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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 487 records · Page 27

Characterization of a new ultra-high pressure shock tube facility for combustion and propulsion studies

A new shock tube facility has been designed, constructed, and characterized at the University of Central Florida. This facility is capable of withstanding pressures of up to 1000 atm, allowing for combustion diagnostics of extreme conditions, such as in rocket combustion chambers or in novel power conversion cycles. For studies with toxic gas impurities, the high initial pressures required the development of a gas delivery system to ensure the longevity of the facility and the safety of the personnel. Data acquisition and experimental propagation were implemented with remote access to ensure safety, paired with a LabVIEW- and Python-based user interface. Thus far, test pressures of 270 atm, blast pressures of 730 atm, and temperatures approaching 10 000 K have been achieved. The extreme limitations of this facility allow for emission spectroscopy to be performed during the oxidation of fuel mixtures, e.g., alkanes diluted in argon and carbon dioxide. Ignition delay times were determined and compared to simulations using chemical kinetic mechanisms. The design, experimental procedures, processes of analysis, and uncertainty determination are outlined, and typical pressure profiles are compared with a new gas dynamics solver and empirical correlations developed across multiple shock tube facilities. Preliminary reactive mixture analyses are included with further investigation of the mixtures outlined.

47 OTHER INSTRUMENTATION↗

Effects of local order parameter dependent transport coefficient in diblock copolymers under applied electric fields

In this work, we present an approach for constructing thermodynamically consistent time-dependent models relevant to thin films of diblock copolymers in applied electric fields. The approach is based on the principles of linear irreversible thermodynamics, and, in this work, it is applied to study the effects of electric fields on thin films of incompressible diblock copolymers. Enforcement of local incompressibility constraint at all times leads to a local order parameter dependent transport coefficient in the model for the diblock copolymers. The dependence of the transport coefficient on the local order parameter is used to relate it with the diffusion constant of Rouse chains and leads to sensitivity of the model to initial conditions. In addition, transient behavior is found to be affected when compared with an ad hoc model assuming a constant transport coefficient. Numerical results such as electric field induced alignment of lamellae domains due to the field are found to be in qualitative agreement with experiments. This approach opens up a systematic way of developing kinetic models for simulating effects of electrolytes added to thin films containing diblock copolymers in the presence of applied electric fields.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Surface coverage dynamics for reversible dissociative adsorption on finite linear lattices

Dissociative adsorption onto a surface introduces dynamic correlations between neighboring sites not found in non-dissociative absorption. We study surface coverage dynamics where reversible dissociative adsorption of dimers occurs on a finite linear lattice. We derive analytic expressions for the equilibrium surface coverage as a function of the number of reactive sites, N, and the ratio of the adsorption and desorption rates. Using these results, we characterize the finite size effect on the equilibrium surface coverage. For comparable N’s, the finite size effect is significantly larger when N is even than when N is odd. Moreover, as N increases, the size effect decays more slowly in the even case than in the odd case. The finite-size effect becomes significant when adsorption and desorption rates are considerably different. These finite-size effects are related to the number of accessible configurations in a finite system where the odd-even dependence arises from the limited number of accessible configurations in the even case. We confirm our analytical results with kinetic Monte Carlo simulations. We also analyze the surface-diffusion case where adsorbed atoms can hop into neighboring sites. As expected, the odd-even dependence disappears because more configurations are accessible in the even case due to surface diffusion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Rotational Dynamics and Transition Mechanisms of Surface-Adsorbed Proteins

Assembly of biomolecules at solid-water interfaces requires molecules to traverse complex orientation-dependent energy landscapes through processes that are poorly understood, largely due to the dearth of in-situ single molecule measurements and statistical analyses of the rotational dynamics that define directional selection. Emerging capabilities in high-speed atomic force microscopy and machine learning have allowed us to directly determine the orientational energy landscape and observe and quantify the rotational dynamics for protein nanorods on the surface of muscovite mica under a variety of conditions. Comparisons with kinetic Monte Carlo simulations show that the transition rates between adjacent orientation-specific energetic minima can largely be understood through traditional models of in-plane Brownian rotation across a biased energy landscape, with resulting transition rates that are exponential in the energy-barriers between states. However, transitions between more distant angular states are decoupled from barrier height, with jump-size distributions showing a power-law decay that is characteristic of a non-classical Levy-flight random walk, indicating that large jumps are enabled by alternative modes of motion via activated states. The findings provide new insights into the dynamics of biomolecules at solid-liquid interfaces that lead to self-assembly, epitaxial matching and other orientationally anisotropic outcomes and define a general procedure for exploring such dynamics with implications for hybrid biomolecular-inorganic materials design.

Orientational energy landscapes, Rotational dynami↗

Single molecule tracking of bacterial cell surface cytochromes reveals dynamics that impact long-distance electron transport

Using a series of multiheme cytochromes, the metal-reducing bacterium Shewanella oneidensis MR-1 can perform extracellular electron transfer (EET) to respire redox-active surfaces, including minerals and electrodes outside the cell. While the role of multiheme cytochromes in transporting electrons across the cell wall is well established, these cytochromes were also recently found to facilitate long-distance (micrometer-scale) redox conduction along outer membranes and across multiple cells bridging electrodes. Recent studies proposed that long-distance conduction arises from the interplay of electron hopping and cytochrome diffusion, which allows collisions and electron exchange between cytochromes along membranes. However, the diffusive dynamics of the multiheme cytochromes have never been observed or quantified in vivo, making it difficult to assess their hypothesized contribution to the collision-exchange mechanism. Here, we use quantum dot labeling, total internal reflection fluorescence microscopy, and single-particle tracking to quantify the lateral diffusive dynamics of the outer membrane-associated decaheme cytochromes MtrC and OmcA, two key components of EET in S. oneidensis. We observe confined diffusion behavior for both quantum dot-labeled MtrC and OmcA along cell surfaces (diffusion coefficients D MtrC = 0.0192 ± 0.0018 µm 2 /s, D OmcA = 0.0125 ± 0.0024 µm 2 /s) and the membrane extensions thought to function as bacterial nanowires. We find that these dynamics can trace a path for electron transport via overlap of cytochrome trajectories, consistent with the long-distance conduction mechanism. The measured dynamics inform kinetic Monte Carlo simulations that combine direct electron hopping and redox molecule diffusion, revealing significant electron transport rates along cells and membrane nanowires.

59 BASIC BIOLOGICAL SCIENCES↗

Fluid-kinetic modeling of a high power density radio frequency inductively coupled positive hydrogen ion source

High power density radio-frequency (RF) inductively coupled positive ion sources are attractive candidates for next-generation neutral beam injection (NBI) systems, where higher injected power and longer pulse lengths are desired without sacrificing source reliability. Operating at absorbed power densities of order $\gt 1~\mathrm{W\,cm}^{-3}$ places these sources in a regime with stronger gas heating, higher dissociation, and non-Maxwellian electron energy distributions. The Large Uniform Plasma for Ionizing Neutrals (LUPIN) is an RF inductively coupled plasma source designed to explore this high power density regime and to provide guidance for a positive ion source upgrade for the DIII-D NBI system. LUPIN is designed to operate at up to 20 kW of RF power at 2 MHz, coupling energy through a cylindrical quartz vessel to achieve target ion current densities of $2100\,\mathrm{A\,m}^{-2}$ . This paper presents fluid-kinetic modeling of LUPIN using the hybrid plasma equipment model where electrons are treated kinetically, and the simulations reveal that electron energy distribution function transitions from nearly Maxwellian in the core to bi-Maxwellian towards the edge. Parametric simulations investigate the effects of RF power, gas pressure, and frequency on plasma density, ion flux, and uniformity. Parametric sweeps reveal that increasing power shifts the primary ionization channel from molecular to atomic with diminishing flux gains due to skin-depth contraction and gas rarefaction. Higher frequency localizes heating and increases $\mathrm{H}_2^+$ and $\mathrm{H}_3^+$ delivery to the grid, while elevated pressure boosts ionization yet hinders ion transport due to increase in collisionality.

inductively coupled plasma↗

Effects of collisional ion orbit loss on tokamak radial electric field and toroidal rotation in an L-mode plasma

Abstract Ion orbit loss has been used to model the formation of a strong negative radial electric field E r in the tokamak edge, as well as edge momentum transport and toroidal rotation. To quantitatively measure ion orbit loss, an orbit-flux formulation has been developed and numerically applied to the gyrokinetic particle-in-cell code XGC. We study collisional ion orbit loss in an axisymmetric DIII-D L-mode plasma using gyrokinetic ions and drift-kinetic electrons. Numerical simulations, where the plasma density and temperature profiles are maintained through neutral ionization and heating, show the formation of a quasisteady negative E r in the edge. We have measured a radially outgoing ion gyrocenter flux due to collisional scattering of ions into the loss orbits, which is balanced by the radially incoming ion gyrocenter flux from confined orbits on the collisional time scale. This suggests that collisional ion orbit loss can shift E r in the negative direction compared to that in plasmas without orbit loss. It is also found that collisional ion orbit loss can contribute to a radially outgoing (counter-current) toroidal-angular-momentum flux, which is not balanced by the toroidal-angular-momentum flux carried by ions on the confined orbits. Therefore, the edge toroidal rotation shifts in the co-current direction on the collisional time scale.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Active control of Alfvén eigenmodes by external magnetic perturbations with different spatial spectra

Alfvén eigenmodes have been suppressed and excited in tokamak plasmas by (just) modifying the poloidal spectra of externally applied static magnetic perturbations. This effect is observed experimentally when toroidal spectra of n = 2, n = 4 as well as a mixed spectrum of n = 2 and n = 4 is applied. Under the n = 2 magnetic perturbations, the modes are excited or suppressed by modifying the coil phasing between the upper and the lower set of coils. Regardless of the absolute rotation, an even parity for the n = 4 perturbation is observed to reduce the amplitude of the Alfvénic instabilities, while an odd parity amplifies it. To combine the stabilizing (and destabilizing) effect of n = 2 and n = 4, a mixed spectrum is applied, finding similar reduction (and amplification) trends. However, the impact on the mode amplitude is more subtle, due to the reduced coil current required for a mixed spectrum. The signal level on the fast-ion loss detector is sensitive to the applied poloidal spectrum, which is consistent with Hamiltonian full-orbit modelling of an edge resonant transport layer activated by the 3D perturbative fields. An internal redistribution of the fast-ion population is induced, modifying the phase-space gradients driving the Alfvénic instabilities, and ultimately determining their existence. The calculated edge resonant layers for both n = 2 and n = 4 toroidal spectra are consistent with the observed suppressed and excited phases. Moreover, hybrid kinetic-magnetohydrodynamic (MHD) simulations reveal that this edge resonant transport layer overlaps in phase-space with the population responsible for the fast-ion drive. The results presented here may help to control fast-ion driven Alfvénic instabilities in future burning plasmas with a significant fusion born alpha particle population.

Alfvén waves↗

Variable-spectrum mode control of high poloidal beta discharges

DIII-D experiments demonstrate that high pressure, broad current profile equilibria can be accessed in the high poloidal beta regime by optimizing the MHD mode control poloidal spectrum. A novel, variable spectrum (VS) magnetic feedback scheme implemented using the DIII-D internal non-axisymmetric coils (I-coils) facilitated access to reduced internal inductance $l$ i operation above the no-wall beta limit compared with both no feedback and fixed spectrum feedback. In addition, the VS feedback helped avoid beta collapses caused by marginally unstable resistive wall mode activity. The lower and upper I-coil rows were configured in two independent feedback loops, allowing the feedback field's poloidal spectrum to vary and track changes in the plasma mode structure as the edge safety factor q 95 varied from 11 to 6 during the discharges. The q 95 dependence of the measured phase difference between the lower and upper I-coil rows during VS feedback is qualitatively compatible with ideal MHD simulations of the least-stable plasma kink mode and with plasma response simulations that included kinetic modifications to ideal MHD. The VS feedback approach is a straightforward way to improve resilience to variations in mode structure that occur as plasma parameters change. The demonstrated expansion of the operating space to lower $l$ i is expected to improve the coupling of the plasma kink mode to external fields and beneficial wall eddy currents, and is compatible with high bootstrap fraction operation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Frequency multiplication with toroidal mode number of kink/fishbone modes on a static HL-2A-like tokamak

In the presence of energetic particles (EPs), the long-lived mode (LLM) frequency multiplication with n = 1, 2, 3, or higher is often observed on HL-2A, where n is the toroidal mode number. Hybrid kinetic-MHD model simulations of the energetic particle (EP) driven kink/fishbone modes on a static HL-2A-like tokamak using NIMROD code find that when the background plasma pressure is relatively high, and the EP pressure and the beam energy are relatively low, the mode frequency increases almost linearly with EP pressure, and the frequency is proportional to n (‘frequency multiplication’), even in the absence of any equilibrium plasma rotation. In addition, the frequency multiplication persists as the safety factor at the magnetic axis q 0 varies. In the absence of EPs, the growth rate of the 1/1 mode is the largest; however, as the EP pressure increases, the growth rate of 2/2 modes or 3/3 modes becomes dominant, suggesting that higher-n modes are more vulnerable to EPs. These results may shed light on the understanding of the toroidal mode number dependence of kink/fishbone modes in the advanced scenarios of tokamaks with weak or reversed central magnetic shear.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Phase transitions in Schloegl's second model for autocatalysis on a Bethe lattice

Schloegl's second model (also known as the quadratic contact process) on a lattice involves spontaneous particle annihilation at rate p and autocatalytic particle creation at empty sites with n ≥ 2 occupied neighbors. The particle creation rate for exactly n occupied neighbors is selected here as n(n - 1)/[z(z - 1)] for lattice coordination number z. We analyze this model on a Bethe lattice. Precise behavior for stochastic models on regular periodic infinite lattices is usually surmised from kinetic Monte Carlo simulation on a finite lattice with periodic boundary conditions. However, the persistence of boundary effects for a Bethe lattice complicates this process, e.g., by inducing spatially heterogenous states. This motivates the exploration of various boundary conditions and unconventional simulation ensembles on the Bethe lattice to predict behavior for infinite size. Here, we focus on z = 3, and predict a discontinuous transition to the vacuum state on the infinite lattice when p exceeds a threshold value of around 0.053.

97 MATHEMATICS AND COMPUTING↗

Statistical mechanics of kinks on a gliding screw dislocation

The ability of a body-centered-cubic metal to deform plastically is limited by the thermally activated glide motion of screw dislocations, which are line defects with a mobility exhibiting complex dependence on temperature, stress, and dislocation segment length. We derive an analytical expression for the velocity of dislocation glide, based on a statistical mechanics argument, and identify an apparent phase transition marked by a crossover temperature above which the activation energy for glide effectively halves, changing from the formation energy of a double kink to that of a single kink. The analysis is in quantitative agreement with direct kinetic Monte Carlo simulations.

36 MATERIALS SCIENCE↗

Hydroxide films on mica form charge-stabilized microphases that circumvent nucleation barriers

Crystal nucleation is facilitated by transient, nanoscale fluctuations that are extraordinarily difficult to observe. Here, we use high-speed atomic force microscopy to directly observe the growth of an aluminum hydroxide film from an aqueous solution and characterize the dynamically fluctuating nanostructures that precede its formation. Nanoscale cluster distributions and fluctuation dynamics show many similarities to the predictions of classical nucleation theory, but the cluster energy landscape deviates from classical expectations. Kinetic Monte Carlo simulations show that these deviations can arise from electrostatic interactions between the clusters and the underlying substrate, which drive microphase separation to create a nanostructured surface phase. This phase can evolve seamlessly from a low-coverage state of fluctuating clusters into a high-coverage nanostructured network, allowing the film to grow without having to overcome classical nucleation barriers.

36 MATERIALS SCIENCE↗

A composite electrodynamic mechanism to reconcile spatiotemporally resolved exciton transport in quantum dot superlattices

Quantum dot (QD) solids are promising optoelectronic materials; further advancing their device functionality requires understanding their energy transport mechanisms. The commonly invoked near-field Förster resonance energy transfer (FRET) theory often underestimates the exciton hopping rate in QD solids, yet no consensus exists on the underlying cause. In response, we use time-resolved ultrafast stimulated emission depletion (STED) microscopy, an ultrafast transformation of STED to spatiotemporally resolve exciton diffusion in tellurium-doped cadmium selenide–core/cadmium sulfide–shell QD superlattices. We measure the concomitant time-resolved exciton energy decay due to excitons sampling a heterogeneous energetic landscape within the superlattice. The heterogeneity is quantified by single-particle emission spectroscopy. This powerful multimodal set of observables provides sufficient constraints on a kinetic Monte Carlo simulation of exciton transport to elucidate a composite transport mechanism that includes both near-field FRET and previously neglected far-field emission/reabsorption contributions. Uncovering this mechanism offers a much-needed unified framework in which to characterize transport in QD solids and additional principles for device design.

36 MATERIALS SCIENCE↗

Water-promoted interfacial pathways in methane oxidation to methanol on a CeO 2 -Cu 2 O catalyst

Highly selective oxidation of methane to methanol has long been challenging in catalysis. Here, we reveal key steps for the pro­motion of this reaction by water when tuning the selectivity of a well-defined CeO 2 /Cu 2 O/Cu(111) catalyst from carbon monoxide and carbon dioxide to methanol under a reaction environment with methane, oxygen, and water. Ambient-pressure x-ray photoelectron spectroscopy showed that water added to methane and oxygen led to surface methoxy groups and accelerated methanol production. These results were consistent with density functional theory calculations and kinetic Monte Carlo simulations, which showed that water preferentially dissociates over the active cerium ions at the CeO 2 –Cu 2 O/Cu(111) interface. The adsorbed hydroxyl species blocked O-O bond cleavage that would dehydrogenate methoxy groups to carbon monoxide and carbon dioxide, and it directly converted this species to methanol, while oxygen reoxidized the reduced surface. Water adsorption also displaced the produced methanol into the gas phase.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Formation of active sites on transition metals through reaction-driven migration of surface atoms

Adopting low-index single-crystal surfaces as models for metal nanoparticle catalysts has been questioned by the experimental findings of adsorbate-induced formation of subnanometer clusters on several single-crystal surfaces. Here we used density functional theory calculations to elucidate the conditions that lead to cluster formation and show how adatom formation energies enable efficient screening of the conditions required for adsorbate-induced cluster formation. We studied a combination of eight face-centered cubic transition metals and 18 common surface intermediates and identified systems relevant to catalytic reactions, such as carbon monoxide (CO) oxidation and ammonia (NH 3 ) oxidation. We used kinetic Monte Carlo simulations to elucidate the CO-induced cluster formation process on a copper surface. Scanning tunneling microscopy of CO on a nickel (111) surface that contains steps and dislocations points to the structure sensitivity of this phenomenon. Metal-metal bond breaking that leads to the evolution of catalyst structures under realistic reaction conditions occurs much more broadly than previously thought.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ultra-high energy density relativistic plasmas from nanostructures: scaling to ultra-high intensities (Final Report)

This project investigated the ultra-high energy density (UHED) regime of matter found in the center of stars, using a compact PW-class laser. These extreme conditions are typically only obtained in the laboratory in the central hot-spot of spherically imploded capsules in inertial confinement fusion experiments driven by the world’s largest lasers. We have shown that near-solid density arrays of aligned nanostructures can be volumetrically heated to multi-keV temperatures by irradiation at relativistic intensity with ultrafast laser pulses of modest energy, opening a path for the generation of UHED plasmas with compact lasers. This new UHED plasma generation approach promises to create an environment with extreme energy densities and degrees of ionization, record conversion of optical laser light into ultrafast x-ray pulses, gigantic magnetic fields and pressures, and directed beams of high energy particles . In this project we achieved record degree of ionization in volumetric heating solid density and near-solid density plasmas. Gold plasmas which spectra is characterized by L shell transition emission from ions with charge up to the Ne-like state, Au+ 72 were generated using ultrafast laser pulses of less than 10 J of energy from a compact laser focused to an intensity of ~ 3x10 21 Wcm -2 . We also conducted measurements to determine the heat penetration depth in Ni nanowire arrays as compared to Ni foil targets by monitoring the line emission of a Co buried tracer underneath a variable amount of Ni. The measurements revealed that the nanowire plasmas are roughly six times larger in depth than the solid density target plasmas. A result of this increased plasma in nanowire arrays is a greatly increased conversion of optical laser light into > 1 KeV x-rays, a record conversion efficiency of 20 %. Critical to the realization of the proposed experiments was the generation of ultrafast laser pulses with ultra-high contrast that can deposit the energy deep into the nanowire arrays before the nanowires explode to create a continuous plasma. Supporting the proposed experiments was the recent demonstration at Colorado State University of a Petawatt-class laser that emits 30 fs pulses at high repetition rates. The experiments combined this unique laser tool with a variety of tailored nanowire arrays fabricated in house and with an extensive suite of diagnostics. The experiments were accompanied by 3-dimensional particle-in-cell simulations and detailed atomic physics simulations with transient kinetics and radiation transport. The proposed research allowed us to continue training Ph.D students and post-docs with broad experience in HEDP Science.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Kinetic effects of self-organization in low-temperature magnetized plasmas

This final report presents the progress made for the DOE-SC0020623 for the period of performance between January 1 2020 and September 30 2024. The research project is entitled "Kinetic effects of self-organization in low-temperature magnetized plasmas", in which kinetic theory and simulations are used to under stand self-organization patterns.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗