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At least 541 records · Page 30
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Dominant Role of Hole Transport Pathway in Achieving Record High Photoconductivity in Two‐Dimensional Metal–Organic Frameworks

Abstract Metal–organic frameworks (MOFs) with mobile charges have attracted significant attention due to their potential applications in photoelectric devices, chemical resistance sensors, and catalysis. However, fundamental understanding of the charge transport pathway within the framework and the key properties that determine the performance of conductive MOFs in photoelectric devices remain underexplored. Herein, we report the mechanisms of photoinduced charge transport and electron dynamics in the conductive 2D M−HHTP (M=Cu, Zn or Cu/Zn mixed; HHTP=2,3,6,7,10,11‐hexahydroxytriphenylene) MOFs and their correlation with photoconductivity using the combination of time‐resolved terahertz spectroscopy, optical transient absorption spectroscopy, X‐ray transient absorption spectroscopy, and density functional theory (DFT) calculations. We identify the through‐space hole transport mechanism through the interlayer sheet π–π interaction, where photoinduced hole state resides in HHTP ligand and electronic state is localized at the metal center. Moreover, the photoconductivity of the Cu−HHTP MOF is found to be 65.5 S m −1 , which represents the record high photoconductivity for porous MOF materials based on catecholate ligands.

14 SOLAR ENERGY↗
DOE OSTI2024

Changes in dislocation punching behavior due to hydrogen-seeded helium bubble growth in tungsten

The accumulation of gas atoms in tungsten is a topic of long-standing interest to the plasma-facing materials community due the metal's use as a divertor material in some tokamak fusion reactors. The nucleation and growth of He/H gas bubbles (along with their isotopes) can result from impinging fluxes of these gases which give rise to damage at the W divertor surface. The inclusion of He or H in W has been studied extensively by the community, finding that He bubbles modify the surface through periodic dislocation punching and bursting mechanisms while H bubbles impact the metal through plastic-strain induced material failure. However, the mechanisms which are present during the combined flux of both He and H is not well-studied atomistically. Motivated by this, an atomistic modeling study is conducted using molecular dynamics to assess the behavior of mixed concentration He:H bubbles in W. Here we find that the introduction of H into a growing He bubble results in a dramatic change in the nature and presence of dislocation loops which are typically generated via dislocation punching in over-pressurized He bubbles. Most notably, at high H concentrations, there is a switchover in energetic favorability from glissile 1/2<111> dislocations to sessile <100> dislocations. This thermodynamic crossover could imply a significant reduction in W surface morphology changes than with pure He bubbles and, additionally, we show this to have implications on the trapping of H in the bubbles and their associated dislocations.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Systematic Study of Different Anion Doping on the Electrochemical Performance of Cobalt-Free Lithium–Manganese-Rich Layered Cathode

Regardless of the appealingly high energy density (1000 Wh kg –1 ) of the lithium–manganese-rich layered oxide cathode (LMR-NMO), this material still suffers from rapid capacity and voltage decay after continuous cycling. LMR-NMO involves the redox reaction of both transition metals and oxygen to gain additional capacity in comparison with a conventional NMC cathode. Due to the use of a high voltage range (beyond 4.4 V), the oxygen release from the structure initiates and in turn generates intergranular cracks and spinel formation, consequently, into rock-salt structure. Here, LMR-NMO with different doping ranges (1–5 mol %) of F, S, and Cl are being examined to summarize the benefits and drawbacks of each anion. This study shows that F is the best candidate as it increases average voltage (voltage retention 96–97% after 200 cycles at 0.5 C), improves ionic conductivity (nearly two times higher than pristine), reduces cation mixing, minimizes oxygen release, and offers high stability during high temperature cycle. However, for S and Cl, the results are conflicted. An optimal amount of anion dopants should be considered as the side effects might overcome the benefits when the doping amount is excessive.

25 ENERGY STORAGE↗
DOE OSTI2021

High-pressure high-temperature synthesis and thermal equation of state of high-entropy transition metal boride

High-entropy transition metal boride (Hf 0.2 Ti 0.2 Zr 0.2 Ta 0.2 Mo 0.2 )B 2 sample was synthesized under high-pressure and high-temperature starting from ball-milled oxide precursors (HfO 2 , TiO 2 , ZrO 2 , Ta 2 O 5 , MoO 3 ) mixed with graphite and boron-carbide. Experiments were conducted in a large-volume Paris Edinburgh press combined with an in-situ Energy Dispersive X-ray Diffraction. The hexagonal AlB 2 phase with an ambient pressure volume V 0 = 27.93 ± 0.03 Å 3 was synthesized at a pressure of 0.9 GPa and temperatures above 1373K. High-pressure high-temperature studies on the synthesized high-entropy transition metal boride sample were performed to 7.6 GPa and 1873 K. The thermal equation of state fitted to the experimental data resulted in an ambient pressure bulk-modulus K 0 = 344 ± 39 GPa, dK/dT = –0.108 ± 0.027 GPa/K, and a temperature dependent volumetric thermal expansion coefficient α = α 0 + α 1 T + α 2 T –2 . The thermal stability combined with a high bulk-modulus establishes this high-entropy transition metal boride as an ultrahard high-temperature ceramic material.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Evolution of the electronic structure in Ta 2 NiSe 5 across the structural transition revealed by resonant inelastic x-ray scattering

We utilized high-energy-resolution resonant inelastic X-ray scattering (RIXS) at both the Ta and Ni L 3 -edges to map out element-specific particle-hole excitations in Ta 2 NiSe 5 across the phase transition. Our results reveal a momentum dependent gap-like feature in the low energy spectrum, which agrees well with the band gap in element-specific joint density of states calculations based on ab initio estimates of the electronic structure in both the low temperature monoclinic and the high temperature orthorhombic structure. Below T c , the RIXS energy-momentum map shows a minimal gap at the Brillouin zone center (~0.16 eV), conforming that Ta 2 NiSe 5 possesses a direct band gap in its low temperature ground state. However, inside the gap, no signature of anticipated collective modes with an energy scale comparable to the gap size can be identified. Upon increasing the temperature to above T c , whereas the gap at the zone center closes, the RIXS map at finite momenta still possesses the gross features of the low temperature map, suggesting a substantial mixing between the Ta and Ni orbits in the conduction and valence bands, which does not change substantially across the phase transition. Our experimental observations and comparison to the theoretical calculations lend further support that the phase transition and the corresponding gap opening in Ta 2 NiSe 5 is largely structural by nature with possible minor contribution from the putative exciton condensate.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Ultra-high Q cavity-based search for the Dark Photon: new exclusion limit from Dark SRF phase 1 and step forward for phase 2

We present here the first results of Dark SRF, a light-shining-through-wall (LSW) experiment that leverages ultra-high quality factor superconducting radio frequency (SRF) cavities to search for dark photons. The use of Nb SRF cavities combined with a strict calibration and measurement protocol increased sensitivity to dark photons by several orders of magnitude compared to other LSW experiments, as demonstrated by our new limit that excluded a broad range of previously unstudied dark photon mass and mixing angle.In addition to the results of the search conducted in liquid helium using 1.3GHz SRF cavities, we also present the first steps of the second phase of the experiment, which will take place in a dilution refrigerator using 2.6GHz SRF cavities. These experiments are part of a wider effort of the Superconducting Quantum Materials and Systems (SQMS) Center to employ ultra-high Q SRF cavities to search for Beyond the SM particles and wavelike dark matter.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Dark SRF, a cavity-based search for the Dark Photon: new exclusion limit and path forward

The dark photon is a hypothesized particle in extension to the Standard Model (SM) that would weakly interact with ordinary SM photons. An effective way to search for hidden sector photons in a laboratory set up is through light-shining-through-wall (LSW) schemes.We present here the first results of Dark SRF, a LSW experiment that leverages ultra-high quality factor superconducting radio frequency (SRF) cavities to search for dark photons. The use of Nb SRF cavities combined with a strict calibration and measurement protocol increased sensitivity to dark photons by several orders of magnitude compared to other LSW experiments, as demonstrated by our new exclusion limit on the dark photon mixing angle.In addition to the results of the search conducted in liquid helium using 1.3GHz SRF cavities, we also present the first steps of the second phase of the experiment, which will take place in a dilution refrigerator using 2.6GHz SRF cavities.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Characterization of Flashback and Flame-Holding in a Jet-in-Crossflow Mixing Configuration with Methane-Hydrogen Fuel Blends

An approach that combines experimental and numerical analyses has been implemented to characterize the fundamentals of flashback events and flame-holding phenomena during high-hydrogen combustion in a jet-in-crossflow (JICF) configuration. Such flame dynamics are visualized experimentally using nanosecond (ns)-based hydroxyl planar laser-induced fluorescence (OH-PLIF) and chemiluminescence diagnostics techniques. The JICF burner has an optically accessible pre-mixing tube allowing the optical diagnostics. The testing was conducted for varied pre-mixer velocities (V) and equivalence ratio (ϕ) for 90%-100% (H2, by mole) H2/CH4 reactant mixtures at atmospheric temperature and pressure conditions. Two distinct flashback events were identified – conventional rich flashback and lean flashback, recorded while increasing ϕ and decreasing ϕ, respectively. The cause of lean flashback was attributed to lower momentum flux ratio which bends the jet sharply, closer toward the injection plane. The mean OH-PLIF images characterized the flame-holding behavior where the flame was found to be stabilized on the leeward side only or on both windward and leeward sides as a lifted flame near the fuel port. A large eddy simulation (LES) with detailed chemistry combustion modeling approach was implemented along with an OH* sub-mechanism, and it showed qualitative agreement with the integrated line-of-sight chemiluminescence results as well as the planar OH-PLIF measurements.

chemiluminescence diagnostic↗
NASA NTRS1969

Predicting transport properties of dilute gases.

Viscosity, thermal conductivity and diffusion predicted for dilute nonpolar, polar and mixed gases, discussing methods for rotational relaxation collision numbers and resonant correction

Brokaw, R. S.↗
NASA NTRS1971

Tracer techniques for urine volume determination and urine collection and sampling back-up system

The feasibility, functionality, and overall accuracy of the use of lithium were investigated as a chemical tracer in urine for providing a means of indirect determination of total urine volume by the atomic absorption spectrophotometry method. Experiments were conducted to investigate the parameters of instrumentation, tracer concentration, mixing times, and methods for incorporating the tracer material in the urine collection bag, and to refine and optimize the urine tracer technique to comply with the Skylab scheme and operational parameters of + or - 2% of volume error and + or - 1% accuracy of amount of tracer added to each container. In addition, a back-up method for urine collection and sampling system was developed and evaluated. This back-up method incorporates the tracer technique for volume determination in event of failure of the primary urine collection and preservation system. One chemical preservative was selected and evaluated as a contingency chemical preservative for the storage of urine in event of failure of the urine cooling system.

Ramirez, R. V.↗
NASA NTRS1989

Understanding transition and turbulence through direct simulations

Direct simulations consist in solving the full Navier-Stokes equations, without any turbulence model, and describing all the detailed features of the flow. Usually the flows are three-dimensional and time-dependent and contain both coarse and fine structures, which makes the numerical task very challenging in terms of both the algorithm and the computational effort. Most of the work until now has involved spectral methods, which are highly accurate but not very flexible in terms of geometry or complex equations. For that reason, future work will also rely on high-order finite-difference or other methods. Direct simulations complement experimental work, and both contribute to the theory and the empirical knowledge of turbulence. Once such a simulation has been shown to be accurate, the flow field is completely known in three dimensions and time, including the pressure, the vorticity and any other quantity. On the other hand, most simulations to date solved the incompressible equations in rather simple geometries, and direct simulations will always be limited to moderate Reynolds numbers. Extensive simulations have been conducted in homogeneous turbulence, channel flows, boundary layers, and mixing layers. Much effort is devoted to addressing flows with compressibility and chemical reactions, and to new geometries such as a backward-facing step.

Spalart, P. R.↗
NASA NTRS1991

Study of Rayleigh scattering for visualization of helium-air mixing at Mach 6

Using an ArF excimer laser, planar Rayleigh scattering measurements were performed to investigate helium mixing into air at supersonic speeds. These experiments were conducted in the Mach 6, high-Reynolds-number facility at NASA Langley Research Center. The capability of the Rayleigh scattering technique for flow visualization of a turbulent environment was demonstrated. The qualitative agreement between the averaged Rayleigh results and the reduced mean-mass-densities obtained from probe measurements substantiate that careful application of the technique, even in the presence of clusters, can give very useful results. It was also demonstrated that planar, quantitative measurements can be made in the absence of clusters.

Shirinzadeh, B.↗
NASA NTRS1992

Scramjet combustor and nozzle computations

The SHIP3D PNS code is used to conduct a 3D parametric study of a scramjet combustor and nozzle configuration at flight Mach numbers of 8, 10, 12, 16, and 20. The study demonstrated the powerful computational strategy of using a highly efficient, modified PNS code and a nonkinetic chemistry model to analyze test data and conduct parametric studies of scramjet combustors and nozzles. The mixing efficiency was found to decrease by 0.2 when the flight Mach number increased from 8 to 12 and showed little change at higher Mach numbers. The protruding ramp injector generated an oblique shock that impinged on the cowl. Ramp-slot injection produced better mixing, both because of the interaction of this shock with the slot fuel, and because of better fuel distribution in the duct. The former effect was enhanced when the ramp angle was increased. Mixing was also enhanced when the ramp fuel injection angle and sweep angle were increased.

Kamath, Pradeep S.↗
NASA NTRS2001

FUSE Observations of Warm Gas in the Cooling Flow Clusters A1795 and A2597

We present far-ultraviolet spectroscopy of the cores of the massive cooling flow clusters Abell 1795 and 2597 obtained with FUSE. As the intracluster gas cools through 3 x 10(exp 5)K, it should emit strongly in the O VI lambda(lambda)1032,1038 resonance lines. We report the detection of O VI (lambda)1032 emission in A2597, with a line flux of 1.35 +/- 0.35 x 10(exp -15) erg/sq cm s, as well as detection of emission from C III (lambda)977. A marginal detection of C III (lambda)977 emission is also reported for A1795. These observations provide evidence for a direct link between the hot (10(exp 7) K) cooling flow gas and the cool (10(exp 4) K) gas in the optical emission line filaments. Assuming simple cooling flow models, the O VI line flux in A2597 corresponds to a mass deposition rate of approx. 40 solar mass /yr within the central 36 kpc. Emission from O VI (lambda)1032 was not detected in A1795, with an upper limit of 1.5 x 10(exp -15) erg/sq cm s, corresponding to a limit on the mass cooling flow rate of M(28 kpc) less than 28M solar mass/ yr. We have considered several explanations for the lack of detection of O VI emission in A1795 and the weaker than expected flux in A2597, including extinction by dust in the outer cluster, and quenching of thermal conduction by magnetic fields. We conclude that a turbulent mixing model, with some dust extinction, could explain our O VI results while also accounting for the puzzling lack of emission by Fe(sub XVII) in cluster cooling flows.

Oegerle, W. R.↗
NASA NTRS2001

The Production of Complex Organics from Interstellar Ices

Infrared spectroscopy of ices in interstellar dense molecular clouds has shown that they contain a variety of simple molecules, as well as aromatic hydrocarbons. While in these clouds, these ices are processed by ultraviolet light and cosmic rays. High vacuum, UV irradiation laboratory simulations conducted using various realistic approx. 10 K interstellar mixed-molecular ice analogs, both with and without polycyclic aromatic hydrocarbons (PAHs), have been carried out in NASA-Ames' Astrochemistry Laboratory. Upon warming, these irradiated ices are found to produce refractory organic residues. These residues have been analyzed using a variety of techniques, including HPLC and laser desorption mass spectrometry, and they have been shown to contain a variety of complex organic compounds. Several of these compounds may be of prebiotic significance. In particular, we will discuss the detection of quinones (substituted PAHs that are used by living systems for electron transport) and amphiphiles (molecules that self-assemble to form membranes). Laboratory simulations have also demonstrated that the organic products can show isotopic enrichments in D that provide clues for the mechanisms of their formation. Similar compounds and D enrichments are seen in the organics found in primitive meteorites, suggesting a direct link between interstellar chemistry and the delivery of organics to newly formed planets.

Sandford, Scott A.↗
NASA NTRS2003

Changes in Polymeric Tether Properties Due to Atomic Oxygen

The Propulsive Small Expendable Deployer System (ProSEDS) mission is designed to provide an on-orbit demonstration of the electrodynamic propulsion capabilities of tethers in space. The ProSEDS experiment will be a secondary payload on a Delta II unmanned expendable booster. A 5-km conductive tether is attached to the Delta II second stage and collects current fiom the low Earth orbit (LEO) plasma to facilitate de-orbit of the spent stage. The conductive tether is attached to a 10-km non-conductive tether, which is then attached to an endmass containing several scientific instruments. Atomic oxygen (AO) erodes most organic materials. As the orbit of the Delta II second stage decas, the AO flux (atoms/sq cm sec) increases. A nominal AO fluence of 1 x l0(exp 21) atoms/sq cm was agreed upon by the investigators as an adequate level for evaluating the performance of the tether materials. A test series was performed to determine the effect of atomic oxygen (AO) on the mechanical integrity and possible strength loss of ProSEDS tether materials. The tether materials in this study were Dyneema, an ultra-high molecular weight polyethylene material used as the non-conducting portion of the ProSEDS tether, and the Kevlar core strength fiber used in the conductive tether. Samples of Dyneema and Kevlar were exposed to various levels of atomic oxygen up to 1.07 x 10(exp 21) atoms/sq cm in the Marshall Space Flight Center Atomic Oxygen Beam Facility (AOBF). Changes in mass were noted after AO exposure. The tethers were then tensile-tested until failure. AO affected both the Dyneema and Kevlar tether material strength. Dyneema exposed to 1.07 x 10(exp 21) atoms/sq cm of atomic oxygen failed due to normal handling when removed fiom the AOBF and was not tensile-tested. Another test series was performed to determine the effect of AO on the electrical properties of the ProSEDS conductive tether. The conductive tether consists of seven individually coated strands of 28 AWG 1350-0 aluminum wire. The conductive coating, developed by Triton Systems, Inc., is a mix of polyanaline and COR, a clear AO-resistant polymer.

Finckenor, Miria M.↗
NASA NTRS2017

LOX/Methane In-Space Propulsion Systems Technology Status and Gaps

Human exploration architecture studies have identified liquid oxygen (LOX)Methane (LCH4) as a strong candidate for both interplanetary and descent ascent propulsion solutions. Significant research efforts into methane propulsion have been conducted for over 50 years, ranging from fundamental combustion mixing efforts to rocket chamber and system level demonstrations. Over the past 15 years NASA and its partners have built upon these early activities that have demonstrated practical components and sub-systems needed to field future methane space transportation elements. These advanced development efforts have formed a foundation of LOXLCH4 propulsion knowledge that has significantly reduced the development risks of future methane based space transportation elements for human exploration beyond earth orbit. As a bipropellant propulsion system, LOXLCH4 has some favorable characteristics for long life and reusability, which are critical to lunar and Mars missions. Non-toxic, non-corrosive, self-venting, and simple to purge. No extensive decontamination process required as with toxic propellants. High vapor pressure provides for excellent vacuum ignition characteristics. Performance is better than current earth storable propellants for human scale spacecraft. Provides the capability for future Mars exploration missions to use propellants that are produced in-situ on Mars Liquid Methane is thermally similar to O2 as a cryogenic propellant, 90,111 K (LO2, LCH4 respectively) instead of the 23 K of LH2. Allows for common components and thus providing cost savings as compared to liquid hydrogen (LH2). Due to liquid methane having a 6x higher density than hydrogen, it can be stored in much smaller volumes. Cryogenic storage aspect of these propellants needs to be addressed. Passive techniques using shielding and orientations to deep space Refrigeration may be required to maintain both oxygen and methane in liquid forms

Propulsion systems↗