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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 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Infrared Microscopy as a Probe of Composition within a Model Biofuel Cell Electrode Prepared from Trametes versicolor Laccase

Abstract Infrared microscopy was applied in the study of laccase biofuel cell electrodes that demonstrated high current and power densities traceable to the use of a low equivalent weight (EW), short side chain (Aquivion) ionomer in the catalyst layer. The electrodes were prepared from a biocatalyst ink composed of orientation‐directing anthracene‐modified multi‐walled carbon nanotubes (An‐MWCNTs) in a dispersion of ionomer exchanged by hydrophobic cations. The ink was applied to an electronically conductive carbon felt support that was hot‐pressed to a Nafion‐NRE 212 (51 μm thickness) membrane, forming the framework for an air‐breathing biofuel cell cathode. Infrared microscopy sampling was performed with the use of a micro‐attenuated total reflection probe that enabled spectra to be recorded from ∼32 μm diameter circular spatial regions on the materials investigated. Sensitivity to deformation of the soft polymer membrane‐based materials was assessed through trial experiments on pure membrane samples before approaching the compositionally more complex biofuel cell electrodes. In studies of laccase cathodes, infrared spectral features of enzyme, buffer anions and surrounding An‐MWCNTs were identified. Heterogeneity in the spatial distribution of components and unexpected bands traceable to insoluble copper salts were detected. The results suggest directions for improving electrode activity and bring to light needs for advancing quantitative interpretations.

Liang, Ying↗
DOE OSTI2019

Probing Molecular Chirality by Orbital-Angular-Momentum-Carrying X-ray Pulses

A twisted X-ray beam with orbital angular momentum is employed in a theoretical study to probe molecular chirality. A nonlocal response description of the matter-field coupling is adopted to account for the field short wavelength and the structured spatial profile. In this study, we use the minimal-coupling Hamiltonian, which implicitly takes into account the multipole contributions to all orders. The combined interactions of the spin and orbital angular momentum of the X-ray beam give rise to circular-helical dichroism signals, which are stronger than ordinary circular dichroism signals, and may serve as a useful tool for the study of molecular chirality in the X-ray regime.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2018

Orientational Pair Correlations in a Dipolar Molecular Liquid: Time-Resolved Resonant and Nonresonant Pump–Probe Spectroscopies

Orientational pair correlations (OPCs), when they are sufficiently strong in a liquid, contain information on the interplay between structure and dynamics that arise from intermolecular interactions. Consequently, the quantification of OPCs remains a subject of substantial interest in current experimental and theoretical work. In the case of benzonitrile, the importance of OPCs remains ambiguous owing to the use of model-dependent analyses or reliance on a single spectroscopic technique. In this work, IR polarization selective pump-probe (PSPP) and optical heterodyne-detected optical Kerr effect (OHD-OKE) experiments were used to quantify OPCs in benzonitrile. These methods measure single molecule and collective relaxation, respectively. Comparison of the orientational correlation function (PSPP) of the naturally abundant 13CN stretching mode and the polarizability anisotropy relaxation (OHD-OKE) of the liquid revealed that collective reorientation was a factor of 1.56 ± 0.08 slower than the single molecule reorientation time. The two types of measurements on dilute benzonitrile in carbon tetrachloride were the same within experimental error. These results support the proposition that OPCs exist and arise from the formation of parallel-aligned intermolecular structures in the neat liquid.

14 SOLAR ENERGY↗
DOE OSTI2019

Reductive Dissolution Mechanisms at the Hematite-Electrolyte Interface Probed by In Situ X-ray Scattering

The electron-catalyzed dissolution and reprecipitation of iron (oxyhydr)oxides constitute critical steps in natural geochemical iron cycling. However, the atomic-scale mechanisms of reductive dissolution and oxidative precipitation of Fe2+ remain poorly understood because they are difficult to directly experimentally probe. Using in situ synchrotron X-ray scattering and a novel electrochemical cell, we interrogate the interfacial structure between the hematite (?-Fe2O3) (11 ¯02) surface and acidic aqueous solution (5 mM Na2SO4, pH 4.0) under controlled electrochemical potential from open circuit to cathodic bias as the reductive dissolution potential is approached and then exceeded. The crystalline order of the surface improves under mild reducing conditions, and the surface Fe stoichiometry changes with cathodic bias. After significant reductive dissolution occurs and cathodic bias is removed, dissolved Fe is re-deposited, forming a disordered interface. Unlike at circumneutral pH, water layers at the hematite interface with acidic solution are poorly ordered, likely due to the adsorption of sulfate from the electrolyte. These results provide a novel atomic-scale view into the behavior of reducible transition metal oxide surfaces under fluctuating (electro)chemical conditions.

McBriarty, Martin E.↗
DOE OSTI2022

Kinetic Probes of the Origin of Activity in MOF-Based C–H Oxidation Catalysis

The development of homogeneous catalysis is enabled by the availability of a rich toolkit of kinetics experiments, such as the Hgdrop test, that differentiate catalytic activity at ligand-supported metal complexes from potential heterogeneous catalysts derived from decomposition of molecular species. Metal-organic frameworks (MOFs) have garnered significant attention as platforms for catalysis at site-isolated, interstitial catalyst sites. Unlike homogeneous catalysis, relatively few strategies have been advanced to evaluate the origin of catalytic activity in MOF-promoted reactions. Many of the MOFs that have been examined as potential catalysts are comprised of molecular constituents that represent viable catalysts in the absence of the extended MOF lattice, and thus interfacial sites and leached homogeneous species represent potential sources of catalyst activity. Here, we demonstrate that analysis of deuterium kinetic isotope effects (KIEs) and olefin epoxidation diastereoselectivity provides probes of the origin of catalytic activity in MOF-promoted oxidation reactions. These analyses support involvement of lattice-based Fe sites in the turnover-limiting step of C–H activation with Fe-MOF-74-based materials (i.e., the MOF functions as a bona fide catalyst) and evidence that Cu 2 -based MOF MIL-125-Cu 2 O 2 functions as a solid-state initiator for solution-phase oxidation chemistry and is not involved in the turnover limiting step (i.e., the MOF does not function as a catalyst for substrate functionalization). furthermore, we anticipate that the simple experiments described here will provide a valuable tool for clarifying the role of MOFs in C–H oxidation reactions.

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

Probing Enhanced Site Activity of Co–Fe Bimetallic Subnanoclusters Derived from Dual Cross-Linked Hydrogels for Oxygen Electrocatalysis

Great efforts have been devoted to unveiling structural contributions of transition heterometallic materials to enhanced catalysis, while effective in situ approaches are still urgently demanded to probe the intrinsic activity on individual electrolyte-accessible sites. Here, we report cobalt–iron subnanoclusters (CoFe-PPy) incorporated on nitrogen-rich nanotubular carbon from dual cross-linked polypyrrole hydrogels. The bimetallic catalyst exhibits obviously improved oxygen electrocatalysis largely attributed to the electronic interaction between cobalt and iron at the atomic scale. Furthermore, the site information and catalytic kinetics of CoFe-PPy were in situ quantified by a surface-interrogation scanning electrochemical microscopy (SI-SECM) technique. Consequently, CoFe-PPy not only provides higher active site density but also achieves rapid kinetics to activate O 2 , greatly promoting the oxygen electroreduction turnover frequency compared with monometallic catalysts. Lastly, our work offers an opportunity to investigate important catalytic parameters of bimetallic electrocatalysis and highlights the heterometallic interaction at the subnanometer scale to promote enhanced electrocatalytic reactivity.

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

Space- and time-resolved small angle X-ray scattering to probe assembly of silver nanocrystal superlattices

Abstract The structure of nanocrystal superlattices has been extensively studied and well documented, however, their assembly process is poorly understood. In this work, we demonstrate an in situ space- and time-resolved small angle X-ray scattering measurement that we use to probe the assembly of silver nanocrystal superlattices driven by electric fields. The electric field creates a nanocrystal flux to the surface, providing a systematic means to vary the nanocrystal concentration near the electrode and thereby to initiate nucleation and growth of superlattices in several minutes. Using this approach, we measure the space- and time-resolved concentration and polydispersity gradients during deposition and show how they affect the superlattice constant and degree of order. We find that the field induces a size-selection effect that can reduce the polydispersity near the substrate by 21% leading to better quality crystals and resulting in field strength-dependent superlattice lattice constants.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Probing squeezed bino-slepton spectra with the Large Hadron Collider

In this study, we consider a minimal supersymmetric Standard Model scenario in which the only light superparticles are a binolike dark matter candidate and a nearly degenerate slepton. It is notoriously difficult to probe this scenario at the Large Hadron Collider (LHC), because the slepton pair-production process yields a final state with soft leptons and small missing transverse energy. We study this scenario in the region of parameter space where the mass difference between the lightest neutralino and the lightest slepton ( Δ m ) is ≲ 60 GeV , focusing on the process in which an additional radiated jet provides a transverse boost to the slepton pair. We then utilize the angular separation of the leptons from each other and from the missing transverse energy, as well as the angular separation between the jet and the missing transverse energy, to distinguish signal from background events. We also use the reconstructed ditau mass, the cos θ ℓ 1 ℓ 2 * variable, and for larger Δ m , a lower bound on the lepton p T . These cuts can dramatically improve both signal sensitivity and the signal-to-background ratio, permitting discovery at the LHC with reasonable integrated luminosity over the interesting region of parameter space. Using our search strategy the LHC will be able to exclude m μ ˜ ≈ 200 GeV for Δ m ≲ 60 GeV at 1.5 – 3 σ with 1000 fb - 1 of integrated luminosity. Although we focus on a particular model, the results generalize to a variety of scenarios in which the dark matter and a leptonic partner are nearly degenerate in mass, and especially to scenarios featuring a scalar mediator.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2018

Simulations of the Ion Current to a Probe in Plasma with Allowance for Ionization and Ion–Neutral Collisions: II. Cylindrical Probe

The ion current to a cylindrical probe is considered with allowance for volume ionization, ion–neutral collisions, and the ion orbital moment. A model based on the molecular dynamics method and applicable in a wide range of plasma parameters (r{sub p}/λ{sub D}= 0.01–100, r{sub i}/λ{sub D}= 0.002–200, ν{sub i}/ω{sub 0i}= 0.01–0.05, and T{sub i}/T{sub e} = 0−0.01) is proposed A convenient representation of the dependence of the relative ion current density on the Langmuir coefficient β{sup 2} and a technique for determining the plasma density from simulation results are offered.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Multi-probe meeting with Harwell II: A discussion of potential areas of cooperation for mutual benefit by the LANL Multi-probe Radiography team [Slides]

In this presentation, we continue a discussion begun in September 2023, with staff from the University of Manchester and the Central Laser Facility-Harwell in the UK exploring the possibilities for cooperative work of mutual interest in the technology underpinning petawatt laser driven Multi-Probe radiography. Since the September Seminar, the US and UK staff have exchanged lists of ideas for possible cooperation and this presentation comprises brief descriptions of five topics that LANL staff would offer for consideration in the area of laser driven radiation sources, applications of machine learning and experiments at Omega (in the US) and Gemini (in the UK).

62 RADIOLOGY AND NUCLEAR MEDICINE↗
NASA NTRS1988

Galileo probe parachute test program: Wake properties of the Galileo probe at Mach numbers from 0.25 to 0.95

The results of surveys of the near and far wake of the Galileo Probe are presented for Mach numbers from 0.25 tp 0.95. The trends in the data resulting from changes in Mach number, radial and axial distance, angle of attack, and a small change in model shape are shown in crossplots based on the data. A rationale for selecting an operating volume suitable for parachute inflation based on low Mach number flight results is outlined.

Canning, Thomas N.↗
NASA NTRS2010

Monolithically Integrated, Mechanically Resilient Carbon-Based Probes for Scanning Probe Microscopy

Scanning probe microscopy (SPM) is an important tool for performing measurements at the nanoscale in imaging bacteria or proteins in biology, as well as in the electronics industry. An essential element of SPM is a sharp, stable tip that possesses a small radius of curvature to enhance spatial resolution. Existing techniques for forming such tips are not ideal. High-aspect-ratio, monolithically integrated, as-grown carbon nanofibers (CNFs) have been formed that show promise for SPM applications by overcoming the limitations present in wet chemical and separate substrate etching processes.

Kaul, Anupama B.↗
NASA NTRS2008

The Experimental Probe of Inflationary Cosmology: A Mission Concept Study for NASA's Einstein Inflation Probe

When we began our study we sought to answer five fundamental implementation questions: 1) can foregrounds be measured and subtracted to a sufficiently low level?; 2) can systematic errors be controlled?; 3) can we develop optics with sufficiently large throughput, low polarization, and frequency coverage from 30 to 300 GHz?; 4) is there a technical path to realizing the sensitivity and systematic error requirements?; and 5) what are the specific mission architecture parameters, including cost? Detailed answers to these questions are contained in this report.

Experimental Probe of Inflationary Cosmology (EPIC↗