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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 1,513 records · Page 84
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Evidence for Interfacial Halogen Bonding

Abstract A homologous series of donor–π–acceptor dyes was synthesized, differing only in the identity of the halogen substituents about the triphenylamine (TPA; donor) portion of each molecule. Each Dye‐X (X=F, Cl, Br, and I) was immobilized on a TiO 2 surface to investigate how the halogen substituents affect the reaction between the light‐induced charge‐separated state, TiO 2 (e − )/ Dye‐X + , with iodide in solution. Transient absorption spectroscopy showed progressively faster reactivity towards nucleophilic iodide with more polarizable halogen substituents: Dye‐F < Dye‐Cl < Dye‐Br < Dye‐I . Given that all other structural and electronic properties for the series are held at parity, with the exception of an increasingly larger electropositive σ‐hole on the heavier halogens, the differences in dye regeneration kinetics for Dye‐Cl , Dye‐Br , and Dye‐I are ascribed to the extent of halogen bonding with the nucleophilic solution species.

Swords, Wesley B.↗
DOE OSTI2018

Stability Considerations Using a Microscopic Stability Model Applied to a 2G Thin Film Coated Superconductor

A numerical, finite element simulation of local temperature fields, critical current and transport current distributions is applied to a 2G thin film coated high-temperature superconductor. The focus is on simulation of quenches originating from transport current locally exceeding critical current density. As in previous reports, a statistical treatment of superconductor parameters (critical temperature, current and magnetic field) is applied for this analysis; it shall take into account uncertainties possibly arising from shortcomings in conductor manufacture or during measurements of their properties. The results of the calculations are used as quasi-boundary (driving) conditions for a subsequent transient microscopic numerical stability analysis. Traditionally, stability analysis usually applies analytic stability functions that incorporate conventional, phonon-related timescales, t and disturbances. The question is whether decay of electron pairs and subsequent relaxation of the excited state to a new dynamic equilibrium carrier concentration, the “electron aspect” of the stability problem, under the same disturbances, proceeds on another timescale, t{sup ′}. Is this timescale identical to the traditional (phonon) timescale, t? If not, how large are the differences? The recently reported microscopic stability model, now applied to a thin film conductor, is consulted to find an answer to these questions. A time limit, t{sub Quench}, can be extracted from the simulations, as the time of immediate onset of a quench. This is a new approach in stability considerations since, conventionally, a temperature limit, T < T{sub Crit}, is set as stability criterion. If electrical operation or cooling conditions cannot immediately respond to this challenge, the thin film superconductor, if this time limit is exceeded, will hardly be able to return to zero loss current transport.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

One-pot electrochemical preparation of BiOCl/BiPO{sub 4} double-layer heterojunction film with efficient photocatalytic performance

Highlights: • A novel BiOCl/BiPO{sub 4} heterojunction film has been synthesized by one-pot electrochemical method. • The as-prepared BiOCl/BiPO{sub 4} heterojunction film exhibited high photocatalytic activity and stability. • The plausible formation process of BiOCl/BiPO{sub 4} heterojunction film has been proposed and demonstrated. • The photocatalytic mechanism of phenol degradation presented by BiOCl/BiPO{sub 4} heterojunction film was investigated and analyzed. - Abstract: A BiOCl/BiPO{sub 4} double-layer heterojunction film on metal Bi plate with reduced recombination of photo-induced carriers has been successfully prepared by one-step electrochemical anodization process. The morphology characterizations displayed that the double-layer film consisted of BiPO{sub 4} rods array at the bottom and BiOCl nanosheets on the top. Meanwhile, the control experiments indicated that the BiPO{sub 4} rods array was transformed by BiOCl rather than Bi{sup 3+} reacting with PO{sub 4}{sup 3−} directly. In addition, the resulting BiOCl/BiPO{sub 4} heterojunction film exhibited excellent photocatalytic activity and stability on the degradation of phenol comparing with pure BiOCl film. Transient photocurrent measurements and PL spectra proved that the enhanced photocatalytic performance of BiOCl/BiPO{sub 4} heterojunction film was attributed to the effective separation of photo-generated electron-hole pairs excited on BiOCl. Moreover, ·O{sub 2}{sup −} and ·OH played a crucial role in the photodegradation process of phenol. Based on these analytical results, a plausible photocatalytic mechanism has been proposed.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Ultrafast Spin Crossover in a Room-Temperature Ferrimagnet: Element-Specific Spin Dynamics in Photoexcited Cobalt Ferrite

Transition metal complexes capable of photoinduced spin crossover have been greatly investigated because of their potential to enable ultrafast optical control of information processing. Yet, any real application of photoswitchable molecules requires that spin crossover be paired with additional functionality such as long-range magnetic order. Important advances combining these functions are notably reported for a number of bimetallic Prussian Blue analogues; however, to date, PBA-based magnetic photoswitches can only operate below 150 K due to loss of magnetic order. In contrast, cobalt ferrite is a ferrimagnetic semiconductor with a Curie temperature of 790 K and extremely favorable magnetic properties by comparison to state-of-the-art PBAs. The mixed valence electronic structure of cobalt ferrite is reminiscent of cobalt–iron PBA, which is a well-known photoswitch. To investigate the potential for photoswitching in this material, we employ transient XUV spectroscopy to probe charge and spin dynamics with element-specific resolution on the femtosecond time scale. Results show that 400 nm light excites a metal-to-metal charge transfer transition, which drives the crossover of high-spin Co 2+ to low-spin Co 3+ with a time constant of 405 ± 29 fs and an internal quantum efficiency of unity. This result establishes the existence of efficient photoswitching in a new class of robust ferrimagnetic spinel ferrites.

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

Ultrafast Reaction Mechanisms in Perovskite Based Photocatalytic C–C Coupling

Solar driven carbon-carbon (C-C) bond formation is a new direction in solar energy utilization. Earth abundant nanocrystal based photocatalysts are highly sought after as they can potentially eliminate expensive noble metal catalysts. A detailed understanding of the underlying reaction mechanisms could provide guidance in designing new systems that can activate a larger class of small molecules. Here, we employ transient absorption spectroscopy to study a model C-C bond formation reaction, i.e., a-alkylation of aldehydes catalyzed by colloidal CsPbBr3 nanocrystals (NCs). We find that both electrons and holes undergo ultrafast charge transfer (~50 ps) from photoexcited perovskite NCs to reactant molecules. A charge separated state lives for more than 0.8 µs, enabling a radical mechanism to form the C-C bonds. We discuss the differences between the NCs photoredox catalysts and the molecular catalyst.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Super-diffusion of excited carriers in semiconductors

The ultrafast spatial and temporal dynamics of excited carriers are important to understanding the response of materials to laser pulses. Here we use scanning ultrafast electron microscopy to image the dynamics of electrons and holes in silicon after excitation with a short laser pulse. We find that the carriers exhibit a diffusive dynamics at times shorter than 200 ps, with a transient diffusivity up to 1,000 times higher than the room temperature value, D 0 ≈30 cm 2 s –1 . The diffusivity then decreases rapidly, reaching a value of D 0 roughly 500 ps after the excitation pulse. We attribute the transient super-diffusive behaviour to the rapid expansion of the excited carrier gas, which equilibrates with the environment in 100–150 ps. Numerical solution of the diffusion equation, as well as ab initio calculations, support our interpretation. Lastly, our findings provide new insight into the ultrafast spatial dynamics of excited carriers in materials.

36 MATERIALS SCIENCE↗
DOE OSTI2016

High-Field High-Repetition-Rate Sources for the Coherent THz Control of Matter

Ultrashort flashes of THz light with low photon energies of a few meV, but strong electric or magnetic field transients have recently been employed to prepare various fascinating nonequilibrium states in matter. Here we present a new class of sources based on superradiant enhancement of radiation from relativistic electron bunches in a compact electron accelerator that we believe will revolutionize experiments in this field. Our prototype source generates high-field THz pulses at unprecedented quasi-continuous-wave repetition rates up to the MHz regime. We demonstrate parameters that exceed state-of-the-art laser-based sources by more than 2 orders of magnitude. The peak fields and the repetition rates are highly scalable and once fully operational this type of sources will routinely provide 1 MV/cm electric fields and 0.3 T magnetic fields at repetition rates of few 100 kHz. In conclusion, we benchmark the unique properties by performing a resonant coherent THz control experiment with few 10 fs resolution.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Reactivity of Zn + aq in high-temperature water radiolysis

For this work, reactivity of transients involving Zn + in high-temperature water radiolysis has been studied in the temperature range of 25–300 °C. The reduced monovalent zinc species were generated from an electron transfer process between the hydrated electron and Zn 2+ ions using pulse radiolysis. The Zn + species can subsequently be oxidized by the radiolytically-produced oxidizing species: ˙OH, H 2 O 2 and ˙H. We find that the absorption of monovalent zinc is very sensitive to the pH of the medium. An absorption maximum at 306–311 nm is most pronounced at pH 7 and the signal then decreases in acidic media where the reducing electrons are competitively captured by protons. At pH values higher than 7, hydroxo-forms of Zn 2+ are created and the maximum of the absorption signal begins to shift to the red spectral region. We find that the optical spectrum of Zn + aq cannot be fully explained in terms of a charge-transfer to solvent (CTTS) process, which was previously proposed. Reaction rates of most of the recombination reactions investigated follow the empirical Arrhenius relationship at temperatures up to 200 °C and have been determined at higher temperatures for the first time. A bimolecular disproportionation reaction of Zn + aq is not observed under the conditions investigated.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Muon detection studied by pulse-height energy analysis: Novel converter arrangements

Muons are conventionally measured by a plastic scintillator–photomultiplier detector. Muons from processes in ultra-dense hydrogen H(0) are detected here by a novel type of converter in front of a photomultiplier. The muon detection yield can be increased relative to that observed with a plastic scintillator by at least a factor of 100, using a converter of metal, semiconductor (Ge), or glass for interaction with the muons penetrating through the metal housing of the detector. This detection process is due to transient formation of excited nuclei by the well-known process of muon capture, giving beta decay. The main experimental results shown here are in the form of beta electron energy spectra detected directly by the photomultiplier. Events which give a high-energy tail in the energy spectra are probably due to gamma photons from the muons. Sharp and intense x-ray peaks from a muonic aluminium converter or housing material are observed. The detection conversion in glass and Ge converters has a time constant of the order of many minutes to reach the final conversion level, while the process in metal converters is stabilized faster. The time constants are not due to lifetimes of the excited nuclei or neutrons but are due to internal charging in the insulating converter material. Interaction of this charging with the high voltage in the photomultiplier is observed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

HOCCO versus OCCO: Comparative spectroscopy of the radical and diradical reactive intermediates

We present a photoelectron imaging study of three glyoxal derivatives: the ethylenedione anion (OCCO{sup −}), ethynediolide (HOCCO{sup −}), and glyoxalide (OHCCO{sup −}). These anions provide access to the corresponding neutral reactive intermediates: the OCCO diradical and the HOCCO and OHCCO radicals. Contrasting the straightforward deprotonation pathway in the reaction of O{sup −} with glyoxal (OHCCHO), which is expected to yield glyoxalide (OHCCO{sup −}), OHCCO{sup −} is shown to be a minor product, with HOCCO{sup −} being the dominant observed isomer of the m/z = 57 anion. In the HOCCO/OHCCO anion photoelectron spectrum, we identify several electronic states of this radical system and determine the adiabatic electron affinity of HOCCO as 1.763(6) eV. This result is compared to the corresponding 1.936(8) eV value for ethylenedione (OCCO), reported in our recent study of this transient diradical [A. R. Dixon, T. Xue, and A. Sanov, Angew. Chem., Int. Ed. 54, 8764–8767 (2015)]. Based on the comparison of the HOCCO{sup −}/OHCCO{sup −} and OCCO{sup −} photoelectron spectra, we discuss the contrasting effects of the hydrogen connected to the carbon framework or the terminal oxygen in OCCO.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1977

Superconducting thermometer for cryogenics

Digital electronic device uses superconducting filaments as sensors. Simple solid-state circuitry combined with filaments comprise highly-reliable temperature monitor. Device has ability to track very fast thermal transients and "on/off" output is adaptable to remote sensing and telemetry.

White, F. A.↗
NASA NTRS1982

Solar energetic photon transients - 50 keV-100 MeV

The observed properties of solar transient photon impulses between a few keV and 100 MeV recorded by the SMM are compared and reasons for continued monitoring of solar photon transients are discussed. Various solar flare events observed are reviewed, along with gamma ray measurements. It is calculated that the emission of energetic photons is due to ion and electron interactions with matter, with both species undergoing acceleration at close time intervals. The gamma ray events and microwave emissions showed time structures similar to previously recorded X ray emissions. Bursts of all three radiation types have displayed a quasi-periodicity of less than 10 sec. Data on the 2.223 MeV neutron capture line have shown a decay in line intensity to take about 50 sec, consistent with Monte Carlo calculation for a He-3/H abundance of 0.00005.

Chupp, E. L.↗
NASA NTRS1987

Advanced Components for Spaceborne Infrared Astronomy

Basic improvements in the technology of low noise read-out systems for low background detectors were demonstrated. Using discrete JFET integrating amplifiers at their optimum temperature of 55 K, read noise less than 7.5 electrons in 128 seconds of integration was obtained. Two models of single channel integrators are now available, the JF-77 for use between 50 and 80 K and the JF-4 for lower temperatures. A 1 x 15 linear array of complete integrators on a single integrated circuit was developed and will be made available in the near future. The successful operation of a superconducting stepper motor was demonstrated. The motor shows a three fold increase in torque over conventional motors operating at room temperature. The success of the motor stems from the use of superconducting coils in conjunction with developments in bearings for cryogenic use, rare-earth rotors, and motor cooling techniques. The current state of development will allow the rapid development of motors optimized for specific applications. An electronic switch capable of resetting cooled JFET integrating amplifiers was developed. The JFET integrating amplifiers that use this switch have demonstrated read noise of less than 10 electrons. The JFET reset device exhibits an extremely high open impedance and low leakage current. Capacitance is sufficiently low so as not to impair amplifier sensitivity. The effects of transient switching charges are minimized by a compensation technique and variable transient current problems inherent to devices of this type are overcome by external circuity.

Davidson, Arnold W.↗
NASA NTRS1987

Radiation damage and defect behavior in proton irradiated lithium-counterdoped n+p silicon solar cells

Two lithium-counterdoped n+p silicon solar cells with different lithium concentrations were irradiated by 10-MeV protons. Cell performance was measured as a function of fluence, and it was found that the cell with the highest concentration of lithium had the highest radiation resistance. Deep level transient spectroscopy which showed two deep level defects that were lithium related. Relating the defect energy levels obtained from this study with those from earlier work using 1-MeV electron irradiation shows no correlation of the defect energy levels. There is one marked similarity: the absence of the boron-interstitial-oxygen-interstitial defect. This consistency strengthens the belief that lithium interacts with oxygen to prevent the formation of the boron interstitial-oxygen interstitial defect. The results indicate that, in general, addition of lithium in small amounts to the p-base of a boron doped silicon solar cell such that the base remains p-type, tends to increase the radiation resistance of the cell.

Stupica, John↗
NASA NTRS1991

A new approach to equipment testing

Considerable controversy has arisen during the recent discussions over a new version of the RTCA DO160C/ED 14C Section 22 document at the European Committee for Aviation Electronics. Section 22 is concerned with lightning waveform tests to equipment. Investigations of some of these controversies with circuit analysis and measurements indicate the impedance characteristics required of the transient generators and the possibility of testing to a voltage limit even for current waveforms.

Hardwick, C. J.↗
DOE OSTI2018

Numerical Simulation and Model Analyses of In-situ Biogeochemical Remediation of Chromium at the LANL - 18306

Environmental management problems associated with contamination of groundwater resources with heavy metals (such as chromium) typically require complex biogeochemical model simulations and analysis of in situ remediation. Frequently, the in situ remediation is the only viable treatment option. In these cases, a three-dimensional reactive transport model of relevant biogeochemical processes is invaluable. Recently, we have developed a novel unique biogeochemical simulator called CHROTRAN (http://chrotran.lanl.gov; Hansen et al. 2017, Vesselinov et al. 2018a) capable to represent the full three-dimensional dynamics of processes associated with in situ biogeochemical remediation of heavy metals in heterogeneous aquifers. CHROTRAN accounts for spatial and temporal transients of (1) the heavy metal to be remediated, (2) introduced amendments (e.g., through well injection), and (3) biomass growth and decay. The introduced amendments can include (1) an electron donor (e.g., molasses), (2) a nontoxic-conservative bio-inhibitor (e.g., ethanol), and (3) a biocide (e.g., dithionite). In addition, direct abiotic reduction by donor-metal interaction as well as donor-driven biomass growth and bio-reduction are modeled in CHROTRAN. Other critical processes, such as donor sorption, bio-fouling and biomass death are also modeled. CHROTRAN can simulate the groundwater flow dynamics introduced due a series of injection and extraction wells and account for reduction of aquifer permeability near the wells due bio clogging. CHROTRAN is based on the existing PFLOTRAN (http://pflotran.org; Lichtner et al, 2017a) code framework, taking advantage of the reaction interface allowing for implementation of complex model features and leverage other facets of PFLOTRAN, such as multi-component geochemistry and high-performance computing. Here, we present numerical simulations and model analyses related to the Los Alamos National Laboratory (LANL) chromium site. The analyses are performed by coupling of CHROTRAN with MADS (Model Analysis and Decision Support; http://mads.lanl.gov; Vesselinov et al., 2018b). We present analyses related to uncertainty quantification of model predictions, sensitivity of model parameters and remedial decision support. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

TEM Study of Zircaloy 2 with FeCrAl Layer under Simulated BWR Environment

Zircaloy 2 is widely used as nuclear fuel cladding in light-water nuclear reactors, which is resistive to corrosion, creep, and swelling. Due to water chemical reactivity and high-temperature steam exposure, oxidation in zirconium cladding is possible during transients. To mitigate the zirconium oxidation and the hydrogen generation at elevated temperature, we have coated Zircaloy 2 with oxide resistant FeCrAl thin film layers using magnetron sputtering. Transmission electron microscopy (TEM), scanning transmission electron microscopy (STEM), and electron energy-dispersive X-ray spectroscopy (EDX) are used to understand the behavior of the protective FeCrAl layer under typical BWR operation conditions. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
NASA NTRS2022

Hybrid simulations of a tangential discontinuity-driven foreshock bubble formation in comparison with a hot flow anomaly formation

Hot flow anomalies (HFAs) and foreshock bubbles (FBs) are significant foreshock transients that can accelerate particles and disturb the magnetosphere-ionosphere system. Yet, their early formation mechanisms are still not fully understood. To investigate the formation of tangential discontinuity (TD)-driven FBs and HFAs, we use 2-D local hybrid simulations where a reflected or an injected warm foreshock ion beam can interact with a TD whose half-thickness is comparable to the ion inertial scale. We show that the foreshock ions perform a partial gyration within, or across, the TD. Bulk motion differences between partially-gyrating foreshock ions and fluid-electrons lead to the generation of currents. As the trigger, these foreshock-driven currents change the magnetic field topology around the TD and force the frozen-in solar wind plasma to redistribute along with the field lines, shaping the foreshock transient. This confirms a recently proposed kinetic formation model. The extent of the magnetic field direction change across the TD within the foreshock ion gyromotion determines the current profile and thus the type of foreshock transient that forms. For a thin TD, the foreshock ions generate a current that is much stronger on the upstream side than the downstream side, forming an FB with one upstream compressional boundary. For the same foreshock ion gyroradius and magnetic shear, a thick TD yields comparable foreshock-driven currents on the upstream and downstream sides, forming an HFA with two compressional boundaries. Our study suggests that the TD thickness is one of the factors that determine the formation of FBs and HFAs

Andrew Vu↗