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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 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Probing the Solvation Shells of Lithium Ions in Glyme-Based Electrolytes

Glymes have been extensively studied as solvents for Li-battery electrolytes, most recently in equimolar mixtures with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), due to their ability to form stable solvates. However, directly quantifying free and coordinated glyme molecules in the liquid state has been challenging due to several experimental limitations. Here, in this work, new vibrational probes are demonstrated for studying the solvation structures of diglyme and triglyme in LiTFSI electrolytes. These IR probes make use of an amine group to report the solvation state of glymes at salt-to-solvent molar ratios ranging from 1:5 to 1:10. Characterization of the thermodynamic properties of the solvent exchange occurring in the first solvation shell of lithium ions (Li + ) showed an equilibrium constant for these probes close to unity at room temperature. This result demonstrates that the probes exhibit a similar solvation behavior to their glyme analogue. Concentration dependence studies also revealed a lack of significant amounts of contact ion pairs at the studied concentrations. Moreover, the first solvation shell of Li + appears to be formed by two partially chelating glyme molecules, establishing that even triglyme with multiple chelation sites does not fully coordinate the cation. Complementary molecular dynamics (MD) simulations agree with the experimental results and suggest that at these concentrations, TFSI – predominantly forms solvent-separated ion pairs. However, the simulations do not properly capture the partial solvation structure of the glyme molecules in the solvation shell of Li + as derived from the experiments.

electrolytes↗
DOE OSTI2024

Anatase TiO 2 Surface Hydration: Infrared Vibrational Assignment and Facet-Specific Stability

Anatase TiO 2 nanoparticles support a subtle diversity of surface aqua and hydroxy coordination environments that are characteristic of distinct facets and defect sites. The disparate properties and stability of each molecularly or dissociatively absorbed water environment may provide unique reactivity for facet- and site-selective atomic layer deposition (ALD). Here we probe the temperature-dependent and facet-specific stretching frequency and stability of surface hydroxyls on faceted anatase TiO 2 nanoparticles via in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). Well-defined truncated octahedra, disks, and rods fabricated through hydrothermal synthesis present dominant (101), (001), and (010) facets, respectively. The selective dehydration of discrete local coordination environments as a function of temperature provides a potential pathway to site-selective and facet-selective ALD on metal oxide nanomaterials.

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

Structure–Activity Relationships for Ethanol Dehydrogenation to Acetaldehyde by Silica-Supported Zinc Oxide Catalysts

Silica-supported ZnO efficiently catalyzes the nonoxidative dehydrogenation of ethanol to acetaldehyde, which is relevant for production of 1,3-butadiene from bioethanol. Characterization with in situ spectroscopies under dehydrated conditions (high sensitivity-low energy ion scattering (HS-LEIS), diffuse reflectance (DR) UV–vis, X-ray absorption spectroscopy (XAS), diffuse reflectance Fourier transform infrared spectroscopy (DRIFTS), inelastic neutron scattering (INS), and UV Raman), and ammonia adsorption probed by temperature-programmed desorption followed by DRIFTS and mass spectrometry (DRIFTS-MS NH 3 -TPD), and DFT calculations revealed that the supported ZnO x phase was present as isolated surface ZnO x sites on SiO 2 , with the vast majority coordinated by two siloxane bonds and one silicon atom with two nonbridging oxygens ((≡SiO) 2 Zn 2+ O 2 Si=), anchored at 4-, 5-, and 6-membered siloxane rings. A minor fraction of surface ZnO x sites possessed Lewis acidity, and even fewer sites possessed a Bro̷nsted acidic Zn(OH) + Si moiety. Ethanol temperature-programmed surface reaction-mass spectrometry (TPSR-MS) with various oxidative or ethanol reaction pretreatments indicated that only sites with Lewis and Bro̷nsted acidic character (Zn(OH) + Si) were active for ethanol dehydrogenation, while the majority surface (≡SiO) 2 Zn 2+ O 2 Si= sites were inactive. Greater heterogeneity among all surface ZnO x sites, as assessed by in situ DR UV–vis spectroscopy, was associated with a greater number of ZnO x sites that were active for ethanol dehydrogenation as well as lower enthalpic barriers for acetaldehyde production among the most active surface ZnO x sites. Turnover frequencies and the apparent activation energy for ethanol dehydrogenation were determined from steady-state kinetics. Together, these findings suggested that anchoring inactive surface (≡SiO) 2 Zn 2+ O 2 Si= sites on the silica support caused a greater number of active surface ZnO x sites to adopt a more strained configuration, promoting ethanol dehydrogenation catalysis. Pretreatments and catalysts that promoted desorption of ethanol during TPSR, taken as a marker of surface dehydroxylation, were associated with an increased number of the most active surface (Zn(OH) + Si) sites. Such findings suggested that inactive surface ZnO x sites were activated for ethanol dehydrogenation by dehydroxylation of the support and/or decreased coordination to hemilabile siloxane ligands.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Observation of a single protein by ultrafast X-ray diffraction

The idea of using ultrashort X-ray pulses to obtain images of single proteins frozen in time has fascinated and inspired many. It was one of the arguments for building X-ray free-electron lasers. According to theory, the extremely intense pulses provide sufficient signal to dispense with using crystals as an amplifier, and the ultrashort pulse duration permits capturing the diffraction data before the sample inevitably explodes. This was first demonstrated on biological samples a decade ago on the giant mimivirus. Since then, a large collaboration has been pushing the limit of the smallest sample that can be imaged. The ability to capture snapshots on the timescale of atomic vibrations, while keeping the sample at room temperature, may allow probing the entire conformational phase space of macromolecules. Here we show the first observation of an X-ray diffraction pattern from a single protein, that of Escherichia coli GroEL which at 14 nm in diameter is the smallest biological sample ever imaged by X-rays, and demonstrate that the concept of diffraction before destruction extends to single proteins. From the pattern, it is possible to determine the approximate orientation of the protein. Our experiment demonstrates the feasibility of ultrafast imaging of single proteins, opening the way to single-molecule time-resolved studies on the femtosecond timescale.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Stimulated excitation of thermal diffusion waves in a magnetized plasma pressure filament

Results are presented from basic heat transport experiments using a magnetized electron temperature filament that behaves as a thermal resonator. Using a small cathode source, low energy electrons are injected along the magnetic field into the afterglow of a pre-existing plasma forming a hot electron filament embedded in a colder plasma. A series of low amplitude, sinusoidal perturbations are added to the cathode discharge bias that creates an oscillating heat source capable of driving large amplitude electron temperature oscillations. Langmuir probes are used to measure the amplitude and phase of the thermal wave field over a wide range of driver frequencies. The results are used to verify the excitation of thermal waves, confirm the presence of thermal resonances, and demonstrate the diagnostic potential of thermal waves through measurement of the parallel thermal diffusivity.

Karbashewski, S. (ORCID:000000034988492X)↗
DOE OSTI2024

Uncertainty analysis of Raman spectra for measuring ortho-parahydrogen compositions

Determining ortho-parahydrogen compositions at cryogenic temperatures is an important quality control for liquid hydrogen custody exchange. High orthohydrogen compositions lead to an exothermic reaction resulting in increased boil off and increased venting losses of liquid hydrogen product by either the supplier or consumer. Traditional methods for measuring ortho-parahydrogen compositions such as hot-wire anemometry, nuclear magnetic resonance, and infrared spectroscopy are typically inconvenient at best. As the number of cryogenic hydrogen systems continue to increase, there is an increased need for flexible, standardized techniques for post processing composition measurements. A Raman spectrometer implemented in the Cryo-Catalysis Hydrogen Experimental Facility (CHEF) has demonstrated incredible flexibility for composition measurements of cryogenic hydrogen flows through a wide range of temperatures and pressures with the Raman probe in-situ at cryogenic temperatures. This article analyzes the uncertainty of Raman spectroscopy data of cryogenic hydrogen equilibrated at temperatures in IONEX catalyst. Spectra from hydrogen catalyzed to the equilibrium ortho-parahydrogen composition are processed and compared to expected statistical distributions for method verification.

08 HYDROGEN↗
DOE OSTI2020

GaN thermal transport limited by the interplay of dislocations and size effects

Measurements and first-principles calculations probe the temperature-dependent thermal conductivity (k) of GaN films with large densities of highly oriented dislocations. We demonstrate that phonon-dislocation scattering is weaker than suggested by previous measurements, likely due to sample and experiment size effects. Nonetheless, dislocation-limited k is observed in samples with large dislocation densities and at lower temperatures where k anisotropy is also observed. Combination of experiment and theory give insights into the interplay of thermal resistance mechanisms limiting GaN functionalities and suggest pathways for tuning k via defect engineering.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Detection of uncompensated magnetization at the interface of an epitaxial antiferromagnetic insulator

We have probed directly the temperature and magnetic field dependence of pinned uncompensated magnetization at the interface of antiferromagnetic FeF 2 with Cu, using FeF 2 -Cu-Co spin valves. Electrons polarized by the Co layer are scattered by the pinned uncompensated moments at the FeF 2 -Cu interface giving rise to giant magnetoresistance. We determined the direction and magnitude of the pinned uncompensated magnetization at different magnetic fields and temperatures using the angular dependencies of resistance. The strong FeF 2 anisotropy pins the uncompensated magnetization along the easy axis independent of the cooling field orientation. Most interestingly, magnetic fields as high as 90 kOe cannot break the pinning at the FeF 2 -Cu interface. This proves that the pinned interfacial magnetization is strongly coupled to the antiferromagnetic order inside the bulk FeF 2 layer. Studies as a function of FeF2 crystalline orientation show that uncompensated spins are only detected in a spin valve with (110) crystal orientation, but not in valves containing FeF 2 (100) and FeF 2 (001). This observation is in agreement with symmetry-related considerations which predict the equilibrium boundary magnetization for the FeF 2 (110) layer.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Prevalence of pretransition disordering in the rutile-to- CaCl 2 phase transition of GeO 2

WE report the ability to tailor a material's electronic properties using density driven disordering has emerged as a powerful route to materials design. The observation of anomalous structural and electronic behavior in the rutile to CaCl 2 phase transition in SnO 2 led to the prediction that such behavior is inherent to all oxides experiencing such a phase transition sequence [Smith et al., J. Phys. Chem. Lett. 10, 5351 (2019)]. Here, the ultrawide band gap semiconductor GeO 2 is confirmed to exhibit anomalous behavior during the rutile to CaCl 2 phase transition. A phase pure rutile GeO 2 sample synthesized under high-pressure, high-temperature conditions is probed using synchrotron diffraction and x-ray and optical spectroscopy under high pressure conditions. Density functional theory calculations show that the enthalpic barrier to displacing an oxygen along the B 1g librational mode decreases with pressure leading up to the rutile to CaCl 2 phase transition. The band structure of the distorted state shows that such oxygen displacements form small polarons.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Ultrafast Raman thermometry in driven YBa 2 C u 3 O 6.48

Signatures of photoinduced superconductivity have been reported in cuprate materials subjected to a coherent phonon drive. A “cold” superfluid was extracted from the transient Terahertz conductivity and was seen to coexist with “hot” uncondensed quasiparticles, a hallmark of a driven-dissipative system of which the interplay between coherent and incoherent responses is not well understood. Here, time resolved spontaneous Raman scattering was used to probe the lattice temperature in the photoinduced superconducting state of YBa 2 ⁢C⁢u 3 ⁢O 6.48 . An increase in lattice temperature of up to 140 K was observed by measuring the time dependent Raman scattering intensity of an undriven “spectator” phonon mode. This value is consistent with the estimated increase in quasiparticle temperature measured under the same excitation conditions. These temperature changes provide quantitative information on the nature of the driven state and its decay, and may suggest a strategy to optimize this effect.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Symmetry-energy expansion with strange dense matter

The quantum chromodynamics (QCD) phase diagram at large densities and low temperatures can be probed using both neutron stars and low-energy heavy-ion collisions. Heavy-ion collisions are nearly isospin-symmetric systems, whereas neutron stars are highly isospin asymmetric since they are neutron rich. The symmetry-energy expansion is used to connect these regimes across isospin asymmetry. However, the current symmetry-energy expansion does not account for strange particles. In this work, we include finite strangeness by redefining the isospin-asymmetry parameter and the symmetry-energy expansion in a way that is consistent with QCD SU(3) flavor symmetry. Furthermore, our new symmetry energy works well beyond typical neutron star central densities and admits a skewness term in the presence of strangeness for the case of weak equilibrium.

Equations of state of nuclear matter↗
DOE OSTI2023

Characterization of a Low-Temperature Plasma (LTP) Ambient Ionization Source Using Temporally Resolved Monochromatic Imaging Spectrometry

The low-temperature plasma (LTP) probe is a common plasma-based source used for ambient desorption–ionization mass spectrometry (MS). While the LTP probe has been characterized in detail with MS, relatively few studies have used optical spectroscopy. In this paper, two-dimensional (2D) imaging at selected wavelengths is used to visualize important species in the LTP plasma jet. First, 2D steady-state images of the LTP plume for N 2 + (391.2 nm), He I (706.5 nm), and N 2 (337.1 nm) emissions were recorded under selected plasma conditions. Second, time-resolved 2D emission maps of radiative species in the LTP plasma jet were recorded through the use of a 200 ns detection gate and varying gate delays with respect to the LTP trigger pulse. Emission from He I, N 2 + , and N 2 in the plasma jet region was found to show a transient behavior (often referred to as plasma bullets) lasting only a few microseconds. The N 2 + and He I maps were highly correlated in spatial and temporal structure. Further, emission from N 2 showed two maxima in time, one before and one after the maximum emission for N 2 + and He I, due to an initial electronic excitation wave and ion–electron recombination, respectively. Third, the interaction of the LTP probe with a sample substrate and an electrically grounded metallic needle was studied. Emission from a fluorophore on the sample substrate showed an initial photon-induced excitation from plasma-generated photons followed by electronic excitation by other plasma species. The presence of a grounded needle near the plasma jet significantly extended the plasma jet lifetime and also generated a long-lived corona discharge on the needle. The effect of LTP operating parameters on emission spectra was correlated with mass-spectral results including reagent-ion signals. Lastly, five movies provide a side-by-side comparison of the temporal behavior of emitting species and insights into the interactions of the emission clouds with a sample surface as well as an external needle. Temporally and spatially resolved imaging provided insights into important processes in the LTP plasma jet, which will help improve analyte ion sampling in LTP–MS.

Chan, George C. -Y.↗
DOE OSTI2024

Four-channel optically pumped magnetometer for a magnetoencephalography sensor array

We present a novel four-channel optically pumped magnetometer (OPM) for magnetoencephalography that utilizes a two-color pump/probe scheme on a single optical axis. We characterize its performance across 18 built sensor modules. The new sensor implements several improvements over our previously developed sensor including lower vapor-cell operating temperature, improved probe-light detection optics, and reduced optical power requirements. The sensor also has new electromagnetic field coils on the sensor head which are designed using stream-function-based current optimization. We detail the coil design methodology and present experimental characterization of the coil performance. The magnetic sensitivity of the sensor is on average 12.3 fT/rt-Hz across the 18 modules while the average gradiometrically inferred sensitivity is about 6.0 fT/rt-Hz. The sensor 3-dB bandwidth is 100 Hz on average. The on-sensor coil performance is in good agreement with the simulations.

Iivanainen, Joonas (ORCID:0000000160344604)↗
DOE OSTI2023

Evaluation of the first version of the new RFPI system dedicated to PIP-II project accelerator

The Low-Level Radio Frequency (LLRF) control system is one of the most critical superconducting linac infrastructures responsible for the parameters of the beam acceleration. The LLRF system mainly focuses on the electromagnetic field parameters inside the cavity. While it incorporates fast feedback algorithms to optimize energy transfer to the passing particle beam it does not follow other cryomodule or cavity parameter changes. The Radio Frequency Protection Interlock (RFPI) system closely monitors various factors (like cryomodule vacuum, beamline vacuum, field emission probe current level, temperature, RF signal leakage, etc). Its simple but reliable logic has to provide an instant decision about the LLRF system or high-power amplifier output signal blocking in case of safety region excitation. This contribution presents a new version of the RFPI system which logic is implemented in the FPGA chip. The initial work on the prototype of the new system design resulted in the PoC (Proof of Concept) device. The PoC offers the possibility of various protection logic configurations, input signals parameters evaluation, and modularity aspects verification. The structure and test results from the device evaluation are summarized and discussed in this contribution.

43 PARTICLE ACCELERATORS↗
DOE OSTI2021

Small bore magnetic measurement system, method for measuring small bore magnets

The invention provides a system for measuring magnets, the system comprising a guide tube removably received by a beam chamber tunnel, wherein said guide tube has a first end terminating at a first end of the tunnel and a second end terminating at a second end of the tunnel; a flexible substrate removably and slidably received by the tube, wherein the flexible substrate has a first end and a second end; a first rotary stage removably attached to the first end of said flexible substrate and a second rotary stage removably attached to the second end of said flexible substrate wherein the first rotary stage and the second rotary stage effects movement of the substrate through the tube; and a Hall probe supported by the flexible substrate. Also provided is a method for measuring magnetic fields, the method comprising extending a measuring probe into a magnetic core while maintaining the probe at ambient temperature and pressure.

Kasa, Matthew T.↗
DOE OSTI2025

Probing the Fine Symmetry Breaking in High-Temperature Superconductor Bi 2 Sr 2 CaCu 2 O 8+δ with Angle-Resolved Nonreciprocal Transport

After decades of research, symmetry breaking in high-temperature cuprate superconductors remains a key issue to resolve and is relevant to understanding their exotic quantum phases. In the prototypical cuprate superconductor, Bi 2 Sr 2 CaCu 2 O 8+δ (Bi2212), the possible symmetry breaking has been mostly examined microscopically with scanning tunneling microscopy and photoemission spectroscopy. However, macroscopic evidence and the direct implications for electronic transport have remained elusive. Using superconductivity-enhanced nonreciprocal transport, we report macroscopic evidence of inversion symmetry breaking in Bi2212. While the inversion symmetry breaking is subtle, its effect on nonreciprocal transport is significantly enhanced by the vortex motion during the superconducting transition, leading to a robust manifestation of inversion symmetry breaking in macroscopic transport. Combining angle-resolved nonreciprocal transport and 3D tight-binding model calculations, we derive that the inversion symmetry breaking is due to subtle crystal distortions that give rise to both in-plane and out-of-plane polar axes. Our work not only establishes nonreciprocal transport as a sensitive macroscopic probe to provide electrical transport-based evidence of fine symmetry breaking in Bi2212, but also paves the way for novel device applications such as high-temperature superconducting diodes and superconducting spintronics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Low-temperature nanoscale heat transport in a gadolinium iron garnet heterostructure probed by ultrafast x-ray diffraction

Time-resolved x-ray diffraction has been used to measure the low-temperature thermal transport properties of a Pt/Gd3Fe5O12//Gd3Ga5O12 metal/oxide heterostructure relevant to applications in spin caloritronics. A pulsed femtosecond optical signal produces a rapid temperature rise in the Pt layer, followed by heat transport into the Gd3Fe5O12 (GdIG) thin film and the Gd3Ga5O12 (GGG) substrate. The time dependence of x-ray diffraction from the GdIG layer was tracked using an accelerator-based femtosecond x-ray source. The ultrafast diffraction measurements probed the intensity of the GdIG (1 −1 2) x-ray reflection in a grazing-incidence x-ray diffraction geometry. The comparison of the variation of the diffracted x-ray intensity with a model including heat transport and the temperature dependence of the GdIG lattice parameter allows the thermal conductance of the Pt/GdIG and GdIG//GGG interfaces to be determined. Complementary synchrotron x-ray diffraction studies of the low-temperature thermal expansion properties of the GdIG layer provide a precise calibration of the temperature dependence of the GdIG lattice parameter. The interfacial thermal conductance of the Pt/GdIG and GdIG//GGG interfaces determined from the time-resolved diffraction study is of the same order of magnitude as previous reports for metal/oxide and epitaxial dielectric interfaces. The thermal parameters of the Pt/GdIG//GGG heterostructure will aid in the design and implementation of thermal transport devices and nanostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Comparison of temperature and doping dependence of elastoresistivity near a putative nematic quantum critical point

Abstract Strong electronic nematic fluctuations have been discovered near optimal doping for several families of Fe-based superconductors, motivating the search for a possible link between these fluctuations, nematic quantum criticality, and high temperature superconductivity. Here we probe a key prediction of quantum criticality, namely power-law dependence of the associated nematic susceptibility as a function of composition and temperature approaching the compositionally tuned putative quantum critical point. To probe the ‘bare’ quantum critical point requires suppression of the superconducting state, which we achieve by using large magnetic fields, up to 45 T, while performing elastoresistivity measurements to follow the nematic susceptibility. We performed these measurements for the prototypical electron-doped pnictide, Ba(Fe 1− x Co x ) 2 As 2 , over a dense comb of dopings. We find that close to the putative quantum critical point, the elastoresistivity appears to obey power-law behavior as a function of composition over almost a decade of variation in composition. Paradoxically, however, we also find that the temperature dependence for compositions close to the critical value cannot be described by a single power law.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗