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NASA NTRS2019

Bayesian Inference and the Effects of Varying Uncertainty Models in Charring Ablator Calibration and Uncertainty Quantification Problems

The Mars Science Laboratory (MSL) vehicle utilized a heat shield constructed from NASA’s Phenolic-Impregnated Carbon Ablator (PICA) material to protect the main structure from the high enthalpy environment encountered during hypersonic atmospheric entry. During the vehicle’s descent through Martian atmosphere, multiple thermocouples embedded within the heat shield captured in-depth material temperature data that allow for studies to be conducted on current material response reconstruction tools. In the present work, material temperature data obtained from thermocouples within the MISP-4 plug (MEDLI (Mars Science Laboratory Entry, Descent, and Landing Instrument) Integrated Sensor Plug) are utilized in the calibration of Theoretical Ablative Composite for Open Testing (TACOT) model parameters in conjunction with NASA’s Porous material Analysis Toolbox (PATO) through Bayesian inference where uncertainty due to parametric, modeling, and experimental sources is simultaneously quantified. Prior to the study, a sensitivity analysis is performed through computation of the robust Sobol indices in an effort to study the relationship between input space and model response and to reduce the dimensionality of the statistical inverse problem. The Bayesian inference methodology necessitates an a-priori choice to be made for the uncertainty model for which numerous possibilities are available. Across most works, however, only basic additive or multiplicative models are utilized with pre-defined magnitudes of uncertainty based on a-priori knowledge or to-be-calibrated multipliers of static covariance matrix structures. The present effort explores the effects of informed uncertainty models, ones with temporal dependence that are simultaneously calibrated through Bayesian inference, on calibrated results for parameters that make up the uncertain input space.

Sensitivity Analysis↗

DOE OSTI2018

The Ablation and Oxidation Behaviors of SiC Coatings on Graphite Prepared by Slurry Sintering and Pack Cementation

SiC coatings were generated on graphite using slurry sintering (SS) and pack cementation (PC). The samples’ ablation features were assessed by an oxyacetylene torch. The rates of mass ablation of the PC–SiC and SS–SiC coatings were approximated 2.17 × 10{sup −3} and 9.52 × 10{sup −3} g s{sup −1}, respectively, decreased by 84.1 and 29.6% compared to the uncoated samples. It was mainly attributed to the formation of a SiO{sub 2} layer on the surface. The continuous SiO{sub 2} molten film formed via the PC–SiC oxidation generates a sealing mechanism which can be an obstacle against the oxygen diffusion and hinder more ablation. This is while discontinuous SiO{sub 2} film formed from the thin SS–SiC cannot protect the graphite effectively. The non-isothermal oxidation test shows that without the SiC coating, the sample weight is lost largely from 25 to 1500 °C, and its weight loss was 2.2% after the TGA. However, after coating, the samples possessed excellent oxidation protection and weight losses of SS–SiC and PC–SiC coatings are down to 1.3 and 0.6%, respectively. The more oxidation of the graphite substrate occurred due to the formation of macrocracks in the coating during the TGA and also the formation of holes on SiO{sub 2} glass layer owing to release of CO or CO{sub 2}.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Fe-carbide/Fe-oxide-based nanocomposites synthesized as magnetic nanomaterials via laser ablation synthesis in solution (LASiS)

Magnetic nanostructured materials (MNMs) have gained prominence in materials technology developments owing to their potential biomedical applications for hyperthermia cancer treatment, and transplant organ cryopreservation. Herein, we report the facile and cost-effective synthesis of Fe-based composite MNMs, comprising both Fe@Fe 2 O 3 and Fe 3 C@C core-shell nanoparticles (NPs), via Laser Ablation Synthesis in Solution (LASiS) using Fe targets ablated under acetone and toluene. Detailed materials characterizations using electron microscopy-based imaging, diffraction studies, and spectroscopic analyses - including Raman and Mössbauer spectroscopy - relate the structure-composition properties for different Fe-oxide/carbide phases in the aforesaid MNMs to their respective magnetic responses. Specifically, we confirm the presence of ultra-small (2–10 nm) amorphous Fe-oxide NPs, as well as Fe@Fe 2 O 3 core-shell NPs (20–40 nm) in the samples synthesized by ablating Fe under acetone. In contrast, samples synthesized under toluene indicate a higher concentration of Fe 3 C@C core-shell NPs (20–40 nm) with a relatively low concentration of Fe 2 O 3 NPs (2–10 nm). Furthermore, the crystallinity of the metallic phases and carbonaceous shell coatings are systematically increased by carrying out LASiS under heated toluene (up to ~95 °C). Importantly, mössbauer spectroscopy results indicate that the elevation in toluene temperature leads to an increase in the concentrations of Fe 3 C@C NPs from ~40 % to ~53 % (at.).

36 MATERIALS SCIENCE↗

DOE OSTI2015

Definitive Management of Oligometastatic Melanoma in a Murine Model Using Combined Ablative Radiation Therapy and Viral Immunotherapy

Purpose: The oligometastatic state is an intermediate state between a malignancy that can be completely eradicated with conventional modalities and one in which a palliative approach is undertaken. Clinically, high rates of local tumor control are possible with stereotactic ablative radiation therapy (SABR), using precisely targeted, high-dose, low-fraction radiation therapy. However, in oligometastatic melanoma, virtually all patients develop progression systemically at sites not initially treated with ablative radiation therapy that cannot be managed with conventional chemotherapy and immunotherapy. We have demonstrated in mice that intravenous administration of vesicular stomatitis virus (VSV) expressing defined tumor-associated antigens (TAAs) generates systemic immune responses capable of clearing established tumors. Therefore, in the present preclinical study, we tested whether the combination of systemic VSV-mediated antigen delivery and SABR would be effective against oligometastatic disease. Methods and Materials: We generated a model of oligometastatic melanoma in C57BL/6 immunocompetent mice and then used a combination of SABR and systemically administered VSV-TAA viral immunotherapy to treat both local and systemic disease. Results: Our data showed that SABR generates excellent control or cure of local, clinically detectable, and accessible tumor through direct cell ablation. Also, the immunotherapeutic activity of systemically administered VSV-TAA generated T-cell responses that cleared subclinical metastatic tumors. We also showed that SABR induced weak T-cell-mediated tumor responses, which, particularly if boosted by VSV-TAA, might contribute to control of local and systemic disease. In addition, VSV-TAA therapy alone had significant effects on control of both local and metastatic tumors. Conclusions: We have shown in the present preliminary murine study using a single tumor model that this approach represents an effective, complementary combination therapy model that addresses the need for both systemic and local control in oligometastatic melanoma.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

DOE OSTI2023

Laser Ablation-Capillary Absorption Spectroscopy: A novel approach for high throughput and increased spatial resolution measurements of δ 13 C in plant-soil systems

Spatial and temporal heterogeneity of nutrient exchange within the rhizosphere is a topic of increasing interest, although challenging to study due to limits in existing analytical capabilities. Here, we developed and demonstrated a new approach applying laser ablation sample introduction to capillary absorption spectroscopy (LA-CAS) to characterize carbon isotopic distribution within plant tissues, rhizosphere, and soil. We exposed switchgrass plants to 13 CO 2 to allow tracing of 13 C-labelled photosynthates within plant biomass and into the associated soil. The LA-CAS methods we describe leverage continuous measurements of a sample stream derived from laser ablation line scans (10-25 µm in width) over a sample surface which enables the user to produce an isotope map with a) higher data density or b) over larger spatial areas versus previously existing techniques. This versatility of LA-CAS is assessed through testing of a range of laser parameters (spot size, scan rates) on various materials (soil, plant biomass/tissues, and rhizosphere). Here, we demonstrate the ability of LA-CAS to provide near instantaneous $δ$ 13 C measurements over isotopically distinct surfaces to enable high spatially resolved mapping of 13 C-labelled material within the rhizosphere. Applying LA-CAS analysis to plant biomass, we observed higher $δ$ 13 C values concentrated within phloem structures, consistent with localized photosynthate transport. When mapping across the rhizosphere, 13 C-enriched soil was typically present within 5-10µm of root boundaries with a steep spatial increase in $δ$ 13 C when the scan approached the middle of the root. As with all LA approaches, care is required to ensure accurate results as phenomena linked to ablation, combustion, and isotopic measurement can impart artifacts if not carefully controlled. Still, taken as a whole, our demonstrations highlight the increased sample throughput, improved data density, and enhanced $δ$ 13 C capability of LA-CAS versus other LA techniques and emphasize the role this method can play in future plant and rhizosphere related studies.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2014

Genetic ablation and short-duration inhibition of lipoxygenase results in increased macroautophagy

12/15-lipoxygenase (12/15-LOX) is involved in organelle homeostasis by degrading mitochondria in maturing red blood cells and by eliminating excess peroxisomes in liver. Furthermore, 12/15-LOX contributes to diseases by exacerbating oxidative stress-related injury, notably in stroke. Nonetheless, it is unclear what the consequences are of abolishing 12/15-LOX activity. Mice in which the alox15 gene has been ablated do not show an obvious phenotype, and LOX enzyme inhibition is not overtly detrimental. We show here that liver histology is also unremarkable. However, electron microscopy demonstrated that 12/15-LOX knockout surprisingly leads to increased macroautophagy in the liver. Not only macroautophagy but also mitophagy and pexophagy were increased in hepatocytes, which otherwise showed unaltered fine structure and organelle morphology. These findings were substantiated by immunofluorescence showing significantly increased number of LC3 puncta and by Western blotting demonstrating a significant increase for LC3-II protein in both liver and brain homogenates of 12/15-LOX knockout mice. Inhibition of 12/15-LOX activity by treatment with four structurally different inhibitors had similar effects in cultured HepG2 hepatoma cells and SH-SY5Y neuroblastoma cells with significantly increased autophagy discernable already after 2 hours. Hence, our study reveals a link between ablation or inhibition of 12/15-LOX and stimulation of macroautophagy. The enhanced macroautophagy may be related to the known tissue-protective effects of LOX ablation or inhibition under various diseased conditions caused by oxidative stress and ischemia. This could provide an important cleaning mechanism of cells and tissues to prevent accumulation of damaged mitochondria and other cellular components. - Highlights: • A relationship between lipoxygenases and autophagy is disclosed. • 12/15-lipoxygenase knockout increases autophagy in mice liver and brain. • Lipoxygenase inhibition boosts autophagy in human hepatoma and neuroblastoma cells. • Lipoxygenase knockout or inhibition triggers selective autophagy.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2015

Measurements of the ablation-front trajectory and low-mode nonuniformity in direct-drive implosions using x-ray self-emission shadowgraphy

Self-emission x-ray shadowgraphy provides a method to measure the ablation-front trajectory and low-mode nonuniformity of a target imploded by directly illuminating a fusion capsule with laser beams. The technique uses time-resolved images of soft x-rays (> 1 keV) emitted from the coronal plasma of the target imaged onto an x-ray framing camera to determine the position of the ablation front. Methods used to accurately measure the ablation-front radius ( ${\it\delta}R=\pm 1.15~{\rm\mu}\text{m}$ ), image-to-image timing ( ${\it\delta}({\rm\Delta}t)=\pm 2.5$ ps) and absolute timing ( ${\it\delta}t=\pm 10$ ps) are presented. Angular averaging of the images provides an average radius measurement of ${\it\delta}(R_{\text{av}})=\pm 0.15~{\rm\mu}\text{m}$ and an error in velocity of ${\it\delta}V/V=\pm 3\%$ . This technique was applied on the Omega Laser Facility and the National Ignition Facility.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2026

Electrode Modification by Laser Ablation to Overcome Mechanical and Scalability Limitations of Solid-State Prealkylation of Electrode Architectures

In this work, laser ablation of Si electrode surfaces is utilized to provide localized strain relief during the Solid State Prealkylation of Electrode Architectures (SPEAR) process, in addition to volumetric expansion relief in the form of free volume channels across the electrode. A hexagonal mesh patterning was employed via laser ablation, where the hexagonal diameter (pitch) was varied from 250 to 1000 µm. It was demonstrated that these channels serve as expansion voids, accommodating the increase in electrode thickness observed during SPEAR and preventing cracking at the electrode surface. Optical microscopy and Raman mapping confirm that Li diffusion is the rate-limiting solid-state process, requiring a 24 h rest period to achieve homogeneous LixSi alloying through the electrode bulk. Electrochemical evaluations in full cells show that a 1000 μm pitch pattern yields a high initial discharge capacity of 2485 mA h g–1 and 86.4% capacity retention after 80 cycles, whereas smaller pitches (<500 μm) result in lithium plating at 4.1 V in full cells paired with NMC 811 due to excessive current collector exposure from the ablation process. XPS analysis reveals that the laser treatment modifies the electrode surface by increasing the Si–O and C–O species, changing the SEI composition observed via an increase in fluorophosphates upon cycling.

Musgrove, Amanda [ORNL] (ORCID:0009000220910389)↗

DOE OSTI2016

High speed direct imaging of thin metal film ablation by movie-mode dynamic transmission electron microscopy

Obliteration of matter by pulsed laser beams is not only prevalent in science fiction movies, but finds numerous technological applications ranging from additive manufacturing over machining of micro- and nanostructured features to health care. Pulse lengths ranging from femtoseconds to nanoseconds are utilized at varying laser beam energies and pulse lengths, and enable the removal of nanometric volumes of material. While the mechanisms for removal of material by laser irradiation, i.e., laser ablation, are well understood on the micrometer length scale, it was previously impossible to directly observe obliteration processes on smaller scales due to experimental limitations for the combination of nanometer spatial and nanosecond temporal resolution. Here, we report the direct observation of metal thin film ablation from a solid substrate through dynamic transmission electron microscopy. Quantitative analysis reveals liquid-phase dewetting of the thin-film, followed by hydrodynamic sputtering of nano- to submicron sized metal droplets. We discovered unexpected fracturing of the substrate due to evolving thermal stresses. This study confirms that hydrodynamic sputtering remains a valid mechanism for droplet expulsion on the nanoscale, while irradiation induced stress fields represent limit laser processing of nanostructured materials. Ultimately, our results allow for improved safety during laser ablation in manufacturing and medical applications.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Femtosecond Laser Ablation Multicollector ICPMS Analysis of Uranium Isotopes in NIST Glass

We have utilized femtosecond laser ablation coupled to multi-collector inductively couple plasma mass spectrometry to measure the uranium isotopic content of NIST 61x (x=0,2,4,6) glasses. The uranium content of these glasses is a linear two-component mixing between isotopically natural uranium and the isotopically depleted spike used in preparing the glasses. Laser ablation results match extremely well, generally within a few ppm, with solution analysis following sample dissolution and chemical separation. In addition to isotopic data, sample utilization efficiency measurements indicate that over 1% of ablated uranium atoms reach a mass spectrometer detector, making this technique extremely efficient. Laser sampling also allows for spatial analysis and our data indicate that rare uranium concentration inhomogeneities exist in NIST 616 glass.

Duffin, Andrew M.↗

DOE OSTI2015

Gas-dynamic acceleration of laser-ablation plumes: Hyperthermal particle energies under thermal vaporization

The expansion of a plume produced by low-fluence laser ablation of graphite in vacuum is investigated experimentally and by direct Monte Carlo simulations in an attempt to explain hyperthermal particle energies for thermally vaporized materials. We demonstrate that the translation energy of neutral particles, ∼2 times higher than classical expectations, is due to two effects, hydrodynamic plume acceleration into the forward direction and kinetic selection of fast particles in the on-axis region. Both effects depend on the collision number within the plume and on the particles internal degrees of freedom. The simulations allow ablation properties to be evaluated, such as ablation rate and surface temperature, based on time-of-flight measurements. Available experimental data on kinetic energies of various laser-produced particles are well described by the presented model.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2017

Enhanced hot-electron production and strong-shock generation in hydrogen-rich ablators for shock ignition

Experiments were performed with CH, Be, C, and SiO 2 ablators interacting with high-intensity UV laser radiation (5 × 10 15 W/cm 2 , λ = 351 nm) to determine the optimum material for hot-electron production and strong-shock generation. Significantly more hot electrons are produced in CH (up to ~13% instantaneous conversion efficiency), while the amount is a factor of ~2 to 3 lower in the other ablators. A larger hot-electron fraction is correlated with a higher effective ablation pressure. As a result, the higher conversion efficiency in CH is attributed to stronger damping of ion-acoustic waves because of the presence of light H ions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2017

Impact of cross-field motion on ablation of high-Z dust in fusion edge plasmas

The impact of cross-field motion of high-Z dust grains on their shielding by ablation cloud in edge plasmas of tokamaks is analyzed. The modification of the existing high-Z dust shielding theory is developed, which takes the dust motion effects into account. We show that the cross-field motion can lead to a large factor increase of the dust ablation rate, as compared to the previous model. It is also shown that the motion effects take place when the dust cross-field velocity exceeds a threshold value. We also obtain the dependencies of the dust ablation flux on the dust velocity and of the threshold velocity on the dust size and the ambient plasma temperature.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2018

Comparison of plastic, high density carbon, and beryllium as indirect drive NIF ablators

Detailed radiation hydrodynamic simulations calibrated to experimental data have been used to compare the relative strengths and weaknesses of three candidate indirect drive ablator materials now tested at the NIF: plastic, High Density Carbon (HDC) or diamond, and beryllium. We apply a common simulation methodology to several currently fielded ablator platforms to benchmark the model and extrapolate designs to the full NIF envelope to compare on a more equal footing. This paper focuses on modeling of the hohlraum energetics which accurately reproduced measured changes in symmetry when changes to the hohlraum environment were made within a given platform. Calculations suggest that all three ablator materials can achieve a symmetric implosion at a capsule outer radius of 1100 m, laser energy of 1.8 MJ, and DT ice mass of 185 g. However, there is more uncertainty in the symmetry predictions for the plastic and beryllium designs. Scaled diamond designs had the most calculated margin for achieving symmetry and the highest fuel absorbed energy at the same scale compared to plastic or beryllium. A comparison of the relative hydrodynamic stability was made using ultra-high resolution capsule simulations and the two dimensional radiation fluxes described in this work. These simulations, which include low and high mode perturbations, suggest that diamond is currently the most promising for achieving higher yields in the near future followed by plastic and more data required to understand beryllium.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2020

Fill tube dynamics in inertial confinement fusion implosions with high density carbon ablators

Plasma jets, such as γ-ray burst jets, Herbig–Haro jets, μ-quasar jets, and active galactic nuclei jets, are found throughout the universe [S. Mendoza et al., Rev. Mex. Astron. Astrofis. 41, 453 (2005)]. Plasma jets are also present in indirect drive inertial confinement fusion experiments originating from the capsule's fill tube and occasionally from divots and voids in the capsules, particles on the exterior of the capsule, or from the tent holding the capsule in the target. This paper looks at two different gas-filled capsule implosions containing a plasma jet resulting from a capsule fill tube and fill channel, both of which utilized high density carbon ablators. Two models were developed, a drag and a snowplow model, which use the time-dependent motion of the injected mass through the hotspot to estimate the mass injected into the hotspot from the fill tube and channel, arriving at an average injected mass of ~84.5 ± 25.5 ng for the first experiment and 91 ± 20 ng for the second experiment. Furthermore, unlike previous methods to estimate fill tube injected mass, these techniques do not assume that the mixed mass is in thermal equilibrium with the hotspot or that the x-ray emission is only coming from within the hotspot itself. This paper also discusses the features seen in these experiments which include limb brightening in the shell for undoped ablators and flattening in the ablator from shadowing by the fill tube.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Considerations for the modeling of the laser ablation region of ICF targets with Lagrangian simulations

Recently, much effort has been dedicated to the improvement of models and modeling choices utilized in radiation hydrodynamic simulations of direct drive inertial confinement fusion experiments in an effort to improve their predictive capability. In this paper, we consider the choice in mesh for the simulation of the laser ablation of a direct-drive-like target and compare Lagrangian simulations with various mesh zoning choices with Eulerian simulations with fixed resolution in the laser energy deposition region. Using these simulations, we demonstrate how errors in ablation pressure, laser deposition rate, shock speed, and density profile arise from insufficient zoning following from the conservation of mass of Lagrangian zones. These considerations place stringent requirements on the initial t = 0 zoning in the solid density shell for simulations aiming at resolving the ablation and laser absorption region. However, with sufficiently fine zoning in the t = 0 shell, agreement with Eulerian simulations and analytic scaling laws can be recovered.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Exploring implosion designs for increased compression on the National Ignition Facility using high density carbon ablators

It has long been recognized that high compression, and hence good confinement, is essential to achieving high yields in inertial confinement fusion implosions. In pursuit of multi-megajoule yields on the National Ignition Facility (NIF), a new campaign has begun aimed at testing the hypothesis that controlling hydrodynamic stability is key to achieving effective higher compression with the high density carbon ablators currently fielded on NIF. This campaign is built around a new implosion design, called SQ-n, that is derived from the uniquely stable Bigfoot design tested on NIF in 2016–2019. While very stable and with performance that was quite close to one-dimensional expectations, Bigfoot was a relatively high adiabat, and consequently lower compression design. The goal of SQ-n is then to evolve Bigfoot toward a higher compression design but without compromising its unique stability characteristics. Specifically, SQ-n adopts a ramped foot pulse shape to minimize early time Richtmyer–Meshkov instability growth and uses an ablator dopant distribution extending all of the way to the fuel–ablator interface that simulations suggest further reduces perturbation growth. In conclusion, this paper describes the design philosophy pursued with SQ-n, the results of instability modeling of the candidate design, and the experimental campaign planned to test these ideas in the near future.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Gamma-ray imaging of inertial confinement fusion implosions reveals remaining ablator carbon distribution

The joint LANL/LLNL nuclear imaging team has acquired the first gamma-ray images of inertial confinement fusion implosions at the National Ignition Facility. The gamma-ray image provides crucial information to help characterize the inertially confined fuel and ablator assembly at stagnation, information that would be difficult to acquire from neutron or x-ray observations. Gamma imaging visualizes both gamma radiation emitted directly in deuterium–tritium (DT) fusion reactions as well as gamma rays produced when DT fusion neutrons scatter inelastically on carbon nuclei in the remaining ablator of the fuel capsule. The resulting image provides valuable information on the position and density of the remaining ablator and potential contamination of the hot spot—a powerful diagnostic window into the capsule assembly during burn.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗