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At least 127 records · Page 7

Multiscale Evaluation of Acetohydroxamic Acid (AHA) Radiolysis Under Used Nuclear Fuel Reprocessing Solvent System Conditions

Acetohydroxamic acid (AHA) has been proposed as an alternative agent for the selective separation of plutonium and neptunium from co-extracted uranium during the reprocessing of used nuclear fuel. However, the fundamental radiolytic behavior of this molecule under envisioned process conditions – i.e., acidic biphasic solvent systems – is not sufficiently understood to support process applications. Here we present a systematic irradiation study (steady-state gamma and time-resolved pulsed electron) into the radiolytic integrity of AHA and formation of degradation products in aqueous nitric acid (HNO3) solutions (0.2 M) in presence and absence of an organic phase, comprising current (tri-butyl phosphate - TBP) and future (N,N-di-(2-ethylhexyl)butyramide - DEHBA and di-2-ethylhexylisobutyramide - DEHiBA) reprocessing ligands dissolved in n-dodecane diluent. Experimental data are complimented by predictive multiscale model calculations for the elucidation of underpinning mechanisms.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Gamma and pulsed electron radiolysis studies of CyMe 4 BTBP and CyMe 4 BTPhen: Identification of radiolysis products and effects on the hydrometallurgical separation of trivalent actinides and lanthanides

The radiolytic stability of the highly selective ligands CyMe 4 BTBP and CyMe 4 BTPhen against ionizing gamma radiation was studied in 1-octanol solution. CyMe 4 BTBP and CyMe 4 BTPhen are important extractants for a potential treatment of used nuclear fuel. They were studied under identical experimental conditions to directly compare the effects of gamma and pulsed electron radiolysis on the ligands and systematically study the influence of structural changes in the ligand backbone. Distribution ratios of Am 3+ , Cm 3+ and Eu 3+ , the residual concentration of CyMe 4 BTBP and CyMe 4 BTPhen in solution, and the formation of radiolysis products were studied as a function of absorbed gamma dose and presence of an acidic aqueous phase during irradiation. Quantitative and semi-quantitative analyses were used to elucidate the radiolysis mechanism for both ligands. Addition products of alpha-hydroxyoctyl radicals formed through radiolysis of the 1-octanol diluent to the ligand molecules were identified as the predominant radiolysis products. These addition products also extract trivalent metal ions, as distribution ratios remained high although the parent molecule concentrations decreased. Therefore, the utilization time of a solvent using these extractants under the harsh conditions of used nuclear fuel treatment could be considerably longer than expected. Understanding the radiolysis mechanism is crucial for designing more radiation resistant extractants.

99 GENERAL AND MISCELLANEOUS↗

Dual particle imaging using time-of-flight neutron classification

Fast-neutron imaging technology is well-suited for passive nuclear material monitoring, secondary inspection of flagged cargo, and wide-area search for lost neutron sources. However, imaging systems that use pulse shape discrimination for event classification require complex pulse waveform analysis. In this work, we evaluate time-of-flight (TOF) based particle classification as an alternative solution for fast-neutron imaging by classifying all events with a TOF above a maximum threshold as neutrons. We measured a Cf-252 source next to Cs-137 using a 12-bar organic-glass scintillator array. By varying the TOF thresholds for neutron identification, we demonstrate a clear trade-off between event yield and backprojection image fidelity, with stricter thresholds improving precision at the cost of statistics, TOF thresholded data generated an image that predicted the neutron source direction with 20% reduced mean central angle prediction error compared to a traditional pulse shape discrimination (PSD) method with comparable event count. Time-of-flight particle classification shows promise as an alternative to pulse shape discrimination systems for fast neutron imaging systems looking to minimize costs and size of electronics with comparable imaging quality. The sources used demonstrate that the method is effective in classifying measured neutrons in a measurement environment with 150 μCi Cs-137 and 1.6 × 10 6 n/s Cf-252 sources positioned at distances of 66 cm and 81 cm from the detector. Additionally, the method classifies low-energy neutron events that pulse shape discrimination removes, so a combination of both methods would result in a higher overall neutron event efficiency.

Heriot, William [Univ. of Michigan, Ann Arbor, MI ↗

Mixed gain detector configurations for time-resolved X-ray solution scattering

X-ray detection at X-ray free-electron lasers is challenging in part due to the XFEL's extremely short and intense X-ray pulses. Experimental measurements are further complicated by the large fluctuations inherent to the self-amplified spontaneous emission process producing the X-rays. At the Linac Coherent Light Source the ePix10ka2M detector offers multiple gain modes, and auto-ranging between these, to increase the dynamic range while retaining low noise. For diffuse scattering techniques, such as time-resolved X-ray solution scattering, where the shape of the scattering pattern largely does not change between exposures, a fixed mix of different gain modes offers many of the same advantages as auto-ranging. We find that configuring individual ASICs in separate gain modes does not impact the intensity linearity of the gain response and has a limited effect on the effective dynamic range in regions with different gain mode settings while avoiding the complexities of auto-ranging. Small (<5%) non-linear gain contributions arise when pixels on the same ASIC are configured in different gain modes. We present a configuration scheme that is designed to select the optimal mixed gain configuration to minimize effects of saturation in the high-/medium-gain region, while maximizing the number of pixels with higher gain to improve the signal-to-noise ratio.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Evolution of Chain Dynamics and Oxidation States with Increasing Chain Length for a Donor–Acceptor-Conjugated Oligomer Series

While it is known that the chain length strongly affects the properties of π-conjugated polymers, the effects of chain length on the molecular structure, chain conformation, and oxidation state properties in donor–acceptor-type conjugated structures remain unclear. This limits our understanding of how the polymer molecular weight impacts material properties. Here, a discrete and monodisperse oligomer series (n = 3, 5, 7, 9, 15, and 21) and polymers (nPB), composed of the donor 3,4-propylenedioxythiophene (ProDOT), the acceptor benzothiadiazole (BTD), and methylthio end-capping groups, are synthesized by C–H-activated cross-coupling. The molecular structure, molecular weight, and dispersity of each oligomer/polymer are thoroughly characterized by nuclear magnetic resonance spectroscopy, mass spectrometry, and gel permeation chromatography. This series reveals a rod-to-coil transition at n = 15 and coil formation at polymer length scales of ~28 units via solution small-angle neutron scattering characterization. The oxidation states are deciphered via cyclic voltammetry, differential pulse voltammetry, spectroelectrochemistry, and density functional theory calculations. Oligomers 3–9 undergo successive one-electron oxidation steps, while 15 and higher undergo multielectron oxidations per step in CH 2 Cl 2 –TBAPF6 at a Pt ultramicroelectrode. The electronic transition of each oxidation state (1+, 2+, 3+, etc.) is tracked by absorption spectroscopy, revealing a “bipolaron to di-polaron” transition at n = 7 at which shorter oligomers prefer bipolaron formation and longer oligomers prefer di-polaron formation in their dication states. Furthermore, oxidized 15 has a lower electronic transition energy compared to its polymer homologue, as shown by spectroelectrochemistry, revealing a synergy between the chain length and the oxidation state properties. This study proves that the convergence limit between small molecule and polymer behavior occurs at approximately 15 units and highlights the property transitions that occur as a function of chain length for a donor–acceptor class of conjugated organic materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Temporal characterization of fundamental plasma parameters in pulsed liquid electrode plasma (LEP) optical emission spectrometry

The fundamental characteristics of liquid electrode plasma (LEP), a pulsed plasma source for optical emission spectrometry, were investigated. Two distinct phases were observed during the process of pulsed plasma generation, namely bubble generation and active plasma discharge. Additionally the ionization efficiency of the LEP, with Mg as a representative analyte, was gauged from the ratio of Mg II 279.553 nm to Mg I 285.213 nm emission and was found to increase from about 5% to 20% in a close-to-linear fashion with the discharge voltage from 800 V to 1200 V. The Mg II/Mg I ratio of the LEP was 2.5 to 3 orders of magnitude less than that typically offered by an inductively coupled plasma (ICP) but was comparable to other solution-based glow discharges. It was found that an off-time interval of more than 150 ms between successive discharge pulses was required to obtain a stable pulse-to-pulse discharge current. Temporally resolved emissions of Mg II 279.6 nm, Mg I 285.2 nm, Fe I 373.5 nm, OH band head at 306 nm, and Hα line at 656.3 nm showed that the background species (OH band and Hα line) reached their maximum emission intensities at around 0.5 ms to 0.7 ms with respect to the onset of the discharge pulse whereas the maximum emissions were observed between 0.7 ms to 0.9 ms for analyte species (Mg and Fe lines). The electron density observed in the present work was in the range from 5.7 × 10 15 cm -3 to 8.2 × 10 15 cm -3 , which was similar to those found in an analytical ICP. The temporal averaged OH rotational temperature was 3300 K, which was comparable to the values of an analytical ICP and solution-based glow discharges. By contrast, the temporally averaged Fe I excitation temperature was around 8900 K, which was even higher than that of an analytical ICP and roughly triple the values obtained by techniques based on glow discharge of liquid samples.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Architecture of the personnel protection systems for Spallation Neutron Source Second Target Station

The Oak Ridge National Laboratory (ORNL) is implementing a major upgrade to the Spallation Neutron Source (SNS) facility, encompassing the addition of the Second Target Station (STS). Preliminary design reviews have been conducted on several STS Personnel Protection Systems (PPS). The reviews focused primarily on the integration with the existing SNS PPS, the new proton transport tunnel, and the target areas. Development of the PPS is ongoing, to ensure a coherent safety system with the mission of protecting users and workers from prompt radiation hazards while providing high beam availability to operations. The STS PPS element in the Integrated Control System (ICS) is a facility-wide system composed of multiple safety subsystems, including the Ring to Second Target (RTST) beam transport tunnel, Target, Bunker and Instruments. Personnel working in all these geographic areas are protected by modular reliable PPS solutions. The safety system enforces access controls, radiation monitoring, beam destination control, and application of critical device inhibit upon detection of abnormal condition. It uses well-documented processes, Common Industrial Protocol (CIP) safety, pulsed test, and redundancy to achieve the desired Safety Integrity Level (SIL). This paper gives an architectural overview of the STS PPS and a detailed safety plan for the SNS facility, addressing safety solutions and human factors.

Michaelides, Tommy [ORNL] (ORCID:0000000190499869)↗

Reinforcement learning pulses for transmon qubit entangling gates

The utility of a quantum computer is highly dependent on the ability to reliably perform accurate quantum logic operations. For finding optimal control solutions, it is of particular interest to explore model-free approaches, since their quality is not constrained by the limited accuracy of theoretical models for the quantum processor—in contrast to many established gate implementation strategies. In this work, we utilize a continuous control reinforcement learning algorithm to design entangling two-qubit gates for superconducting qubits; specifically, our agent constructs cross-resonance and CNOT gates without any prior information about the physical system. Using a simulated environment of fixed-frequency fixed-coupling transmon qubits, we demonstrate the capability to generate novel pulse sequences that outperform the standard cross-resonance gates in both fidelity and gate duration, while maintaining a comparable susceptibility to stochastic unitary noise. We further showcase an augmentation in training and input information that allows our agent to adapt its pulse design abilities to drifting hardware characteristics, importantly, with little to no additional optimization. Our results exhibit clearly the advantages of unbiased adaptive-feedback learning-based optimization methods for transmon gate design.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Benchmarking magnetised three-wave coupling for laser backscattering: analytic solutions and kinetic simulations

Understanding magnetised laser–plasma interactions is important for controlling magneto-inertial fusion experiments and developing magnetically assisted radiation and particle sources. For nanosecond pulses at non-relativistic intensities, interactions are dominated by coherent three-wave interactions, whose nonlinear coupling coefficients became known only recently when waves propagate at oblique angles with the magnetic field. In this paper, backscattering coupling coefficients predicted by warm-fluid theory are benchmarked using particle-in-cell simulations in one spatial dimension, and excellent agreements are found for a wide range of plasma temperatures, magnetic field strengths and laser propagation angles, when the interactions are mediated by electron-dominant hybrid waves. Systematic comparisons between theory and simulations are made possible by a rigorous protocol. On the theory side, the initial boundary value problem of linearised three-wave equations is solved, and the transient-time solutions allow the effects of growth and damping to be distinguished. On the simulation side, parameters are carefully chosen and calibration runs are performed to ensure that comparisons are well controlled. Fitting simulation data to analytical solutions yields numerical growth rates that match theory predictions within error bars. Although warm-fluid theory is found to be valid for a wide parameter range, genuine kinetic effects have also been observed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Strong, Nonresonant Radiation Enhances Cis–Trans Photoisomerization of Stilbene in Solution

Previously, it has been demonstrated that external electric fields may be used to exert control over chemical reactivity. In this paper, the impact of a strong, nonresonant IR field (1064 nm) on the photoisomerization of cis-stilbene is investigated in cyclohexane solution. The design of a suitable reaction vessel for characterization of this effect is presented. The electric field supplied by the pulsed, near-IR radiation (ε 1 = 4.5 × 10 7 V/cm) enhances the cis → trans photoisomerization yield at the red edge of the absorption spectrum (wavelengths between 337 and 340 nm). Within the microliter focal volume, up to 75% of all cis-stilbene molecules undergo isomerization to trans-stilbene in the strong electric-field environment, indicating a significant increase relative to the 35% yield of trans-stilbene under field-free conditions. This result correlates with a 1–3% enhancement in the trans-stilbene concentration throughout the bulk solution. Theoretical analysis suggests that the observed change is the result of dynamic Stark shifting of the ground and first excited states, leading to a significant redshift in cis-stilbene’s absorption spectrum. The predicted increase in the absorption cross section in this range of excitation wavelengths is qualitatively consistent with the experimental increase in trans-stilbene production.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-Voltage Pulsed Power Generator for Beam Injection Systems

Beam injection systems in hadron colliders require kickers generating ±50 kV peak voltages into a 50 Ω impedance, with peak currents of 1000 A and sub-10 ns rise and fall times. This paper presents a novel high-voltage pulse power generator utilizing a distributed pulser architecture. It combines gallium nitride (GaN) transistors in a Marx topology with an inductive adder, achieving nanosecond-scale switching speeds and high-power efficiency. Compared to other solutions such as based on MOSFETs or fast ionization dynistors, our development offers superior peak and average power performance, reduced system complexity, and enhanced reliability, marking a significant step forward in high-voltage pulse generation for accelerator applications.

Smirnov, Alexander (ORCID:0000000280631691)↗

DevOps and Data: Faster-Time-to-Knowledge through SageOps, MLOps, and DataOps

This report describes the approach, investigation, and prototyping efforts to develop an efficient, reusable methodology and reference framework for applying DevOps to disparate data for data science and data analytics at scale, based on focused application of this methodology and reusable reference framework within Sandia National Laboratories’ Pulsed Power community. Additionally, this report reviews: engineered instantiation of the reference framework used for development and production solutions, our experiences and results in using the reference framework, and future plans regarding research and development.

97 MATHEMATICS AND COMPUTING↗

Discovery, Timing, and Multiwavelength Observations of the Black Widow Millisecond Pulsar PSR J1555–2908

Abstract We report the discovery of PSR J1555−2908, a 1.79 ms radio and gamma-ray pulsar in a 5.6 hr binary system with a minimum companion mass of 0.052 M ⊙ . This fast and energetic ( E ̇ = 3 × 10 35 erg s −1 ) millisecond pulsar was first detected as a gamma-ray point source in Fermi Large Area Telescope (LAT) sky survey observations. Guided by a steep-spectrum radio point source in the Fermi error region, we performed a search at 820 MHz with the Green Bank Telescope that first discovered the pulsations. The initial radio pulse timing observations provided enough information to seed a search for gamma-ray pulsations in the LAT data, from which we derive a timing solution valid for the full Fermi mission. In addition to the discovery and timing of radio and gamma-ray pulsations, we searched for X-ray pulsations using NICER but no significant pulsations were detected. We also obtained time-series r -band photometry that indicates strong heating of the companion star by the pulsar wind. Material blown off the heated companion eclipses the 820 MHz radio pulse during inferior conjunction of the companion for ≈10% of the orbit, which is twice the angle subtended by its Roche lobe in an edge-on system.

79 ASTRONOMY AND ASTROPHYSICS↗

Non-Equilibrium Plasma Interactions with Biomaterials, Biological Solutions and Tissues

Cold atmospheric pressure plasma discharges offer an abundant source of reactive oxygen and nitrogen species (RONS) at room temperature enabling unique interactions with biomaterials, biological solutions and tissues. These interactions particularly with living matter are presently an important intellectual frontier in plasma science with promising potential applications ranging from human health care to advanced biomaterial processing. Exciting case studies have been reported that illustrate the huge potential of cold atmospheric plasma technology in wound healing and cancer treatment. The interaction of plasma with conducting and dielectric biomaterials such as tissue strongly influences the plasma properties. In turn this changes the impact of the plasma on the biomaterial. Particularly in the case of living matter, liquid based solutions are ubiquitous which complicates interfacial processes. The lack of insight into the underlying mechanisms of the interaction of plasma with wounds and tumors is currently a bottleneck for the further development of the technology and gives rise to many interesting scientific questions. This project was focused on plasma properties and kinetics during plasma-biomaterial interactions. Both DC pulsed and RF driven atmospheric pressure plasma jets, extensively used by the plasma community were studied. The bio-interfaces included hydrogel as a tissue model, (saline) solutions, bacteria and virus. Plasma diagnostics used include Thomson scattering, Rayleigh scattering, Raman scattering, (two-photon absorption) laser induced fluorescence, optical emission spectroscopy, absorption spectroscopy, molecular beam mass spectrometry and fast imaging allowing to determine electron densities and temperatures, ionic species, reactive species including radicals, gas temperatures, gas composition, electric fields and solution components transferred to the gas phase.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Solving the Pulsed-Power Driven Inertial Fusion Energy Standoff Problem (Abbreviated Final Report)

The standoff problem in pulsed-power driven IFE (Inertial Fusion Energy) refers to the problem of electrically connecting a fusion target with the driver in a way that preserves the driver/target interface in the presence of a large fusion energy release (100’s of megajoules to 1000 megajoules). High yield fusion drivers for stockpile stewardship applications have similar concerns, but without the complication of the high repetition rate needed for energy production. All proposed IFE or high yield systems have the challenge of protecting the reactor vessel and driver from the energy release, but pulsed power drivers have the additional challenge of establishing an electrical connection in a way that does not create excessive debris or require costly/massive structures that must be expendable. Fortunately, there are conceptual solutions in the form of very low mass transmission lines, usually in the form of wires or foils, since very little mass is needed to overcome the magnetic forces driving the transmission lines apart or provide a low resistance pathway given the short pulse duration of the driver. Several important aspects of the standoff problem were analyzed in the course of this LDRD project. Conceptual means of introducing the low mass transmission lines into the reactor chamber were proposed, including analysis of methods to retain the power flow gap between the electrodes in the presence of the chamber environment. The energy losses due to ohmic dissipation and magnetic acceleration of the low mass transmission lines were evaluated for candidate driver pulses and different transmission line masses, and the fluence of x-ray and neutron energy on the persistent power flow structures that must survive the pulse of energy were evaluated. Finally, means of rapidly pumping down the chamber were explored as a way to return the system to low pressure following the multi-atmosphere post-pulse pressure rise. The overall conclusion from the analysis is that, while the reactor environment creates stressful conditions for a low mass transmission line standoff system, there are concepts expending 10 kg or less of electrode mass each pulse with the potential to mitigate the stresses and successfully drive fusion targets. Whether such a system could lead to a practical and economical fusion reactor would require extensive research and development beyond the scope of the feasibility study.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Mechanical Property Evaluation of CuNb Composites Manufactured with High-Pressure Torsion

Copper is under consideration as the optimum material for both high heat flux applications and high pulsed magnets. One challenge is that copper has low strength which is problematic to deployment in these applications. One solution is to alloy copper with BCC elements to improve its mechanical properties. However, the limited solubility of the BCC elements in copper requires high deformation processes to be used in order to manufacture these 3D composites. Here, high energy ball milling combined with high pressure torsion was used to manufacture 3D Cu-Nb composites. After the consolidation the mechanical properties of the composites were measured using micro- and nanohardness testing at room and elevated temperature. The results indicated that after 10 turns during the high-pressure torsion consolidation, the mechanical properties of the composites were completely saturated displaying uniform properties across the manufactured disk. Performing the high pressure torsion at temperature further improved consolidation of the disk. The high temperature nanoindentation also indicated a change in the deformation mechanism between 200 and 500 ºC.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Non-inductive plasma vertical position measurement for the 1056 s discharge on EAST

Vertical position stability plays a crucial role in maintaining safe and reliable plasma operation for long-pulse fusion devices. In general, the vertical position is measured by using inductive magnetic coils installed inside the vacuum vessel; however, the integration drift effects are inherent for steady-state or long-pulse plasma operation. Further, developing a non-magnetic approach provides a fusion reactor-relevant steady-state solution that avoids the negative impact of integration drift. In this paper, we compare the non-inductively determined vertical position achieved by line-integrated interferometer and polarimeter measurements to that employing an inductive flux loop for a 1056 s discharge recently achieved on EAST (Experimental Advanced Superconducting Tokamak). Experimental results show that the non-inductive measurement is more robust than flux loops after 300 s if the integrator is not reset to suppress integrator drift. Real-time vertical position control using the non-inductive system is proposed for the next EAST experimental campaign.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Turbulence suppression at extreme plasma densities on DIII-D and EAST

Recent high-poloidal-beta (high-βP) experiments on DIII-D and EAST have made coordinated breakthroughs for high confinement quality at high density near the Greenwald limit. Density gradient amplification of turbulence suppression at high βP can explain both of these achievements. Experiments on DIII-D have achieved Greenwald fraction (fGr = line-averaged density/Greenwald density) above 1 simultaneously with normalized energy confinement (H98y2) around 1.5, as required in fusion reactor designs but never before verified in tokamak experiments with the divertor configuration. A synergy between increased H98y2 and fGr is observed with strong gas puffing, due to the build-up of an internal transport barrier at large radius in the temperature and density channels. Transport simulations reveal that the favorable trend of reduced turbulent energy transport at higher density is only expected when increasing the density gradient at high local safety factor and high β, thus at high βP to ensure strong α-stabilization. These conditions are crucial to many conceptual designs for steady-state reactors. New experiments on EAST have nearly doubled the ion temperature at fGr ∼ 0.9, consistent with predict-first modeling results based on the same physics revealed from the DIII-D analysis. All previous EAST long-pulse H-modes have Ti ≪ Te near plasma axis. Transport modeling indicates that the profiles are limited by ion-temperature-gradient modes at mid-radius. The modeling also suggested potential solutions, including reducing magnetic shear, enhancing density gradients, and higher impurity concentration. Following this guidance, EAST experiments directly show a strong enhancement of Ti achieved with a combination of a second plasma current ramp-up, a density gradient increase, and a Zeff perturbation by a short pulse (100 ms) of impurity injection, as predicted by the earlier modeling.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗