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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 OSTI2025

Chemical Interface Damping Revealed by Single-Particle Absorption Spectroscopy

Plasmon-induced interfacial charge separation is a promising way to efficiently extract energetic carriers through direct plasmon decay. This mechanism of charge transfer has been investigated by single-particle scattering spectroscopy, which measures the homogeneous plasmon line width. The line width is broadened by charge transfer, generally known as chemical interface damping. However, conflicting reports exist regarding the effect of chemical interface damping on the corresponding single-particle absorption spectrum, which is needed to accurately determine absolute light conversion efficiencies. This work aims to resolve this question by directly correlating absorption and scattering spectra of individual gold nanorods in the presence and absence of a charge-accepting interface. We find that for TiO 2 coated nanorods, the absorption line width is indeed broadened due to chemical interface damping but is overall narrower than the scattering line width. Here, chemical interface damping is furthermore found to increase with larger resonance energies. The observed differences in line widths between absorption and scattering are elucidated within the context of an analytically tractable model describing the lowest energy optically bright and higher-order optically dark plasmon modes of the nanorod, including bulk, radiative, and chemical interface damping effects. Taken together, these results establish that single-particle absorption spectroscopy is capable of revealing interfacial charge injection by direct plasmon decay.

absorption↗
NASA NTRS2021

INTEGRAL reloaded: Spacecraft, instruments and ground system

The European Space Agency’s INTErnational Gamma-Ray Astrophysics Laboratory (ESA/INTEGRAL) was launched aboard a Proton-DM2 rocket on 17 October 2002 at 06:41 CEST, from Baikonur in Kazakhstan. Since then, INTEGRAL has been providing long, uninterrupted observations (up to about 47 h, or 170 ksec, per satellite orbit of 2.7 days) with a large field-of-view (FOV, fully coded: 100 deg), millisecond time resolution, keV energy resolution, polarization measurements, as well as additional wavelength coverage at optical wavelengths. This is realized by two main instruments in the 15 keV to 10 MeV energy range, the spectrometer SPI (spectral resolution 3 keV at 1.8 MeV) and the imager IBIS (angular resolution: 12 arcmin FWHM), complemented by X-ray (JEM-X; 3–35 keV) and optical (OMC; Johnson V-band) monitor instruments. All instruments are co-aligned to simultaneously observe the target region. A particle radiation monitor (IREM) measures charged particle fluxes near the spacecraft. The Anti-coincidence subsystems of the main instruments, built to reduce the background, are also very efficient all-sky γ-ray detectors, which provide virtually omni-directional monitoring above ~75 keV. Besides the long, scheduled observations, INTEGRAL can rapidly (within a couple of hours) re-point and conduct Target of Opportunity (ToO) observations on a large variety of sources. INTEGRAL observations and their scientific results have been building an impressive legacy: The discovery of currently more than 600 new high-energy sources; the first-ever direct detection of (56)Ni and (56)Co radio-active decay lines from a Type Ia supernova; spectroscopy of isotopes from galactic nucleo-synthesis sources; new insights on enigmatic positron annihilation in the Galactic bulge and disk; and pioneering gamma-ray polarization studies. INTEGRAL is also a successful actor in the new multi-messenger astronomy introduced by non-electromagnetic signals from gravitational waves and from neutrinos: INTEGRAL found the first prompt electromagnetic radiation in coincidence with a binary neutron star merger. Up to now more than 1750 scientific papers based on INTEGRAL data have been published in refereed journals. In this paper, we will give a comprehensive update of the satellite status after more than 18 years of operations in a harsh space environment, and an account of the successful Ground Segment.

Erik Kuulkers↗
DOE OSTI2020

Shape evolution of neutron-rich 106,108,110 Mo isotopes in the triaxial degree of freedom

Background: Neutron-rich nuclei with mass number between 100 and 110 attract much attention, since several kinds of shapes, such as spherical, prolate, oblate, and triaxial shapes, are predicted. In particular, for neutron-rich Mo isotopes, different models predict different magnitudes and rigidity of triaxial deformation. Previous interpretations of experimental results based solely on low-lying $2^+_2$ states are insufficient to distinguish between the rigid triaxial shape, $\gamma$ vibration, or $\gamma$-soft rotor. Purpose: The shape evolution of 106 Mo, 108 Mo, and 110 Mo is investigated through their $2^+_1$-state lifetimes, decay-branching ratios of the $2^+_2$ state, and energies of the low-lying collective excited states with $K^π = 0^+, 2^+$, and $4^+$. Method: $\beta$-delayed $\gamma$-ray spectroscopy was employed for neutron-rich Nb and Zr isotopes produced at the RIKEN RI Beam Factory to populate excited states in 106 Mo, 108 Mo, and 110 Mo. The EUroball-RIKEN Cluster Array was used for high-resolution $\gamma$-ray detection and lifetimes of the $2^+_1$ states were determined using the UK fast-timing array of LaBr 3 (Ce) detectors. Results: New $\gamma$-ray transitions and levels are reported, including newly assigned $0^+_2$ states in 108,110 Mo. Quadrupole deformations were obtained for 106,108,110 Mo from their $2^+_1$ energies and lifetimes. The $\beta$-delayed neutron-emission probabilities of 108 Nb and 110 Nb were determined by examining the $\gamma$ rays of their respective daughter decays. Conclusions: In this work, the even-odd energy staggering in the $2^+_2$ band was compared with typical patterns of the $\gamma$-vibrational band, rigid triaxial rotor, and $\gamma$-soft rotor. The very small even-odd staggering of 106 Mo, 108 Mo, and 110 Mo favors a $\gamma$-vibrational band assignment. The kinematic moment of inertia for the $2^+_2$ band showed a trend similar to the ground-state band, which is as expected for the $\gamma$-vibrational band. Beyond-mean-field calculations employing the constrained Hartree-Fock-Bogoliubov and local quasiparticle-random-phase approximation method using the SLy5 + T interaction reproduced the ground and $2^+_2$ bands in 106 Mo and 108 Mo. The collective wave functions are consistent with the interpretation of the $2^+_2$ band as the $\gamma$-vibrational band of the prolate shape. However, the staggering pattern observed in 110 Mo differs from the one suggested in the calculations which predict a $\gamma$-soft rotor. There was no experimental indication of the oblate shape or the $\gamma$-soft rotor predicted in these Mo isotopes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2026

Isospin symmetry holds beyond the proton drip line: First observation of excited states in 55Cu

Isospin symmetry, combined with shell-model description, has long been successful in reproducing nuclear structure and predicting mirror energy differences. However, these descriptions have been primarily limited to mirror nuclei with well-bound ground states. As one approaches the proton drip line, coupling to the continuum becomes important. Despite this, little is known about medium-mass nuclei at the drip line. Here we report the measurement of the excitation energies of several unbound states in a nucleus beyond the proton drip line, 55Cu, performed via γ-ray spectroscopy at the Radioactive Isotope Beam Factory (RIKEN). Several low-lying yrast states are observed to decay predominantly by γ-ray emission. In contrast, the state–predicted to be strongly populated in the one-proton knockout reaction–is notably absent, suggesting that it decays primarily via prompt proton emission. We show that even for such an unbound system, shell-model calculations based on a harmonic oscillator potential reproduce the observed mirror energy differences remarkably well in all the observed states. Based on this result, we propose that a general pattern might emerge where, in medium-mass systems at the proton drip line, the stronger Coulomb barrier together with the centrifugal barrier effectively confines the wave functions, so that the shell model is able to describe low-lying states, enabling accurate predictions of mirror energy differences between isobaric analogue states.

Pigliapoco, S [Dipartimento di Fisica e Astronomia↗
DOE OSTI2023

Extracting spinon self-energies from two-dimensional coherent spectroscopy

Two-dimensional coherent spectroscopy (2DCS) is a nonlinear spectroscopy technique capable of identifying whether apparent continua in linear response are made out of multiplets of sharp deconfined quasiparticles. This makes it a potent tool for experimental identification of fractionalized phases. Previous discussions have focused on limits where the quasiparticles in question are infinitely long lived. In this paper we discuss 2DCS in the regime where the fractionalized quasiparticles can themselves decay. We introduce a powerful path-integral-based approach, whereby the computation of nonlinear susceptibilities reduces to an efficient exercise in diagrammatic perturbation theory. Here, we apply this method to compute the 2DCS response of the one-dimensional transverse field Ising model, in the presence of integrability-breaking perturbations. We discuss aspects of the self-energy of the fractionalized quasiparticles that may be extracted via 2DCS, such as the momentum-dependent decay rate.

1-dimensional spin chains↗
DOE OSTI2022

Dual Passivation of Cathode and Anode through Electrode–Electrolyte Interface Engineering Enables Long-Lifespan Li Metal–SPAN Batteries

The reliability and durability of lithium metal (Li 0 )–sulfur batteries are largely limited by the undesired Li 0 plating-stripping irreversibility and the detrimental polysulfide dissolution, yet approaches that can simultaneously address the above anodic and cathodic problems are scarce. In this study, we report the stable operation of a Li 0 -SPAN (sulfurized polyacrylonitrile) battery via an anode–cathode dual-passivation approach. By combination of a fluorinated localized high concentration electrolyte (LHCE) and a Li 3 N-forming additive (TMS-N 3 ), robust and highly conductive electrode passivation layers are formed in situ on the surface of both the Li 0 anode and the SPAN cathode. The resulting highly reversible, dendrite-free, and high-density Li 0 plating morphology enables a high Coulombic efficiency of 99.4%. Advanced tender energy X-ray spectroscopy also reveals the eliminated Li 2 S formation and minimized polysulfide dissolution in SPAN cathodes, leading to a high capacity of 580 mAh/g SPAN and stable cycling with negligible capacity decay (0.7%) for 800 cycles. This electrode–electrolyte interphase engineering strategy has tackled the major limitations of Li–S batteries in both ether- and carbonate-based electrolyte systems and under a wide temperature range from –10 to +50 °C, thus providing insightful guidelines for the rational design of highly durable and high-energy-density Li 0 -S batteries.

25 ENERGY STORAGE↗
DOE OSTI2020

Ultrafast dynamics of 2-thiouracil investigated by time-resolved Auger spectroscopy

In this paper, we present time-resolved ultraviolet-pump x-ray probe Auger spectra of 2-thiouracil. An ultraviolet induced shift towards higher kinetic energies is observed in the sulfur 2p Auger decay. The difference Auger spectra of pumped and unpumped molecules exhibit ultrafast dynamics in the shift amplitude, in which three phases can be recognized. In the first 100 fs, a shift towards higher kinetic energies is observed, followed by a 400 fs shift back to lower kinetic energies and a 1 ps shift again to higher kinetic energies. We use a simple Coulomb-model, aided by quantum chemical calculations of potential energy states, to deduce a C-S bond expansion within the first 100 fs. The bond elongation triggers internal conversion from the photoexcited S 2 to the S 1 state. Based on timescales, the subsequent dynamics can be interpreted in terms of S 1 nuclear relaxation and S 1 -triplet internal conversion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Using cyclotron radiation emission for ultra-high resolution x-ray spectroscopy

Abstract Cyclotron radiation emission spectroscopy (CRES) is an approach to measuring the energy of an electron trapped in an externally applied magnetic field. The bare electron can come from different interactions, including photoelectric absorption, Compton scatters, beta decay, and pair production. CRES relies on measuring the frequency of the electron’s cyclotron motion, and because the measurement times extend over 10 6 –10 7 cycles, the energy resolution is on the order of a single electronvolt. To date, CRES has only been performed on internal beta-emitting radioisotopes, but the technology can be applied to x-ray spectrometery through appropriate selection of a target gas and sufficient intensity of the distinct x-ray source. The applications of this technology range from high-precision measurements of atomic energy levels to calibrations of basic science experiments, to trace element identification. In this work we explore the use of CRES for x-ray spectroscopy within the rubric of measuring the energy levels of argon. Though the energy levels of argon are well established, we adopt this motivation as an example question around which a detector may be designed. The issues we explore include target material, density, electron trapping depth, noise levels, and overall efficiency. We also discuss spectral deconvolution and how the multiple peaks obtained from a single target/source pair can be used to enhance the robustness of the measurement.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2024

237 Np Fission Spectrum Cumulative Fission Product Yield Measurement Using Godiva IV Critical Assembly

Precise integral measurement of fast neutron-induced fission product yields for various actinides is of high interest for applied nuclear science. The goal of this effort is to improve uncertainties in fission product yield values of 237 Np. Fission was induced in a NpO 2 (NO 3 ) target using the Godiva IV critical assembly in burst mode. The irradiated sample was transferred to a high-resolution γ-ray detection setup within 50 minutes. γ-ray list mode data was collected from 50 minutes to 1 week after the irradiation. γ-ray spectroscopy was performed to analyze the time dependent γ-ray yields using an automated peak search algorithm to identify isotopes by their decay γ-ray energy and half-life. Finally, the initial activity for each isotope identified was used to calculate their fission product yield.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

239 Pu Fission Spectrum Cumulative Fission Product Yield Measurement Using Godiva IV Critical Assembly

Precise integral measurement of fast neutron-induced fission product yields for various actinides is of high interest for applied nuclear science. The goal of this effort is to improve uncertainties in fission product yield values of 239 Pu. Fission was induced in a pure 239 Pu (>99%) target using the Godiva IV critical assembly in burst mode. Further, the irradiated sample was transferred to a high-resolution γ-ray detector within 45 minutes. γ-ray list mode data was collected from 45 minutes to 1 week after the irradiation. γ-ray spectroscopy was performed to analyze the time dependent γ-ray yields using an automated peak search algorithm to identify isotopes by their decay γ-ray energy and half-life. The initial activity for each isotope identified was used to calculate their fission product yield.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Cyclotron radiation emission spectroscopy signal classification with machine learning in project 8

The Cyclotron Radiation Emission Spectroscopy (CRES) technique pioneered by Project 8 measures cyclotron radiation from individual electrons in a background magnetic field to construct a highly precise energy spectrum for beta decay studies and other applications. The detector, magnetic trap geometry, and electron dynamics give rise to a multitude of complex electron signal structures which carry information about distinguishing physical traits. Here, we develop machine learning models to classify CRES signals with high accuracy based on these traits, improve the resultant frequency spectrum, and offer the potential for a sophisticated analysis which will help Project 8 achieve tritium endpoint measurement in the future.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Positron Emission Intensity in the Decay of 86 gY for Use in Dosimetry Studies

The β + -emitting radionuclide 86 gY (t 1/2 = 14.7 h) forms a matched-pair with the β – -emitting therapeutic radionuclide 90Y (t 1/2 = 2.7 d) for theranostic application in medicine. This approach demands a precise knowledge of the positron emission probability of the PET nuclide which was until recently rather uncertain for 86 gY. In this work, an 86 gY source of high radionuclidic purity was prepared and a direct measurement of the positron emission intensity per 100 decay of the parent (hereafter “positron emission intensity”) was performed using high-resolution HPGe detector γ-ray spectroscopy. The electron capture intensity was also determined as an additional check by measuring the K α and K β X-rays of energies 14.1 and 15.8 keV, respectively, using a low energy HPGe detector. From those measurements, normalized values of 27.2 ± 2.0% for β + -emission and 72.8 ± 2.0% for EC were obtained. These results are in excellent agreement with values recently reported in the literature based on a detailed decay scheme study.

61 RADIATION PROTECTION AND DOSIMETRY↗
DOE OSTI2021

Fluorination-Enhanced Surface Stability of Cation-Disordered Rocksalt Cathodes for Li-Ion Batteries

Cation-disordered rocksalt (DRX) materials have emerged as a class of novel high-capacity cathodes for Li-ion batteries. However, commercialization of DRX cathodes will require reducing their capacity decay, which has been associated with oxygen loss during cycling. Recent studies have shown that fluorination of DRX cathodes can effectively reduce the oxygen loss and improve the cycling stability; however, the underlying atomic-scale mechanisms remain elusive. Herein, using a combination of electrochemical measurements, scanning transmission electron microscopy, and electron energy loss spectroscopy, we examine the correlation between the electrochemical properties and structural evolution in Mn-redox-based DRX cathodes, Li1.2Ti0.4-xMn0.4+xO2.0-xFx (x = 0 and 0.2). We find that fluorination strongly suppresses structural amorphization and void formation initiated from the particle surface, therefore greatly enhancing the cyclability of the cathode. We further reveal a novel rocksalt-to-spinel-like structural transformation in the DRX bulk, which surprisingly contributes to a gradual capacity increase during cycling. Our results provide important insight for the design of novel DRX cathodes with high capacity and long cycle life.

Li, Linze↗
DOE OSTI2021

The JLab Eta Factory (JEF) experiment

The new experiment, JLab Eta Factory (JEF), in the experimental Hall D at Jefferson Lab will extend the physics potential of the GlueX detector beyond the main spectroscopy program and perform precision measurements of various ?(?)decays with emphasis on rare neutral modes. The physics program of the experiment spans from precision tests of low-energy QCD to search of gauge bosons in the mass range below 1 GeV coupling the SM sector to the dark sector. Photoproduction of highly boosted ?(?)mesons using a tagged photon beam, good detection of recoil proton and multi-photon final states will allow to suppress background and collect high-statistics data sample of ?mesons. All these provide many advantages over other ?(?)experiments. The JEF experiment requires to upgrade the inner part of the forward lead glass calorimeter of the GlueX detector with high-granularity, high-resolution lead tungstate PbWO4 scintillating crystals. The calorimeter insert is currently under construction at Jeffeson Lab. The detector will be ready to take data in 2024. An overview of the JEF project will be presented.

Somov, Alexander↗
DOE OSTI2025

Energy Dependent Fission Product Yields

This project utilized a 10-meter Fast Transfer System (called RABITTS) and Decay Station. FPYs are measured using neutron activation of U-235 and Pu-239 followed by gamma ray spectroscopy. We irradiated targets with mono-energetic neutrons produced at the TUNL tandem accelerator laboratory. The gamma spectra collected in these target irradiations are being analyzed to determine FPY values.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2026

Unimolecular Dynamics of Partially Deuterated Hydroperoxyalkyl Intermediates (•QOOD) in Cyclohexane and Cyclopentane Oxidation

The hydroperoxyalkyl radicals (•QOOH) formed in cyclohexane and cyclopentane oxidation with carbon radical center at the β site relative to the hydroperoxy group have recently been observed through their infrared fingerprint and time- and energy-resolved unimolecular dissociation dynamics to hydroxyl (OH) radical and cyclic ether products. Partial deuteration shifts the IR transitions associated with OH/OD motion to lower frequencies, providing a new window on the IR spectroscopy and unimolecular dynamics of these transient intermediates. Specifically, the overtone OD stretch (2ν OD ) has been identified at 5215.0 cm –1 and 5216.0 cm –1 for the β-QOOD intermediates in cyclohexane and cyclopentane oxidation, respectively. Unimolecular decay rates of the •QOOD intermediates at these energies have been obtained from the time-resolved appearance of OD products. The experimental rates are compared with statistical microcanonical rates evaluated using RRKM theory, including heavy-atom tunneling associated with simultaneous O–O bond elongation and C–O–O angle contraction along the reaction pathway. The experimental rates provide a further test of the previously determined transition state (TS) barriers, which were computed utilizing a benchmarking approach that builds on higher-level reference calculations for the smaller ethane oxidation system. Here, the experimental rate measurements for both •QOOD intermediates agree well with the computed rates after accounting for small changes in zero-point energy and a minor empirical adjustment of the TS barriers in both systems.

Ethers↗
DOE OSTI2020

Experimental and theoretical studies of the doubly substituted methyl-ethyl Criegee intermediate: Infrared action spectroscopy and unimolecular decay to OH radical products

In this work the infrared (IR) action spectrum of the doubly substituted methyl-ethyl Criegee intermediate (MECI) is observed in the CH stretch overtone region with detection of OH products. The MECI exhibits four conformers, all of which undergo unimolecular decay via a 1,4 H-atom transfer mechanism, followed by the rapid release of OH products. Conformers with different orientations of the carbonyl oxide group with respect to the methyl and ethyl substituents (i.e., anti and syn ) decay via distinct transition state barriers (16.1 kcal mol –1 and 15.4 kcal mol –1 , respectively). The observed IR action spectrum is in good agreement with the predicted anharmonic IR absorption spectrum, but exhibits significant congestion, which is attributed to couplings between spectroscopic bright states and nearby dark states. Energy-dependent OH appearance rates are measured upon IR excitation of the strongest features in the IR action spectrum and are found to be on the order of 10 6 –10 7 s –1 . The experimental rates are in good agreement with computed Rice–Ramsperger–Kassel–Marcus rates for the unimolecular decay of MECI at these energies, which incorporate quantum mechanical tunneling and sophisticated hindered rotor treatments, as well as high-level theoretical calculations of the TS barrier heights, rovibrational properties, and torsional barriers associated with the MECI conformers. Master equation modeling is used to predict thermal rates for the unimolecular decay of anti - and syn -MECI of 473 s –1 and 660 s –1 , respectively. Comparison with other previously studied Criegee intermediate systems provides insights into substituent effects on unimolecular decay under both energy-dependent and thermal conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Evidence against the Efimov effect in 12 C from spectroscopy and astrophysics

Background: The Efimov effect is a universal phenomenon in physics whereby three-body systems are stabilized via the interaction of an unbound two-body subsystems. A hypothetical state in 12 C at 7.458-MeV excitation energy, comprising a loose structure of three α particles in mutual two-body resonance, has been suggested in the literature to correspond to an Efimov state in nuclear physics. The existence of such a state has not been demonstrated experimentally. Purpose: Using a combination of γ spectroscopy, charged-particle spectroscopy, and astrophysical rate calculations allowing for strict limits on the existence of such a state to been established here. Method: Using the combined data sets from two recent experiments, one with the TexAT (Texas Active Target) TPC (Time Projection Chamber) to measure α decay and the other with Gammasphere to measure γ decay of states in 12 C populated by 12 N and 12 B β decay, respectively, we achieve high sensitivity to states in close proximity to the α threshold in 12 C. Results: No evidence of a state at 7.458 MeV is seen in either data set. Using a likelihood method, the 95% confidence limit γ -decay branching ratio is determined as a function of the β-decay feeding strength relative to the Hoyle state. In parallel, calculations of the 3α reaction rate show the inclusion of the Efimov corresponds to a large increase in the reaction rate around 5 × 10 7 K. Conclusion: From decay spectroscopy—at the 95% confidence limit, the Efimov state cannot exist at 7.458 MeV with any γ-decay branching ratio unless the β strength is less than 0.7% of the Hoyle state. This limit is evaluated for a range of different excitation energies and the results are not favorable for existence of the hypothetical Efimov state in 12 C . Furthermore, the 3α reaction rate with the inclusion of a state between 7.43 and 7.53 MeV exceeds the rate required for stars to undergo the red giant phase.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗