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DOE OSTI2023

Analytic insights into nonlocal energy transport: Steady state Fokker Planck theory in arbitrary Z plasmas

The generation of energetic electrons in laser fusion in an important issue. The electrons may either arise from a laser plasma instability, or from the uncoupled high temperature tail of a Maxwellian distribution. To study these in a laser fusion context, it is important to find a method accurate enough to be useful, and simple enough to be incorporated into a radiation hydrodynamics numerical simulation, the main workhorse for studying the laser fusion target. That is why analytic insights become important, they allow one to simplify the Fokker Planck theory so that a solution of it can be incorporated into a radiation hydrodynamic simulation. This work develops and analyzes a steady state Fokker Planck theory for plasmas of arbitrary Z. It develops a method of solving the simplified Fokker Planck method with a technique called sparse eigenfunction analysis. As a result, this method appears to work reasonably well when compared to the experimental results from the Rochester/NIF on plastic spherical targets with and without a silicon layer.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Plasma catalytic non-oxidative methane conversion to hydrogen and value-added hydrocarbons on zeolite 13X

Non-thermal plasma has unfolded highly efficient, safe to operate novel routes for methane conversion to hydrogen. In this work, methane conversion is performed under atmospheric dielectric barrier discharge (DBD) plasma with and without 13X zeolite-based catalysts i.e., 13X, Ga/13X, Pd/13X, and Pd-Ga/13X. Experimental results indicate that the plasma catalytic process delivered almost twofold higher product yield than the plasma only route. The binary Pd-Ga catalyst possesses highest catalytic performance with about 40 % CH 4 conversion at an input flowrate of 5 cm 3 min -1 and 2W due to the formation of the Pd-Ga alloy, which acts as catalytic active centre for activating C–H bonds. Product yield can be tailored by the catalyst design where the bimetallic Pd-Ga/13X preferably favours the hydrocarbon formation while H 2 is the dominant product obtained over the Pd/13X. The cleavage of C–H bonds of methane molecule over the plasma only route is mainly governed by energetic electrons in the gaseous phase the catalyst activity, and plasma-catalyst synergism play a significant role in the plasma catalysis process. Further, the findings from this work provide significant insights into the methane activation for subsequent optimization of the methane conversion processes operated on floating production, storage, and offloading vessels (FPSOVs). Exploiting untapped offshore natural gas reserves, where conventional pipeline systems are less economical.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Status of the Mu2e experiment

The Mu2e experiment at Fermilab searches for the coherent, neutrino-less conversion of a μ − to e − in the Coulomb field of Al nuclei, that represents one of the cleanest Charged Lepton Flavor Violating (CLFV) processes for exploring Beyond the Standard Model (BSM) physics. Mu2e aims to improve previous sensitivity by four orders of magnitude, with a distinctive signature provided by identifying mono-energetic electrons with energy slightly below the muon rest mass. To reach this goal, the experiment will use the highest intensity pulsed muon beam in the world, with up to 6 × 1 0 9 stopped muons/sec. This is achieved using the Fermilab proton beam and the design and realization of a unique 25 m long superconducting solenoidal system. The high beam intensity relies upon minimizing beam losses in the slow extraction region, indicating an opportunity of using bent crystals for shadowing. A high-resolution straw tracker and a fast CsI crystal calorimeter identify the conversion electron. Both detectors are inserted behind the Stopping Target in the last solenoid section. A Cosmic Ray Veto covers a large part of the solenoids to suppress background produced by cosmic rays. In this paper, we report the details of the experimental layout, the construction status of the magnetic system and detectors, and a short description of the simulation and realization of the bent crystals. Performing crystal channeling in front of the first slow extraction septa will allow beam shadowing and largely reduce beam losses. •Charge Lepton Flavor Violation processes: μ − → e − conversion.•Large Superconducting Solenoid system.•High-Intensity beams•High precision detectors.•Crystal channeling.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

Resistance of Boron Nitride Nanotubes to Radiation-Induced Oxidation

We present unprecedented results on the damage thresholds and pathways for boron nitride nanotubes (BNNT) under the influence of energetic electrons in an oxidative gas environment, using an environmental aberration-corrected electron microscope over a range of oxygen pressures. We observe a damage cascade process that resists damage until a higher electron dose, compared with carbon nanotubes, initiating at defect-free BNNT sidewalls and proceeding through the conversion from crystalline nanotubes to amorphous boron nitride (BN), resisting oxidation throughout. We compare with prior results on the oxidation of carbon nanotubes and present a model that attributes the onset of damage in both cases to a physisorbed oxygen layer that reduces the threshold for damage onset. Surprisingly, increased temperatures offer protection against damage, as do electron dose rates that significantly exceed the oxygen dose rates, and our model attributes both effects to a physisorbed oxygen population.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Cryogenic “Iodide-Tagging” Photoelectron Spectroscopy: A Sensitive Probe for Specific Binding Sites of Amino Acids

This work showcases cryogenic and temperature-dependent “iodide-tagging” photoelectron spectroscopy to probe specific binding sites of amino acids using the glycine-iodide complex (Gly?I-) as a case study. Multiple Gly?I- isomers were generated from ambient electrospray ionization and kinetically isolated in a cryogenic ion trap. These structures were characterized with temperature-dependent “iodide-tagging” negative ion photoelectron spectroscopy (NIPES) where iodide was used as the “messenger” to interpret electronic energetics and structural information of various Gly?I- isomers. Accompanied by theoretical computations and Franck-Condon simulations, a total of five cluster structures have been identified along with their various binding motifs. This work demonstrates that “iodide-tagging” NIPES is a powerful general means for probing specific binding interactions in biological molecules of interest.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Ni and Co Incorporation in Forsterite: A Density Functional Theory Study with Hubbard Correction

Ni and Co are critical elements for the world economy and modern technologies. Mafic and ultramafic deposits represent low-grade yet abundant alternatives to traditional Ni and Co ores. Here, in this work, density functional theory (DFT) with the Hubbard U correction (DFT+U) was used to simulate the incorporation of Ni and Co in forsterite (Mg 2 SiO 4 ), the Mg endmember of olivine, a common mineral in mafic and ultramafic rocks. Hubbard U terms for Ni and Co were parametrized using a series of oxide, hydroxide, carbonate, silicate, and sulfide minerals relevant to extraction and recovery of Ni and Co from mafic and ultramafic deposits. Electronic, energetic, magnetic, and structural properties were considered in the parametrization. For each of Ni and Co, an effective Hubbard correction (U eff ) value that optimized agreement with either experimental data or a hybrid exchange-correlation functional for all of the minerals considered is reported. DFT+U ab initio molecular dynamics (AIMD) simulations of Ni and Co incorporated into the M1 and M2 octahedral sites of forsterite were then performed. Ni and Co substitution in the M1 site was more energetically favorable than substitution in the M2 site, in agreement with published partition coefficients. AIMD trajectories were used to compute extended X-ray absorption fine structure (EXAFS) spectra of Ni in the M1 and M2 sites for direct fitting to a published experimental spectrum of Ni in a natural San Carlos olivine sample. The results of the fit indicated that ordering of Ni in the M1 site was not as strong at the low Ni concentrations relevant to mafic and ultramafic silicate minerals as that at the higher concentrations of the Ni-Mg olivine solid solutions studied to date.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Hydrogen from Sunlight and Water: A Side-by-Side Comparison between Photoelectrochemical and Solar Thermochemical Water-Splitting

Photoelectrochemical (PEC) and solar thermochemical (STCH) water-splitting represent two promising pathways for direct solar hydrogen generation. PEC water-splitting integrates multiple functional materials and utilizes energetic electrons and holes generated from sunlight to produce hydrogen and oxygen in two half-reactions, while STCH water-splitting couples a series of consecutive chemical reactions and uses absorbed heat from sunlight to generate hydrogen and oxygen in two full reactions. In this Focus Review, the basic operating principles, sunlight utilization, device architecture, reactor design, instantaneous and annually averaged solar-to-hydrogen (STH) conversion efficiency, and the operating conditions and constraints of both pathways are compared. A side-by-side comparison addresses some common sources of confusion and misinterpretation, especially in the evaluation of STH conversion efficiencies, and reveals distinct features and challenges in both PEC and STCH technologies. Furthermore, this Focus Review also addresses materials and device challenges in PEC and STCH for cost-competitive hydrogen generation.

08 HYDROGEN↗

DOE OSTI2021

Pro‐ L * ‐ A Probabilistic L * Mapping Tool for Ground Observations

Abstract Both ground and space observations are used extensively in the modeling of space weather processes within the Earth’s magnetosphere. In radiation belt physics modeling, one of the key phase‐space coordinates is L *, which indicates the location of the drift paths of energetic electrons. Global magnetic field models allow a subset of locations on the ground (mainly subauroral) to be mapped along field lines to a location in space and transformed into L *, provided that the initial ground location maps to a closed drift path. This allows observations from ground, or low‐altitude space‐based platforms to be mapped into space in order to inform radiation belt modeling. Many data‐based magnetic field models exist; however, these models can significantly disagree on mapped L * values for a single point on the ground, during both quiet times and storms. We present a state of the art probabilistic L * mapping tool, Pro‐ L *, which produces probability distributions for L * corresponding to a given ground location. Pro‐ L * has been calculated for a high resolution magnetic latitude by magnetic local time grid in the Earth’s Northern Hemisphere. We have developed the probabilistic model using 11 years of L * calculations for seven widely used magnetic field models. Usage of the tool is highlighted for both event studies and statistical models, and we demonstrate a number of potential applications.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2023

Verifying Ray Tracing Amplitude Methods for Global Magnetospheric Modeling

Abstract Ray tracing is a commonly used method for modeling the propagation of electromagnetic waves in Earth's magnetosphere. To apply ray tracing results to global models of wave‐particle interaction such as energetic electron scattering, it is useful to map the discrete rays to a volume filling mesh. However, some methods have inherent losses of energy from the wave source, or do not account for the full range of wave properties within a sample volume. We have developed and tested a 3D magnetospheric ray tracing code “MESHRAY” which resolves these issues. MESHRAY uses the conservation of Poynting flux through ray triplets with finite volume to determine the local field amplitudes. Electromagnetic wave energy density from all ray data points is mapped to a mesh and verified against the wave source power for energy conservation varying time step length, number of rays, and total time steps. We find that the method is self‐consistent and numerically robust. We further investigate whether the neglect of phase information and superposition has a significant impact on the accuracy of mapping wave intensity to a mesh. We find excellent agreement between the analytic solution for waves emitted by a line source in a plane‐stratified medium and an equivalent ray tracing solution. When phase information is excluded, ray tracing reproduces an average amplitude spread over regions of coherent constructive and destructive interference. This may be an important consideration for interpolating ray tracing results of longer wavelength waves such as magnetosonic, electromagnetic ion cyclotron, or ULF waves.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2026

Signatures of nonthermal carriers in nonlinear photoluminescence

Ultrafast light emission from plasmonic nanostructures provides a sensitive probe of the energetic electrons generated by intense optical excitation. The way this emission scales with excitation intensity has long been read through the lens of heated electron populations at an elevated temperature, yet this picture cannot reconcile the variety of behaviors seen across different materials and experiments. We argue that transient nonthermal electrons play a far larger role than has been appreciated. We present a unified description that reproduces emission behavior across diverse systems and outline experiments needed to resolve their signatures.

nanoscale materials↗

DOE OSTI2022

Data-driven design of novel halide perovskite alloys

The great tunability of the properties of halide perovskites presents new opportunities for optoelectronic applications as well as significant challenges associated with exploring combinatorial chemical spaces. Here, in this work, we develop a framework powered by high-throughput computations and machine learning for the design and prediction of mixed cation halide perovskite alloys. In a chemical space of ABX 3 perovskites with a selected set of options for A, B, and X species, pseudo-cubic structures with B-site mixing are simulated using density functional theory (DFT) and several properties are computed, including stability, lattice constant, band gap, vacancy formation energy, refractive index, and optical absorption spectrum, using both semi-local and hybrid functionals. Neural networks (NN) are used to train predictive models for every property using tabulated elemental properties of A, B, and X site species as descriptors. Starting from a DFT dataset of 229 points, we use the trained NN models to predict the structural, energetic, electronic, and optical properties of an extensive dataset of 17955 compounds, and perform high-throughput screening in terms of stability, band gap, and defect tolerance, to obtain 392 promising compounds that are ranked as potential absorbers according to their photovoltaic figure of merit. Compositional trends in the screened set of attractive mixed cation halide perovskites are revealed and additional computations are performed on selected compounds. The data-driven design framework developed here is promising for designing novel mixed compositions and can be extended to a wider perovskite chemical space in terms of A, B, and X species, different kinds of mixing at the A, B, or X sites, non-cubic phases, and other properties of interest.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Investigation of the correlation patterns and the Compton dominance variability of Mrk 421 in 2017

We present a detailed characterisation and theoretical interpretation of the broadband emission of the paradigmatic TeV blazar Mrk 421, with a special focus on the multi-band flux correlations. The dataset has been collected through an extensive multi-wavelength campaign organised between 2016 December and 2017 June. The instruments involved are MAGIC, FACT, Fermi-LAT, Swift, GASP-WEBT, OVRO, Medicina, and Metsähovi. Additionally, four deep exposures (several hours long) with simultaneous MAGIC and NuSTAR observations allowed a precise measurement of the falling segments of the two spectral components. The very-high-energy (VHE; E> 100 GeV) gamma rays and X-rays are positively correlated at zero time lag, but the strength and characteristics of the correlation change substantially across the various energy bands probed. The VHE versus X-ray fluxes follow different patterns, partly due to substantial changes in the Compton dominance for a few days without a simultaneous increase in the X-ray flux (i.e., orphan gamma-ray activity). Studying the broadband spectral energy distribution (SED) during the days including NuSTAR observations, we show that these changes can be explained within a one-zone leptonic model with a blob that increases its size over time. The peak frequency of the synchrotron bump varies by two orders of magnitude throughout the campaign. Our multi-band correlation study also hints at an anti-correlation between UV-optical and X-ray at a significance higher than 3σ. A VHE flare observed on MJD 57788 (2017 February 4) shows gamma-ray variability on multi-hour timescales, with a factor ten increase in the TeV flux but only a moderate increase in the keV flux. The related broadband SED is better described by a two-zone leptonic scenario rather than by a one-zone scenario. We find that the flare can be produced by the appearance of a compact second blob populated by high energetic electrons spanning a narrow range of Lorentz factors, from γ' min =2x10 4 to γ' max =6x10 5 .

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2026

Development of a broadband hard x-ray radiography platform for pulsed-power experiments

In this article, we develop and demonstrate a broadband hard x-ray radiography platform at the Zebra Pulsed Power Laboratory that integrates point-projection radiography, bremsstrahlung measurements, and hard x-ray pinhole imaging, designed to diagnose current-driven, cylindrically compressed matter. Initial laser-pulsed-power coupled experiments revealed that intense background radiation generated during 1 MA Zebra current shots overwhelmed laser-produced hard x-rays, obscuring radiographic images. Using combined spectral and spatial diagnostics, we identify energetic electrons accelerated by return currents as the dominant source of background hard x-rays, with electron energies inferred to be 3–4 MeV based on Monte Carlo simulations, and demonstrate mitigation through modifications to the radiation shielding and return-current configuration. The diagnostic platform was validated using a wire-pinch hard x-ray source, allowing radiographs of static 1-mm-diameter aluminum wires to be obtained while simultaneously measuring x-ray source spectra and spatial emission distributions within a single shot. Measured wire transmission profiles were quantitatively reconstructed using radiation transport simulations that incorporate an experimentally inferred two-temperature exponential x-ray spectrum from bremsstrahlung signal analysis and spatially distributed emission sources identified by pinhole imaging. Agreement between measured and simulated transmission profiles demonstrates the validity of the radiographic and x-ray source characterization approach, establishing this diagnostic platform as a promising tool for diagnosing magnetically driven, high-density plasmas relevant to warm dense matter and inertial fusion energy research.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Creating pair plasmas with observable collective effects

Although existing technology cannot yet directly produce fields at the Schwinger level, experimental facilities can already explore strong-field QED phenomena by taking advantage of the Lorentz boost of energetic electron beams. Recent studies show that QED cascades can create electron-positron pairs at sufficiently high density to exhibit collective plasma effects. Signatures of the collective pair plasma effects can appear in exquisite detail through plasmainduced frequency upshifts and chirps in the laser spectrum. Maximizing the magnitude of the QED plasma signature demands high pair density and low pair energy, which suits the configuration of colliding an over 10 18 Jm -3 energy-density electron beam with a 10 22 -10 23 Wcm -2 intensity laser pulse. The collision creates pairs that have a large plasma frequency, made even larger as they slow down or reverse direction due to both the radiation reaction and laser pressure. This paper explains at a tutorial level the key properties of the QED cascades and laser frequency upshift, and at the same time finds the minimum parameters that can be used to produce observable QED plasma.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

The principle of minimal power

This article is devoted to the memory of Yuri P Raizer, who passed away in 2021. He left a noticeable trace in gas discharge physics. The principle of minimal power (the state that requires minimal power is most probable) is thoroughly used in his books. Although the fundamental laws of physics do not imply this ad hoc principle, a detailed analysis of underlying phenomena can often reveal why nature prefers this path. Raizer illustrated this principle for plasma stratification, formation of electrode spots, discharge constriction, the shape of an arc channel, etc. We argue that the nonlinearity of equations describing gas discharges can often justify the realization of a plasma state maintained at minimal electric power. This nonlinearity appears because small groups of energetic electrons often control the ionization processes. The number of these electrons depends strongly on the ratio of the electric field to gas density, E/N. Under certain conditions, the ionization rate can also depend nonlinearly on electron density due to stepwise ionization and Coulomb collisions. Here, we use the principle of minimal power to illustrate some of Raizer's contributions to gas discharge physics from a single point of view. We demonstrate that nonlinearity of ionization processes in gas discharges can substantiate this principle for plasma stratification. However, striations of s, p, and r types in neon could exist with minimal or no ionization enhancement. This reminds us of Raizer's warning that applying the minimal power principle could lead to erroneous predictions, and a proper theory is required in each case to justify its use. 'The phenomenon of striations satisfies the principle of minimal power' – Yuri Raizer

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2024

RF antenna helicity dependent particle heating in a helicon source

Experiments have demonstrated that ion phenomena, such as the lower hybrid resonance, play an important role in helicon source operation. Damping of the slow branch of the bounded whistler wave at the edge of a helicon source (i.e. the Trivelpiece-Gould mode) has been correlated with the creation of energetic electrons, heating of ions at the plasma edge, and anisotropic ion heating. Here we present ion velocity distribution function measurements, electron density and temperature measurements, and magnetic fluctuation measurements on both sides of an m = |1| helical antenna in a helicon source as a function of the driving frequency, magnetic field strength, and magnetic field orientation relative to the antenna helicity. Significant electron and ion heating (up to two times larger) occurs on the side of the antenna consistent with the launch of the m = +1 mode. The electron and ion heating occurs within one electron skin depth of the plasma edge, where slow wave damping is expected. The source parameters for enhanced particle heating are also consistent with lower hybrid resonance effects, which can only occur for Trivelpiece-Gould wave excitation.

wave modes↗

DOE OSTI2024

Dataset for "Resistance of Boron Nitride Nanotubes to Radiation-Induced Oxidation" as published in The Journal of Physical Chemistry C

Adsorption↗

DOE OSTI2023

Enhanced cutoff energies for direct and rescattered strong-field photoelectron emission of plasmonic nanoparticles

Abstract The efficient generation, accurate detection, and detailed physical tracking of energetic electrons are of applied interest for high harmonics generation, electron-impact spectroscopy, and femtosecond time-resolved scanning tunneling microscopy. We here investigate the generation of photoelectrons (PEs) by exposing plasmonic nanostructures to intense laser pulses in the infrared (IR) spectral regime and analyze the sensitivity of PE spectra to competing elementary interactions for direct and rescattered photoemission pathways. Specifically, we measured and numerically simulated emitted PE momentum distributions from prototypical spherical gold nanoparticles (NPs) with diameters between 5 and 70 nm generated by short laser pulses with peak intensities of 8.0 × 10 12 and 1.2 × 10 13 W/cm 2 , demonstrating the shaping of PE spectra by the Coulomb repulsion between PEs, accumulating residual charges on the NP, and induced plasmonic electric fields. Compared to well-understood rescattering PE cutoff energies for strong-field photoemission from gaseous atomic targets (10× the ponderomotive energy), our measured and simulated PE spectra reveal a dramatic cutoff-energy increase of two orders of magnitude with a significantly higher contribution from direct photoemission. Our findings indicate that direct PEs reach up to 93 % of the rescattered electron cutoff energy, in contrast to 20 % for gaseous atoms, suggesting a novel scheme for the development of compact tunable tabletop electron sources.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗