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At least 145 records · Page 8

Use of a deuterium-deuterium neutron generator for the Add-A-Source waste matrix correction technique

Neutron generators offer an alternative to radioactive sources in the application of active techniques for nondestructive assay of nuclear materials. The Add-A-Source technique has enabled improvements in the ability to accurately measure waste bearing nuclear materials by measuring and correcting for the non-nuclear matrix effect. The technique has historically been performed with a Cf-252 spontaneous fission source. Here, in this work, we have demonstrated the use of a Deuterium-deuterium neutron generator in place of the Cf-252 source. A DD generator enables operational advantages and allows the simplification of the instrument design, while offering equivalent corrective performance as a Cf-252 source.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Gas stopping and reacceleration techniques at the Facility for Rare Isotope Beams (FRIB)

The Facility for Rare Isotope Beams (FRIB) at Michigan State University provides a wide range of beams and energies for science with fast, stopped and reaccelerated rare-isotope beams. FRIB was commissioned in 2022 with the science program beginning in May 2022. Here, the combination of fast beams followed by gas stopping of rare-isotope beams together with reacceleration is unique to FRIB. Stopping techniques and beam manipulation at very-low energies are important to slow down fast beams for use in either stopped-beam experimental devices, or subsequent injection in the reaccelerator for experiments at energies ranging from 0.3 MeV/u to 12 MeV/u, depending on the Q/A of the ion. Innovative stopped-beam techniques to optimize the stopping and extraction efficiencies across a wide range of atomic numbers, as well as to reduce contamination and increase extraction speed, were developed. Reacceleration of those beams involve cooling, bunching, charge breeding and acceleration by a state-of-the-art superconducting reaccelerator, ReA. In this contribution we present the latest results of various gas stoppers and techniques to eliminate contaminants after reacceleration by the ReA.

43 PARTICLE ACCELERATORS↗

An adaptive knowledge-based data-driven approach for turbulence modeling using ensemble learning technique under complex flow configuration: 3D PWR sub-channel with DNS data

This work describes a new approach to increase the accuracy of Reynolds-averaged Navier–Stokes (RANS) in modeling turbulence flow leveraging the machine learning technique. Traditionally, different turbulence models for Reynolds stress are developed for different flow patterns based on human knowledge. Each turbulence model has a certain application domain and prediction uncertainty. In recent years, with the rapid improvements of machine learning techniques, researchers start to develop an approach to compensate for the prediction discrepancy of traditional turbulence models with statistical models and data. However, the approach has deficiencies in several aspects. For example, the amount of human knowledge introduced to the statistical model couldn’t be controlled, which makes the statistical model learn from a very naïve stage and limits its application. In this work, a new approach is developed to address those deficiencies. Here, the new approach uses the “ensemble learning” technique to control the amount of human knowledge introduced into the statistical model. Therefore, the new approach could be adaptive to the multiple application domains. In conclusion, according to the results of case study, the new approach shows higher accuracy than both traditional turbulence models and the previous machine learning approach.

42 ENGINEERING↗

Modeling simultaneous particle shrinkage, dissolution and breakage using the modified moving grid technique

Simultaneous shrinkage, dissolution and breakage are important particle size reduction phenomena that characterize processes like the reactive degradation of solid chemicals. The dynamics of the particle size distribution (PSD) for such processes are non-trivial to model due to the number expending processes brought about by the eventual dissolution of particles. To this end, Population Balance Model (PBM) resolved through the sectional techniques is the natural approach. Here, we introduce a modified Moving Grid technique (m-MGT) to accurately resolve the particle size reduction phenomena. Our technique mimics the perpetual particle shrinkage through a continuously left-moving size grid and incorporates a strategic grid removal routine to capture the disappearance of particles. Coupled with the Fixed Pivot (FP) discretization for breakage, our m-MGT not only preserves the moment-related properties, but also benchmarked very well against the analytical number densities and exhibited a minimum of first-order convergence in all assessed case studies.

97 MATHEMATICS AND COMPUTING↗

Formation and degradation mechanism of methylammonium lead iodide perovskite thin film fabricated by electrospray technique

Electrospray deposition technique has been reported previously for fabricating effective and stable perovskite thin film, leading to efficient perovskite solar cells. Here, in this work, a comprehensive investigation of the formation mechanism of methylammonium lead iodide perovskite (CH 3 NH 3 PbI 3 ) film by electrospray technique is demonstrated and compared to the formation mechanism through the conventional spin coating technique. In the electrospray process, charged MAI nanoparticles are gradually introduced onto the PbI 2 film, intercalating within the PbI 2 structure to produce the perovskite film. In contrast, the spin-coating method involves supplying the MAI solution in bulk, leading to perovskite crystal formation through the dissolution of the PbI 2 layer by the MAI solution, followed by recrystallization into perovskite oriented in the [110] direction, 30° inclined to the substrate. The impact of charge and the electric field on the formation of perovskite film using the electrospray is explored. Furthermore, the intrinsic stability of perovskite films is monitored in real-time in a highly humid environment (≥80 % relative humidity (RH)) using in-situ Grazing Incidence Wide Angle X-ray Scattering (GIWAXS), and a degradation mechanism is proposed to enhance the durability of the perovskite-based devices. The study further delves into the comparison of the stability of electrosprayed and spin-coated perovskite film, and the impact of humidity level and the presence of a hole-transporting layer on the stability of the perovskite layer. Overall, this work provides a detailed understanding of the formation and humidity-induced degradation mechanism of electrosprayed perovskite films, offering insights that can extend to various applications of perovskite materials.

14 SOLAR ENERGY↗

An Open-Cell Environmental Transmission Electron Microscopy Technique for In Situ Characterization of Samples in Aqueous Liquid Solutions

The desire to image specimens in liquids has led to the development of open-cell and closed-cell techniques in transmission electron microscopy (TEM). The closed-cell approach is currently more common in TEM and has yielded new insights into a number of biological and materials processes in liquid environments. The open-cell approach, which requires an environmental TEM (ETEM), is technically challenging but may be advantageous in certain circumstances due to fewer restrictions on specimen and detector geometry. Here, we demonstrate a novel approach to open-cell liquid TEM, in which we use salt particles to facilitate the in situ formation of droplets of aqueous solution that envelope specimen particles coloaded with the salt. This is achieved by controlling sample temperature between 1 and 10°C and introducing water vapor to the ETEM chamber above the critical pressure for the formation of liquid water on the salt particles. Our use of in situ hydration enables specimens to be loaded into a microscope in a dry state using standard 3 mm TEM grids, allowing specimens to be prepared using trivial sample preparation techniques. Furthermore, our future aim will be to combine this technique with an in situ light source to study photocorrosion in aqueous environments.

47 OTHER INSTRUMENTATION↗

A Deep Learning-Driven Sampling Technique to Explore the Phase Space of an RNA Stem-Loop

The folding and unfolding of RNA stem-loops are critical biological processes; however, their computational studies are often hampered by the ruggedness of their folding landscape, necessitating long simulation times at the atomistic scale. Here, we adapted DeepDriveMD (DDMD), an advanced deep learning-driven sampling technique originally developed for protein folding, to address the challenges of RNA stem-loop folding. Although tempering- and order parameter-based techniques are commonly used for similar rare-event problems, the computational costs or the need for a priori knowledge about the system often present a challenge in their effective use. DDMD overcomes these challenges by adaptively learning from an ensemble of running MD simulations using generic contact maps as the raw input. DeepDriveMD enables on-the-fly learning of a low-dimensional latent representation and guides the simulation toward the undersampled regions while optimizing the resources to explore the relevant parts of the phase space. We showed that DDMD estimates the free energy landscape of the RNA stem-loop reasonably well at room temperature. Our simulation framework runs at a constant temperature without external biasing potential, hence preserving the information on transition rates, with a computational cost much lower than that of the simulations performed with external biasing potentials. Here, we also introduced a reweighting strategy for obtaining unbiased free energy surfaces and presented a qualitative analysis of the latent space. This analysis showed that the latent space captures the relevant slow degrees of freedom for the RNA folding problem of interest. Finally, throughout the manuscript, we outlined how different parameters are selected and optimized to adapt DDMD for this system. We believe this compendium of decision-making processes will help new users adapt this technique for the rare-event sampling problems of their interest.

Gupta, Ayush↗

Lithium–Sulfur Batteries: 3D Printed Tools and Assembly Techniques for Repeatable Lab-Scale Coin Cell Manufacturing

The coin cell form factor has become a standard in energy storage research owing to its relatively low cost, low quantity of requisite electroactive material, fast experimental turnover, and capability to generate publishable quality data. Coin cell assembly at the lab-scale requires precise manual alignment of the many internal components of a cell to yield a properly functioning device. Truly repeatable device assembly presents a significant challenge to the acquisition of reliable data. In this report, we present a three-dimensional (3D) printable design for a coin cell alignment device and describe techniques for a generalized workflow to achieve reproducible coin cell assembly of lithium-based batteries. Standardized assembly techniques using readily accessible, purpose-built tools were demonstrated for labscale production of lithium−sulfur (Li−S) coin cells. Li−S batteries fabricated using the alignment device as well as conductive adhesive incorporated workflows afforded coin cells with up to 35% reduction of assembly times, comparable or better functional cell yields, and improved electrochemical device performance with more consistent and up to 150 mAh/g higher average discharge capacities coupled with Coulombic efficiency increases of up to 2.0% over manually aligned cell assembly techniques.

Batteries↗

How May the Choice of Downscaling Techniques and Meteorological Reference Observations Affect Future Hydroclimate Projections?

Abstract We present an intercomparison of a suite of high‐resolution downscaled climate projections based on a six‐member General Circulation Model (GCM) ensemble from Coupled Models Intercomparison Project (CMIP6). The CMIP6 GCMs have been downscaled using dynamical and statistical downscaling techniques based on two meteorological reference observations over the conterminous United States. We use the regional climate model, RegCM4, for dynamical downscaling, double bias correction constructed analogs method for statistical downscaling, and Daymet and Livneh datasets as the reference observations for statistical training and bias‐correction. We evaluate the performances of downscaled data in both historical and future periods under the SSP585 scenario. While dynamical downscaling improves the simulation of some performance evaluation indices, it adds an extra bias in others, highlighting the need for statistical correction before its use in impact assessments. Downscaled datasets after bias‐correction compare exceptionally well with observations. However, the choice of downscaling techniques and the underlying reference observations influence the hydroclimate characteristics of downscaled data. For instance, the statistical downscaling generally preserves the GCMs climate change signal but overestimates the frequency of hot extremes. Similarly, simulated future changes are sensitive to the choice of reference observations, particularly for precipitation extremes that exhibit a higher projected increase in the ensembles trained and/or corrected by Daymet than Livneh. Overall, these results demonstrate that multiple factors, including downscaling techniques and reference observations, can substantially influence the outcome of downscaled climate projections and stress the need for a comprehensive understanding of such method‐based uncertainties.

54 ENVIRONMENTAL SCIENCES↗

Comparison of machine learning techniques to optimize the analysis of plutonium surrogate material via a portable LIBS device

The utilization of machine learning techniques has become commonplace in the analysis of optical emission spectra. These methods are often limited to variants of principal components analysis (PCA), partial-least squares (PLS), and artificial neural networks (ANNs). A plethora of other techniques exist and are well established in the world of data science, yet are seldom investigated for their use in spectroscopic problems. In this study, machine learning techniques were used to analyze optical emission spectra of laser-induced plasma from ceria pellets doped with silicon in order to predict silicon content. Additionally, a boosted regression ensemble model was created, and its predictive accuracy was compared to that of traditional PCA, PLS, and ANN regression models. Boosted regression tree ensembles yielded fits with R-squared (R2) values as high as 0.964 and mean-squared errors of prediction (MSEPs) as low as 0.074, providing the most accurate predictive model. Neural networks performed with slightly lower R2 values and higher MSEPs compared to the ensemble methods, thus indicating susceptibility to overfitting.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Atomic force microscopy: Emerging illuminated and operando techniques for solar fuel research

Integrated photoelectrochemical devices rely on the synergy between components to efficiently generate sustainable fuels from sunlight. The micro- and/or nanoscale characteristics of the components and their interfaces often control critical processes of the device, such as charge-carrier generation, electron and ion transport, surface potentials, and electrocatalysis. Understanding the spatial properties and structure–property relationships of these components can provide insight into designing scalable and efficient solar fuel components and systems. These processes can be probed ex situ or in situ with nanometer-scale spatial resolution using emerging scanning-probe techniques based on atomic force microscopy (AFM). In this Perspective, we summarize recent developments of AFM-based techniques relevant to solar fuel research. We review recent progress in AFM for (1) steady-state and dynamic light-induced surface photovoltage measurements; (2) nanoelectrical conductive measurements to resolve charge-carrier heterogeneity and junction energetics; (3) operando investigations of morphological changes, as well as surface electrochemical potentials, currents, and photovoltages in liquids. Opportunities for research covered here include: (1) control of ambient conditions for performing AFM measurements; (2) in situ visualization of corrosion and morphological evolution of electrodes; (3) operando AFM techniques to allow nanoscale mapping of local catalytic activities and photo-induced currents and potentials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Techniques for studying materials under extreme states of high energy density compression

The properties of materials under extreme conditions of pressure and density are of key interest to a number of fields, including planetary geophysics, materials science, and inertial confinement fusion. In geophysics, the equations of state of planetary materials, such as hydrogen and iron, under ultrahigh pressure and density provide a better understanding of their formation and interior structure [Celliers et al., “Insulator-metal transition in dense fluid deuterium,” Science 361, 677–682 (2018) and Smith et al., “Equation of state of iron under core conditions of large rocky exoplanets,” Nat. Astron. 2, 591–682 (2018)]. The processes of interest in these fields occur under conditions of high pressure (100 GPa–100 TPa), high temperature (>3000 K), and sometimes at high strain rates (>103 s−1) depending on the process. With the advent of high energy density (HED) facilities, such as the National Ignition Facility (NIF), Linear Coherent Light Source, Omega Laser Facility, and Z, these conditions are reachable and numerous experimental platforms have been developed. To measure compression under ultrahigh pressure, stepped targets are ramp-compressed and the sound velocity, measured by the velocity interferometer system for any reflector diagnostic technique, from which the stress-density of relevant materials is deduced at pulsed power [M. D. Knudson and M. P. Desjarlais, “High-precision shock wave measurements of deuterium: Evaluation of exchange-correlation functionals at the molecular-to-atomic transition,” Phys. Rev. Lett. 118, 035501 (2017)] and laser [Smith et al., “Equation of state of iron under core conditions of large rocky exoplanets,” Nat. Astron. 2, 591–682 (2018)] facilities. To measure strength under high pressure and strain rates, experimenters measure the growth of Rayleigh–Taylor instabilities using face-on radiography [Park et al., “Grain-size-independent plastic flow at ultrahigh pressures and strain rates,” Phys. Rev. Lett. 114, 065502 (2015)]. The crystal structure of materials under high compression is measured by dynamic x-ray diffraction [Rygg et al., “X-ray diffraction at the national ignition facility,” Rev. Sci. Instrum. 91, 043902 (2020) and McBride et al., “Phase transition lowering in dynamically compressed silicon,” Nat. Phys. 15, 89–94 (2019)]. Medium range material temperatures (a few thousand degrees) can be measured by extended x-ray absorption fine structure techniques, Yaakobi et al., “Extended x-ray absorption fine structure measurements of laser-shocked V and Ti and crystal phase transformation in Ti,” Phys. Rev. Lett. 92, 095504 (2004) and Ping et al., “Solid iron compressed up to 560 GPa,” Phys. Rev. Lett. 111, 065501 (2013), whereas more extreme temperatures are measured using x-ray Thomson scattering or pyrometry. This manuscript will review the scientific motivations, experimental techniques, and the regimes that can be probed for the study of materials under extreme HED conditions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

A super-resolution technique to analyze single-crystal inelastic neutron scattering measurements using direct-geometry chopper spectrometers

Direct-geometry time-of-flight chopper neutron spectroscopy is instrumental in studying dynamics in liquid, powder, and single crystal systems. We report here that real-space techniques in optical imagery can be adapted to obtain reciprocal-space super resolution dispersion for phonon or magnetic excitations from single-crystal neutron spectroscopy measurements. The procedure to reconstruct super-resolution energy dispersion of excitations relies on an accurate determination of the momentum and energy-dependent point spread function and a dispersion correction technique inspired by an image disparity calculation technique commonly used in stereo imaging. Here by, applying these methods to spinwave dispersion data from a virtual neutron experiment demonstrates ~5-fold improvement over nominal energy resolution.

47 OTHER INSTRUMENTATION↗

An updated technique to obtain explosive kinetics data on microsecond timescales

There are few techniques available for chemists to obtain time-to-explosion data with known temperature inputs at the early stages of the design and synthesis of new explosives. In the 1960s, a technique was developed to rapidly heat milligram-quantities of confined explosives to ~1000 K on microsecond timescales. Wenograd loaded explosives inside stainless steel hypodermic needles, connected them to a fireset and rapidly discharged a capacitor through the steel. He obtained the temperature by measuring the needle resistance in a Wheatstone bridge arrangement and the time to explosion from a needle rupture. However, owing to the narrow-gauge needles used in the original research, the experiment was only possible with melt-castable explosives; it was never replicated, and modern diagnostics are now available with advances beyond the 1960s. Here, we report the development of the High Explosives Initiation Time (HEIT) test, which utilizes a 250 J pulsed power system to heat the needles. This work extends the Wenograd approach by using optical diagnostics, computational modeling, and advanced techniques to measure needle resistance and needle rupture. Preliminary rate information for pentaerythritol tetranitrate (PETN) will be presented.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

Optimization techniques in self-similar compressible flow

We investigate the one-dimensional (1D) inviscid compressible flow equations for an ideal gas through the lens of optimization techniques. It is the case that, to our knowledge, optimization analysis applied to the so-called “linear velocity” solutions of the Euler compressible flow equations has not been previously conducted. Through both gradient-based and variational techniques, new variants of well-studied flow scenarios, i.e., self-similar, 1D, linear velocity solution class to idealized inviscid compressible flow equations, are determined, as encoded in both the kinematic and thermodynamic properties of this self-similar solution class. With the kinematics of the said solutions being driven by a self-similar “scale radius” and the thermodynamics being driven separately through the appearance of an arbitrary function, a myriad of new solution classes is possible. Acting as a guide to more realistic physical circumstances as well as discovery, it is the hope that the presented cases serve as the framework for future investigations into the intersection of self-similarity and optimization techniques. Fields of study that may find this work to be of interest include aerodynamic design, flow control, inertial confinement fusion, physics-informed neural networks, and other related areas of interest.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Interfacial solvation-structure regulation for stable Li metal anode by a desolvation coating technique

Rechargeable lithium (Li) metal batteries face challenges in achieving stable cycling due to the instability of the solid electrolyte interphase (SEI). The Li-ion solvation structure and its desolvation process are crucial for the formation of a stable SEI on Li metal anodes and improving Li plating/stripping kinetics. This research introduces an interfacial desolvation coating technique to actively modulate the Li-ion solvation structure at the Li metal interface and regulate the participation of the electrolyte solvent in SEI formation. Through experimental investigations conducted using a carbonate electrolyte with limited compatibility to Li metal, the optimized desolvation coating layer, composed of 12-crown-4 ether-modified silica materials, selectively displaces strongly coordinating solvents while simultaneously enriching weakly coordinating fluorinated solvents at the Li metal/electrolyte interface. This selective desolvation and enrichment effect reduce solvent participation to SEI and thus facilitate the formation of a LiF-dominant SEI with greatly reduced organic species on the Li metal surface, as conclusively verified through various characterization techniques including XPS, quantitative NMR, operando NMR, cryo-TEM, EELS, and EDS. The interfacial desolvation coating technique enables excellent rate cycling stability (i.e., 1C) of the Li metal anode and prolonged cycling life of the Li||LiCoO 2 pouch cell in the conventional carbonate electrolyte (E/C 2.6 g/Ah), with 80% capacity retention after 333 cycles.

42 ENGINEERING↗

Noise suppression for MHD characterization with electron cyclotron emission imaging 1D technique

Significant noise suppression for magnetohydrodynamics (MHD) mode characterization in the spatial and spectral domain is achieved by processing two-dimensional (2D) electron cyclotron emission imaging (ECEI) data with a one-dimensional (1D) ECEI technique using a short time window ($1\;{\text{ms}}$). The technique is applied to detect toroidal Alfven eigenmodes (TAEs) in the temporal spectrum and fit their radial envelope using the data from the DIII-D tokamak W-band 2D ECEI system. Using the data length (time window) of only 1 ${\text{ms}}$, the 1D ECEI can clearly detect the TAEs (~100 ${\text{kHz}}$) on the spectrum, while similar spectrum quality requires ~10 ${\text{ms}}$ data length with the cross power spectrum between two midplane ECEI channels. The 1D ECEI technique also effectively avoids biased fitting when resolving the fine structure of the TAE's radial envelope. The radially spatial resolution of 1D ECEI is constrained by the finite ECE radiation volume of the ECEI receiver. Here, with forward radiation modeling, we find the DIII-D ECEI system can sensitively measure the even parity MHD activities, for which the mode width is >15 mm, and tearing modes (odd parity MHD activities), for which the island full width is >30 mm.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Novel fabrication technique for high-resolution spherical crystal analyzers using a microporous aluminium base

Modern inelastic X-ray spectrometers employ curved, bent and diced analyzers to capture sufficiently large solid angles of radially emitted scattered radiation emanating from the sample. Fabricating these intricate analyzers, especially when a high energy resolution of a few millielectronvolts is required, is very time-consuming, expensive and often a hit-or-miss affair. A novel fabrication technique is introduced, utilizing a concave-spherical, microporous aluminium base to hold an assembly of a thin glass substrate with a diced crystal wafer bonded to it. Under uniform vacuum forces, the glass substrate is drawn into the aluminium base, achieving the desired bending radius, while dicing of the diffracting crystal layer prevents bending strain from being imposed on the individual crystal pixels. This technique eliminates the need for permanently bonding the crystal assembly to the concave lens, offering the opportunity for correcting figure errors, avoiding long-term degradation of the permanent bond, and making both lens and crystal reusable. Process and material costs are thus substantially decreased. Two analyzers, Si(844) and Ge(337) with intrinsic resolutions of 14.6 meV and 36.5 meV, respectively, were produced in this fashion and characterized in resonant inelastic X-ray scattering (RIXS) measurements. The achieved overall energy resolutions for both analyzers were 29.4 meV for Si(844) and 56.6 meV for Ge(337). Although the RIXS technique is veru sensitive to analyzer imperfections, the analyzers were found to be equal, if not superior, in quality to their traditional, permanently bonded counterparts.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗