast switching times ( ~ 500 ms as opposed to minutes for past three-terminal thermal transistors) due to its small thermal mass. Our experiments are supported by detailed calculations that highlight the mechanism of thermal modulation. We anticipate that the advances reported here will open new opportunities for designing thermal circuits or thermal logic devices for advanced thermal management.

42 ENGINEERING↗

Predicting Radiation-Induced Plutonium Redox Chemistry using Multi-scale Modeling Methods

Over the the last 70 years plutonium (Pu) has been integral in the development of several technologies that have changed the world, yet our fundamental understanding of its chemistry is still far from complete. This is a testament to this element’s unique and complex properties, such as its ability to coexist as multiple oxidation states in aqueous solution. Careful manipulation of plutonium oxidation states is essential in the study and utilization of its rich chemistry. To achieve this level of control, a comprehensive mechanistic understanding of radiation-induced plutonium redox chemistry is critical due to the unavoidable exposure of plutonium to ionizing radiation fields, both inherent and from in-process applications. For this reason, we have developed an experimentally evaluated multi-scale computer model for the prediction of gamma radiation-induced Pu(IV) redox chemistry in concentrated nitric acid solutions (1.0, 3.0, and 6.0 M). Under these acidic, aqueous solution conditions, cobalt-60 gamma irradiation afforded negligible net change in the steady-state oxidation state distribution of Pu(IV). Multi-scale calculations, which are in excellent agreement with experimental data, indicate that this observation is due to radiation-induced redox cycling between Pu(IV) and Pu(III), as achieved by the reduction of Pu(IV) by radiolytic nitrous acid and hydrogen peroxide, and the oxidation of Pu(III) by nitrate and hydroxyl radicals. These radiation-induced redox processes are augmented by plutonium’s inherent disproportionation reactions.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Hygrothermal aging and recycling effects on mechanical and thermal properties of recyclable thermoplastic glass fiber composites

Abstract Glass fiber‐reinforced polymer composites are widely used in marine applications, including renewable energy devices and submarines, due to their strength‐to‐weight ratios and corrosion resistance. As sustainability becomes more important, recyclable thermoplastic composites are gaining attention in marine energy applications. These materials face harsh conditions such as high chloride water, UV radiation, pressurization, and thermal cycling, which can affect their durability and recyclability. This study examines the impact of hygrothermal aging on the recyclability of an Elium glass fiber (GF) composite. Samples were mechanically ground for recycling, and mechanical and thermal properties were compared between aged and unaged samples. After seawater aging, the tensile strength and modulus of the unaged composite dropped by 25% and 13% respectively, due to water ingress along the fiber‐matrix interface. The recycled composite showed reduced flexural strength as the long fiber composite was converted into short fibers during the process. Differential scanning calorimetry (DSC) revealed no change in glass transition temperature after aging. Weight loss (25%) was attributed to the thermal stability of the glass fibers. Dynamic mechanical analysis (DMA) showed that the storage modulus increased with aging, and fracture analysis confirmed a mixed mode of failure for aged composites. Highlights Hygrothermal aging lowers mechanical performance of Elium® GF composites. Failure mechanism tends to be matrix cracking and interface bonding. Glass transition temperature is not reduced by hygrothermal aging. Fractured composite was successfully recycled via thermoforming. Flexural strength of the recycled composite is lower.

17 WIND ENERGY↗

𝐴𝑏 initio density-matrix approach to exciton coherence: Phonon scattering, Coulomb interactions, and radiative recombination

Relaxation processes following light excitation in semiconductors are key in materials-based quantum technology applications. These processes are broadly studied in atomically thin transition-metal dichalcogenides, quasi-two-dimensional excitonic semiconductors in which atomistic design allows for tunable excited-state properties, such as relaxation lifetimes and photoinduced coherence. In this work, we present a density-matrix-based approach to compute exciton relaxation within a many-body ab initio perspective. We expand our previously developed Lindblad density-matrix formalism to capture multichannel electron-hole pair relaxation processes, including phonon and Coulomb scattering as well as radiative recombination, and we study their effect on the time-resolved excited-state propagation. Using monolayer MoSe 2 as a prototypical example, we examine many-body effects on the time-dependent dynamics of photoactive excitations, exploring how the electron-hole pair interactions are reflected in variations of the excitation energy, spectral signature, and state coherence. In conclusion, our method supplies a detailed understanding of exciton relaxation mechanisms in realistic materials, offering a previously unexplored pathway to study excited-state dynamics in semiconductors from first principles.

Band structure methods↗

Near-field-driven radiative thermal dynamics in aperiodic photonic nanostructures

Harnessing structural correlations in near-field plasmonic and polaritonic systems hold untapped potential for controlling light–matter interactions at the nanoscale. By tuning these correlations, one can reshape mode localization, coupling, and spectral distribution which are properties central to manipulating energy transport and field enhancement in nanophotonic platforms. We exploit Vogel spirals, an aperiodic geometry where a single parameter dictates spatial correlations, to show how correlation strength reshapes the modal spectrum and transient dynamics of near-field coupling. As a proof of concept, we demonstrate that aperiodic configurations outperform both uncorrelated (random) and periodic arrays in controlling near-field radiative heat-transfer dynamics. These results establish deterministic aperiodic order as a powerful platform for tailoring correlated electromagnetic responses in next-generation nanophotonic devices.

36 MATERIALS SCIENCE↗

CsPbBr3 perovskite single crystals for X- and -radiation detectors

Methods were developed for the synthesis and growth of halide lead perovskites CsPbBr3, which can be used as detectors of optical, X-ray, and -radiation. The growth of single crystals was carried out by the Bridgman method in quartz ampoules using zone-refined starting material. The electro-physical properties of the inorganic perovskite lead cesium tribromide CsPbBr3 were studied. Two types of structures with Cr/CsPbBr3/Ni rectifying and Ni/CsPbBr3/Ni ohmic contacts were fabricated. The resistivity of (  7×109 Ohmcm), and the activation energy of the dark conductivity (E  0.8 eV) were determined. From the measurements of the optical transmission spectra, the CsPbBr3 energy gap at 300 K was found to be Еg = 2.27 eV. The temperature dependence of the forbidden gap (Eg(T) = 2.4 - 4*10-4 T, eV) was also determined. A significant increase in photosensitivity for the Cr/CsPbBr3/Ni structure was observed at elevated temperatures. The Cr/CsPbBr3/Ni structures were shown to be sensitive to -radiation. The FWHM of the energy resolution for 241Am source was measured to be 15.8 keV.

Sklyarchuk, V.↗

Dark field X-ray microscopy below liquid-helium temperature: The case of NaMnO 2

Dark field X-ray microscopy (DFXM) is an experimental technique employed to investigate material properties by probing their ‘mesoscale,’ or microscale structures, in a bulk-sensitive manner using hard X-rays at synchrotron radiation sources. However, challenges remain when it comes to applications of this technique to examine low-temperature phenomena in quantum materials, which exhibit complex phase transitions at cryogenic temperatures. One such material is NaMnO 2 , which hosts an antiferromagnetic transition at 45 K that is suspected to coincide with local structural transitions from its majority monoclinic phase to nanoscale triclinic domains. Direct observation of local heterogeneities and this effect at low temperatures in NaMnO 2 is an important step in understanding this material and serves as an ideal candidate study for expanding the DFXM experimental design space. This paper details a foundational high-resolution DFXM study, down to liquid-helium temperature and below, conducted to explore phase transitions in NaMnO 2 . In conclusion, the outlined experiment ushers in the evaluation of other functional materials at low temperatures using this technique.

36 MATERIALS SCIENCE↗

Theoretical investigation of plasma wave generation by pulsed electron beams in space

Here, we report theoretical calculations of plasma wave generation in the whistler modes and in the extraordinary modes, by pulsed electron beams in a magnetized plasma. The numerical simulations of the wave generation take into account the longitudinal expansion of the electron beam due to the space charge force and the energy spread. The work presented in this article provides predictions for the wave generation performance of the beam plasma interactions experiment (Beam PIE), where pulsed electron beams were produced by a spaceborne radio frequency (RF) linear accelerator. We also theoretically explore the desirable properties of the pulsed electron beam for future space experiments, which will be the next step toward eventually demonstrating the radiation-belt remediation (RBR).

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Effects from Time Dependence of Ice Nucleus Activity for Contrasting Cloud Types

Abstract The role of time-dependent freezing of ice nucleating particles (INPs) is evaluated with the “Aerosol–Cloud” (AC) model in 1) deep convection observed over Oklahoma during the Midlatitude Continental Convective Cloud Experiment (MC3E), 2) orographic clouds observed over North California during the Atmospheric Radiation Measurement (ARM) Cloud Aerosol Precipitation Experiment (ACAPEX), and 3) supercooled, stratiform clouds over the United Kingdom, observed during the Aerosol Properties, Processes And Influences on the Earth’s climate (APPRAISE) campaign. AC uses the dynamical core of the WRF Model and has hybrid bin–bulk microphysics and a 3D mesoscale domain. AC is validated against coincident aircraft, ground-based, and satellite observations for all three cases. Filtered concentrations of ice (>0.1–0.2 mm) agree with those observed at all sampled levels. AC predicts the INP activity of various types of aerosol particles with an empirical parameterization (EP), which follows a singular approach (no time dependence). Here, the EP is modified to represent time-dependent INP activity by a purely empirical approach, using our published laboratory observations of time-dependent INP activity. In all simulated clouds, the inclusion of time dependence increases the predicted INP activity of mineral dust particles by 0.5–1 order of magnitude. However, there is little impact on the cloud glaciation because the total ice is mostly (80%–90%) from secondary ice production (SIP) at levels warmer than about −36°C. The Hallett–Mossop process and fragmentation in ice–ice collisions together initiate about 70% of the total ice, whereas fragmentation during both raindrop freezing and sublimation contributes <10%. Overall, total ice concentrations and SIP are unaffected by time-dependent INP activity. In the simulated APPRAISE case, the main causes of persistence of long-lived clouds and precipitation are predicted to be SIP in weak embedded convection and reactivation following recirculation of dust particles in supercooled layer cloud.

54 ENVIRONMENTAL SCIENCES↗