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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 685 records · Page 38
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

A Template-based Approach to the Photometric Classification of SN 1991bg-like Supernovae in the SDSS-II Supernova Survey

The use of SNe Ia to measure cosmological parameters has grown significantly over the past two decades. However, there exists a significant diversity in the SN Ia population that is not well understood. Overluminous SN 1991T-like and subluminous SN 1991bg-like objects are two characteristic examples of peculiar SNe. The identification and classification of such objects is an important step in studying what makes them unique from the remaining SN population. With the upcoming Vera C. Rubin Observatory promising on the order of a million new SNe over a 10 year survey, spectroscopic classifications will be possible for only a small subset of observed targets. As such, photometric classification has become an increasingly important concern in preparing for the next generation of astronomical surveys. Using observations from the Sloan Digital Sky Survey II (SDSS-II) SN Survey, we apply here an empirically based classification technique targeted at the identification of SN 1991bg-like SNe in photometric data sets. By performing dedicated fits to photometric data in the rest-frame redder and bluer bandpasses, we classify 16 previously unidentified 91bg-like SNe. Using SDSS-II host galaxy measurements, we find that these SNe are preferentially found in host galaxies with an older average stellar age than the hosts of normal SNe Ia. We also find that these SNe are found at a further physical distance from the center of their host galaxies. We find no statistically significant bias in host galaxy mass or specific star formation rate for these targets.

Astronomy & Astrophysics↗
DOE OSTI2024

Excitonic Shockley-Read-Hall recombination in organic semiconductors

Trap-mediated recombination influences the performance of a wide range of electronic devices. The well-known Shockley-Read-Hall (SRH) expression for inorganic semiconductors is often invoked to describe the recombination rate in organic materials, although without a clear understanding of how its parameters relate to the underlying material properties or how it should be modified to account for the finite lifetime of exciton intermediates in, for example, the doped emissive layer of an organic light-emitting diode (OLED). Here, we formalize SRH recombination for organic semiconductors based on diffusive trapping and Langevin recombination. We show that including the exciton state suppresses the recombination rate in host-guest systems with type II energy level alignment whenever the interfacial gap between the host and guest molecular orbitals is comparable to the exciton energy. Furthermore, these results quantify the balance between bimolecular and trap-mediated recombination in doped OLED emissive layers, and indicate that devices with type II host-guest pairings can, in principle, beat the thermodynamic limit of their neat guest counterparts.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Rossi-alpha Uncertainty Quantification by Analytic, Bootstrap, and Sample Methods to Inform Fitting Best Practices

The prompt neutron period (the negative reciprocal of the prompt neutron decay constant) can be estimated using the Rossi-alpha technique that is predicated on fitting Rossi alpha histograms and of interest in nuclear criticality safety and nonproliferation. The histograms are traditionally fit with a one-exponential model; however, recent work has proposed a two-exponential model to account for reflector induced phenomenon. Until recently, the uncertainty quantification for either model was inadequate (inaccurate and demanded large measurement times). Measurement uncertainty quantification by sample and analytic methods was developed and validated in Ref. The purpose of this transaction is to (i) validate a new bootstrap method by comparing bin-by-bin error bar estimates and (ii) demonstrate how to choose bin widths and reset times to optimize precision and accuracy.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Fiber-Optic Raman Probe for On-line EAF Slag Analysis

Here, in Electric Arc Furnace (EAF) steelmaking, the push for improved efficiency requires accurate analysis of the chemical composition of its slag system to control slag foaming, provide refractory protection, and maintain high furnace iron yield. Therefore, the ability to obtain real-time slag chemistry data would provide a useful tool to improve the control and efficiency of the process. The work reported here aims to assess the structure and chemistry of EAF slags at high temperatures using a portable fiber-optic Raman probe. As a result, the ability to relate Raman spectra peaks to chemistry and structure is demonstrated in experimental result with EAF slags at 1550°C.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

13 C ENDOR Characterization of the Central Carbon within the Nitrogenase Catalytic Cofactor Indicates That the CFe 6 Core Is a Stabilizing “Heart of Steel”

Substrates and inhibitors of Mo-dependent nitrogenase bind and react at Fe ions of the active-site FeMo-cofactor [7Fe–9S–C–Mo–homocitrate] contained within the MoFe protein α-subunit. The cofactor contains a CFe 6 core, a carbon centered within a trigonal prism of six Fe, whose role in catalysis is unknown. Targeted 13 C labeling of the carbon enables electron-nuclear double resonance (ENDOR) spectroscopy to sensitively monitor the electronic properties of the Fe–C bonds and the spin-coupling scheme adopted by the FeMo-cofactor metal ions. Here this report compares 13 CFe 6 ENDOR measurements for (i) the wild-type protein resting state (E 0 ; α-Val 70 ) to those of (ii) α-Ile 70 , (iii) α-Ala 70 -substituted proteins; (iv) crystallographically characterized CO-inhibited “hi-CO” state; (v) E 4 (4H) Janus intermediate, activated for N 2 binding/reduction by accumulation of 4[ e– /H + ]; (vi) E 4 (2H)* state containing a doubly reduced FeMo-cofactor without Fe-bound substrates; and (vii) propargyl alcohol reduction intermediate having allyl alcohol bound as a ferracycle to FeMo-cofactor Fe6. All states examined, both S = 1/2 and 3/2 exhibited near-zero 13 C isotropic hyperfine coupling constants, $^Ca$ = [-1.3 ↔ +2.7] MHz. Density functional theory computations and natural bond orbital analysis of the Fe-C bonds show that this occurs because a (3 spin-up/3 spin-down) spin-exchange configuration of CFe 6 Fe-ion spins produces cancellation of large spin-transfers to carbon in each Fe–C bond. Previous X-ray diffraction and DFT both indicate that trigonal-prismatic geometry around carbon is maintained with high precision in all these states. The persistent structure and Fe–C bonding of the CFe 6 core indicate that it does not provide a functionally dynamic (hemilabile) “beating heart”-instead it acts as “a heart of steel”, stabilizing the structure of the FeMo-cofactor-active site during nitrogenase catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Metasomatic Alteration of Type 3 Ordinary and Carbonaceous Chondrites

Metasomatism refers to the process during which a pre-existing rock undergoes compositional and mineralogical transformations associated with chemical reactions triggered by the reaction of fluids which invade the protolith. It changes chemical compositions of minerals, promotes their dissolution and precipitation of new minerals. In this paper, we review metasomatic alteration of type 3 ordinary (H, L, LL) and carbonaceous (CV, CO, CK) chondrites, including (i) secondary mineralization, (ii) physicochemical conditions, (iii) chronology ( 53 Mn- 53 Cr, 26 Al- 26 Mg, 129 I- 129 Xe) of metasomatic alteration, (iv) records of metasomatic alteration in H, O, N, C, S, and Cl isotopic systematics, (v) effects of metasomatic alteration on O- and Al-Mg-isotope systematics of primary minerals in chondrules and refractory inclusions, and (vi) sources of water ices in metasomatically altered CV, CO, and ordinary chondrites, and outline future studies.

129I-129Xe chronology↗
DOE OSTI2022

Single-Photon-Induced Electron Spin Polarization of Two Exchange-Coupled Stable Radicals

Transient electron paramagnetic resonance spectroscopy has been used to probe photoinduced electron spin polarization of a stable exchange-coupled organic biradical in a Pt(II) complex comprising 4,4'-di-tert-butyl-2,2'-bipyridine (bpy) and 3,6-bis(ethynyl-para-phenyl-nitronyl nitroxide)-o-catecholate (CAT(o-C$\equiv$C-Ph-NN) 2 ). Photoexcitation results in four unpaired spins in excited states of this complex, with spins being localized on each of the two radicals, CAT •+ and bpy •– . The four spins are all exchange-coupled in these excited states, and an off-diagonal matrix element in the CAT •+ -NN exchange allows for exchange-enhanced intersystem crossing to the 3 T 1a state, which possesses (bpy •– )Pt(CAT •+ ) chromophoric triplet character. Further, fast mixing between this 3 T 1a state and other thermally accessible excited LL'CT state(s) followed by fast relaxation provides spin polarization of the exchange-coupled NN radicals in the 3 S 0 ground state of the complex. Our results demonstrate that well-defined quantum states of a ground-state biradical can be initialized with single-photon excitation and have the potential for further spin manipulation directed toward quantum information science applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Impact of Thermonuclear Reaction Rate Uncertainties on the Identification of Presolar Grains from Classical Novae

Approximately 30%–40% of classical novae generate dust between 20 and 100 days following the eruption. However, there has yet to be a definitive identification of presolar stardust grains originating from classical novae. While multiple studies have suggested a nova origin for specific grains, aligning simultaneously all measured isotopic ratios of a specific grain with those predicted from simulations remains challenging. Using Monte Carlo simulations, this work investigates how uncertainties in thermonuclear reaction rates influence the isotopic ratios predicted in simulations of classical novae, specifically impacting the identification of presolar grains. In particular, we address two questions: (i) What is the impact of uncertainties in reaction rates on the range of isotopic ratios predicted by classical nova simulations? (ii) Which reaction rate uncertainties most significantly influence the predicted abundance ratios in presolar grains? Our results show that current reaction rate uncertainties affect the isotopic ratios of 12 C/ 13 C, 14 N/ 15 N, 16 O/ 17 O, 16 O/ 18 O, 24 Mg/ 25 Mg, 24 Mg/ 26 Mg, 26 Al/ 27 Al, and 28 Si/ 29 Si by less than 20% in either carbon–oxygen or oxygen–neon (ONe) novae, especially when considering the mixing of matter throughout the entire envelope. However, the isotopic ratios of 28 Si/ 30 Si, 32 S/ 33 S, and 32 S/ 34 S in ONe novae are exceptions: their variability greatly exceeds a factor of 2 due to the uncertainties in the reaction rates of 30 P(p,γ) 31 S, 33 S(p,γ) 34 Cl, and 34 S(p,γ) 35 Cl, respectively. These results highlight the significant influence of specific reaction rates on the predicted abundance ratios and underscore the necessity for accurate nuclear measurements to reduce these uncertainties.

Classical novae↗
DOE OSTI2023

Method for conversion of diols to olefin products

A method for converting a diol in solution to an olefin fraction, the method comprising: (i) reacting a diol of the formula HO—R—OH in solution with a carbonyl-containing molecule of the formula: in the presence of an acid catalyst to result in a dioxolane molecule of the formula: wherein R is a hydrocarbon linker containing 1-12 carbon atoms, and R 1 and R 2 are independently selected from hydrogen atom and hydrocarbon groups containing 1-12 carbon atoms, wherein R 1 and R 2 optionally interconnect; (ii) removing the dioxolane molecule from the solution by phase separation; and (iii) contacting the dioxolane molecule with a metal-loaded zeolite at a temperature of 100-500° C. to convert the dioxolane molecule to an olefin fraction.

Li, Zhenglong↗
DOE OSTI2024

Atomically dispersed platinum-group metal-free catalysts and method for synthesis of the same

Atomically dispersed platinum-group metal-free catalyst and method for synthesizing the same. According to one embodiment, the catalyst is made by a method in which, in a first step, a metal oxide/zeolitic imidazolate frameworks (ZIF) composite is formed by combining (i) nanoparticles of an oxide of at least one of iron, cobalt, nickel, manganese, and copper, (ii) a hydrated zinc salt, and (iii) an imidazole. Then, in a second step, the metal oxide/ZIF composite is thermally activated, i.e., carbonized, to form an M-N—C catalyst. Thereafter, the M-N—C catalyst may be mixed with a quantity of ammonium chloride, and then the M-N—C/NH 4 Cl mixture may be pyrolyzed. The foregoing NH 4 Cl treatment may improve the intrinsic activity of the catalyst. Then, a thin layer of nitrogen-doped carbon may be added to NH 4 Cl-treated M-N—C catalyst by chemical vapor deposition (CVD). Such CVD treatment may improve the stability of the catalyst.

Wu, Gang↗
DOE OSTI2022

Kinetic Model for the Reduction of Cu II Sites by NO + NH 3 and Reoxidation of NH 3 -Solvated Cu I Sites by O 2 and NO in Cu-SSZ-13

In this work, a kinetic model is developed for the reduction of Cu II sites by NO + NH 3 and the reoxidation of NH 3 -solvated Cu I sites by O 2 and NO in Cu-SSZ-13. Fourier transform infrared (FTIR) spectroscopy and spatially resolved capillary inlet mass spectrometry (SpaciMS) measurements during transient reactor experiments are utilized to identify the rate parameters associated with NO + NH 3 RHC (reduction half-cycle), proposed to occur via two distinct pathways involving adsorbed NH 3 and gas-phase NH 3 . The resulting NO + NH 3 RHC model is validated using spatiotemporal N 2 measurements covering a wide range of temperatures (200–450 °C) and space velocities (53,000–640,000 h –1 ). N 2 O formation is observed and modeled during NO + NH 3 RHC, with quantitative validation under standard selective catalytic reduction (SCR) conditions. Experimentally measured enthalpic and entropic changes associated with O 2 adsorption on NH 3 -solvated Cu I (ZCu(NH 3 ) 2 ) complexes [ Kamasamudram, K. Catal. Today 2010 , 151 (3–4), 212-222], along with activation energies estimated computationally for the intercage diffusion of ZCu(NH 3 ) 2 complexes [ Paolucci, C. Science 2017 , 357 (6 354), 898-903], are incorporated into a mean field kinetic model for the low-temperature oxidation half-cycle (OHC). Significant NH 3 release is observed during the isothermal oxidation of Cu I sites, attributed to desorption of NH 3 ligands from NH 3 -solvated Cu II dimers (Z 2 Cu 2 (NH 3 ) 4 O 2 ). Reduction of these dimeric complexes leads to the consumption of one NO/Cu II , contradicting the expected reduction stoichiometry. Inclusion of a global Arrhenius rate for the NO titration of Z 2 Cu 2 (NH 3 ) 4 O 2 complexes provides accurate representations of standard SCR on reduced and oxidized catalysts, predicting transient NO and NH 3 consumption between 150 and 250 °C as a function of hydrothermal aging. Deactivation of low-temperature standard SCR by NH 3 is observed at high NH 3 pressures, modeled via the formation of superoxo amino (ZCu(NH 3 ) 3 OO*) complexes during NH 3 titration of Z 2 Cu 2 (NH 3 ) 4 O 2 complexes [ Negri, C. J. Am. Chem. Soc. 2020 , 142 (37), 15884-15896]. The redox kinetic model presented here provides a foundational description of active site redox during low-temperature standard SCR, combining the recent kinetic, spectroscopic, and computational findings on the mechanism of standard SCR over Cu-SSZ-13.

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

Towards Elucidating Structure–Spectra Relationships in Rhamnogalacturonan II: Computational Protocols for Accurate 13C and 1H Shifts for Apiose and Its Borate Esters

Apiose is a naturally occurring, uncommon branched-chain pentose found in plant cell walls as part of the complex polysaccharide Rhamnogalacturonan II (RG-II). The structural elucidation of the three-dimensional structure of RG-II by nuclear magnetic resonance (NMR) spectroscopy is significantly complicated by the ability of apiose to cross-link via borate ester linkages to form RG-II dimers. Here, we developed a computational approach to gain insight into the structure–spectra relationships of apio–borate complexes in an effort to complement experimental assignments of NMR signals in RG-II. Our protocol involved structure optimizations using density functional theory (DFT) followed by isotropic magnetic shielding constant calculations using the gauge-invariant atomic orbital (GIAO) approach to predict chemical shifts. We evaluated the accuracy of 23 different functional–basis set (FBS) combinations with and without implicit solvation for predicting the experimental 1 H and 13 C shifts of a methyl apioside and its three borate derivatives. The computed NMR predictions were evaluated on the basis of the overall shift accuracy, relative shift ordering, and the ability to distinguish between dimers and monomers. We demonstrate that the consideration of implicit solvation during geometry optimizations in addition to the magnetic shielding constant calculations greatly increases the accuracy of NMR chemical shift predictions and can correctly reproduce the ordering of the 13 C shifts and yield predictions that are, on average, within 1.50 ppm for 13 C and 0.12 ppm for 1 H shifts for apio–borate compounds.

BASIC BIOLOGICAL SCIENCES,BIOMASS FUELS↗
DOE OSTI2025

Suppression of neutral-pion production in deep-inelastic scattering off nuclei with the CLAS detector

We present the first threefold differential measurement for neutral-pion multiplicity ratios produced in semi-inclusive deep-inelastic electron scattering on carbon, iron, and lead nuclei normalized to deuterium from CLAS at Jefferson Lab. We found that the neutral-pion multiplicity ratio is maximally suppressed for the leading hadrons (energy fraction 𝑧 → 1), suppression varying from 25% in carbon up to 75% in lead. An enhancement of the multiplicity ratio at low 𝑧 and high 𝑝$^2_𝑇$ is observed, suggesting an interconnection between these two variables. This behavior is qualitatively similar to the previous twofold differential measurement of charged pions by the HERMES Collaboration and, recently, by CLAS Collaboration. The largest enhancement was observed at high 𝑝$^2_𝑇$ for heavier nuclei, namely, iron and lead, while the smallest enhancement was observed for the lightest nucleus, carbon. This behavior suggests a competition between partonic multiple scattering, which causes enhancement, and hadronic inelastic scattering, which causes suppression.

color confinement↗
DOE OSTI2022

Mechanisms of Retention and Transport of Fission Products in Virgin and Irradiated Nuclear Graphite

To fulfill the design and licensing requirements for advanced reactors, the U.S. Department of Energy (DOE) is specifically interested in targeted research to quantify the mechanisms of fission product transport and retention in graphitic grades that will likely be used in next-generation very/high temperature reactors, fluoride salt-cooled high temperature reactors and molten salt reactors. We have examined an integrated experimental-computational approach to determine the diffusivities of selected fission products – ruthenium (Ru) and silver (Ag) in five nuclear graphite grades – POCO AXF-5Q, POCO ZXF-5Q, PCEA, IG110, and NBG-18. Experimental investigation for diffusion of other fission products (iodine, cesium, and krypton) in graphite could not be carried out due to extreme evaporation due to high vapor pressure, despite several attempts incorporating various experimental schemes. Experimental investigation with irradiated graphite could not be carried out because necessary approval to transport irradiated graphite could not be obtained due to procedural reasons at ORNL and national policy change in UK. An effort was made to “produce” by ion sputtering, but it was discontinued because the outcome did not adequately represent irradiated graphite. Thin film and “cup-and-cap” methods were employed to deposit fission products, diffusion annealed were carried out in an argon atmosphere, and concentration profiles were determined by dynamic secondary ion mass spectroscopy depth profiling technique. Regardless of graphite type, anomalous diffusion behavior of Ru (i.e., lower than expected based on Arrhenius temperature dependence) at an intermediate temperature, around 600 to 700 °C, was observed. Diffusion behavior of silver on the other hand agreed well to the Arrhenius temperature dependence although the excessive evaporation of silver hampered the accurate determination of diffusivities at temperature higher than 900 °C. In general, silver was observed to diffuse faster than Ru in the temperature range compared from 500 to 900 °C, had consistently had higher pre-exponential factor corresponding to higher jump frequency. To understand the abnormal diffusional behavior of Ru in graphite in intermediate temperature range, a detailed microstructural analysis was carried out. Clustering of Ru into particles on the surface of graphite was observed around 700 °C corresponding to de-wetting and spheroidization. This change would influence the boundary condition of diffusion, although features of clustering was much smaller (<1 mm) than the SIMS raster size (120 x 120 mm). Raman spectroscopy also demonstrated that Raman peak intensity for Ru decreased significantly for samples annealed higher than 700 °C and presence of Ru in graphite altered the crystallinity of graphite. To further elucidate the abnormal diffusion behavior observed in intermediate temperature investigated, the vibrational properties of graphene, bilayer graphene and Kr atoms in bilayer graphene were investigated with molecular dynamics. Krypton, which is a fission product, was introduced between a bilayer graphene system to evaluate (i) whether the phonon dispersion curves change with high temperature in bilayer graphene (ii) whether the addition of Kr atoms between the bilayer introduces any significant change in the vibrational properties, and (iii) whether any change in the vibrational properties can be correlated to the diffusive behavior of Kr atoms. The results show that the Kr atoms indeed exhibit an anomalous diffusive behavior at 550°C. Phonon analysis shows that a few phonon frequencies are enhanced as much as 20 to 30 % with the addition of just 0.2 at.% Kr. So, this may explain the unexpected self-diffusivity of fission products.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Measurement of beam-recoil observables 𝐶 𝑥 and 𝐶 𝑧 for 𝐾 + ⁢Λ photoproduction

Exclusive photoproduction of 𝐾 + ⁢Λ final states off a proton target has been an important component in the search for missing nucleon resonances and our understanding of the production of final states containing strange quarks. Polarization observables have been instrumental in this effort. The current work is an extension of previously published CLAS results on the beam-recoil transferred polarization observables 𝐶 𝑥 and 𝐶 𝑧 . Here, we extend the kinematic range up to invariant mass 𝑊 = 3.33 GeV from the previous limit of 𝑊 = 2.5 GeV with significantly improved statistical precision in the region of overlap. These data will provide for tighter constraints on the reaction models used to unravel the spectrum of nucleon resonances and their properties by not only improving the statistical precision of the data within the resonance region, but also constraining 𝑡-channel processes that dominate at higher 𝑊 but extend into the resonance region.

Electrons↗
DOE OSTI2022

Four-Coordinate Fe N 2 and Imido Complexes Supported by a Hemilabile NNC Heteroscorpionate Ligand

Inspired by mechanistic proposals for N 2 reduction at the nitrogenase FeMo cofactor, we report herein a new, strongly σ-donating heteroscorpionate ligand featuring two weak-field pyrazoles and an alkyl donor. This ligand supports four-coordinate Fe(I)-N 2 , Fe(II)-Cl, and Fe(III)-imido complexes, which we have characterized using a variety of spectroscopic and computational methods. Structural and quantum mechanical analysis reveal the nature of the Fe–C bonds to be essentially invariant between the complexes, with conversion between the (formally) low-valent Fe-N 2 and high-valent Fe-imido complexes mediated by pyrazole hemilability. This presents a useful strategy for substrate reduction at such low-coordinate centers and suggests a mechanism by which FeMoco might accommodate the binding of both π-acidic and π-basic nitrogenous substrates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Sub-quarter micrometer periodically poled Al 0.68 Sc 0.32 N for ultra-wideband photonics and acoustic devices

In this study, we demonstrate the ability of polarity inversion of sputtered aluminum scandium nitride thin films through post-fabrication processes with domain widths as small as 220 nm at a periodicity of 440 nm. An approach using photo- and electron-beam lithography to generate sub-quarter micrometer feature size with adjustable duty cycle through a lift-off process is presented. Here, the film with a coercive field $E_c^+$ of 5.35 MV/cm was exercised first with a 1 kHz triangular double bipolar wave and ultimately poled with a 0.5 kHz double monopolar wave using a Radiant Precision Premier II tester. The metal polar (M-polar) and nitrogen polar (N-polar) domains were identified and characterized through potassium hydroxide wet etching as well as piezoresponse force microscopy (PFM). Well-distinguished boundaries between the oppositely polarized domain regions were confirmed through the phase diagram of the PFM results. The relationship between the electrode width, poling voltage, and domain growth was experimentally studied and statistically analyzed, where 7.96 nm/V domain width broadening vs escalating poling voltage was observed. This method produces extremely high domain spatial resolution in III-nitride materials via poling and is transferable to a CMOS-compatible photolithography process. The spatial resolution of the periodically poled Al 0.68 Sc 0.32 N is suitable for second-harmonic generation of deep ultraviolet through quasi-phase-matching and RF MEMS operating in the X-Band spectrum.

36 MATERIALS SCIENCE↗