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At least 667 records · Page 37

Co-Free Cathode Materials and Their Novel Architectures

To enable cobalt-free LiNi 0.5 Mn 1.5 O 4 (LNMO) electrode and novel electrolyte formulation for use in next-generation Li-ion batteries (LIB) capable of high energy density, long cycle life and low cost, several methods were developed throughout this project. To enhance the performance of LNMO, Fe-doping on LNMO, laser treatment and atomic layer deposition (ALD) were adopted. Moreover, dry electrode method has successfully helped to fabricate ultra-high loading LNMO with stable performance. The improvement at anode side includes ALD-coating as well as pre-lithiation of graphite anode. In the novel electrolyte development, it was found that all-fluorinated electrolyte with appropriate additives can effectively extend both cycle and calendar life of LNMO full cells at practical loadings. Additional diagnosis of LNMO full cells showed that different types of carbon and porosity of separator play a critical role in the success of LNMO’s high voltage operation. The combined effort throughout the project pushed forward the understanding and commercialization of LNMO at practical level.

25 ENERGY STORAGE↗

Defect And Damage Characterization Of Additively Manufactured Titanium Alloy Ti-5553 Using Traditional Computed Tomography Volume Segmentation And Machine Learning Algorithms

The mechanical response of a component is affected by defects, such as porosity, arising from the laser powder bed fusion (LPBF) fabrication process. Thus, it is important to develop accurate and efficient inspection methods for identifying porosity. In this work, porosity identified in an X-ray computed tomography (XCT) volume of a Ti-5553 coupon was compared to pores identified in a serial sectioned volume that represented the ground truth. The porosity of the XCT scan was identified using contrast-based, ISO-based, and machine learning (ML) methods for segmentation. Large inherent porosity was easy to identify, but the ISO thresholding still struggled due to the intensity gradient resulting from both the beam hardening in XCT and the uneven lighting of the serial sectioning panels. Further, the results show that ML-based methods were better suited for identifying small pores and reducing the amount of false positives. Additionally, high strain-rate impact testing was done on some of the XCT samples as well as post-mortem XCT inspection, and the same suite of segmentation and quantification tools were used to identify the large spallation cavities. The comparison of porosity pre- and post-mortem provides insight on the influence of the LPBF porosity on the formation of spall cavities.

36 MATERIALS SCIENCE↗

Sapphire advanced mitigation process: wet etch to expose sub-surface damage and increase laser damage resistance and mechanical strength

In this study, a novel, to the best of our knowledge, method of wet chemical etching of sapphire workpieces (such as optics, wafers, windows, and cones), called the sapphire advanced mitigation process (or sapphire AMP), has been developed that exposes sub-surface mechanical damage created during the optical fabrication process and significantly enhances the surface laser damage resistance (> 2×) and mechanical strength (up to ~ 2.6×). Sapphire AMP involves first treating the workpiece with a mixture of sulfuric and phosphoric acid ([H 2 SO 4 ]:[H 3 PO 4 ]= 1 : 3) at 220°C, followed with phosphoric acid at 160°C, then with sodium hydroxide base (NaOH) and surfactant at 40°C, and finally with a high-pressure deionized water spray rinse. Sapphire AMP has been demonstrated on both A- and C-plane sapphire workpieces. The mechanism of this etch process involves the reaction of the sapphire (Al 2 O 3 ) surface with sulfuric acid (H 2 SO 4 ) forming aluminum sulfate [Al2(SO4)3], which has low solubility. The high phosphoric acid content in the first and second steps of sapphire AMP results in the efficient conversion of Al 2 (SO 4 ) 3 to aluminum phosphate (AlPO 4 ), which is very soluble, greatly reducing reaction product redeposition on the workpiece surface. Sapphire AMP is shown to expose sub-surface mechanical damage on the sapphire surface created during the grinding and polishing processes, whose etched morphology has either isotropic or anisotropic evolution depending on the nature of the initial surface damage. Sapphire AMP was also designed to remove the key known surface, laser absorbing precursors (namely, foreign chemical impurities, the fracture surface layer of preexisting sub-surface damage, and reaction product or foreign species redeposition or precipitation). Static and sliding indention induced surface microfractures on sapphire are shown after sapphire AMP to have a significant decrease in the fast photoluminescence intensity (a known metric for measuring the degree of laser damaging absorbing precursors). In addition, the onset of laser damage (at 351 nm 3 ns) on sapphire AMP treated workpieces was shown to increase in fluence from ~ 4 to >9.5J/cm 2 . Finally, biaxial ball-on-ring mechanical tests on sapphire disks showed an increase in the failure stress from 340 MPa (with pre-existing 28 µm flaws) to ~ 900MPa after sapphire AMP, which is attributed to the blunting of the surface microfractures.

36 MATERIALS SCIENCE↗

The X-Ray Emission Effectiveness of Plasma Mirrors: Reexamining Power-Law Scaling for Relativistic High-Order Harmonic Generation

Ultrashort pulsed lasers provide uniquely detailed access to the ultrafast dynamics of physical, chemical, and biological systems, but only a handful of wavelengths are directly produced by solid-state lasers, necessitating efficient high-power frequency conversion. Relativistic plasma mirrors generate broadband power-law spectra, that may span the gap between petawatt-class infrared laser facilities and x-ray free-electron lasers; despite substantial theoretical work the ultimate efficiency of this relativistic high-order-harmonic generation remains unclear. We show that the coherent radiation emitted by plasma mirrors follows a power-law distribution of energy over frequency with an exponent that, even in the ultrarelativistic limit, strongly depends on the ratio of laser intensity to plasma density and exceeds the frequently quoted value of -8/3 over a wide range of parameters. The coherent synchrotron emission model, when adequately corrected for the finite width of emitting electron bunches, is not just valid for p-polarized light and thin foil targets, but generally describes relativistic harmonic generation, including at normal incidence and with finite-gradient plasmas. Our numerical results support the ω-4/3 scaling of the synchrotron emission model as a limiting efficiency of the process under most conditions. The highest frequencies that can be generated with this scaling are usually restricted by the width of the emitting electron bunch rather than the Lorentz factor of the fastest electrons. The theoretical scaling relations developed here suggest, for example, that with a 20-PW 800-nm driving laser, 1 TW/harmonic can be produced for 1-keV photons.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

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↗

Development and investigation of efficient resonance ionization mass spectrometry schemes of gadolinium

Resonance ionization mass spectrometry of gadolinium can be used for nuclear forensics and to further the understanding of stellar nucleosynthesis but has been used only a handful of times due to the high laser power required and interference from non-resonant ionization of molecules of other elements. Herein we present the development of two novel resonance ionization spectroscopy schemes for gadolinium that provide improvements in isotopic fractionation and ionization efficiency, respectively, opening new applications for gadolinium analysis. The schemes are demonstrated and compared in a mixed sample of gadolinium and neodymium.

and nuclear chemistry↗

Delivery of H - / H + Beams to Area A

We explore the relative merits of transporting the beam from the H + ion source and from the H - ion source to Area-A for low current applications. Transporting the H - beam to Area-A using the laser neutralization approach has some risk associated with it and will require some development. Alternative method of delivering H - beam to Area-A includes replacing LDBM00 bending magnet with kicker for sharing beam between Line D and modified Line A. Transporting the H + beam to Area-A will have significant impact on the operation the IPF facility and maintaining high pulse rate to IPF will require major modifications to the transition region of the accelerator and Drift Tube Linac.

43 PARTICLE ACCELERATORS↗

Analytic insights into nonlocal energy transport. III. steady state Fokker Planck theory in spherical and planar geometry

This paper develops an approximate steady state Fokker Planck theory for energetic electron transport in a spherical laser fusion target. First, we apply the theory to only a small population of electrons, which is specified at the outset. Then, one determines the nonlocal electron energy flux of these electrons at a particular position. These energetic electrons may either come from the tail of the thermal distribution function or be generated by an instability. This paper develops two approximate methods of solution, which we call the “characteristic method” and “sparse eigenfunction.” The former works only in planar geometry and the latter in both planar and spherical geometry. Comparison of the two methods in planar geometry shows that even though the approximations are very different, they give about the same result, increasing their credibility. For the example we have chosen, spherical effects are not important for electrons from the tail of the distribution function but may well be for instability generated electrons, which have much higher energy. Comparing planar to spherical, one finds an additional spherical barrier protecting the fuel. It turns out that the associated fuel preheat a Fokker Planck model predicts is considerably less than that predicted by the Krook models as developed at both NRL and other places.

Manheimer, Wallace (ORCID:0000000163342591)↗

Optimization of laser-induced breakdown spectroscopy for liquid sodium analysis

Next-generation nuclear power reactors based on liquid sodium coolant are in development to improve efficiency and safety. Fast breeder reactors could potentially achieve considerably higher fuel burn-up while producing less nuclear waste compared with current commercial technology. Monitoring of impurities in these types of reactors is important in order to prevent blockage of the cooling system or hazardous reactions due to the high reactivity of sodium with water. In this work, laser-induced breakdown spectroscopy is performed on a liquid sodium sample using a custom-built immersion probe system. The probe provides direct line of sight to the sample vessel in argon atmosphere for laser delivery and signal collection. Signatures of sodium, and impurities such as potassium and oxygen have been obtained. The probe height and immersion have a strong influence on the signal level and stability. Argon flow rates of 2 to 5 liters per minute produce no substantial change in signal, suggesting a steady laminar flowing regime. A high signal-to-noise ratio for impurity elements confirms the suitability of this technique for reliable impurity detection and monitoring in the reactor environment.

Gardette, V. [University of Michigan, Ann Arbor, M↗

Structural, optical, and thermal properties of BN thin films grown on diamond via pulsed laser deposition

Heterostructures based on ultrawide-bandgap (UWBG) semiconductors (bandgap > 4.0 eV), such as BN and diamond, hold significant importance for the development of high-power electronics in the next generation. However, achieving in situ heteroepitaxy of BN/diamond or vice versa remains exceptionally challenging due to the complex growth kinetics involved. In this work, we grew BN thin film on (100) single-crystal diamonds using pulsed laser deposition and investigated its structural, magnetic, optical, and thermal properties. Throughout this study, the structural analyses confirmed the growth of BN films, which exhibited diamagnetic behavior at room temperature. Notably, the film demonstrated anisotropic refractive index characteristics within the visible-to-near-infrared wavelength range. The room-temperature cross-plane thermal conductivity of BN is 1.53 ± 0.77 W/mK, while the thermal conductance of the BN/diamond interface is 20 ± 2 MW/m 2 ⁢K. These findings have significant implications for a range of device applications based on UWBG BN/diamond heterostructures.

36 MATERIALS SCIENCE↗

Laser metal deposition of refractory high-entropy alloys for high-throughput synthesis and structure-property characterization

Progress in materials development is often paced by the time required to produce and evaluate a large number of alloys with different chemical compositions. This applies especially to refractory high-entropy alloys (RHEAs), which are difficult to synthesize and process by conventional methods. To evaluate a possible way to accelerate the process, high-throughput laser metal deposition was used in this work to prepare a quinary RHEA, TiZrNbHfTa, as well as its quaternary and ternary subsystems by in-situ alloying of elemental powders. Compositionally graded variants of the quinary RHEA were also analyzed. Our results show that the influence of various parameters such as powder shape and purity, alloy composition, and especially the solidification range, on the processability, microstructure, porosity, and mechanical properties can be investigated rapidly. The strength of these alloys was mainly affected by the oxygen and nitrogen contents of the starting powders, while substitutional solid solution strengthening played a minor role.

additive manufacturing↗

High-Fidelity Velocity and Concentration Measurements of Turbulent Buoyant Jets

Accurate models of turbulent buoyant flows are essential for the design of the cooling circuit of nuclear reactors and passive safety systems. However, available models fail to fully capture the physics of turbulent mixing when buoyancy becomes predominant with respect to momentum. Therefore, high-fidelity experiments of well-controlled fundamental flows are needed to develop and validate more accurate models. We analyze experiments of positive and negative turbulent buoyant jets, both in uniform and stratified environments, with the aim of understanding the thermal hydraulics of turbulent mixing with variable density and providing high-fidelity data for the development and validation of turbulence models. Non-intrusive, simultaneous particle image velocimetry and laser-induced fluorescence measurements were carried out to acquire instantaneous velocity and concentration fields on a vertical section parallel to the axis of a jet in the self-similar region. The refractive index matching method was applied to measure high-resolution buoyant jets with up to 8.6% density difference. These data are free of the typical errors that characterize optical measurements of buoyancy-driven flows (e.g. natural and mixed convection) where the refractive index of the fluid is inhomogeneous throughout the measurement domain. Turbulent statistics and entrainment of buoyant jets in uniform and stratified environments are presented. These data are compared with non-buoyant jets in a uniform environment, as a reference to investigate the effects of buoyancy and stratification on turbulent mixing. The results will be used for the assessment of current turbulence models and as a basis for the development of a new model that captures turbulent mixing.

laser induced fluorescence↗

Materials synthesis at terapascal static pressures

Theoretical modelling predicts very unusual structures and properties of materials at extreme pressure and temperature conditions. Hitherto, their synthesis and investigation above 200 gigapascals have been hindered both by the technical complexity of ultrahigh-pressure experiments and by the absence of relevant in situ methods of materials analysis. Here we report on a methodology developed to enable experiments at static compression in the terapascal regime with laser heating. We apply this method to realize pressures of about 600 and 900 gigapascals in a laser-heated double-stage diamond anvil cell, producing a rhenium–nitrogen alloy and achieving the synthesis of rhenium nitride Re 7 N 3 —which, as our theoretical analysis shows, is only stable under extreme compression. Full chemical and structural characterization of the materials, realized using synchrotron single-crystal X-ray diffraction on microcrystals in situ, demonstrates the capabilities of the methodology to extend high-pressure crystallography to the terapascal regime.

36 MATERIALS SCIENCE↗

Exploring 3D elastic-wave scattering at interfaces using high-resolution phased-array system

The elastic-wave scattering at interfaces, such as cracks, is essential for nondestructive inspections, and hence, understanding the phenomenon is crucial. However, the elastic-wave scattering at cracks is very complex in three dimensions since microscopic asperities of crack faces can be multiple scattering sources. We propose a method for exploring 3D elastic-wave scattering based on our previously developed high-resolution 3D phased-array system, the piezoelectric and laser ultrasonic system (PLUS). We describe the principle of PLUS, which combines a piezoelectric transmitter and a 2D mechanical scan of a laser Doppler vibrometer, enabling us to resolve a crack into a collection of scattring sources. Subsequently, we show how the 3D elastic-wave scattering in the vicinity of each response can be extracted. Here, we experimentally applied PLUS to a fatigue-crack specimen. We found that diverse 3D elastic-wave scattering occurred in a manner depending on the responses within the fatigue crack. This is significant because access to such information will be useful for optimizing inspection conditions, designing ultrasonic measurement systems, and characterizing cracks. More importantly, the described methodology is very general and can be applied to not only metals but also other materials such as composites, concrete, and rocks, leading to progress in many fields.

36 MATERIALS SCIENCE↗

Radiative cooling effects on reverse shocks formed by magnetized supersonic plasma flows

We study the structure of reverse shocks formed by the collision of supersonic, magnetized plasma flows driven by an inverse (or exploding) wire array with a planar conducting obstacle. We observe that the structure of these reverse shocks varies dramatically with wire material, despite the similar upstream flow velocities and mass densities. For aluminum wire arrays, the shock is sharp and well-defined, consistent with magneto-hydrodynamic theory. In contrast, we do not observe a well-defined shock using tungsten wires, and instead we see a broad region dominated by density fluctuations on a wide range of spatial scales. We diagnose these two very different interactions using interferometry, Thomson scattering, shadowgraphy, and a newly developed imaging refractometer that is sensitive to small deflections of the probing laser corresponding to small-scale density perturbations. We conclude that the differences in shock structure are most likely due to radiative cooling instabilities, which create small-scale density perturbations elongated along magnetic field lines in the tungsten plasma. These instabilities grow more slowly and are smoothed by thermal conduction in the aluminum plasma.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

The crucial role of diagnostics in achieving ignition on the National Ignition Facility (NIF)

Well over 100 diagnostics can operate on the National Ignition Facility (NIF) as a result of several decades of development on NIF, and before that on Nova, OMEGA, and earlier LLNL lasers. A subset of these have guided the approach to achieving ignition on the NIF in 2022 [H. Abu-Shawareb et al. (Indirect Drive ICF Collaboration), Phys. Rev. Lett. 129(7), 075001 (2022)]. Achieving ignition on NIF has required many types of experiments with this core set of diagnostics, some constraining known unknowns and some revealing surprises—arguably unknown unknowns. Early design work realized that the extreme precision required for ignition on NIF would require fine-tuning by experiment, that is, measuring and adjusting known unknowns. Many examples are given where the use of the core set of ignition diagnostics in experimental arrangements called platforms demonstrated control of the key theoretical parameters defined as shape, adiabat, velocity, and mix. The direction of the adjustments to input conditions is found either by trend analysis or, in many cases, by observing from the diagnostic data the direction to make an adjustment. In addition, diagnostics have revealed some unexpected or neglected known issues, which degrade performance, or unexpected issues, unknown unknowns. Some of these factors had been previously considered, but underestimated or difficult to calculate at the time. The overall methodology can be described as a variant of Popper's falsifiability philosophy [K. Popper, The Logic of Scientific Discovery (Hutchinson, 1974)]. This paper summarizes the role of ignition diagnostics in terms of falsification or validation of theory or experimental setup as well as uncovering unexpected issues. The journey to ignition started in the seventies with a 1-µm wavelength laser producing disastrous results. Diagnostics have guided us to the recent multi-decadal goal of demonstrating ignition and burn in the laboratory.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Ultracold Electrons via Near-Threshold Photoemission from Single-Crystal Cu(100)

Achieving a low mean transverse energy or temperature of electrons emitted from the photocathode-based electron sources is critical to the development of next-generation and compact x-ray free electron lasers and ultrafast electron diffraction, spectroscopy, and microscopy experiments. In this Letter, we demonstrate a record low mean transverse energy of 5 meV from the cryo-cooled (100) surface of copper using near-threshold photoemission. Further, we also show that the electron energy spread obtained from such a surface is less than 11.5 meV, making it the smallest energy spread electron source known to date: more than an order of magnitude smaller than any existing photoemission, field emission, or thermionic emission based electron source. Overall, our measurements also shed light on the physics of electron emission and show how the energy spread at few meV scale energies is limited by both the temperature and the vacuum density of states.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗