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Sodium tracer measurements of an expanded dense aluminum plasma from e-beam isochoric heating

Spatially and temporally resolved visible absorption spectroscopy is performed on sodium D-lines present as surface contaminants on an expanded dense aluminum plasma plume. An 80-ns FWHM, intense, relativistic electron beam deposits 5.4 J into a 100- μ m-thick Al foil, which isochorically heats and subsequently hydrodynamically expands the material through the warm dense matter state and into a classical-like plasma state, with a coupling parameter of approximately 0.2 and a degeneracy parameter of approximately 270. The Na contamination, carried along with the expanding plume, shows saturated absorption features in the dense Al continuum for λ > 450 nm. X-ray photoelectron spectroscopy and laser-induced breakdown spectroscopy confirm Na is a surface contaminant with an atomic concentration of ~ 0.1 % when interrogating identical foil samples. Additioanlly, a spectroscopic-quality radiation transport model is used to post-process 2D hydrodynamic simulations to interpret the plasma conditions based on the measured Na 3p-3s doublet line profiles. A sodium number density of 3 × 10 15 cm -3 best matches the experimental spectra, which originate from a dense surface plasma with n e = 3.0 ± 0.8 × 10 18 cm -3 .

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Permeation Properties of Disordered Metal-Organic Framework Membranes Made by Vapor Phase Ligand Treatment

Zeolitic imidazolate frameworks (ZIFs) are nanoporous molecular sieves offering exciting opportunities for membrane- and adsorption-based gas separations. The Tsapatsis group developed an all-vapor-phase ligand induced permselectivation (LIPS) method for the fabrication of ZIF nanocomposite membranes. The LIPS method consists of a combination of atomic layer deposition of a dense oxide inside the mesopores of a porous support followed by transformation of the dense oxide deposit to nanoporous ZIF by exposure to sublimated vapors of an imidazolate ligand. It enables the formation of thin nanocomposite films consisting of ZIF deposited inside pores with diameters smaller than 10 nm. Vapor-phase conversion of the impermeable ZnO to ZIF increases flux of certain gases more than others. Vapor phase linker/ligand treatment (VPLT) can further modify the properties of LIPS and other membranes. The combination of LIPS with VPLT provides an all-vapor methodology for making and modifying ZIF membranes with the ability to control the ZIF deposit composition and the level of confinement in a variety of mesoporous supports. The propylene/propane separation performance of LIPS/VPLT ZIF membranes confined (entirely or partially) inside mesopores is remarkably superior to that of most conventional ZIF membranes consisting of unconfined (deposited on the external surface of porous supports) polycrystalline films. The accomplishments of this award are: (i) understanding of the LIPS process using mathematical models of atomic layer deposition (ALD), (ii) development of surface modification methods (vapor, e-beam, plasma, and X-ray treatments) to tune permeation properties, (iii) microstructural control of ZIF-8 films using ALD (support modification, direct ALD, and by use of in situ permeability monitoring), (iv) molecular simulations, and (v) thin film characterization and adsorption measurements using spectroscopy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Measurement and reduction of Ar metastable densities by nitrogen admixing in electron beam-generated plasmas

Abstract Electron beam (e-beam) generated plasmas are useful for material processing applications such as deposition and etching because the plasmas deliver a large fluence of very low energy of ions to surfaces. Metastable species produced in the beam-region can also transport significant energy to the plasma periphery and surfaces. In this work, we have investigated the spatially resolved density of metastable Ar 1s 5 species produced in an Ar and Ar/N 2 e-beam generated plasma at pressures of 60–67 mTorr using laser-induced fluorescence (LIF). The experiments provide the first direct measure of absolute density and reduction of Ar 1s 5 in an e-beam generated plasma when argon is diluted with nitrogen. These results are consistent with previous predictions of numerical modeling and measurements using optical emission spectroscopy. The present spatially resolved LIF measurements directly quantify the reduction of Ar 1s 5 in the e-beam generated plasma by nitrogen admixing. This reduction was observed in the region of the electron beam and in the plasma periphery, where substrates are usually placed. For example, up to a threefold reduction of the density of Ar 1s 5 was measured when the argon background was diluted with 15.5% nitrogen at pressure of 60 mTorr. Ar 1s 5 reduction is attributed to excitation exchange with nitrogen molecules as well as the cooling of plasma electrons via inelastic collisions with nitrogen molecules.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Anticathode effect on electron kinetics in electron beam generated E × B plasma

Electron beam (e-beam) generated plasmas with applied crossed electric and magnetic (E x B) fields are promising for low damage processing of materials with applications to microelectronics and quantum information systems. In cylindrical e-beam E x B plasmas, radial confinement of electrons and ions is achieved by an axial magnetic field and radial electric field, respectively. To control the axial confinement of electrons, such e-beam generated plasma sources may incorporate a conducting boundary known as an anticathode, which is placed on the axially opposite side of the plasma from the cathode. In this work, it is shown that varying the anticathode voltage bias can control the degree to which the anticathode collects or repels incident electrons, allowing control of warm electron (electron energies in 10–30 eV range) and beam electron population confinement. It is suggested that the effect of the anticathode bias on the formation of these distinct electron populations is also associated with the transition between weak turbulence and strong Langmuir turbulence.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Anticathode effect on multimodal azimuthal oscillations in electron beam generated E×B plasma

Electron beam (e-beam) generated plasmas with applied crossed electric and magnetic (⁠E x B⁠) fields are promising for low-damage (gentle) material processing. However, these plasmas can be subject to the formation of plasma non-uniformities propagating in the ⁠E x B direction. These rotating plasma structures (or “spokes”) enhance the transport of charged species across the magnetic field, which can harm the gentle processing capability of the plasma. In this work, we investigate the role of electrostatically active boundaries on the spoke formation by incorporating a variable bias conducting boundary (known as an anticathode) placed on the axially opposite side of the cathode. Our findings indicate azimuthal mode suppression occurs when the anticathode is electron collecting. Furthermore, we show selective azimuthal mode suppression by biasing the anticathode to an intermediate potential between the cathode and anode potentials. In conclusion, these findings suggest a link between the axial electron confinement in the e-beam generated plasma and azimuthally propagating plasma structure formation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Multimodal azimuthal oscillations in electron beam generated E×B plasma

Electron beam (e-beam) generated plasmas with applied crossed electric and magnetic (E×B) fields are promising for low-damage material processing. However, these plasmas can be subject to the formation of azimuthally propagating structures that enhance the radial transport of energetic charged species, which can harm the gentle processing capability of the plasma. In this work, we investigate the azimuthal structure formation in an e-beam generated E×B plasma using experimental diagnostics and 2D3V particle-in-cell simulations. Our findings demonstrate the formation of multiple simultaneously occurring azimuthally propagating modes that exhibit nontrivial radial dependence. It is suggested that the multimodal azimuthal spectrum is caused in part by the radial outflow of ions in the plasma.

electron beams↗

Production of warm ions in electron beam generated E × B plasma

Several recent experiments have demonstrated low-damage processing of 2D materials, such as graphene and single crystal diamond, using electron beam (e-beam) generated plasmas with applied crossed electric and magnetic (E × B) fields. Here, the low damage of these sensitive materials is commonly attributed to the low energy of ions incident to the substrate surface and the ion confinement in E x B fields. In this work, measurements of atom and ion velocity distribution functions in an e-beam E × B plasma at sub-mTorr argon pressures using a laser-induced fluorescence diagnostic revealed the presence of a warm population of ions with temperatures of ~ 1 eV that are sufficient to destroy the ion confinement in E × B fields and drive the ion flux by cross field diffusion in the direction opposite to the applied electric field, toward the plasma-bounded walls or substrate. Thus, it is this nearly ambipolar diffusion process that is responsible for the flux of charged particles impinging on the wall/substrate surface.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

6000 lines/mm blazed grating for a high-resolution x-ray spectrometer

We have designed and fabricated a high groove density blazed grating for a Resonant Inelastic X-ray Scattering spectrometer for the new Qerlin beamline at the Advanced Light Source (ALS) synchrotron facility. The gratings were fabricated using a set of nanofabrication techniques including e-beam lithography, nanoimprint, plasma etch, and anisotropic wet etching. Two gratings with groove density of 6000 lines/mm and 3000 lines/mm and optimized for operation in the 1st and 2nd negative diffraction order respectively were fabricated and tested. We report on fabrication details and characterization of the gratings at beamline 6.3.2 of the ALS.

36 MATERIALS SCIENCE↗

Spatial profile of argon (1s 5 ) metastables in an electron beam generated plasma

Electron beams with an applied magnetic field generate a secondary cold plasma with a selective chemical composition, featuring low-energy ions and metastable species in the discharge periphery, ideal for low-damage plasma treatment of material substrates. In this work, we studied the plasma generated by an e-beam using a 4 kV voltage in a pure argon gas environment under a magnetic field of 150 G and in the pressure range of 25–90 mTorr. We measured the absolute spatial density profile of argon (1 s 5 ) metastables in an electron beam generated plasma by laser-induced fluorescence and found it to be of the order of 10 16 m −3 . The electron temperature and the electron density measured by a Langmuir probe were of the order of 10 16 m −3 and less than an eV respectively. Electron-impact quenching was identified as a significant loss mechanism for the Ar(1s 5 ) state, leading to the saturation of the metastable density at higher pressures. Outside the primary ionization region, the spatial distribution of argon metastables followed a linear diffusion profile, indicating negligible additional production in those regions.

EEDF↗

LICS Modeling [Slides]

We propose to design a new diagnostic based on laser inverse Compton scattering (LICS) to study the dynamics of runaway electron formation during killer-pellet triggered disruptions in DIII-D, and their subsequent loss. Obtaining a better understanding of transient runaway electrons (and how to suppress them) is one of the highest priorities of the US fusion program. To enable this, we need better measurements of the runaway electron population during and after disruptions. We intend to measure point-wise time-resolved spatial profile and energy distributions of the runaway electrons while they are in the core of the tokamak plasma. While LICS measurements of relativistic e-beams have been successfully made on accelerators, they have never been done in a tokamak. We bring two innovations to this diagnostic concept which should enable 10 times better signal-to-noise ratios than previously envisioned. In particular, we will marry bright short pulse (10’s of picosecond) laser technologies with the availability of short-pulse gated x-ray imagers developed at Los Alamos for the National Ignition Facility (NIF), to reject noise generated by the tokamak and plasma environment. We will generate a Conceptual Physics Basis, a Preliminary Design, and a Final Design package, with associated DIII-D reviews, along with prototype component testing for the diagnostic over the course of the two year duration of this proposal.

42 ENGINEERING↗

Investigation of UV, ns-laser damage resistance of hafnia films produced by electron beam evaporation and ion beam sputtering deposition methods

Laser-induced damage in coating materials with a high index of refraction, such as hafnia, limits the performance of high power and high energy laser systems. Understanding the underlying physics responsible for laser damage holds the key for developing damage-resistant optical films. Previous studies have reported a substantial difference in laser damage onset for hafnia films produced by different deposition methods, yet the underlying mechanisms for the observed difference remain elusive. We combined laser damage testing with analytical characterizations and theoretical simulations to investigate the response of hafnia films produced by electron (e-) beam evaporation vs ion beam sputtering (IBS) methods upon UV ns-laser exposure. We found that e-beam produced hafnia films were overall more damage resistant; in addition, we observed a polarization anisotropy associated with the onset of damage in the e-beam films, while this effect was absent in the latter films. The observed differences can be attributed to the stark contrast in the pressure inside the pores inherent in both films. The high pressure inside the IBS-induced nanobubbles has been shown to reduce the threshold for laser-induced plasma breakdown leading to film damage. The polarization effects in the e-beam coatings can be related to the asymmetric electric field intensification induced by the columnar void structure. Our findings provide a fundamental basis for developing strategies to produce laser damage-resistant coatings for UV pulsed laser applications.

36 MATERIALS SCIENCE↗

Application of electron beam technology to decompose persistent emerging drinking water contaminants: poly- and perfluoroalkyl substances (PFAS) and 1,4-Dioxane

Poly- and perfluoroalkyl substances (PFAS) and 1,4-dioxane are persistent emerging contaminants that are currently under consideration for federal and state-specific regulations in drinking water. Both PFAS and 1,4-dioxane are highly resistant to degradation and are not effectively removed by conventional drinking water treatment systems. Results from the Unregulated Contaminant Monitoring Rule 3 survey showed that >540 sites across the nation are contaminated with both PFAS and 1,4-dioxane. Hence, there is a need to identify technologies that can effectively remove both these contaminants. Water treatment via electron beam (e-beam) has been proven effective at treating a wide range of contaminants, including perfluorooctane sulfonate (PFOS), perfluorooctanoate (PFOA), polychlorinated biphenyls, and trichloroethylene. While the e-beam process is often considered similar to advanced oxidation processes (AOPs), e-beam technology is unique in that it produces both highly oxidizing and reducing species at the same time. The specific objectives of this study were to: (i) determine the effectiveness of 9 MeV electrons provided by the Fermilab’s Accelerator Application Development and Demonstration (A2D2) tool to decompose PFAS and 1,4-dioxane; (ii) assess the formation of byproducts during water treatment; (iii) apply the optimized treatment to field groundwater samples contaminated with PFAS and 1,4-dioxane, and (iv) assess the energy demands for the treatment of these contaminants using e-beam. Results from this study showed that e-beam is effective in treating both 1,4-dioxane and PFAS. Complete degradation of 1,4-dioxane was observed at a dose of 5 kGy for an initial concentration of up to 1 ppm without the need for any sample modification. The electrical energy per order (EEo) for treatment of 1,4-dioxane ranged from 0.46 to 0.72 kWh/m 3 /order and was comparable and even lower, in some cases, than other AOP technologies. Alkaline conditions (pH 13) and low dissolved oxygen concentration (2 mg/L) highly favored the treatment of PFAS by e-beam. Greater than 90% removal of PFOA and PFOS from an initial concentration of 100 to 500 ppb was achieved at a dose of 250 kGy and 500 kGy, respectively, under optimized conditions. The degradation efficiency was not significantly changed when treating other PFAS of fluorinated carbon chain length of 5 to 7 individually at 250 kGy with a removal ranging from 85¬–99% for different compounds. Short chain PFAS (perfluorobutanoate: PFBA and perfluorobutane sulfonate: PFBS) did not degrade under the same conditions at 250 kGy, but 70 to 99% degradation was observed at a higher dose of 1000 kGy. Short chain PFAS (perfluorohexanoate: PFHxA (C5) and perfluoroheptanoate: PFHpA (C6)) were detected after treatment of PFOA, but not after PFOS treatment. Inability to close the mass balance through targeted analysis suggests the presence of other intermediates not detectable by available analytical methods. When treating PFAS mixture containing ten compounds at equimolar concentration of 0.05 µM each, preferential degradation of polyfluorinated compound (6:2 fluorotelomer sulfonate or 6:2 FTS) followed by C8 and C7 compounds was observed as a function of increasing e-beam dose. About 30% degradation of ΣPFAS was observed at 250 kGy and no further removal was observed up to a dose of 1000 kGy. C4 to C6 PFASs showed no degradation, while C3 PFAS (PFBS) showed an increase in concentration by 34% at 1000 kGy due to formation from the breakdown of other long chain PFAS. These results suggested that (a) the reaction kinetics is likely different for different PFAS based on chain length, functional group, and the degree of fluorination of the carbon chain, and (b) there may be intermediates generated from the degradation of 6:2 FTS and C7/C8 compounds that can potentially scavenge hydrated electrons needed for reaction with the untreated PFAS molecules. Treatment of three PFAS-contaminated groundwater samples from two US states showed similar trends as observed in the treatment of equimolar PFAS mixtures. Up to 71% removal of ΣPFAS was achieved in real groundwater samples at 750 kGy and data trend suggested that higher degradation is feasible if higher doses (>1MGy) are applied to treat field samples to overcome matrix effects and competing species. Calculated EEo for PFAS ranged from as low as ~48 to 1081 kWh/m 3 /order depending on the type of PFAS treated. These values are comparable and even lower, in some cases, than other destructive technologies employed for PFAS treatment such as ultrasound, plasma, and photochemical treatment. The results from this study indicate e-beam is a promising approach under favorable conditions and should be explored further as an end-of-train treatment option for PFAS destruction.

1,4-Dioxane↗

Los Alamos LDRD Appraisal Final Report for 20190124ER [Hot Electron Beam Generation and Transport for Fast Ignition]

This project was successful in addressing key technical issues of the cone-guided electron fast ignition concept for ICF. The development of an e-beam to deliver energy of 10’s of kilojoules to HED targets would be useful for myriad experimental applications relevant to the Laboratory’s mission. For example, ICF ignition and the development of a burning plasma is a high priority for the national high energy density physics effort and this work is aligned with that mission. Moreover, other technologies (e.g., MeV laser radiography) would be advanced by the R&D advancements from this project, so this work has broader implications for other LANL missions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Divertor Component Testing

Power exhaust is an immense challenge in tokamaks. Commonwealth Fusion Systems (CFS), in collaboration with MIT and others, is working on the design of a compact (R 0 = 1.85 m), high-field (B 0 = 12 T) tokamak for the demonstration of net fusion energy, called SPARC. Empirical scaling laws indicate that the unmitigated heat flux in the boundary plasma will exceed 10 GW/m 2 . Such high heat fluxes will be a formidable challenge. The scope of this work is to utilize the HHF testing expertise maintained by ORNL, used in support of NSTX-U and to demonstrate the thermal performance of tungsten-coated graphitic foam targets, to help CFS and its collaborators to assess the performance of (1) base materials (tungsten and its alloys) and (2) divertor mockups under SPARC-like divertor heat flux conditions. These activities will be performed by ORNL personnel using electron beam exposure facilities at the Pennsylvania State University’s Applied Research Laboratory (ARL). ARL is a Department of Defense University Affiliated Research Center where ORNL has successfully executed NSTX-U and graphitic foam high heat flux testing using electron beam (e-beam) facilities, which is a nonstandard service. For the assessment of base materials, CFS will do an initial thermal analysis, in consultation with ORNL, to understand under what scenarios the materials are most likely to fail. CFS will supply to ORNL various tungsten-based material samples to test with testing taking 3 weeks. ORNL will thermally stress the samples under SPARC divertor-like conditions to either failure or to a prescribed number of pulses. ORNL will record experimental data, including IR surface temperature and embedded thermocouple readings, and report results to CFS

36 MATERIALS SCIENCE↗

A multi-institution collaboration to study copper wire hybrid and laser-cut foil X-pinches

X-pinches are a pulsed power wire-array configuration that produce nanosecond and micron-scale X-ray sources with numerous applications. The earliest embodiment of the X-pinch inspired its name, as it is typically composed of two or more fine (5-50 µm) wires crossed into the shape of an X (Fig. 1a). The ‘X’ ablates when subjected to large (10 1 -10 4 kA), fast-rising (~1 kA/ns) currents, and extreme magnetic pressure at the cross-point constricts the ablated plasma, which develops instabilities and then pinches to near-zero radius, localized ‘hot spots’, emitting X-rays from a sub-nanosecond and 1 µm scale source characteristic of a hot (~1 keV), dense (10% solid density) plasma. A subsequent gap forms where the hot spot(s) occurred, across which substantial potential accelerates electron beams (e-beams) that generate larger, longer-lasting X-ray bursts composed of harder X-rays.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗