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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Ultrasound-Assisted Nonthermal, Nonequilibrium Separation of Organic Molecules from Their Binary Aqueous Solutions: Effect of Solute Properties on Separation

The separation of organic molecules in downstream processes, such as distillation, plays a vital role in biobased chemical production. A comprehensive study was performed here using ultrasonic energy to separate 11 organic molecules from their binary aqueous solutions under nonthermal, nonequilibrium, and phase-change free conditions. A batch sonoseparator with a three-stage mist collection unit allowed direct analysis of ultrasound-generated mist with an HPLC/GC and differentiation and quantification of the vapor and mist. The results showed that the alcohols (1-butanol, ethanol, 1-propanol, and methanol) and acetone were enriched in the ultrasound-generated mist with enrichment ratios of 3.2–5. On the other hand, ethylene glycol, glycerol, γ-valerolactone (GVL), glucose, and sucrose were diluted with dilution ratios in the range of 2.04–15.7 in the mist and vapor generated by ultrasound (or concentrated in the bulk solution). No enrichment nor dilution of acetic acid was observed. The role of various physicochemical parameters such as dynamic viscosity, surface tension, Henry’s law of solubility constant, vapor pressure, and octanol–water partition coefficient in the enrichment was examined. Furthermore, the hydrophobicity of the organic molecules represented by the octanol–water partition coefficient was found to play a crucial role in determining the separation characteristics of the molecules in ultrasound-generated mist and vapor.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Energetic Nonthermal Electrons within the Above-the-looptop Regions in Solar Flares: Acceleration, Feedback, and Quasiperiodic Pulsations

Solar flares are among the most dramatic events in the solar system, releasing substantial magnetic energy and accelerating a large number of electrons to high energies. Notably, in certain events, the above-the-looptop region may contain a significant population of nonthermal electrons, both in number and energy. For the first time, we adopt a novel numerical method that combines magnetohydrodynamics with energetic particles incorporating feedback from nonthermal electrons to investigate electron acceleration and transport in solar flares. We find that a large fraction of energetic electrons are accelerated via the current sheet and termination shock regions. Most energetic electrons are concentrated in the above-the-looptop region, carrying a sizable amount of the released energy. We observe that greater feedback of nonthermal electrons leads to steeper energy spectra. The energy density of the nonthermal electrons oscillates due to the periodic impact of magnetic islands into the above-the-looptop region, which may help explain the observed quasiperiodic pulsations. Our simulations provide new insights into the origin of nonthermal electrons and associated emissions in the above-the-looptop region.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Nanoparticle dynamics in the spatial afterglows of nonthermal plasma synthesis reactors

Nonthermal plasma flow tube reactors are industrially scalable systems for the production of nanocrystal (NC) based materials and coatings. One key advantage of nonthermal plasma synthesis is the ability to both synthesize NCs and deposit films in a single reactor, as at the reactor outlet, NCs can be inertially deposited onto a target substrate. The size and morphology of deposited particles can substantially influence the film structure and function. Though NCs are typically near-spherical and monodispersed as-produced in plasma synthesis reactors, NC charge and growth dynamics can be altered substantially when NCs are sampled out of the plasma and through the spatial afterglow region, affecting deposition. Experiments have demonstrated changes of NC size and charge in the spatial afterglow; however, these dynamics remain unexplored and unexplained via theory and simulation. To address this, we developed a constant number Monte Carlo (CNMC) simulation model to examine the mechanisms of NC decharging and growth in the spatial afterglow of plasma flow tube reactors. Collisions between NC and plasma species, diffusive deposition, and electron desorption from NCs are incorporated in the CNMC simulation. The simulation results are specifically compared with previous experiments on Si NCs synthesized from a low pressure Ar-SiH 4 nonthermal plasma reactor. Furthermore, the experiment-model comparison shows that CNMC models can be implemented which accurately model NC size distribution evolution in a spatial afterglow. Simultaneously, results show that improved collision models, energetic species diffusion models, and electron desorption models will be necessary to accurately depict NC dynamics in spatial afterglows.

42 ENGINEERING↗
DOE OSTI2023

Plasma-Catalyst Synergy in the One-Pot Nonthermal Plasma-Assisted Synthesis of Aromatics from Methane

Electrification of the methane dehydroaromatization reaction with the use of nonthermal plasmas could alleviate the high-temperature requirement for this process while promoting the formation of valuable aromatics. Here, in this work, we evaluate the use of nonthermal plasma to investigate methane activation and conversion to aromatics by systematically varying bulk gas temperature in a one-pot, plasma-stimulated catalytic reactor over Mo/H-ZSM-5 and metal-free H-ZSM-5 catalysts. We report that Mo is not required for methane activation under low-temperature plasma conditions (573–773 K), and methane conversions up to ~15% with a 1:1 methane/N 2 feed are obtained under a 10 W plasma. However, Mo contributes to the formation of aromatics in the presence of a plasma at 773 K, achieving close to a 2-fold increase in the production of aromatics when compared to unmodified H-ZSM-5. Further, the exposure of as-prepared Mo/H-ZSM-5 to the methane plasma feed induces the formation of Mo-carbide phases in the temperature range studied. These findings highlight the complex roles of nonthermal plasmas in the direct activation of methane and the importance of plasma-catalyst design to facilitate aromatization reactions under plasma-assisted reaction conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

New Insights into Nonthermal Plasma-Assisted Poly(vinyl alcohol) Depolymerization Catalyzed by TiO 2

Here, in this study, we investigated the solid residual poly(vinyl alcohol) (PVA) and TiO 2 after nonthermal air, CO 2 , and N 2 plasma depolymerization in the absence and presence of TiO 2 . Scanning electron microscopy studies showed the absence of highly viscous tar and carbonaceous residues on the surfaces of PVA and TiO 2 . In the absence of TiO 2 , PVA particles exhibited micron-sized holes on their surfaces, whereas in the presence of TiO 2 , the surface roughness of PVA particles was observed at the submicron scale. These observations suggest that TiO 2 facilitates the even distribution of nonthermal plasma at a submicron scale, leading to a more uniform depolymerization of PVA surfaces. Raman, Fourier transform infrared spectroscopy, and X-ray absorption spectroscopy showed that (i) the surface of residual PVA contains mainly ketone functional groups and less C-H bonds than the pristine PVA and (ii) further confirmed the absence of highly viscous tar and carbonaceous residues on both used TiO 2 and residual PVA. The nuclear magnetic resonance and mass spectroscopy suggested that the PVA is growing back to poly polyvinyl acetate by the esterification reaction, and the ethers are produced by the acetal reaction between PVA and aldehyde. The transmission electron microscopy and X-ray diffraction analysis indicated no major crystal structural change of the TiO 2 catalyst after the plasma reactions. This study demonstrates that nonthermal plasma-assisted depolymerization is a viable alternative to thermal depolymerization, offering the unique advantage of converting polymer wastes into gaseous small organic molecules without generating recalcitrant viscous tar and carbonaceous residues on the surfaces of the polymer and TiO 2 catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Lower hybrid drift instability in nonthermal plasmas

Lower hybrid drift instability (LHDI) is driven by the cross-field current and operates in the vicinity of the lower-hybrid frequency, between the ion- and electron-gyro frequencies, and with wavelengths between the electron and ion thermal gyro radii. The free energy source that drives this instability resides in the density gradient associated with an inhomogeneous plasma. The existing literature on LHDI assumes that the charged particle distribution function is given by a Maxwellian form, but the space plasma is pervasively observed to feature nonthermal characteristics. This paper extends the theory of LHDI to nonthermal plasmas. The generalized theory of LHDI is, thus, applicable to various space plasma environments characterized by nonthermal plasma velocity distribution functions.

Arya, Neetasha (ORCID:0009000236075605)↗
DOE OSTI2022

The seeds and homogeneous nucleation of photoinduced nonthermal melting in semiconductors due to self-amplified local dynamic instability

Laser-induced nonthermal melting in semiconductors has been studied over the past four decades, but the underlying mechanism is still under debate. Here, by using an advanced real-time time-dependent density functional theory simulation, we reveal that the photoexcitation-induced ultrafast nonthermal melting in silicon occurs via homogeneous nucleation with random seeds originating from a self-amplified local dynamic instability. Because of this local dynamic instability, any initial small random thermal displacements of atoms can be amplified by a charge transfer of photoexcited carriers, which, in turn, creates a local self-trapping center for the excited carriers and yields the random nucleation seeds. Because a sufficient amount of photoexcited hot carriers must be cooled down to band edges before participating in the self-amplification of local lattice distortions, the time needed for hot carrier cooling is the response for the longer melting time scales at shorter laser wavelengths. This finding provides fresh insights into photoinduced ultrafast nonthermal melting.

42 ENGINEERING↗
DOE OSTI2025

Constraints on Nonthermal Pressure at Galaxy Cluster Outskirts from a Joint SPT and XMM-Newton Analysis

We present joint South Pole Telescope and XMM-Newton observations of eight massive galaxy clusters (0.8–2 × 10$^{15}$ M$_{⊙}$) spanning a redshift range of 0.16–0.35. Employing a novel Sunyaev–Zel’dovich + X-ray fitting technique, we effectively constrain the thermodynamic properties of these clusters out to the virial radius. The resulting best-fit electron density, deprojected temperature, and deprojected pressure profiles are in good agreement with previous observations of massive clusters. For the majority of the cluster sample (five out of eight clusters), the entropy profiles exhibit a self-similar behavior near the virial radius. We further derive hydrostatic mass, gas mass, and gas fraction profiles for all clusters up to the virial radius. Comparing the enclosed gas fraction profiles with the universal gas fraction profile, we obtain nonthermal pressure fraction profiles for our cluster sample at >0.5R$_{500}$, demonstrating a steeper increase between R$_{500}$ and R$_{200}$ that is consistent with the hydrodynamical simulations. Our analysis yields nonthermal pressure fraction ranges of 8%–28% (median: 15% ± 11%) at R$_{500}$ and 21%–35% (median: 27% ± 12%) at R$_{200}$. Notably, weak-lensing mass measurements are available for only four clusters in our sample, and our recovered total cluster masses, after accounting for nonthermal pressure, are consistent with these measurements.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2024

Observation and Characterization of Vibrationally Active Surface Species Accessed with Nonthermal Nitrogen Plasmas

Polycrystalline Ni, Pd, Cu, Ag, and Au foils exposed to nonthermal plasma (NTP)-activated N 2 are found to exhibit a vibrational feature near 2200 cm –1 in polarization-modulation infrared reflection-absorption spectroscopy (PM-IRAS) observations that are not present in the same materials exposed to N 2 under nonplasma conditions. The feature is similar to that reported elsewhere and is typically assigned to chemisorbed N 2 . We employ a combination of temperature-dependent experiments, sequential dosing, X-ray photoelectron spectroscopy, isotopic labeling, and density functional theory calculations to characterize the feature. Results are most consistent with a triatomic species, likely NCO, with the C and O likely originating from ppm-level impurities in the ultrahigh-purity (UHP) Ar and/or N 2 gas cylinders. Here, this work highlights the potential for nonthermal plasmas to access adsorbates inaccessible thermally as well as the potential contributions of ppm-level impurities to corrupt the interpretation of plasma catalytic chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Ternary SiGeSn alloy nanocrystals via nonthermal plasma synthesis

We report on the synthesis of ternary SiGeSn nanocrystals (NCs) produced via nonthermal plasma synthesis from silane (SiH 4 ), germane (GeH 4 ), and tetramethylstannane (Sn(CH 3 ) 4 ) precursor sources. Detailed structural, chemical, and vibrational analyses show that all three elements are incorporated both on the NC surface and within the NC core. Incorporation of Sn into the NC core is realized using a secondary injection of SiH 4 and GeH 4 precursor gases in the after-glow region of the plasma, which kinetically traps Sn in the core. We demonstrate compositional tunability of the SiGeSn NCs in which the Si and Ge ratios can be varied broadly at low Sn concentrations. We also show tunability of the Sn content up to ~2 atomic percent as revealed by ICP-MS analysis. More generally, this report demonstrates how nonthermal plasma synthesis can be used to produce metastable ternary nanostructured alloys involving thermodynamically insoluble constituents.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Relativistic Magnetic Reconnection in Astrophysical Plasmas: A Powerful Mechanism of Nonthermal Emission

Magnetic reconnection—a fundamental plasma physics process, where magnetic field lines of opposite polarity annihilate—is invoked in astrophysical plasmas as a powerful mechanism of nonthermal particle acceleration, able to explain fast-evolving, bright high-energy flares. Near black holes and neutron stars, reconnection occurs in the relativistic regime, in which the mean magnetic energy per particle exceeds the rest mass energy. This review reports recent advances in our understanding of the kinetic physics of relativistic reconnection (RR): ▪ Kinetic simulations have elucidated the physics of plasma heating and nonthermal particle acceleration in RR. ▪ The physics of radiative RR, with its self-consistent interplay between photons and reconnection-accelerated particles—a peculiarity of luminous, high-energy astrophysical sources—is the new frontier of research. ▪ RR plays a key role in global models of high-energy sources, in terms of both global-scale layers and reconnection sites generated as a by-product of local magnetohydrodynamic instabilities. We summarize themes of active investigation and future directions, emphasizing the role of upcoming observational capabilities, laboratory experiments, and new computational tools.

acceleration of particles↗
DOE OSTI2024

Nonthermal hydrogen plasma-enabled ambient, fast lignin hydrogenolysis to valuable chemicals and bio-oils

The reduction of fossil fuel resources and the ongoing surge in global energy demand have captured the interest of researchers worldwide, prompting a focus on developing renewable energy sources. For this reason, biomass conversion has emerged as a crucial pathway for renewable fuel production. Lignin, constituting 10–35% of woody biomass, represents a significant and largely untapped sustainable feedstock. Despite the potential of lignin, a substantial portion of this lignocellulosic residue remains unused, with approximately 60% considered waste. This study addresses the challenge of underutilized lignin by introducing an innovative approach to its hydrogenolysis. Despite their potential, existing hydrogenolysis methods face obstacles such as complexity, high cost, and the need for high temperatures or pressures. Herein we report a noncatalytic nonthermal hydrogen plasma method for lignin hydrogenolysis, conducted under ambient temperature and pressure conditions. Our method proves to be highly effective in breaking lignin bonds, achieving complete conversion, and generating valuable gaseous and bio-oil products including methane and aromatic dimers and monomers obtained from guaiacyl and syringyl units within the lignin structure. Our results showed an increase in gaseous products, especially methane, and aromatic monomer yields, as well as a reduction in total bio-oil and biochar yields and lignin functional groups by increasing reaction time, input power, and H2 partial pressure. This research confirms the considerable promise of utilizing noncatalytic nonthermal hydrogen plasma-assisted hydrogenolysis as an effective technique for producing gaseous and liquid fuels from lignin.

Pishva, Parsa↗
DOE OSTI2024

Toward sustainable production of N-containing products via nonthermal plasma-enhanced conversion of natural gas resources

Nonthermal plasmas can directly activate and cleave the strong chemical bonds in molecular nitrogen and methane to facilitate the transformation of these inherently stable molecules through the application of electrical energy. Here, we report a low temperature, atmospheric pressure, nonthermal plasma for the “one-pot” synthesis of olefins, alkynes, higher molecular weight hydrocarbons, ammonia, and nitrogen-containing liquids from a representative shale gas feed enriched with nitrogen. Furthermore, we reproducibly observe a wide range of valuable and synthetically challenging gas-phase and liquid-phase products containing C-N, C-C, and N-H bonding by controlling the N 2 concentration in the inlet feed stream. In nitrogen-lean regimes, hydrocarbon products dominate (e.g., ethylene, acetylene, etc.), while nitrogen-rich regimes promote incorporation of nitrogen into the products, leading to the formation of ammonia and liquid products containing a variety of functionalities (e.g., nitriles, amines, heterocycles). High resolution electrospray ionization mass spectrometry was used to measure molecular weights and identify the chemical formulas of the liquid products. Van Krevelen diagrams were created and showed many products with compositions around H/C = 2 and N/C = 0.5, indicating the potential importance of intermediate species with these ratios for liquid formation (e.g., CH 3 CN + H).

03 NATURAL GAS↗
DOE OSTI2020

Nonthermal electron and ion acceleration by magnetic reconnection in large laser-driven plasmas

Magnetic reconnection is a fundamental plasma process that is thought to play a key role in the production of nonthermal particles associated with explosive phenomena in space physics and astrophysics. Experiments at high-energy-density facilities are starting to probe the microphysics of reconnection at high Lundquist numbers and large system sizes. We have performed particle-in-cell (PIC) simulations to explore particle acceleration for parameters relevant to laser-driven reconnection experiments. We study particle acceleration in large system sizes that may be produced soon with the most energetic laser drivers available, such as at the National Ignition Facility. In these conditions, we show the possibility of reaching the multi-plasmoid regime, where plasmoid acceleration becomes dominant. Our results show the transition from X point to plasmoid-dominated acceleration associated with the merging and contraction of plasmoids that further extend the maximum energy of the power-law tail of the particle distribution for electrons. We also find for the first time a system-size-dependent emergence of nonthermal ion acceleration in driven reconnection, where the magnetization of ions at sufficiently large sizes allows them to be contained by the magnetic field and energized by direct X point acceleration. For feasible experimental conditions, electrons and ions can attain energies of ϵ max , e / k B T e > 100 and ϵ max , i / k B T i > 1000 . Using PIC simulations with binary Monte Carlo Coulomb collisions, we study the impact of collisionality on plasmoid formation and particle acceleration. The implications of these results for understanding the role reconnection plays in accelerating particles in space physics and astrophysics are discussed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Nonthermal breaking of magnetic order via photogenerated spin defects in the spin-orbit coupled insulator Sr 3 Ir 2 O 7

In many strongly correlated insulators, antiferromagnetic order competes with exotic and technologically relevant phases, like superconductivity. While control of spin order is critical to stabilize different functional states, elucidating the mechanism of laser-induced demagnetization in complex oxides remains a challenge. It is unknown if the optical pulse can quench magnetization nonthermally or if it instead only acts as a heat source. In this study, we used ultrafast, broadband, optical spectroscopy to track the responses of the electronic, lattice, and spin degrees of freedom and their relation to antiferromagnetism in the strongly spin-orbit coupled insulator Sr 3 Ir 2 O 7 . We find that magnetization can be rapidly and strongly suppressed on a sub-150 fs timescale. At low excitation fluences, the magnetic recovery is fast; however, the recovery time increases dramatically with the magnitude of demagnetization. At the same time, we show that the lattice, evidenced through the A g phonon frequencies, appears to remain below T N , suggesting that the system remains nonthermal during the optical modulation of spin order. We suggest that photogenerated spin defects are responsible for the long-lived demagnetized state and discuss its implications for optical control of solids.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Collisional-energy-cascade model for nonthermal velocity distributions of neutral atoms in plasmas

Nonthermal velocity distributions with much greater tails than a Maxwellian have been observed for radical atoms in plasmas for a long time. Historically, such velocity distributions have been modeled by a two-temperature Maxwell distribution. In this paper, I propose a model based on collisional energy cascade, which has been studied in the field of granular materials. In the collisional energy cascade, a particle ensemble undergoes energy input at the high-energy region, entropy production by elastic collisions among particles, and energy dissipation. For radical atoms, energy input may be caused by the Franck-Condon energy of molecular dissociation or charge-exchange collision with hot ions, and the input energy is eventually dissipated by collisions with the walls. Here, I show that the steady-state velocity distribution in the collisional energy cascade is approximated by the generalized Mittag-Leffler distribution, which is a one-parameter extension of the Maxwell distribution. This parameter indicates the degree of the nonthermality and is related to the relative importance of energy dissipation over entropy production. This model is compared with a direct molecular dynamics simulation for simplified gaseous systems with energy input, as well as some experimentally observed velocity distributions of light radicals in plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Plasma Dynamics and Nonthermal Particle Acceleration in 3D Nonrelativistic Magnetic Reconnection

Understanding plasma dynamics and nonthermal particle acceleration in 3D magnetic reconnection has been a long-standing challenge. In this paper, we explore these problems by performing large-scale fully kinetic simulations of multi-X-line plasmoid reconnection with various parameters in both the weak- and strong-guide-field regimes. In each regime, we have identified its unique 3D dynamics that lead to field-line chaos and efficient acceleration, and we have achieved nonthermal acceleration of both electrons and protons into power-law spectra. The spectral indices agree well with a simple Fermi acceleration theory that includes guide-field dependence. In the low-guide-field regime, the flux rope kink instability governs the 3D dynamics for efficient acceleration. The weak dependence of the spectra on the ion-to-electron mass ratio and β ($\ll$1) implies that the particles are sufficiently magnetized for Fermi acceleration in our simulations. While both electrons and protons are injected at reconnection exhausts, protons are primarily injected by perpendicular electric fields through Fermi reflections and electrons are injected by a combination of perpendicular and parallel electric fields. The magnetic power spectra agree with in situ magnetotail observations, and the spectral index may reflect a reconnection-driven size distribution of plasmoids instead of the Goldreich–Sridhar vortex cascade. As the guide field becomes stronger, the oblique flux ropes of large sizes capture the main 3D dynamics for efficient acceleration. Intriguingly, the oblique flux ropes can also experience flux rope kink instability, to drive extra 3D dynamics. This work has broad implications for 3D reconnection dynamics and particle acceleration in heliophysics and astrophysics.

79 ASTRONOMY AND ASTROPHYSICS↗