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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 1,279 records · Page 71
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Electron Spin-Polarization Dependent Damage to Chiral Amino Acid l-Histidine

The damage of approximately monolayer films of L-histidine by low-energy spin-polarized electrons (SPE) ejected from a magnetized cobalt substrate has been probed using X-ray photoelectron spectroscopy (XPS). Average damage cross sections for N-containing motifs of L-histidine are 25-30 and 2-5 Mb for zwitterions and neutral molecules, respectively. Here, the magnetization direction of the substrate, which controls the ejected SPE helicity, was reversed in situ, and statistically significant differences in the damage cross sections of 10-30% were measured between positive and negative electron helicities. This is the first measurement of spin dichroism (SD) in an amino acid. The differential cross sections suggest that inelastic scattering of SPE with chiral molecules could contribute to the persistence of one enantiomer vs the other under certain irradiation conditions, particularly for the zwitterionic species.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Lattice Strain Measurement of Core@Shell Electrocatalysts with 4D Scanning Transmission Electron Microscopy Nanobeam Electron Diffraction

Strain engineering enables the direct modification of atomic bonding and is currently an active area of research aimed at improving electrocatalytic activity. However, directly measuring the lattice strain of individual catalyst nanoparticles is challenging, especially at the scale of a single unit cell. In this study, we quantitatively map the strain present in rhodium@platinum (core@shell) nanocube electrocatalysts using conventional aberration-corrected scanning transmission electron microscopy (STEM) and the recently developed technique of 4D-STEM nanobeam electron diffraction. We demonstrate that 4D-STEM combined with data preconditioning allows for quantitative lattice strain mapping with subpicometer precision and without the influence of scan distortions. When combined with multivariate curve resolution, 4D-STEM allows us to distinguish the nanocube core from the shell and to quantify the unit cell size as a function of distance from the core–shell interface. Our results demonstrate that 4D-STEM has significant precision and accuracy advantages in strain metrology of catalyst materials compared to aberration-corrected STEM imaging and is beneficial for extracting information about the evolution of strain in catalyst nanoparticles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Structural Characterization of Loblolly Pine Derived Biochar by X-ray Diffraction and Electron Energy Loss Spectroscopy

Biochar from lignocellulosic biomass is emerging as a sustainable material with versatile applications, but its detailed properties are poorly understood because of its structural complexity. We propose a biochar structural development model based on experimental results including composition analysis, surface area and pore analysis, X-ray diffraction analysis, electron microscopy imaging, and electron energy loss spectroscopy. Loblolly pine derived biochars were produced at different carbonization temperatures between 300 to 1000 °C. Fixed carbon, sp 2 content, and number of graphene layers increased with increased carbonization temperature. Alternating average C–C bond length, interlayer spacing distance, and layer coherence length were observed. Bulk plasmon excitation energy was correlated to the average C–C bond length, and it serves as a good indicator of the carbon structure development when compared to the perfect graphitic carbon structure. On the basis of the experimental results, four different structural development phases are identified, which provide a comprehensive understanding of biochar nanocarbon crystallite development. Unlike previous biochar structure models, which proposed radially growing polyaromatic carbon crystallite, we propose a lengthwise growing polyaromatic carbon crystallite model. Furthermore, this experiment-based biochar model should be helpful when determining the structure of unknown biomass-derived carbon materials and disordered pyrolytic carbon materials.

Biomass carbonization↗
DOE OSTI2020

Phase Transitions in Metal–Organic Frameworks Directly Monitored through In Situ Variable Temperature Liquid-Cell Transmission Electron Microscopy and In Situ X-ray Diffraction

Zr 6 -based metal–organic frameworks (MOFs) with tetratopic organic linkers have been extensively investigated owing to their versatile structural tunability. While diverse topologies and polymorphism in the resulting MOFs are often encountered with tetratopic linkers and Zr 6 nodes, reports on phase transitions within these systems are rare. Thus, we have a limited understanding of polymorph transformations, hindering the rational development of pure phase materials. In this study, a phase transition from a microporous MOF, scu-NU-906, to a mesoporous MOF, csq-NU-1008, was discovered and monitored through in situ variable temperature liquid-cell transmission electron microscopy (VT-LCTEM), high-resolution transmission electron microscopy (HRTEM), and in situ variable temperature powder X-ray diffraction (VT-PXRD). Furthermore, it was found that the microporous- to-mesoporous transformation in the presence of formic acid occurs via a concomitant dissolution–reprecipitation process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Femtosecond X-ray induced changes of the electronic and magnetic response of solids from electron redistribution

Resonant X-ray absorption, where an X-ray photon excites a core electron into an unoccupied valence state, is an essential process in many standard X-ray spectroscopies. With increasing X-ray intensity, the X-ray absorption strength is expected to become nonlinear. Here we report the onset of such a nonlinearity in the resonant X-ray absorption of magnetic Co/Pd multilayers near the Co L 3 edge. The nonlinearity is directly observed through the change of the absorption spectrum, which is modified in less than 40 fs within 2 eV of its threshold. This is interpreted as a redistribution of valence electrons near the Fermi level. For our magnetic sample this also involves mixing of majority and minority spins, due to sample demagnetization. Our findings reveal that nonlinear X-ray responses of materials may already occur at relatively low intensities, where the macroscopic sample is not destroyed, providing insight into ultrafast charge and spin dynamics.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Importance of proton-coupled electron transfer in cathodic regeneration of organic hydrides

Electrochemical regeneration of organic hydrides is often hindered by the rapid dimerization of organic radicals produced as the first intermediates of these electrochemical transformations. Here, we utilize proton-coupled electron transfer to outcompete the undesired dimerization and achieve successful hydride regenerations of two groups of organic hydrides – acridines and benzimidazoles. An analysis of the critical factors that control the regeneration pathways of organic hydrides is demonstrated in this report.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2012

Structural, magnetic, and electron transport properties of MnBi:Fe thin films

The structural, magnetic, and electron transport properties of Mn{sub 55-x}Fe{sub x}Bi{sub 45} (x = 0, 2, 4, 5, 8, 11, 13, 16) films prepared by multilayer deposition and annealing using e-beam evaporation have been investigated. Fe doping has produced a significant change in the magnetic properties of the samples including the decrease in saturation magnetization and magnetocrystalline anisotropy and increase in coercivity. Although the magnetization shows a smooth decrease with increasing Fe concentration, the coercivity jumps abruptly from 8.5 kOe to 22 kOe as Fe content changes from 4% to 5%, but the change in coercivity is small as the concentration goes beyond 5%. The temperature dependence of resistivity shows that the samples with low Fe concentration ({<=}4%) are metallic, but the resistivity increases unexpectedly as the concentration reaches 5%, where the resistance increases with decreasing temperature below 300 K. First-principle calculations suggest that the observed magnetic properties can be understood as the consequences of competing ferromagnetic and antiferromagnetic exchange interactions between the interstitial atom and the rest of the MnBi lattice.

36 MATERIALS SCIENCE↗
DOE OSTI2012

Three-Dimensional Quantitative Chemical Roughness Of Buried ZrO2/In2O3 Interfaces Via Energy-Filtered Electron Tomography

The protocol to calculate the chemical roughness from three-dimensional (3-D) data cube acquired by energy-filtered electron tomography has been developed and applied to analyze the 3-D Zr distribution at the arbitrarily shaped interfaces in the ZrO2/In2O3 multilayer films. The calculated root-mean-square roughness quantitatively revealed the chemical roughness at the buried ZrO2/In2O3 interfaces, which is the deviation of Zr distribution from the ideal flat interface. Knowledge of the chemistry and structure of oxide interfaces in 3-D provides information useful for understanding changes in the behavior of a model ZrO2/In2O3 heterostructure that has potential to exhibit mixed conduction behavior. VC 2012 American Institute of Physics.

Zhong, X Y↗
DOE OSTI2013

Rigid-body rotation of an electron cloud in divergent magnetic fields

For a given voltage across a divergent poloidal magnetic field, two electric potential distributions, each supported by a rigid-rotor electron cloud rotating with a different frequency, are found analytically. The two rotation frequencies correspond to the slow and fast rotation frequencies known in uniform plasma. Due to the centrifugal force, the equipotential surfaces, that correspond to the two electric potential distributions, diverge more than the magnetic surfaces do, the equipotential surfaces in the fast mode diverge largely in particular. The departure of the equipotential surfaces from the magnetic field surfaces may have a significant focusing effect on the ions accelerated by the electric field. The focusing effect could be important for laboratory plasma accelerators as well as for collimation of astrophysical jets.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2013

Constrained γZ correction to parity-violating electron scattering

We update the calculation of γZ interference corrections to the weak charge of the proton. We show how constraints from parton distributions, together with new data on parity-violating electron scattering in the resonance region, significantly reduce the uncertainties on the corrections compared to previous estimates.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2013

GaInN light-emitting diodes using separate epitaxial growth for the p-type region to attain polarization-inverted electron-blocking layer, reduced electron leakage, and improved hole injection

A GaInN light-emitting diode (LED) structure is analyzed that employs a separate epitaxial growth for the p-type region, i.e., the AlGaN electron-blocking layer (EBL) and p-type GaN cladding layer, followed by wafer or chip bonding. Such LED structure has a polarization-inverted EBL and allows for uncompromised epitaxial-growth optimization of the p-type region, i.e., without the need to consider degradation of the quantum-well active region during p-type region growth. Simulations show that such an LED structure reduces electron leakage, reduces the efficiency droop, improves hole injection, and has the potential to extend high efficiencies into the green spectral region.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2013

Determination of the individual atomic site contribution to the electronic structure of 3,4,9,10-perylene-tetracarboxylic-dianhydride (PTCDA)

We have studied the element and orbital-specific electronic structure of thin films of 3,4,9,10-perylene-tetracarboxylic-dianhydride (PTCDA) using a combination of synchrotron radiation-exited resonant x-ray emission spectroscopy, x-ray absorption spectroscopy, x-ray photoelectron spectroscopy, as well as density functional theory calculations. Resonant and non-resonant x-ray emission spectroscopies were used to measure the C and O 2p partial densities of state in PTCDA. Furthermore, resonant x-ray emission at the C and O K-edges is shown to be able to measure the partial densities of states associated with individual atomic sites. The flat molecular orientation of PTCDA on various substrates is explained in terms of the carbonyl O atom acting as a hydrogen-bond acceptor leading to multiple in-plane intermolecular C=O···H−C hydrogen bonding between carbonyl groups and the perylene core of the neighboring PTCDA molecules. We support this conclusion by comparison of our calculations to measurements of the electronic structure using element-, site-, and orbital-selective C and O K-edge resonant x-ray emission spectroscopy, and photoemission spectroscopy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Electronic structure, magnetic properties, and magnetostructural transformations in rare earth dialuminides

We report electronic structure, magnetic properties, and magnetostructural transformations of selected rare earth dialuminides calculated by using local spin density approximation (LSDA), including the Hubbard U parameter (LSDA + U) approach. Total energy calculations show that CeAl{sub 2} and EuAl{sub 2} adopt antiferromagnetic (AFM) ground states, while dialuminides formed by other magnetic lanthanides have ferromagnetic (FM) ground states. The comparison of theoretical and experimental magnetic moments of CeAl{sub 2} indicates that the 4f orbital moment of Ce in CeAl{sub 2} is quenched. Theoretical calculations confirm that Eu in EuAl{sub 2} and Yb in YbAl{sub 2} are divalent. PrAl{sub 2} exhibits a tetragonal distortion near FM transition. HoAl{sub 2} shows a first order magnetostructural transition while DyAl{sub 2} shows a second order transformation below magnetic transition. The dialuminides formed by Nd, Tb, and Er are simple ferromagnets without additional anomalies in the FM state.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Gas mixing system for imaging of nanomaterials under dynamic environments by environmental transmission electron microscopy

A gas mixing manifold system that is capable of delivering a stable pressure stream of a desired composition of gases into an environmental transmission electron microscope has been developed. The system is designed to provide a stable imaging environment upon changes of either the composition of the gas mixture or upon switching from one gas to another. The design of the system is described and the response of the pressure inside the microscope, the sample temperature, and sample drift in response to flow and composition changes of the system are reported.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2014

Computing the reconnection rate in turbulent kinetic layers by using electron mixing to identify topology

Three-dimensional kinetic simulations of magnetic reconnection for parameter regimes relevant to the magnetopause current layer feature the development of turbulence, driven by the magnetic and velocity shear, and dominated by coherent structures including flux ropes, current sheets, and flow vortices. Here, we propose a new approach for computing the global reconnection rate in the presence of this complexity. The mixing of electrons originating from separate sides of the magnetopause layer is used as a proxy to rapidly identify the magnetic topology and track the evolution of magnetic flux. The details of this method are illustrated for an asymmetric current layer relevant to the subsolar magnetopause and for a flow shear dominated layer relevant to the lower latitude magnetopause. While the three-dimensional reconnection rates show a number of interesting differences relative to the corresponding two-dimensional simulations, the time scale for the energy conversion remains very similar. These results suggest that the mixing of field lines between topologies is more easily influenced by kinetic turbulence than the physics responsible for the energy conversion.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2014

Electron-stimulated reactions in layered CO/H{sub 2}O films: Hydrogen atom diffusion and the sequential hydrogenation of CO to methanol

Low-energy (100 eV) electron-stimulated reactions in layered H{sub 2}O/CO/H{sub 2}O ices are investigated. For CO layers buried in amorphous solid water (ASW) films at depths of 50 monolayers (ML) or less from the vacuum interface, both oxidation and reduction reactions are observed. However, for CO buried more deeply in ASW films, only the reduction of CO to methanol is observed. Experiments with layered films of H{sub 2}O and D{sub 2}O show that the hydrogen atoms participating in the reduction of the buried CO originate in the region that is 10–50 ML below the surface of the ASW films and subsequently diffuse through the film. For deeply buried CO layers, the CO reduction reactions quickly increase with temperature above ∼60 K. We present a simple chemical kinetic model that treats the diffusion of hydrogen atoms in the ASW and sequential hydrogenation of the CO to methanol to account for the observations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗