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At least 343 records · Page 19

Elemental fractionation in aerosol laser-induced breakdown spectroscopy with nanosecond and femtosecond laser ablation

For the purpose of realizing atmospheric radiation plume tracking, laser-induced breakdown spectroscopy (LIBS) was performed to characterize Cs atomic emissions from airborne nanoparticles in a binary particle matrix using nanosecond and femtosecond laser ablation. As a surrogate to multi-element nuclear fallout particulates, both Cs and Na solutions were mixed with Cu at a 1:1.45 M concentration ratio and aerosolized to study elemental fractionation in atomic emissions, revealing Na I resonance emissions are enhanced whereas Cs I resonance emissions are reduced with Cu present despite sharing similar electronic and chemical properties. Femtosecond laser ablation reduced elemental fractionation effects by more than 50% while retaining the same temporal fractionation trends for Cs and Na. The origin of elemental fractionation in aerosol LIBS was further investigated using Al and Ti aerosols which revealed that the particle matrix induces changes to the local plasma temperature, population of atomic states, and subsequent molecular association and emission.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Metal DiSulfide thin films synthesized by pulsed ion beam ablation: Self-assembled structures with improved mechanical properties in humid conditions

Thin films composed of transition metal dichalcogenides such as molybdenum disulfide (MoS 2 ) or tungsten disulfide (WS 2 ) are well known for their solid lubricating behavior in dry environments such as space, but deteriorate rapidly in environments where oxygen is present. There have been many attempts over recent decades to improve MoS 2 lubricating performance in humid environments by addition of metals such as titanium to the film. The additions have come in the form of co-sputtering with the MoS 2 , or formation of nano multilayer coatings. We have previously reported on the synthesis of MoS 2 films by high-power ion beam ablation [Prasad et al, Matls. Lett. 65 (2010) 4–6]. The resulting films are observed to contain spheres of pure Mo of 10–100 nm size evenly dispersed throughout the ~1 μm-thick film, a form of self-assembly not before seen in films produced by sputtering or by pulsed laser deposition (PLD). The remaining Mosingle bondS matrix was observed to crystalize in situ under frictional contact into MoS 2 with the basal planes orienting themselves in the direction of sliding underneath the wear surface. The present study concerns metal additions in the form of alternating layers with MoS 2 deposited in between from an ablation target. The addition of Ti resulted in the extension of good tribological performance to humid air conditions, but the path to good performance appears to be relatively narrow. The same distributed Mo spheres were present in the new film, and similar self-assembled morphologies when V was substituted for the Ti, and when multilayers were formed of WS 2 with Zr additions. Furthermore, it appears that addition of Ti resulted in improvements in mechanical film strength that contributed to the wear ability in humid conditions.

Intense ion beams↗

Uranium Single Particle Analysis for Simultaneous Fluorine and Uranium Isotopic Determinations via Laser-Induced Breakdown Spectroscopy/Laser Ablation–Multicollector–Inductively Coupled Plasma–Mass Spectrometry

Uranyl fluoride (UO 2 F 2 ) particles (<20 μm) were subjected to first-of-its-kind analysis via simultaneous laser-induced breakdown spectroscopy (LIBS) and laser ablation multi-collector inductively coupled plasma–mass spectrometry (LA–MC–ICP–MS). Briefly, a nanosecond pulsed high-energy laser was focused onto the sample (particle) surface. In a single laser pulse, the UO 2 F 2 particle was excited/ionized within the microplasma volume, and the emission of light was collected via fiber optics such that emission spectroscopy could be employed for the detection of uranium (U) and fluorine (F). The ablated particle was simultaneously transported into the MC–ICP–MS for high precision isotopic (i.e., 234 U, 235 U, and 238 U) analysis. This method, LIBS/LA–MC–ICP–MS was optimized and employed to rapidly measure 80+ UO 2 F 2 particles, which were subjected to different calcination processes, which results in varying degrees of F loss from the individual particles. In measuring the particles, the average F/U ratios for the populations treated at 100 and 500 °C were 2.78 ± 1.28 and 1.01 ± 0.50, respectively, confirming loss of F through the calcination process. The average 235 U/ 238 U on the particle populations for the 100 and 500 °C were 0.007262 (22) and 0.007231 (23), which was determined to be <0.2% from the expected value. The 234 U/ 238 U ratios on the same particles were 0.000053 (11) and 0.000050 (10) for the 100 and 500 °C, respectively, <10% from the expected value. Notably, each population was analyzed in under 5 min, demonstrating the truly rapid analysis technique presented here in this paper.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

The effect of oxygen concentration on the speciation of laser ablated uranium

Abstract In order to model the fate and transport of particles following a nuclear explosion, there must first be an understanding of individual physical and chemical processes that affect particle formation. One interaction pertinent to fireball chemistry and resultant debris formation is that between uranium and oxygen. In this study, we use laser ablation of uranium metal in different concentrations of oxygen gas, either 16 O 2 or 18 O 2 , to determine the influence of oxygen on rapidly cooling uranium. Analysis of recovered particulates using infrared absorption and Raman spectroscopies indicate that the micrometer-sized particulates are predominantly amorphous UO x (am-UO x , where 3 ≤ x ≤ 4) and UO 2 after ablation in 1 atm of pure O 2 and a 1% O 2 /Ar mixture, respectively. Energy dispersive X-ray spectroscopy (EDS) of particulates formed in pure O 2 suggest an O/U ratio of ~ 3.7, consistent with the vibrational spectroscopy analysis. Both am-UO x and UO 2 particulates convert to α-U 3 O 8 when heated. Lastly, experiments performed in 18 O 2 environments show the formation of 18 O-substituted uranium oxides; vibrational frequencies for am-U 18 O x are reported for the first time. When compared to literature, this work shows that cooling timescales can affect the structural composition of uranium oxides (i.e., crystalline vs. amorphous). This indicator can be used in current models of nuclear explosions to improve our predicative capabilities of chemical speciation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Time resolved ablator areal density during peak fusion burn on inertial confinement fusion implosions

Near peak compression, inertial confinement fusion implosions release both deuterium–tritium (DT) fusion gamma rays and neutron induced gamma rays from carbon from the areal density of the remaining ablator shell. The gamma reaction history diagnostic makes a time resolved measurement of both. Across many recent implosions, the carbon gamma ray peak arrives systematically 11 ± 10 ps later compared to DT fusion burn. The timing shift is consistent with the carbon areal density increasing throughout the peak of the fusion burn, implying that the carbon portion of the capsule continues to converge. A model finds that the observed timing shift is consistent with a 4π averaged carbon ablator inward velocity of 80 μm/ns for the contemporary National Ignition Facility implosions. In this work, the timing shift is possibly related to the energy balance of the implosion, with the expectation that a high performing, igniting capsule would see the carbon gamma rays arrive before the DT fusion peak.

Nuclear fusion↗

Faster ablative Kelvin–Helmholtz instability growth in a magnetic field

Shear flows along a plasma interface will quickly grow unstable due to the Kelvin–Helmholtz instability. If there is a concurrent temperature gradient across the interface, higher modes are stabilized by the thermal diffusion. These ablative effects must be considered in, for example, jet features in inertial confinement fusion hot-spots, or plasma plumes in young supernovae. We show that magnetization of the plasma can greatly affect the instability, even if magnetic pressure is small. This is because electrons are localized by their gyromotion, reducing the heat flux and material ablation. We use a two-dimensional numerical extended-magnetohydrodynamics approach to assess this effect for dense fusion conditions. In comparison with the unmagnetized case, self-generated Biermann fields make only a minor difference to growth rates. However, simulations with a large 50 kT external field found that the growth rate of the least stable mode increased by 40%. In conclusion, this has implications for mix processes in Z-pinches and magnetized inertial confinement fusion concepts.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Measurement and simulation of small cryogenic neon pellet Ne-I 640 nm photon efficiency during ablation in DIII-D plasma

Small (~1 mm) neon pellet fragments are fired into DIII-D H-mode plasmas, and resulting trajectory-averaged photon efficiencies (neutral neon ionization events for every photon emitted) of S/XB ≈ 85 are estimated for Ne-I 640 nm by dividing the estimated initial pellet fragment mass by the measured number of emitted Ne-I photons. The experiments are modeled by running the Lagrangian particle (LP) fluid/magneto-hydrodynamic pellet code to estimate axial ablation plume neon density profiles and temperature profiles at each pellet position. These solutions are then fed into the PrismSPECT collisional-radiative code, which calculates resulting neon charge states and photon emission rates, giving a profile-average of S/XB ≈ 109. The burnthrough plasma minor radius predicted by LP (ρ ≈ 0.63) is reasonably close to the experimental observation ρ ≈ 0.6. Furthermore, the modeling indicates that local S/XB is not constant along the pellet trajectory but tends to increase with increasing ablation rate. Non-equilibrium kinetics are predicted to be very important, while line trapping is predicted to be relatively unimportant (for Ne-I 640 nm S/XB).

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Evolution and persistence of SiO emission in nanosecond laser ablation plumes

Analyzing laser-produced plasmas in a controlled oxygen-containing environment provides insight into the formation and evolution of molecular species through gas-phase oxidation. This study explores the role of ambient pressure and oxygen availability in forming SiO molecular species in laser ablation plumes. The self-emission emanating during the reactive ablation of Si targets was characterized by optical emission spectroscopy and optical time-of-flight techniques. Our results showed that the SiO species formation was greatly influenced by both the ambient pressure and oxygen availability. The intensity and the persistence of SiO emission bands are lower at higher oxygen concentrations, indicating they are depopulated by the formation of more complex silicon oxides. The oxygen partial pressure effects on plume chemistry showed that SiO formation is favored even with a minimal oxygen concentration in the environment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Self-consistent investigation of density fueling needs on ITER and CFETR utilizing the new Pellet Ablation Module

Abstract Self-consistent modeling using the stability, transport, equilibrium, and pedestal (STEP) workflow in the OMFIT integrated modeling framework (predicting pedestal with EPED, core profiles with TGYRO, current profile with ONETWO, and EFIT for equilibrium) suggests ITER and future devices such as China Fusion Engineering Test Reactor (CFETR) Zhuang et al (2019 Nucl. Fusion 59 112010) will benefit from high-density operation (Greenwald limit fraction f g w ≈ 0.7−1.3). Regimes with an operational density near the Greenwald limit will likely need peaked density profiles so that the pedestal density remains below the Greenwald limit. Peaked density profiles can be achieved with the help of pellet injection. A flexible Pellet Ablation Module (PAM), which predicts the density source based on a comprehensive analytical pellet ablation model, has been developed for predicting pellet fueling for transport studies, and has been incorporated into the STEP workflow for predictive modeling. This workflow is applied to DIII-D and finds good agreement with experiments. On ITER the effect of pellet fueling is examined in an advanced inductive scenario, where a fusion gain of up to Q = 9 is predicted with strong central pellet fueling. On CFETR, with a mid-radius density source, an average of 1.5 × 10 22 electrons s −1 are required to achieve the density and temperature profiles necessary for the 1000 MW advanced scenario with a tritium burn-up fraction of ∼ 3 % .

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Numerical investigation of liquid wall ablation in inertial fusion energy chambers

This paper presents a novel approach for modeling liquid wall ablation in liquid wall-protected inertial fusion energy (IFE) chambers. These systems are promising candidates for the implementation of fusion technology, yet significant gaps remain in understanding the underlying physical processes and their implications for design. Following target ignition, a portion of the fusion energy is released as x-rays, which deposit their energy into an array of liquid jets, leading to partial vaporization. Accurately modeling this heat deposition and vaporization process remains challenging due to the complex geometries typical of (pre-conceptual) IFE chamber designs. Furthermore, the subsequent expansion of vaporized material into the chamber’s vacuum environment poses difficulties for conventional CFD methods based on continuum assumptions, which can lead to significant inaccuracies. To address some aspects of these challenges, this work introduces a ray-tracing-based methodology to map the spatial distribution of ablated material in liquid wall-protected systems. In addition, a vacuum-tracking scheme is developed to extend the applicability of an OpenFOAM-based solver to gas dynamics in rarefied environments. The proposed approach has been verified through numerical benchmarks and applied to a practical case involving the HYLIFE-II (High Yield Lithium Injection Fusion Energy) chamber. The methodology advances the modeling capabilities for liquid wall-protected IFE systems and provides valuable tools to support their design and optimization.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Implementing a microphysics model in hydrodynamic simulations to study the initial plasma formation in dielectric ablator materials for direct-drive implosions

A microphysics model to describe the photoionization and impact ionization processes in dielectric ablator materials like plastic has been implemented into the 1-D hydrodynamic code LILAC for planar and spherical targets. Currently, the initial plasma formation during the early stages of a laser drive are modeled in an ad hoc manner, until the formation of a critical surface. Implementation of the physics-based models predict higher values of electron density, electron temperature, and pressure than the ad hoc model. Moreover, the numerical predictions are consistent with previous experimental observations of the shinethrough mechanism in plastic ablators. For planar targets, a decompression of the rear end of the target was observed, that is similar to recent experiments. An application of this model is to understand the laser-imprint mechanism that is caused by nonuniform laser irradiation due to single beam speckle.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Magnetic Signatures of Radiation-Driven Double Ablation Fronts

In experiments performed with the OMEGA EP laser system, magnetic field generation in double ablation fronts was observed. Proton radiography measured the strength, spatial profile, and temporal dynamics of self-generated magnetic fields as the target material was varied between plastic (CH), aluminum, copper, and gold. Two distinct regions of magnetic field are generated in mid-Z targets -- one produced by gradients from electron thermal transport and the second from radiation-driven gradients. Extended magnetohydrodynamic simulations including radiation transport reproduced key aspects of the experiment, including field generation and double ablation front formation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Direct Measurement of Ice-Ablator Interface Motion for Instability Mitigation in Indirect Drive ICF Implosions

In indirect drive inertial confinement fusion (ICF) implosions hydrodynamic instability growth at the imploding capsule ablator-DT fuel interface can reduce fuel compressibility and inject ablator into the hot spot hence reducing hot spot pressure and temperature. As a mitigation strategy, a gentle acceleration of this interface is predicted by simulations and theory to significantly reduce this instability growth in the early stage of the implosion. We have performed high-contrast, time-resolved x-ray refraction enhanced radiography (RER) to accurately measure the level of acceleration as a function of the initial laser drive time history for indirect-drive implosions on the National Ignition Facility. Here, we demonstrate a transition from no acceleration to 20 ± 1.8μm ns -2 acceleration by tweaking the drive that should reduce the initial instabilities by an order of magnitude at high modes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Laser pulse-length dependent ablation and shock generation in silicon at 5 × 10 14 W/ cm 2 intensities

The effect of laser pulse duration on energy coupling into a planar silicon target is investigated in experiments at the OMEGA-EP facility by varying the laser pulse length τ —spanning 3 orders of magnitude from 100 ps to 10 ns—while maintaining a constant peak laser intensity, I 0 = 5 × 10 14 W/ cm 2 . In theoretical models, the ablation pressure primarily scales for a given material with laser intensity and wavelength, which are all fixed variables here, allowing us to explore the specific role of laser pulse duration. Two-dimensional radiation-hydrodynamics simulations benchmarked with optical probing of the expanding plasma show that the pulse duration is critical for the ablation pressure to reach a steady state. Moreover, the pulse duration impacts shock decay and multiple wave effects, which strongly dictate the evolving shock profile that propagates within the laser-shocked target as ultimately measured by rear-surface diagnostics. The shock velocities inferred from the theoretical model, after considering shock decay, impedance matching, and shock Hugoniot, are found to be in good agreement with velocimetry measurements. However, discrepancies are observed with simulations for the shorter (0.1 ns) and longer (10 ns) pulse durations, which are respectively attributed to unaccounted contributions of kinetic absorption mechanisms and instabilities in simulations. Published by the American Physical Society 2024

Bailly-Grandvaux, M. (ORCID:0000000175294013)↗

Characterization of ablator dynamics initiated by picket-pulse conditions

Direct-drive laser-fusion targets may include low-cost plastic ablator material. Here, this work describes a tabletop experimental system designed to enable the investigation of the interaction of such ablator material as a function of the laser wavelength and the associated excitation mechanism. This experimental system offers time-resolved imaging of the material response with subpicosecond temporal resolution and ≈1-μm spatial resolution. The system involves synchronized femtosecond and picosecond lasers to initiate and characterize the dynamics of polystyrene planar targets irradiated by conditions similar to a “picket” prepulse from a direct-drive pulse shape. Ultrafast imaging of the initial excitation process followed by the resulting critical plasma formation, shock-wave propagation, and blowoff plasma expansion is used to compare the impact of excitation wavelength, 355 nm or 266 nm, on the ensuing dynamics. This work aims to investigate fundamental laser material interactions to help advance physics models that can inform the development of laser driver and target designs.

42 ENGINEERING↗

Single-shot, double-pulse determination of the detonation energy in nanosecond-laser ablation using the blast model

We demonstrate a novel single-shot method to determine the detonation energy of laser-induced plasma and investigate its performance. This approach can be used in cases where there are significant shot-to-shot variations in ablation conditions, such as laser fluctuations, target inhomogeneity, or multiple filamentation with ultrashort pulses. The Sedov blast model is used to fit two time-delayed shadowgrams measured with a double-pulse laser. We find that the reconstruction of detonation parameters is insensitive to the choice of interpulse delay in double-pulse shadowgraphy. In contrast, the initial assumption of expansion dimensionality has a large impact on the reconstructed detonation energy. The method allows for a reduction in the uncertainties of blast wave energy measurements as a diagnostic technique employed in various laser ablation applications.

42 ENGINEERING↗

Detection limits for laser absorption spectroscopy of Li in laser ablation plumes

A high-sensitivity laser absorption spectroscopy (LAS) method is demonstrated for rapid and non-contact analysis of Li in solids. Glass samples with Li concentrations ranging from 1-500 ppm by mass are ablated in 5 Torr air, and time-resolved Li atomic absorption is measured using a tunable laser near 671 nm. Significant improvements in analytical performance over prior laser-induced breakdown techniques are demonstrated. Here, a single-shot limit of detection (LOD) of 180 ppb is shown for fixed wavelength operation, improving to 6 ppb with averaging over 1000 ablation shots (100 s acquisition time). Isotope-resolved Li absorption spectra are measured with a 17 ppb LOD in 40 s. Methods for optimizing LOD based on noise/averaging properties of LAS experiments in LA plumes are discussed.

(020.3260) Isotope shifts↗

Method Development for Measuring U Isotope Ratios by Laser Ablation MC-ICP-MS. Task 1: Hardware Setup

The aim of this project is to develop methodology to identify and analyze U and Pu containing particles using laser ablation MC-ICP-MS. The final methodology will ultimately be described in a detailed procedural document that will be shared with IAEA-NWAL laboratories. In this report, we describe the Task-1 deliverable; the setup and optimization of hardware required to perform U isotopic analyses by laser ablation MC-ICP-MS.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗