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At least 109 records · Page 6

Acoustic Measurements of Solvent Extraction Processes in Support of Safeguards

The proposed poster focuses on using acoustic monitoring to advance detection techniques for reprocessing equipment in support of nuclear safeguards. The usage of free air acoustic monitoring has been previously demonstrated at Idaho National Laboratory (INL) at facilities such as the Advanced Test Reactor and the National Security Test Range. However, this work focuses on a deployment environment dedicated to monitoring separation processes, using solvent extraction equipment such as centrifugal contactors. This environment offers an opportunity for signal discovery and in characterizing acoustic signatures of the equipment in operation. This data can support the development of safeguards by design and security by design measures for aqueous reprocessing facilities. Furthermore, this type of monitoring can aid in early detection and identification of removed materials indicating diversion, which is essential for initiating material recovery and actor identification. The results of this work include data from nine low-frequency acoustic sensors used to investigate potential acoustic characteristics of centrifugal contactors used in multi-stage processes. The results also discuss the correlation between the signatures and the operation of the contactor banks.

98 - NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL↗

Fast, Accurate, and Reliable Thermal Metrology to Assess the Thermal Resistivity on Small Samples of Thermal Insulation

Developing new insulation materials having a thermal resistivity greater than 69 m K/W (10 hr ft2 °F/Btu/inch) can be appealing for building envelope retrofit and construction of new buildings. Multiple institutions are involved in the development of innovative insulation materials with high thermal resistivity. However, these projects have struggled in the development of new materials due to the difficulty associated with the measurement of small sections of high thermal resistivity materials. As new materials are being developed, the size of each test specimen impacts the cost of development. Given the lack of a reliable method to measure the thermal resistivity on small samples of such materials, we evaluated experimental techniques that can be improved to satisfy the need for testing small sections of high thermal resistivity materials and developed standardized test methods to enable the rapid thermal evaluation of advanced insulation materials. This paper presents the study results and potential techniques for fast, accurate, and reliable effective thermal resistivity measurement on small samples of insulation materials.

Desjarlais, Andre Omer↗

Three-dimensional (3D) velocity map imaging: from technique to application

The velocity map imaging (VMI) technique was first introduced by Eppink and Parker in 1997, as an improvement to the original ion imaging method by Houston and Chandler in 1987. The method has gained huge popularity over the past two decades and has become a standard tool for measuring high-resolution translational energy and angular distributions of ions and electrons. VMI has evolved gradually from 2D momentum measurements to 3D measurements with various implementations and configurations. The most recent advancement has brought unprecedented 3D performance to the technique in terms of resolutions (both spatial and temporal), multi-hit capability as well as acquisition speed while maintaining many attractive attributes afforded by conventional VMI such as being simple, cost-effective, visually appealing and versatile. Here, in this tutorial, we will discuss many technical aspects of the recent advancement and its application in probing correlated chemical dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Predicting Si-Anode Calendar Life Using Machine Learning: Correlating Electrolyte Properties and Electrochemical Signals

This study evaluates novel electrolytes tailored for Si-containing anodes to promote calendar-life. Drawing inspiration from advancements in electrolytes for Li-metal cells, the work investigates correlations between predicted electrolyte properties and measured electrochemical performance using several machine-learning models. By leveraging machine learning and advanced modeling techniques, this study aims to establish predictive frameworks that accelerate calendar-aging experiments and inform rational electrolyte design for Si-containing cells. In the present study, fifteen different electrolytes are evaluated in a Si-containing cell using an accelerated calendar-life protocol. For each electrolyte considered, 87 properties (features) from the Advanced Electrolyte Model were produced to identify key property/performance relationships. In this study, the best performing electrolytes were generally those formulations that included non-coordinating fluoroether solvents, and the most predictive features for long-term calendar-life were features related to salt concentration and electrolyte viscosity as well as early capacity, ionic conductivity, and Coulombic efficiency measurements. The framework developed in this study correlating electrolyte properties to measured electrochemical performance is expected to accelerate electrolyte design for Si-containing anodes and ultimately enable high-energy-density, long-life Li-ion batteries.

25 - ENERGY STORAGE↗

At-wavelength characterization of X-ray wavefronts in Bragg diffraction from crystals

The advent of next-generation synchrotron radiation sources and X-ray free-electron lasers calls for high-quality Bragg-diffraction crystal optics to preserve the X-ray beam coherence and wavefront. This requirement brings new challenges in characterizing crystals in Bragg diffraction in terms of Bragg-plane height errors and wavefront phase distortions. Here, a quantitative methodology to characterize crystal optics using a state-of-the-art at-wavelength wavefront sensing technique and statistical analysis is proposed. The method was tested at the 1-BM-B optics testing beamline at the Advanced Photon Source for measuring silicon and diamond crystals in a self-referencing single-crystal mode and an absolute double-crystal mode. The phase error sensitivity of the technique is demonstrated to be at the λ/100 level required by most applications, such as the characterization of diamond crystals for cavity-based X-ray free-electron lasers.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Markov Chain Monte Carlo Parameter Estimation of Deflagration Losses in a Rotating Detonation Engine

One of the practical challenges of the studies of rotating detonation engines (RDEs) is the direct estimation of losses from experimental measurements. This study attempts at resolving this limitation by combining a reduced order model (ROM) of the detonation wave characteristics with a Markov chain Monte Carlo parameter estimation framework. The model considers simple deflagration losses and the overall impact of deflagration on RDE performance. To evaluate this model, a Markov Chain Monte Carlo (MCMC) sampling technique was applied to estimate the loss parameters within the model for a set of conditions operated in hydrogen-air over a range of mass flow rates and equivalence ratios. The MCMC parameter estimation framework allowed for the determination of a posterior distribution of the loss parameters for each test condition, an examination of the correlation between the loss parameters and measured performance metrics of the RDE, and an uncertainty propagation of these parameters. The predicted model loss parameters were then compared to indirect experimental measurements of the deflagration combustion fractions to evaluating the validity of the approach, and shed light on the benefits and drawbacks of the model, measurement techniques, and the estimation framework.

33 ADVANCED PROPULSION SYSTEMS↗

MicroPulse DIAL (MPD) – a diode-laser-based lidar architecture for quantitative atmospheric profiling

Abstract. Continuous water vapor and temperature profiles are critically needed for improved understanding of the lower atmosphere and potential advances in weather forecasting skill. Ground-based, national-scale profiling networks are part of a suite of instruments to provide such observations; however, the technological method must be cost-effective and quantitative. We have been developing an active remote sensing technology based on a diode-laser-based lidar technology to address this observational need. Narrowband, high-spectral-fidelity diode lasers enable accurate and calibration-free measurements requiring a minimal set of assumptions based on direct absorption (Beer–Lambert law) and a ratio of two signals. These well-proven quantitative methods are known as differential absorption lidar (DIAL) and high-spectral-resolution lidar (HSRL). This diode-laser-based architecture, characterized by less powerful laser transmitters than those historically used for atmospheric studies, can be made eye-safe and robust. Nevertheless, it also requires solar background suppression techniques such as narrow-field-of-view receivers with an ultra-narrow bandpass to observe individual photons backscattered from the atmosphere. We discuss this diode-laser-based lidar architecture's latest generation and analyze how it addresses a national-scale profiling network's need to provide continuous thermodynamic observations. The work presented focuses on general architecture changes that pertain to both the water vapor and the temperature profiling capabilities of the MicroPulse DIAL (MPD). However, the specific subcomponent testing and instrument validation presented are for the water vapor measurements only. A fiber-coupled seed laser transmitter optimization is performed and shown to meet all of the requirements for the DIAL technique. Further improvements – such as a fiber-coupled near-range receiver, the ability to perform quality control via automatic receiver scanning, advanced multi-channel scalar capabilities, and advanced processing techniques – are discussed. These new developments increase narrowband DIAL technology readiness and are shown to allow higher-quality water vapor measurements closer to the surface via preliminary intercomparisons within the MPD network itself and with radiosondes.

Spuler, Scott M.↗

Single-shot spatiotemporal plasma density measurements with a chirped probe pulse

In this work, we present the development and demonstration of a diagnostic for the measurement of the spatial and temporal evolution of plasma density in a single shot. Single-shot Advanced Plasma Probe HolographIc REconstruction (SAPPHIRE) utilizes a chirped probe pulse, a diffractive optical element, a self-referenced interferometer, and an interference bandpass filter to achieve high-fidelity electron density measurements suitable for underdense plasmas that exhibit cylindrical symmetry. The method overcomes limitations in conventional diagnostics, such as reliance on shot-to-shot reproducibility, while capturing plasma dynamics on picosecond timescales with micron-level spatial resolution. The capabilities of SAPPHIRE are demonstrated through measurements of laser-driven plasma channels in helium–nitrogen gas jets. SAPPHIRE demonstrates the formation and expansion of plasma channels in a single shot and the propagation of supersonic ionization fronts while revealing shot-to-shot variations in the plasma profiles. Experimental results are validated against theoretical models and scaling laws, underscoring the robustness and accuracy of this technique. By enabling ultrafast, high-resolution plasma diagnostics in a single exposure, SAPPHIRE represents a transformative advancement in plasma measurement technology.

Grace, Elizabeth S. [Lawrence Livermore National L↗

Speciation mapping of the oxidation layer on aged uranium dioxide using scanning transmission x-ray spectromicroscopy

In this study, UO 2 was aged in humid air and prepared as a thin section using a focused ion beam (FIB) instrument. The specimen was measured using synchrotron radiation spectromicroscopy techniques at the Beamline 11.0.2 STXM end station of the Advanced Light Source (ALS). Non-negative matrix factorization (NMF) methods were used to identify and map three component x-ray absorption near-edge structure (XANES) spectra in the oxygen K-edge data, revealing a surface layer of U 4 O 9 with a thickness of 206 ± 21 nm, and the bulk of the sample remaining as UO 2 . Uranium N 4,5 -edge XANES spectromicroscopy supports these results. The diffusion-controlled parabolic rate constant for UO 2 oxidation to U 4 O 9 was calculated from the observed layer thickness and compared to literature values. Complementary transmission electron microscopy (TEM) was used to image the sample and identify the phases present in various regions, confirming the STXM results.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Light–ferroelectric interaction in two-dimensional lead iodide perovskites

The unique physical properties of two-dimensional (2D) metal halide perovskites (MHPs) such as nonlinear optics, anisotropic charge transport, and ferroelectricity have made these materials promising candidates for multifunctional applications. Recently, fluorine derivatives such as 4,4-difluoropiperidinium lead iodide perovskite or (4,4-DFPD, C 5 H 10 F 2 N) 2 PbI 4 have shown strong ferroelectricity as compared to other 2D MHPs. Although it was previously addressed that the ferroelectricity in MHPs can be affected by illumination, the underlying physical mechanisms of light–ferroelectricity interaction in 2D MHPs are still lacking. Here, we explore the electromechanical responses in 4,4-(DFPD) 2 PbI 4 thin films using advanced scanning probe microscopy techniques revealing ferroelectric domain structures. In this work, hysteretic ferroelectric loops measured by contact-Kelvin probe force microscopy are dependent on domain structures under dark conditions, while ferroelectricity weakens under illumination. The X-ray diffraction patterns exhibit significant changes in preferential orientation of individual lattice planes under illumination. Particularly, the reduced intensity of the (1 1 1) lattice plane under illumination leads to transitioning from a ferroelectric to a paraelectric phase. The instability of positive ions, especially molecular organic cations, is observed under illumination by time-of-flight secondary ion mass spectrometry. The combination of crystallographic orientation and chemical changes under illumination clearly contributes to the origin of light–ferroelectricity interaction in 2D (4,4-DFPD, C 5 H 10 F 2 N) 2 PbI 4 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

PyDA: A Hands-On Introduction to Dynamical Data Assimilation with Python

Dynamic data assimilation offers a suite of algorithms that merge measurement data with numerical simulations to predict accurate state trajectories. Meteorological centers rely heavily on data assimilation to achieve trustworthy weather forecast. With the advance in measurement systems, as well as the reduction in sensor prices, data assimilation (DA) techniques are applicable to various fields, other than meteorology. However, beginners usually face hardships digesting the core ideas from the available sophisticated resources requiring a steep learning curve. In this tutorial, we lay out the mathematical principles behind DA with easy-to-follow Python module implementations so that this group of newcomers can quickly feel the essence of DA algorithms. We explore a series of common variational, and sequential techniques, and highlight major differences and potential extensions. We demonstrate the presented approaches using an array of fluid flow applications with varying levels of complexity.

97 MATHEMATICS AND COMPUTING↗

Generation of macro- and microplastic databases by high-throughput FTIR analysis with microplate readers

Abstract FTIR spectral identification is today’s gold standard analytical procedure for plastic pollution material characterization. High-throughput FTIR techniques have been advanced for small microplastics (10–500 µm) but less so for large microplastics (500–5 mm) and macroplastics (> 5 mm). These larger plastics are typically analyzed using ATR, which is highly manual and can sometimes destroy particles of interest. Furthermore, spectral libraries are often inadequate due to the limited variety of reference materials and spectral collection modes, resulting from expensive spectral data collection. We advance a new high-throughput technique to remedy these problems using FTIR microplate readers for measuring large particles (> 500 µm). We created a new reference database of over 6000 spectra for transmission, ATR, and reflection spectral collection modes with over 600 plastic, organic, and mineral reference materials relevant to plastic pollution research. We also streamline future analysis in microplate readers by creating a new particle holder for transmission measurements using off-the-shelf parts and fabricating a nonplastic 96-well microplate for storing particles. We determined that particles should be presented to microplate readers as thin as possible due to thick particles causing poor-quality spectra and identifications. We validated the new database using Open Specy and demonstrated that additional transmission and reflection spectra reference data were needed in spectral libraries. Graphical abstract

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Cyclotron radiation emission spectroscopy of electrons from tritium $β$ decay and 83m Kr internal conversion

Project 8 has developed a novel technique, cyclotron radiation emission spectroscopy (CRES), for direct neutrino mass measurements. A CRES-based experiment on the beta spectrum of tritium has been carried out in a small-volume apparatus. Here, we provide a detailed account of the experiment, focusing on systematic effects and analysis techniques. In a Bayesian (frequentist) analysis, we measure the tritium endpoint as ${18}$ ${553}_{—19}^{+18}$ (${18}$ ${548}_{—19}^{+19}$) eV and set upper limits of 155 (152) eV (90% C.L.) on the neutrino mass. No background events are observed beyond the endpoint in 82 days of running. We also demonstrate an energy resolution of 1.66 ± 0.19 eV in a resolution-optimized magnetic trap configuration by measuring 83m Kr 17.8-keV internal-conversion electrons. These measurements establish CRES as a low-background, high-resolution technique with the potential to advance neutrino mass sensitivity

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Bridging the length scales on mechanical property evaluation (Final Report)

The development of small-scale mechanical testing in combination with microstructural investigation is of great interest to the nuclear materials community for both materials development and monitoring applications. Dramatically reducing the sample sizes to reduce radioactivity and obtaining mechanical properties of irradiated samples is truly intriguing. Moreover, such studies promise a range of benefits including cost reduction, fundamental insight in structure-property relationships, increased statistics on less sample material, and reinvestigation of prior irradiated and tested reactor samples while simultaneously enabling the generation of mechanical test data on ion beam irradiated materials with limited penetration depths. Small scale materials testing on sub-sized samples has been studied for several decades, though it has only been after the development of micro-testing based on Focused Ion Beam (FIB) sample manufacturing in that orders of magnitude smaller samples could really be investigated in a quantitative manner. In recent years, small scale mechanical testing techniques at a number of length scales has been developed for both unirradiated and irradiated (ion and neutron) materials. Technological advances made in this field have enabled ex-situ and in-situ transmission electron microscopy (TEM) and scanning electron microscopy (SEM) examination, thus leading to more accurate measurements as well as additional mechanistic information. A recent review of the benefits of these techniques show that these techniques are at a stage to tackle multi-scale ranges of materials investigations and can be utilized to obtain fundamental science-based understanding of nuclear materials. Considering the tremendous advances made, one can see how small-scale mechanical testing techniques combined with modeling can enable true small scale to bulk scale mechanical property correlations. However, for the engineering community to adapt this approach fully, one needs to demonstrate that a) that these techniques can produce results with high fidelity and reproducibility, b) generate engineering stress-strain data that one can utilize to understand bulk behavior, and c) generate new insight into relevant phenomena fostering the true understanding of radiation damage and microstructure in materials for nuclear applications. It is the objective of this proposal to bridge the length scale between macro- and micro- scale mechanical testing of unirradiated and irradiated materials. This involves the development and demonstration of procedures for multi-scale mechanical testing that enable high fidelity reproducibility of data and the generation bulk property data from small-scale mechanical tests. Through this, the proposal aims to enhance the confidence in the obtained data at the smaller length scales and enhance the insight provided from these techniques for bulk scale applications on both unirradiated and irradiated materials.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

High-fidelity retrieval from instantaneous line-of-sight returns of nacelle-mounted lidar including supervised machine learning

Abstract. Wind turbine applications that leverage nacelle-mounted Doppler lidar are hampered by several sources of uncertainty in the lidar measurement, affecting both bias and random errors. Two problems encountered especially for nacelle-mounted lidar are solid interference due to intersection of the line of sight with solid objects behind, within, or in front of the measurement volume and spectral noise due primarily to limited photon capture. These two uncertainties, especially that due to solid interference, can be reduced with high-fidelity retrieval techniques (i.e., including both quality assurance/quality control and subsequent parameter estimation). Our work compares three such techniques, including conventional thresholding, advanced filtering, and a novel application of supervised machine learning with ensemble neural networks, based on their ability to reduce uncertainty introduced by the two observed nonideal spectral features while keeping data availability high. The approach leverages data from a field experiment involving a continuous-wave (CW) SpinnerLidar from the Technical University of Denmark (DTU) that provided scans of a wide range of flows both unwaked and waked by a field turbine. Independent measurements from an adjacent meteorological tower within the sampling volume permit experimental validation of the instantaneous velocity uncertainty remaining after retrieval that stems from solid interference and strong spectral noise, which is a validation that has not been performed previously. All three methods perform similarly for non-interfered returns, but the advanced filtering and machine learning techniques perform better when solid interference is present, which allows them to produce overall standard deviations of error between 0.2 and 0.3 m s−1, or a 1 %–22 % improvement versus the conventional thresholding technique, over the rotor height for the unwaked cases. Between the two improved techniques, the advanced filtering produces 3.5 % higher overall data availability, while the machine learning offers a faster runtime (i.e., ∼ 1 s to evaluate) that is therefore more commensurate with the requirements of real-time turbine control. The retrieval techniques are described in terms of application to CW lidar, though they are also relevant to pulsed lidar. Previous work by the authors (Brown and Herges, 2020) explored a novel attempt to quantify uncertainty in the output of a high-fidelity lidar retrieval technique using simulated lidar returns; this article provides true uncertainty quantification versus independent measurement and does so for three techniques rather than one.

47 OTHER INSTRUMENTATION↗

Oxide– and Silicate–Water Interfaces and Their Roles in Technology and the Environment

Interfacial reactions drive all elemental cycling on Earth and play pivotal roles in human activities such as agriculture, water purification, energy production and storage, environmental contaminant remediation, and nuclear waste repository management. The onset of the 21st century marked the beginning of a more detailed understanding of mineral aqueous interfaces enabled by advances in techniques that use tunable high-flux focused ultrafast laser and X-ray sources to provide near-atomic measurement resolution, as well as by nanofabrication approaches that enable transmission electron microscopy in a liquid cell. This leap into atomic- and nanometer-scale measurements has uncovered scale-dependent phenomena whose reaction thermodynamics, kinetics, and pathways deviate from previous observations made on larger systems. A second key advance is new experimental evidence for what scientists hypothesized but could not test previously, namely, interfacial chemical reactions are frequently driven by “anomalies” or “non-idealities” such as defects, nanoconfinement, and other nontypical chemical structures. Third, progress in computational chemistry has yielded new insights that allow a move beyond simple schematics, leading to a molecular model of these complex interfaces. In combination with surface-sensitive measurements, we have gained knowledge of the interfacial structure and dynamics, including the underlying solid surface and the immediately adjacent water and aqueous ions, enabling a better definition of what constitutes the oxide– and silicate–water interfaces. This critical review discusses how science progresses from understanding ideal solid–water interfaces to more realistic systems, focusing on accomplishments in the last 20 years and identifying challenges and future opportunities for the community to address. Further, we anticipate that the next 20 years will focus on understanding and predicting dynamic transient and reactive structures over greater spatial and temporal ranges as well as systems of greater structural and chemical complexity. Closer collaborations of theoretical and experimental experts across disciplines will continue to be critical to achieving this great aspiration.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Development of a Reference Database for Beta-Delayed Neutron Emission

Beta-delayed neutron emission is important for nuclear structure and astrophysics as well as for reactor applications. Significant advances in nuclear experimental techniques in the past two decades have led to a wealth of new measurements that remain to be incorporated in the databases. In this work, we report on a coordinated effort to compile and evaluate all the available β-delayed neutron emission data. The different measurement techniques have been assessed and the data have been compared with semi-microscopic and microscopic-macroscopic models. The new microscopic database has been tested against aggregate total delayed neutron yields, time-dependent group parameters in 6-and 8-group re-presentation, and aggregate delayed neutron spectra. New recommendations of macroscopic delayed-neutron data for fissile materials of interest to applications are also presented. The new Reference Database for Beta-Delayed Neutron Emission Data is available online.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Ultimate brightness of a medium-energy synchrotron light source at operational beam intensity

Synchrotron light sources are key instruments of modern science, providing unique opportunities for groundbreaking studies in diverse scientific disciplines and driving innovation in numerous scientific and technological fields. Fourth-generation light sources provide unprecedented capabilities in imaging, spectroscopy and diffraction techniques. Ultimate brightness is the key to advancing to a smaller scale, faster response, and higher data measurement and processing rate. The brightness is primarily determined by the electron beam emittance and energy spread at operational intensity. A common feature of fourth-generation synchrotrons is the short length of the electron bunches combined with a very small transverse beam size. Consequently, the high particle density leads to strong collective effects that significantly increase the emittance and limit the achievable brightness at operational beam intensity. In this article, we summarize our studies of the emittance and brightness scaled with the beam energy and intensity, taking into account the effects of intrabeam scattering, beam-impedance interaction and bunch lengthening provided by higher-harmonic RF systems to identify optimal combinations of machine and beam parameters.

36 MATERIALS SCIENCE↗