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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 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Cation-Dependent Light-Induced Halide Demixing in Hybrid Organic–Inorganic Perovskites

Mixed cation metal halide perovskites with increased power conversion efficiency, negligible hysteresis, and improved long-term stability under illumination, moisture, and thermal stressing have emerged as promising compounds for photovoltaic and optoelectronic applications. In this paper, we shed light on photoinduced halide demixing using in situ photoluminescence spectroscopy and in situ synchrotron X-ray diffraction (XRD) to directly compare the evolution of composition and phase changes in CH(NH 2 ) 2 CsPb-halide (FACsPb-) and CH 3 NH 3 Pb-halide (MAPb-) perovskites upon illumination, thereby providing insights into why FACs-perovskites are less prone to halide demixing than MA-perovskites. We find that halide demixing occurs in both materials. However, the I-rich domains formed during demixing accumulate strain in FACsPb-perovskites but readily relax in MA-perovskites. The accumulated strain energy is expected to act as a stabilizing force against halide demixing and may explain the higher Br composition threshold for demixing to occur in FACsPb-halides. In addition, we find that while halide demixing leads to a quenching of the high-energy photoluminescence emission from MA-perovskites, the emission is enhanced from FACs-perovskites. This behavior points to a reduction of nonradiative recombination centers in FACs-perovskites arising from the demixing process and buildup of strain. FACsPb-halide perovskites exhibit excellent intrinsic material properties with photoluminescence quantum yields that are comparable to MA-perovskites. Finally, because improved stability is achieved without sacrificing electronic properties, these compositions are better candidates for photovoltaic applications, especially as wide bandgap absorbers in tandem cells.

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

Turning on the protonation-first pathway for electrocatalytic CO 2 reduction by manganese bipyridyl tricarbonyl complexes

Electrocatalytic reduction of CO 2 to CO is reported for the complex, { fac -Mn I ([(MeO) 2 Ph] 2 bpy)(CO) 3 (CH 3 CN)}(OTf), containing four pendant methoxy groups, where [(MeO) 2 Ph] 2 bpy = 6,6'-bis(2,6-dimethoxyphenyl)-2,2'-bipyridine. In addition to a steric influence similar to that previously established for the 6,6'-dimesityl-2,2'-bipyridine ligand in [ fac -MnI(mes 2 bpy)(CO) 3 (CH 3 CN)](OTf), which prevents Mn 0 –Mn 0 dimerization, the [(MeO) 2 Ph] 2 bpy ligand introduces an additional electronic influence combined with a weak allosteric hydrogen-bonding interaction that significantly lowers the activation barrier for C–OH bond cleavage from the metallocarboxylic acid intermediate. This provides access to the thus far elusive protonation-first pathway, minimizing the required overpotential for electrocatalytic CO 2 to CO conversion by Mn(I) polypyridyl catalysts, while concurrently maintaining a respectable turnover frequency. Comprehensive electrochemical and computational studies here confirm the positive influence of the [(MeO) 2 Ph] 2 bpy ligand framework on electrocatalytic CO 2 reduction and its dependence upon the concentration and p K a of the external Bronsted acid proton source (water, methanol, trifluoroethanol, and phenol) that is required for this class of manganese catalyst. Linear sweep voltammetry studies show that both phenol and trifluoroethanol as proton sources exhibit the largest protonation-first catalytic currents in combination with { fac -Mn I ([(MeO) 2 Ph] 2 bpy)(CO) 3 (CH 3 CN)}(OTf), saving up to 0.55 V in overpotential with respect to the thermodynamically demanding reduction-first pathway, while bulk electrolysis studies confirm a high product selectivity for CO formation. As a result, to gain further insight into catalyst activation, time-resolved infrared (TRIR) spectroscopy combined with pulse-radiolysis (PR-TRIR), infrared spectroelectrochemistry, and density functional theory calculations were used to establish the v (CO) stretching frequencies and energetics of key redox intermediates relevant to catalyst activation.

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

Activity-based cell sorting reveals responses of uncultured archaea and bacteria to substrate amendment

Metagenomic studies have revolutionized our understanding of the metabolic potential of uncultured microorganisms in various ecosystems. However, many of these genomic predictions have yet to be experimentally tested, and the functional expression of genomic potential often remains unaddressed. In order to obtain a more thorough understanding of cell physiology, novel techniques capable of testing microbial metabolism under close to in situ conditions must be developed. Here, we provide a benchmark study to demonstrate that bioorthogonal non-canonical amino acid tagging (BONCAT) in combination with fluorescence-activated cell sorting (FACS) and 16S rRNA gene sequencing can be used to identify anabolically active members of a microbial community incubated in the presence of various growth substrates or under changing physicochemical conditions. We applied this approach to a hot spring sediment microbiome from Yellowstone National Park (Wyoming, USA) and identified several microbes that changed their activity levels in response to substrate addition, including uncultured members of the phyla Thaumarchaeota, Acidobacteria, and Fervidibacteria. Because shifts in activity in response to substrate amendment or headspace changes are indicative of microbial preferences for particular growth conditions, results from this and future BONCAT-FACS studies could inform the development of cultivation media to specifically enrich uncultured microbes. Most importantly, BONCAT-FACS is capable of providing information on the physiology of uncultured organisms at as close to in situ conditions as experimentally possible.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

Spectroscopic characterization of a new Re(i) tricarbonyl complex with a thiosemicarbazone derivative: towards sensing and electrocatalytic applications

This work describes the preparation of a new thiosemicarbazone derivative, (Z)- N -ethyl-2-(6-oxo-1,10-phenanthrolin-5(6 H )-ylidene)hydrazinecarbothioamide (phet) and its respective Re( I ) tricarbonyl chloro complex, fac -[ReCl(CO) 3 (phet)]. The spectroscopic, photophysical and electrochemical properties of the new complex were fully investigated through steady state and time-resolved techniques along with computational calculations. In fac -[ReCl(CO) 3 (phet)], the new ligand is coordinated to the metal center through the pyridyl rings of the phenanthroline moiety. The unbound electron pairs in the S atom of the bending thiosemicarbazone group induce new low energy lying electronic transitions. Consequently, enhanced visible light absorption up to 550 nm is observed in acetonitrile due to the overlap between MLCT Re→phet and IL phet(n→π*) transitions. The absorption bands and emission quantum yields of fac -[ReCl(CO) 3 (phet)] are sensitive to proton concentration due to an acid-basic equilibrium in the N atoms of the thiosemicarbazone. Proton dissociation constants of 10.0 ± 0.1 and 11.4 ± 0.2 were determined respectively for the ground and excited states of the new complex. Spectral changes could also be observed in the presence of Zn 2+ cations which can be further explored for sensing applications. The electrochemical behavior of the new complex was studied in detail, revealing up to four one electron reduction processes in the range from 0 to -2.4 V vs. Fc + /Fc. With support of DFT calculations, the first three processes are ascribed to the reduction of the coordinated phet ligand followed by the Re I/0 reduction and consequent Cl - release. Furthermore, the new complex was able to act as an electrocatalyst for CO 2 reduction into CO ( E onset = -1.92 V vs. Fc + /Fc), with a turnover frequency of 2.81 s -1 and turnover number of 24 ± 1 in anhydrous acetonitrile, being the first Re( I ) tricarbonyl complex with a thiosemicarbazone derivative described for this goal. The detailed characterization carried out here can drive the development of new Re( I )-thiosemicarbazone derivatives for different applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Poster - 15: Air kerma rate measurements using a cylindrical free-air ionization chamber on the 05B1-1 beamline at the Canadian Light Source

Purpose: The BioMedical Imaging and Therapy (BMIT) beamlines at the Canadian Light Source offer the opportunity for investigating novel imaging and therapy applications of synchrotron radiation. A necessary component in advancing this research, and in progressing toward clinical applications, is the availability of accurate dosimetry that is traceable to a standards institution. However, dosimetry in this setting is challenging. These beams are typically small, non-uniform, and highly intense. This work describes air kerma rate measurements on a BMIT beamline using a free-air ionization chamber (FAC). Methods: The measurements were taken at the 05B1-1 beamline (∼8 – 100 keV) for several beam qualities with mean energies between 20.0 and 84.0 keV. The Victoreen Model 480 cylindrical FAC, with a specially fabricated 0.52 mm diameter aperture, was used to measure air kerma rates. The required correction factors were determined using a variety of methods: tabulated data, measurements, theoretical calculations and Monte Carlo simulations (EGSnrc user code egs-fac). Results: The experimental air kerma rates measured between 0.270 ± 13.6% and 312 ± 2.7% Gy/min. At lower energies (low filtration), the most impactful correction factors were those for ion recombination and for x-ray attenuation. Conclusions: These measurements marked the first absolute dosimetry performed at the BMIT beamlines. The experimental and Monte Carlo methods developed will allow air kerma rates to be measured under other experimental conditions, provide a benchmark to which other dosimeters will be compared, and provide a reference for imaging and therapy research programs on this beamline.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2022

Multiplexed Probing for Functional Capacity Measurements in Complex and Limited-Size Samples

A new strategy using glass as a solid support for functionalization with chemical probes has been recently developed with successful results. The next step in glass functionalization is to pair chemical probes with fluorescent glass microspheres. This approach gives us a way to directly quantify probe-bound protein using Fluorescence-Activated Cell Sorting (FACS). FACS has already shown to be amendable to glass microspheres, demonstrating changes in probe-bound protein concentration. Suitable probing conditions for gram-positive and negative microbes, complex microbial communities from myriad ecosystems, and eukaryotic cells/tissues have traditionally suffered from set-backs, such as limited protein per sample and conditions atypical for probing. To remedy this, we propose to: (1) Demonstrate probe functionalization specific to glass microspheres by paired fluorophore and use those activity probes successfully with proteomics. Probes that are currently available (CYP5, GSH/GST, Glycoside Hydrolase) can be easily prepared onto glass surfaces. Probe-bound microspheres can be tested in ratios, first with known amounts of purified protein and then complex microbiome lysates. (2) Our validated microspheres are then used to determine quantitative amounts of protein through FACS sorting. Complimenting these results by proteomics, prepared microspheres are then optimized and condensed into a user-friendly kit. Once successfully commercialized, this multiplexed assay can be used with little to no technical expertise, making this available to various industries users.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Few-Atom Copper Catalyst for the Electrochemical Reduction of CO to Acetate: Synergetic Catalysis between Neighboring Cu Atoms

Single-atom catalysts (SACs) are gaining increasing recognition because of their superior catalytic properties for various reactions. However, the performance of SACs is often limited by the lack of neighboring metal centers to cooperate in catalysis. Herein, a synergetic interaction between neighboring Cu atoms of a few-atom catalyst (FAC) on graphdiyne is found to greatly enhance the production of acetate in CO electroreduction reaction relative to Cu SACs. In a 1.0 M KOH electrolyte, this Cu FAC exhibits an acetate Faradaic efficiency of 53.8±1.5 % and an ultrahigh relative purity of up to 97 wt% for liquid products, and excellent stability of over 23 h continuous electrolysis at -0.8 V versus reversible hydrogen electrode (RHE). Theoretical studies suggest that the intersite catalytic communication between two neighboring metal atoms confined in each pore of GDY facilitates the formation of acetic acid through either stepwise hydrogenation of CH 2 CO* or the direct reaction of H 2 O with CH 2 CO*. Our study demonstrates the unprecedented synergetic catalysis of Cu FAC in promoting the selective CO electroreduction toward acetate production.

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

Laboratory Calibrations of Fe xii–xiv Line-Intensity Ratios for Electron Density Diagnostics

In this work, we have used an electron beam ion trap to measure electron-density-diagnostic line-intensity ratios for extreme ultraviolet lines from Fe xii, xiii, and xiv at wavelengths of ≈185–205 and 255–276 Å. These ratios can be used as density diagnostics for astrophysical spectra and are especially relevant to solar physics. We found that density diagnostics using the Fe xiii 196.53/202.04 and the Fe xiv 264.79/274.21 and 270.52A/274.21 line ratios are reliable using the atomic data calculated with the Flexible Atomic Code (FAC). On the other hand, we found a large discrepancy between the FAC theory and experiment for the commonly used Fe xii (186.85 + 186.88)/195.12 line ratio. These FAC theory calculations give results similar to the data tabulated in CHIANTI, which are commonly used to analyze solar observations. Our results suggest that the discrepancies seen between solar coronal density measurements using the Fe xii (186.85 + 186.88)/195.12 and Fe xiii 196.54/202.04 line ratios are likely due to issues with the atomic calculations for Fe xii.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS1985

ISEE-1 and 2 observations of field-aligned currents in the distant midnight magnetosphere

Magnetic field measurements obtained in the nightside magnetosphere by the co-orbiting ISEE-1 and 2 spacecraft have been examined for signatures of field-aligned currents (FAC). Such currents are found on the boundary of the plasma sheet both when the plasma sheet is expanding and when it is thinning. Evidence is often found for the existence of waves on the plasma sheet boundary, leading to multiple crossings of the FAC sheet. At times the boundary layer FAC sheet orientation is nearly parallel to the X-Z GSM plane, suggesting 'protrusions' of plasma sheet into the lobes. The boundary layer current polarity is, as expected, into the ionosphere in the midnight to dawn local time sector, and outward near dusk. Current sheet thicknesses and velocities are essentially independent of plasma sheet expansion or thinning, having typical values of 1500 km and 20-40 km/s respectively. Characteristic boundary layer current densities are about 10 nanoamps per square meter.

Elphic, R. C.↗
NASA NTRS1988

Finite area combustor theoretical rocket performance

Previous to this report, the computer program of NASA SP-273 and NASA TM-86885 was capable of calculating theoretical rocket performance based only on the assumption of an infinite area combustion chamber (IAC). An option was added to this program which now also permits the calculation of rocket performance based on the assumption of a finite area combustion chamber (FAC). In the FAC model, the combustion process in the cylindrical chamber is assumed to be adiabatic, but nonisentropic. This results in a stagnation pressure drop from the injector face to the end of the chamber and a lower calculated performance for the FAC model than the IAC model.

Gordon, Sanford↗
NASA NTRS1991

DMSP F7 observations of a substorm field-aligned current

Observations are described of a substorm field-aligned current (FAC) system traversed by the DMSP F7 spacecraft just after 0300 UT on April 25, 1985. It is shown that the substorm FAC portion of the current system was located equatorward of the boundary between open and closed field lines. The equatorward boundary of the substorm FAC into the magnetotail was mapped using the Tsyganenko (1987) model, showing that the boundary corresponds to 6.9 earth radii. The result is consistent with the suggestion of Akasofu (1972) and Lopez and Lui (1990) that the region of substorm initiation lies relatively close to the earth and the concept that an essential feature of substorms is the disruption and diversion of the near-earth current sheet.

Lopez, R. E.↗
NASA NTRS1995

Simultaneous prenoon and postnoon observations of three field-aligned current systems from Viking and DMSP-F7

The spatial structure of dayside large-scale field-aligned current (FAC) systems is examined by using Viking and Defense Meteorological Satellite Program-F7 (DMSP-F7) data. We focus on four events in which the satellites simultaneously observed postnoon and prenoon three FAC systems: the region 2, the region 1, and the mantle (referred to as midday region O) systems, from equatorward to poleward. These events provide the most solid evidence to date that the midday region O system is a separate and unique FAC system, and is not an extension of the region 1 system from other local times. The events are examined comprehensively by making use of a mulit-instrumental data set, which includes magnetic field, particle flux, electric field, auroral UV image data from the satellites, and the Sondrestrom convection data. The results are summarized as follows: (1) Region 2 currents flow mostly in the central plasma sheet (CPS) precipitation region, often overlapping with the boundary plasma sheet (BPD) at their poleward edge. (2) The region 1 system is located in the core part of the auroral oval and is confined in a relatively narrow range in latitude which includes the convection reversal. The low-latitude boundary layer, possibly including the outer part of the plasma sheet, and the external cusp are the major source regions of dayside region 1 currents. (2) Midday region O currents flow on open field lines and are collocated with the shear of antisunward convection flows with velocites decreasing poleward. On the basis of these results we support the view that both prenoon and postnoon current systems consist of the three-sheet structure when the disctortion ofthe convection pattern associated with interplanetary magnetic field (IMF) B(sub Y) is small and both morningside and eveningside convection cells are crescent-shaped. We also propose that the midday region O and a part of the region 1 systems are closely coupled to the same source.

Ohtani, S.↗
NASA NTRS2001

Magnetosphere-Regolith/Exosphere Coupling: Differences and Similarities to the Earth Magnetosphere-Ionosphere Coupling

Of the three Mercury passes made by Mariner 10, the first and third went through the Mercury magnetosphere. The third encounter which occurred during northward IMF (interplanetary magnetic field) showed quiet time magnetic fields. In contrast the third encounter observed clear substorm signatures including dipolarization, field-aligned currents (FACs) and injection of energetic electrons at geosynchronous orbit. However, the determined cross-tail potential drop and the assumed height integrated conductance indicate that the FAC should be 2-50 times weaker than observed. We address this inconsistency and the fundamental problem of FAC closure whether this takes place in the regolith or in the exosphere. The current state of knowledge of the magnetosphere-exosphere/regolith coupling is addressed and similarities and differences to the Earth magnetosphere-ionosphere coupling are discussed.

Gjerleov, J. W.↗
NASA NTRS2004

Improved Ionospheric Electrodynamic Models and Application to Calculating Joule Heating Rates

Improved techniques have been developed for empirical modeling of the high-latitude electric potentials and magnetic field aligned currents (FAC) as a function of the solar wind parameters. The FAC model is constructed using scalar magnetic Euler potentials, and functions as a twin to the electric potential model. The improved models have more accurate field values as well as more accurate boundary locations. Non-linear saturation effects in the solar wind-magnetosphere coupling are also better reproduced. The models are constructed using a hybrid technique, which has spherical harmonic functions only within a small area at the pole. At lower latitudes the potentials are constructed from multiple Fourier series functions of longitude, at discrete latitudinal steps. It is shown that the two models can be used together in order to calculate the total Poynting flux and Joule heating in the ionosphere. An additional model of the ionospheric conductivity is not required in order to obtain the ionospheric currents and Joule heating, as the conductivity variations as a function of the solar inclination are implicitly contained within the FAC model's data. The models outputs are shown for various input conditions, as well as compared with satellite measurements. The calculations of the total Joule heating are compared with results obtained by the inversion of ground-based magnetometer measurements. Like their predecessors, these empirical models should continue to be a useful research and forecast tools.

Weimer, D. R.↗
NASA NTRS2004

An Overview of the Formation and Attitude Control System for the Terrestrial Planet Finder Formation Flying Interferometer

The Terrestrial Planet Finder formation flying Interferometer (TPF-I) will be a five-spacecraft, precision formation operating near the second Sun-Earth Lagrange point. As part of technology development for TPF-I, a formation and attitude control system (FACS) is being developed that achieves the precision and functionality needed for the TPF-I formation and that will be demonstrated in a distributed, real-time simulation environment. In this paper we present an overview of FACS and discuss in detail its formation estimation, guidance and control architectures and algorithms. Since FACS is currently being integrated into a high-fidelity simulation environment, component simulations demonstrating algorithm performance are presented.

Scharf, Daniel P.↗
NASA NTRS2008

Space Technology 5 Observations of Auroral Field-Aligned Currents

During its three month long technology validation mission, Space Technology 5 (ST-5) returned high quality multi-point measurements of the near-Earth magnetic field. Its three micro-satellites were launched into a 300 x 4500 km, dawn - dusk, sun synchronous orbit (inclination = 105.60) orbit with a period of 138 min by a Pegasus launch vehicle on March 22, 2006. The spacecraft were maintained in a "pearls on a sting" constellation with controlled spacings ranging from just over 5000 km down to under 50 km. The individual micro-satellites were 48 cm tall octagons with diameters of 50 cm. They were spin-stabilized at approximately 20 rpm at deployment and slowly spun-down to about 15 rpm by the end of the mission. Each spacecraft carried a miniature tri-axial fluxgate magnetometer (MAG) provided by the University of California at Los Angeles mounted at the end of a ultra-low mass 72 cm boom. These data allow, for the first time, the separation of temporal and spatial variations in field-aligned current (FAC) perturbations measured in low-Earth orbit on time scales of 10 sec to 10 min. The constellation measurements are used to directly determine field-aligned current sheet motion, thickness. and current density. Two multi-point methods for the inference of FAC current density that have not previously been possible in low-Earth orbit are demonstrated: 1) the -standard method." based upon s/c velocity, but corrected for FAC current sheet motion. and 2) the "gradiometer method" which uses simultaneous magnetic field measurements at two points with known separation. Future studies will apply these methods to the entire ST-5 data sct and expand to include horizontal ionospheric currents. ULF waves and geomagnetic field gradient analyses.

Slavin, James↗
NASA NTRS2007

Space Technology 5 Multi-point Measurements of Near-Earth Magnetic Fields: Initial Results

The Space Technology 5 (ST-5) mission successfully placed three micro-satellites in a 300 x 4500 km dawn-dusk orbit on 22 March 2006. Each spacecraft carried a boom-mounted vector fluxgate magnetometer that returned highly sensitive and accurate measurements of the geomagnetic field. These data allow, for the first time, the separation of temporal and spatial variations in field-aligned current (FAC) perturbations measured in low-Earth orbit on time scales of approximately 10 sec to 10 min. The constellation measurements are used to directly determine field-aligned current sheet motion, thickness and current density. In doing so, we demonstrate two multi-point methods for the inference of FAC current density that have not previously been possible in low-Earth orbit; 1) the "standard method," based upon s/c velocity, but corrected for FAC current sheet motion, and 2) the "gradiometer method" which uses simultaneous magnetic field measurements at two points with known separation. Future studies will apply these methods to the entire ST-5 data set and expand to include geomagnetic field gradient analyses as well as field-aligned and ionospheric currents.

Slavin, James A.↗
NASA NTRS2010

Alfven Wave Reflection Model of Field-Aligned Currents at Mercury

An Alfven Wave Reflection (AWR) model is proposed that provides closure for strong field-aligned currents (FACs) driven by the magnetopause reconnection in the magnetospheres of planets having no significant ionospheric and surface electrical conductance. The model is based on properties of the Alfven waves, generated at high altitudes and reflected from the low-conductivity surface of the planet. When magnetospheric convection is very slow, the incident and reflected Alfven waves propagate along approximately the same path. In this case, the net field-aligned currents will be small. However, as the convection speed increases. the reflected wave is displaced relatively to the incident wave so that the incident and reflected waves no longer compensate each other. In this case, the net field-aligned current may be large despite the lack of significant ionospheric and surface conductivity. Our estimate shows that for typical solar wind conditions at Mercury, the magnitude of Region 1-type FACs in Mercury's magnetosphere may reach hundreds of kilo-Amperes. This AWR model of field-aligned currents may provide a solution to the long-standing problem of the closure of FACs in the Mercury's magnetosphere. c2009 Elsevier Inc. All rights reserved.

Lyatsky, Wladislaw↗