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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 631 records · Page 35
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Imaging Valence Electron Rearrangement in a Chemical Reaction Using Hard X-Ray Scattering

We have observed the signatures of valence electron rearrangement in photoexcited ammonia using ultrafast hard x-ray scattering. Time-resolved x-ray scattering is a powerful tool for imaging structural dynamics in molecules because of the strong scattering from the core electrons localized near each nucleus. Such core-electron contributions generally dominate the differential scattering signal, masking any signatures of rearrangement in the chemically important valence electrons. Ammonia represents an exception to the typically high core-to-valence electron ratio. Here, we measured 9.8 keV x-ray scattering from gas-phase deuterated ammonia following photoexcitation via a 200 nm pump pulse to the 3s Rydberg state. We observed changes in the recorded scattering patterns due to the initial photoexcitation and subsequent deuterium dissociation. Ab initio calculations confirm that the observed signal is sensitive to the rearrangement of the single photoexcited valence electron as well as the interplay between adiabatic and nonadiabatic dissociation channels. The use of ultrafast hard x-ray scattering to image the structural rearrangement of single valence electrons constitutes an important advance in tracking valence electronic structure in photoexcited atoms and molecules.

Gabalski, Ian [SLAC National Accelerator Laborator↗
DOE OSTI2024

Differentiating Three-Dimensional Molecular Structures Using Laser-Induced Coulomb Explosion Imaging

Coulomb explosion imaging (CEI) with x-ray free electron lasers has recently been shown to be a powerful method for obtaining detailed structural information of gas-phase planar ring molecules [R. Boll et al., X-ray multiphoton-induced Coulomb explosion images complex single molecules, Nat. Phys. 18, 423 (2022).]. In this Letter, we investigate the potential of CEI driven by a tabletop laser and extend this approach to differentiating three-dimensional structures. We study the static CEI patterns of planar and nonplanar organic molecules that resemble the structures of typical products formed in ring-opening reactions. Here, our results reveal that each molecule exhibits a well-localized and distinctive pattern in three-dimensional fragment-ion momentum space. We find that these patterns yield direct information about the molecular structures and can be qualitatively reproduced using a classical Coulomb explosion simulation. Our findings suggest that laser-induced CEI can serve as a robust method for differentiating molecular structures of organic ring and chain molecules. As such, it holds great promise as a method for following ultrafast structural changes, e.g., during ring-opening reactions, by tracking the motion of individual atoms in pump-probe experiments.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Evolution of Thyroglobulin Loop Kinetics in EpCAM

Epithelial cell-activating molecule (EpCAM) is an important cancer biomarker and therapeutic target given its elevated expression in epithelial cancers. EpCAM is a type I transmembrane protein that forms cis-dimers along the thyroglobulin type-1A-like domain (TYD) in the extracellular region. The thyroglobulin loop (TY loop) within the TYD is structurally dynamic in the monomer state of human EpCAM, binding reversibly to a TYD site. However, it is not known if this flexibility is prevalent across different species. Here, we conduct over 17 μs of all-atom molecular dynamics simulations to study EpCAM TY loop kinetics of five different species, including human, mouse, chicken, frog, and fish. We find that the TY loop remains dynamic across evolution. In addition to the TYD binding site, we discover a second binding site for the TY loop in the C-terminal domain (CTD). Calculations of the dissociation rate constants from the simulation trajectories suggest a differential binding pattern of fish EpCAM and other organisms. Whereas fish TY loop has comparable binding for both TYD and CTD sites, the TY loops of other species preferably bind the TYD site. A hybrid construct of fish EpCAM with human TY loop restores the TYD binding preference, suggesting robust effects of the TY loop sequence on its dynamic behavior. Our findings provide insights into the structural dynamics of EpCAM and its implication in physiological functions.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2025

Surface deposition of nanometer scale carbon structures on Bi 2 Sr 2 CaCu 2 O 8+δ using a low-cost scanning electron microscope

In this work, we investigate optically active nanostructures on Bi 2 Sr 2 CaCu 2 O 8+δ (BSCCO). The nanostructures are constructed from carbon nanocrystals formed using the electron beam of a scanning electron microscope to locally decompose residual hydrocarbons at the BSCCO surface. Atomic force microscopy is used to characterize the dimensions of these structures as a function of beam exposure time. This technique has been used to induce localized intercalation to form carbon nanoparticles up to tens of nanometers into a variety of 2D materials. Cross-sectional scanning transmission electron microscopy in BSCCO shows the presence of these carbon deposits on the surface, but there is no evidence they penetrate into the BSCCO substrate. Therefore, this technique is not suitable for localized intercalation in BSCCO, and it does have promise as a cost-effective approach to pattern nanometer scale etch stops.

2D materials↗
DOE OSTI2021

Designing Anion-Exchange Ionomers with Oriented Nanoscale Phase Separation at a Silver Interface

We report performance of polymer electrolyte-based energy systems is significantly impacted by transport within the electrode catalyst layer, where ionomer thin films coat catalyst particles. Proton exchange ionomer thin films have been thoroughly characterized, but few studies have critically examined anion-exchange ionomer (AEI) thin films. Further, none have reported nanoscale phase separation for hydrocarbon AEIs, which is critical to mitigate transport resistances. In this work, a set of hydrocarbon-based AEIs with nanoscale phase separation are developed from tunable block copolymer systems composed of polyisoprene (PIp) and polychloromethylstyrene (PCMS). The effect of the PIp/PCMS ratio, architecture, and thickness on the thin-film morphology of the neutral block copolymer precursors on silicon and silver substrates is investigated using grazing-incidence small-angle X-ray scattering (GISAXS) and atomic force microscopy (AFM). AEIs are prepared by quaternizing with trimethylamine or methylpiperidine and their cation-dependent morphology is characterized at 60 °C and 95% RH. A perpendicularly aligned morphology is observed on silver, while no phase separation is observed on silicon, indicating that silver-polymer interfacial interactions drive phase separation. After quaternization, dipole-dipole interactions induce some disorder, but nanoscale phase separation is still maintained. GISAXS patterns are modeled using a Unified Fit approach to understand water uptake and swelling, and recommendations for AEI design are presented.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Nanoscale electrostatic control in ultraclean van der Waals heterostructures by local anodic oxidation of graphite gates

In an all-van der Waals heterostructure, the active layer, gate dielectrics and gate electrodes are assembled from two-dimensional crystals that have a low density of atomic defects. This design allows two-dimensional electron systems with very low disorder to be created, particularly in heterostructures where the active layer also has intrinsically low disorder, such as crystalline graphene layers or metal dichalcogenide heterobilayers. A key missing ingredient has been nanoscale electrostatic control, with existing methods for fabricated local gates typically introducing unwanted contamination. Here we describe a resist-free local anodic oxidation process for patterning sub-100 nm features in graphite gates, and their subsequent integration into an all-van der Waals heterostructure. We define a quantum point contact in the fractional quantum Hall regime as a benchmark device and observe signatures of chiral Luttinger liquid behaviour, indicating an absence of extrinsic scattering centres in the vicinity of the point contact. In the integer quantum Hall regime, we demonstrate in situ control of the edge confinement potential, a key requirement for the precision control of chiral edge states. In conclusion, this technique may enable the fabrication of devices capable of single anyon control and coherent edge-state interferometry in the fractional quantum Hall regime.

36 MATERIALS SCIENCE↗
NASA NTRS1982

Nitridation of Si(111) by nitrogen atoms. II

The reaction between Si(111) and nitrogen atoms has been investigated by LEED, Auger, and electron energy loss (ELS) techniques. The early stage of the reaction at 850-1050 C involves the formation of a chemically reacted monolayer which grows in islands. The sticking coefficient for the submonolayer is estimated to be of the order of unity. Two electronically different surface structures can be formed during these stages, yielding the '8 x 8' and the quadruplet LEED patterns; the quadruplet unit cell is the one with the highest nitrogen density. A pure quadruplet structure is obtained from samples with a carbon contamination of the Si monolayer of about 5 pct. During the multilayer stages, the influence of the substrate is not as important, and the reactions at 850 C and above produce quadruplet-like local structures.

Schrott, A. G.↗
NASA NTRS1998

Potential for EMU Fabric Damage by Electron Beam and Molten Metal During Space Welding for the International Space Welding Experiment

As a consequence of preparations concerning the International Space Welding Experiment (ISWE), studies were performed to better understand the effect of molten metal contact and electron beam impingement with various fabrics for space suit applications. The question arose as to what would occur if the electron beam from the Ukrainian Universal Hand Tool (UHT) designed for welding in space were to impinge upon a piece of Nextel AF-62 ceramic cloth designed to withstand temperatures up to 1427 C. The expectation was that the electron beam would lay down a static charge pattern with no damage to the ceramic fabric. The electron beam is capable of spraying the fabric with enough negative charge to repel further electrons from the fabric before significant heating occurs. The static charge pattern would deflect any further charge accumulation except for a small initial amount of leakage to the grounded surface of the welder. However, when studies were made of the effect of the electron beam on the insulating ceramic fabric it was surprisingly found that the electron beam did indeed burn through the ceramic fabric. It was also found that the shorter electron beam standoff distances had longer burnthrough times than did some greater electron beam standoff distances. A possible explanation for the longer burnthrough times for the small electron beam standoff distance would be outgassing of the fabric which caused the electron beam hand-tool to cycle on and off to provide some protection for the cathodes. The electron beam hand tool was observed to cycle off at the short standoff distance of two inches likely due to vapors being outgassed. During the electron beam welding process there is an electron leakage, or current leakage, flow from the fabric. A static charge pattern is initially laid down by the electron beam current flow. The static charge makes up the current leakage flow which initially slightly heats up the fabric. The initially laid down surface charge leaks a small amount of current. The rate at which the current charge leaks from the fabric controls how fast the fabric heats up. As the ceramic fabric is heated it begins to outgass primarily from contamination/impurities atoms or molecules on and below the fabric surface. The contaminant gases ionize to create extra charge carriers and multiply a current of electrons. The emitted gas which ionized in the electron leakage flow promotes further leakage. Thus, the small leakage of charge from the fabric surface is enhanced by outgassing. When the electron beam current makes up the lost current, the incoming electrons heat the fabric and further enhance the outgassing. The additional leakage promotes additional heating up of the ceramic fabric. The electrons bound to the ceramic fabric surface leak off more and more as the surface gets hotter promoting even greater leakage. The additional electrons that result also gain energy in the field and produce further electrons. Eventually the process becomes unstable and accelerates to the point where a hole is burned through the fabric.

Fragomeni, James M.↗
NASA NTRS2020

Global-scale distribution of ozone in the remote troposphere from ATom and HIPPO airborne field missions

Ozone is a key constituent of the troposphere, where it drives photochemical processes, impacts air quality, and acts as a climate forcer. Large-scale in situ observations of ozone commensurate with the grid resolution of current Earth system models are necessary to validate model outputs and satellite retrievals. In this paper, we examine measurements from the Atmospheric Tomography (ATom; four deployments in 2016–2018) and the HIAPER Pole-to-Pole Observations (HIPPO; five deployments in 2009–2011) experiments, two global-scale airborne campaigns covering the Pacific and Atlantic basins. ATom and HIPPO represent the first global-scale, vertically resolved measurements of O3 distributions throughout the troposphere, with HIPPO sampling the atmosphere over the Pacific and ATom sampling both the Pacific and Atlantic. Given the relatively limited temporal resolution of these two campaigns, we first compare ATom and HIPPO ozone data to longer-term observational records to establish the representativeness of our dataset. We show that these two airborne campaigns captured on average 53 %, 54 %, and 38 % of the ozone variability in the marine boundary layer, free troposphere, and upper troposphere–lower stratosphere (UTLS), respectively, at nine well-established ozonesonde sites. Additionally, ATom captured the most frequent ozone concentrations measured by regular commercial aircraft flights in the northern Atlantic UTLS. We then use the repeated vertical profiles from these two campaigns to confirm and extend the existing knowledge of tropospheric ozone spatial and vertical distributions throughout the remote troposphere. We highlight a clear hemispheric gradient, with greater ozone in the Northern Hemisphere, consistent with greater precursor emissions and consistent with previous modeling and satellite studies. We also show that the ozone distribution below 8 km was similar in the extra-tropics of the Atlantic and Pacific basins, likely due to zonal circulation patterns. However, twice as much ozone was found in the tropical Atlantic as in the tropical Pacific, due to well-documented dynamical patterns transporting continental air masses over the Atlantic. Finally, we show that the seasonal variability of tropospheric ozone over the Pacific and the Atlantic basins is driven year-round by transported continental plumes and photochemistry, and the vertical distribution is driven by photochemistry and mixing with stratospheric air. This new dataset provides additional constraints for global climate and chemistry models to improve our understanding of both ozone production and loss processes in remote regions, as well as the influence of anthropogenic emissions on baseline ozone.

ATom, aircraft profiles, Atlantic pollution, ozone↗
DOE OSTI2022

Importance of imposing gauge invariance in time-dependent density functional theory calculations with meta-generalized gradient approximations

It has been known for more than a decade that the gauge variance of the kinetic energy density τ leads to additional terms in the magnetic orbital rotation Hessian used in linear-response time-dependent density functional theory (TDDFT), affecting excitation energies obtained with τ-dependent exchange–correlation functionals. While previous investigations found that a correction scheme based on the paramagnetic current density has a small effect on benchmark results, we report more pronounced effects here, in particular, for the popular M06-2X functional and for some other meta-generalized gradient approximations (mGGAs). In the first part of this communication, this is shown by a reassessment of a set of five Ni(II) complexes for which a previous benchmark study that did not impose gauge invariance has found surprisingly large errors for excitation energies obtained with M06-2X. These errors are more than halved by restoring gauge invariance. The variable importance of imposing gauge invariance for different mGGA-based functionals can be rationalized by the derivative of the mGGA exchange energy integrand with respect to τ. In the second part, a large set of valence excitations in small main-group molecules is analyzed. For M06-2X, several selected n → π* and π→π$^{*}_{⊥}$ excitations are heavily gauge-dependent with average changes of –0.17 and –0.28 eV, respectively, while π→π$^{*}_{∥}$ excitations are marginally affected (–0.04 eV). Similar patterns, but of the opposite signs, are found for SCAN0. Here, the results suggest that reevaluation of previous gauge variant TDDFT results based on M06-2X and other mGGA functionals is warranted.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Pair distribution function analysis of nano-object assemblies

The atomic pair distribution function (aPDF) analysis technique, also known as the total scattering method, which considers both Bragg and diffuse scattering, has been used extensively to probe local atomic arrangements in crystalline and disordered materials. In contrast, there have been limited applications of the PDF in self-assembled nanomaterials, which represent a class of materials built from nanoscale objects, such as nano-colloids, micelles and proteins. As distinguished from atoms, nano-objects have polydispersity in size and shape, and such form-factor effects complicate the application of PDF analysis to nano-systems. Here, in this paper, the application of the PDF is extended to spherical nano-object assemblies and the formulae for the nano-PDF (nPDF) are derived, showing some differences from the aPDF. By numerical simulations, the properties of the nPDF (peak broadening and pattern profile) are studied systematically as a function of structural features, such as nano-object parameters (size and size polydispersity) and assembly structural features (size, shape, structure type and lattice disorder), and of data processing parameters ( q cut-off and `missing' data in ultra-small-angle regions). The nPDF analysis method is found to provide an effective route to revealing not only nanoscale but also mesoscale structural properties, for example the morphology of a nano-assembly.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2026

The Focus of an Ultraintense Laser Pulse

Back in 1885, von Lommel studied the diffraction of a circular opening. His study was one step further than the Airy diffraction model (describing patterns in the focal plane) because von Lommel’s model was able to describe what the light distribution before and after the focus is. Today’s extreme lasers have a flat-top profile whose diffraction pattern in the vicinity of the focus is very much reminiscent of von Lommel’s description. In the present Chapter, we will compute, based on a Huygens-Fresnel integral method, the laser field distribution around the focus. This modelling is particularly important because the intensity distribution before and after the focal plane (where the Airy disk exists) is very relevant to many contemporary experiments, and is key to the ionization of atoms and the dynamics of liberated electrons. For clarity, we are going to analyze three cases corresponding to three f-numbers: f/10, f/1.8, and f/1.1. Our computed results reveal the present-day significance of von Lommel’s pioneering results. Here, they help us understand the light distribution in the entire focal region of an ultraintense laser pulse including the full vectorial fields, not just the focal plane.

Roso, Luis [Universidad de Salamanca (Spain)]↗
DOE OSTI2024

Flash healing of laser-induced graphene

The advancement of laser-induced graphene (LIG) technology has streamlined the fabrications of flexible graphene devices. However, the ultrafast kinetics triggered by laser irradiation generates intrinsic amorphous characteristics, leading to high resistivity and compromised performance in electronic devices. Healing graphene defects in specific patterns is technologically challenging by conventional methods. Herein, we report the rapid rectification of LIG’s topological defects by flash Joule heating in milliseconds (referred to as F-LIG), whilst preserving its overall structure and porosity. The F-LIG exhibits a decreased I D /I G ratio from 0.84 – 0.33 and increased crystalline domain from Raman analysis, coupled with a 5-fold surge in conductivity. Pair distribution function and atomic-resolution imaging delineate a broader-range order of F-LIG with a shorter C-C bond of 1.425 Å. The improved crystallinity and conductivity of F-LIG with excellent flexibility enables its utilization in high-performance soft electronics and low-voltage disinfections. Notably, our F-LIG/polydimethylsiloxane strain sensor exhibits a gauge factor of 129.3 within 10% strain, which outperforms pristine LIG by 800%, showcasing significant potential for human-machine interfaces.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Stability of the peroxide group in BaO 2 under high pressure

Alkaline earth metal peroxides are typical examples of ionic compounds containing polyanions. We herein report a stable BaO 2 phase at high pressure up to 130 GPa found via a first-principles computational structure searches and high-pressure experimental investigations. The identified monoclinic structure (space group C2/m) can be derived by sublattice distortions of Ba atoms and peroxide groups associated with the phonon mode softening of the lower-pressure Cmmm structure. Contrary to the previous expectation of polymerization of the peroxide group at elevated pressure, the new phase retains the peroxide group and interestingly exhibits an insulating behavior demonstrating an increase of the band gap under compression. Our synchrotron XRD measurements could not distinguish between Cmmm and C2/m BaO 2 definitively because the difference in XRD patterns is very subtle. However, our data do not show any sign of polymerization transition up to 120 GPa. Raman spectra of the O-O peroxide vibration show a small anomaly in frequency at 110 GPa, which is qualitatively similar to that predicted theoretically due to the Cmmm to C2/m phase transition thus supporting the predicted transformation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Self referencing attosecond interferometer with zeptosecond precision

In this work we demonstrate the generation of two intense, ultrafast laser pulses that allow a controlled interferometric measurement of higher harmonic generation pulses with 12.8 attoseconds in resolution (half the atomic unit of time) and a precision as low as 680 zeptoseconds (10–21 seconds). We create two replicas of a driving femtosecond pulse which share the same optical path except at the focus where they converge to two foci. An attosecond pulse train emerges from each focus through the process of high harmonic generation. The two attosecond pulse trains from each focus interfere in the far field producing a clear interference pattern in the extreme ultraviolet region. By controlling the relative optical phase (carrier envelope phase for pulsed fields) between the two driving laser pulses we are able to actively influence the delay between the pulses and are able to perform very stable and precise pump-probe experiments. Because of the phase shaping operation occurs homogeneously across the entire spatial profile, we effectively create two indistinguishable intense laser pulses or a common path interferometer for attosecond pulses. Commonality across the two beams means that they are extremely stable to environmental and mechanical fluctuations up to a Rayleigh range from the focus. In our opinion this represents an ideal source for homodyne and heterodyne spectroscopic measurements with sub-attosecond precision.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1976

Tropical F region winds from O I 1356-A and forbidden OI 6300-A emissions. I - Theory

The paper theoretically investigates the relationship of neutral winds and E x B plasma drifts to the time-dependent distribution of 1356-A and 6300-A airglow intensities in the region of the Appleton anomaly. Radiative recombination, ion-ion neutralization, and dissociative recombination are considered as main mechanisms in producing the atomic oxygen tropical nightglow. A quantitative relation is determined between the neutral wind velocities and the resultant asymmetry in the emissions about the dip equator. The height difference at northern and southern conjugate points is shown to be linearly related to the vector sum of the wind velocity components along the magnetic meridian at the latitude of the conjugate points. The height difference at conjugate points may be used to study the pattern of neutral wind velocities in the tropical ionosphere.

Bittencourt, J. A.↗
NASA NTRS1992

Atomic oxygen in the Martian thermosphere

The Mariner 9 Ultraviolet Spectrometer (UVS) made extensive observations of air-glow emissions from the thermosphere of Mars throughout the nominal mission (November 1971 - February 1972), during late summer in the southern hemisphere. Limb and disc measurements of the 130 nm triplet emission from thermospheric atomic oxygen were modelled by Strickland et al. Recently, the thermospheric general circulation models (TGCMs) developed for the Earth and Venus have been applied to Mars; we refer to it as the MTGCM. Our analysis shows that the oxygen mixing ratio is the fundamental unknown controlling the 130 nm brightness. Our radiative transport calculation shows that the emergent intensity at 130 nm is not very sensitive to variations in thermospheric temperature. The pattern of diurnal variation derived from our analysis is roughly the same as Strickland et al. although with somewhat lower values for the O mixing ratio. The main reasons for this difference are the more important role played by the photoelectron source in our model, and the somewhat larger 130 nm solar flux; thus, we require less oxygen to match the observed brightnesses. Strickland et al. also found that the OI 130 nm emission on Mars is correlated with solar activity. We find that the correlation is virtually non-existent during the early orbits when the planet was covered with a thick global dust storm, but later orbits, during the clearing of the storm, show a persistent correlation.

Stewart, A. I. F.↗
DOE OSTI2019

Molecular Dynamics Simulation Study of Uniaxial Ratcheting Behaviors for Ultrafine-Grained Nanocrystalline Nickel

In this paper, molecular dynamics (MD) simulation-based study of deformation behavior of ultrafine-grained nanocrystalline nickel under asymmetric cyclic loading having stress ratios (R) such as − 0.2, − 0.4 and − 0.6 for different temperatures, viz. 100, 300 and 500 K, has been performed using embedded atom method potential. The predicted ratcheting strain by MD simulation for nanocrystalline Ni varies from 15 to 30%. A significant increase in ratcheting strain has been observed with the increase in temperature. It has been observed that the number of vacancies increases, and the number of clusters decreases with the increase in temperature. Slight reduction in crystallinity is identified at the middle of the each loading cycle from the performed cluster analysis. Zigzag pattern of dislocation density has been observed and leads to the decrease in dislocation density with the increase in temperature. Stress ratio does not show any significant effect on the number of vacancies, clusters and dislocation density on structural evolution during the asymmetric cyclic loading. Slight change in the grain rotation has been observed with the increase in temperature, and there is almost no change in the final texture evolved. From the post-tensile tests, ultimate tensile strength that remains same may be due to constant average dislocation density.

36 MATERIALS SCIENCE↗