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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 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Optical transient grating pumped X-ray diffraction microscopy for studying mesoscale structural dynamics

Abstract A fundamental understanding of materials’ structural dynamics, with fine spatial and temporal control, underpins future developments in electronic and quantum materials. Here, we introduce an optical transient grating pump and focused X-ray diffraction probe technique (TGXD) to examine the structural evolution of materials excited by modulated light with a precisely controlled spatial profile. This method adds spatial resolution and direct structural sensitivity to the established utility of a sinusoidal transient-grating excitation. We demonstrate TGXD using two thin-film samples: epitaxial BiFeO 3 , which exhibits a photoinduced strain (structural grating) with an amplitude proportional to the optical fluence, and FeRh, which undergoes a magnetostructural phase transformation. In BiFeO 3 , structural relaxation is location independent, and the strain persists on the order of microseconds, consistent with the optical excitation of long-lived charge carriers. The strain profile of the structural grating in FeRh, in comparison, deviates from the sinusoidal excitation and exhibits both higher-order spatial frequencies and a location-dependent relaxation. The focused X-ray probe provides spatial resolution within the engineered optical excitation profile, resolving the spatiotemporal flow of heat through FeRh locally heated above the phase transition temperature. TGXD successfully characterizes mesoscopic energy transport in functional materials without relying on a specific transport model.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Magnetoquantum oscillations in the specific heat of a topological Kondo insulator

Surprisingly, magnetoquantum oscillations (MQOs) characteristic of a metal with a Fermi surface have been observed in measurements of the topological Kondo insulator SmB 6 . As these MQO have only been observed in measurements of magnetic torque (dHvA) and not in measurements of magnetoresistance (SdH), a debate has arisen as to whether the MQO are an extrinsic effect arising from rare-earth impurities, defects, and/or aluminum inclusions or an intrinsic effect revealing the existence of charge-neutral excitations. In this work, we report the first observation of MQO in the low-temperature specific heat of SmB 6 . The observed frequencies and their angular dependence for these flux-grown samples are consistent with previous results based on magnetic torque for SmB 6 but the inferred effective masses are significantly larger than previously reported. Such oscillations can only be observed if the MQO are of bulk thermodynamic origin; the measured magnetic-field dependent oscillation amplitude and effective mass allow us to rule out suggestions of an extrinsic, aluminum inclusion-based origin for the MQO.

topological materials↗
DOE OSTI2022

Root-N Krylov-space correction vectors for spectral functions with the density matrix renormalization group

In this work, we propose a method to compute spectral functions of generic Hamiltonians using the density matrix renormalization group (DMRG) algorithm directly in the frequency domain, based on a modified Krylov-space decomposition to compute the correction vectors. Our approach entails the calculation of the root-N (N=2 is the standard square root) of the Hamiltonian propagator using Krylov-space decomposition and repeating this procedure N times to obtain the actual correction vector. We show that our method greatly alleviates the burden of keeping a large bond dimension at large target frequencies, a problem found with conventional correction-vector DMRG, whereas achieving better computational performance at large N. We apply our method to spin and charge spectral functions of t-J and Hubbard models in the challenging two-leg ladder geometry and provide evidence that the root-N approach reaches a much improved spectral resolution compared to the conventional correction vector.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Nonlinear self-focusing in strongly magnetized pair plasma

An intense radiation field can modify plasma properties and the corresponding refractive index and lead to nonlinear propagation effects such as self-focusing. In this work, we estimate the corresponding effects in pair plasmas for circularly polarized waves, in both unmagnetized and strongly magnetically dominated cases. First, in the unmagnetized pair plasma the ponderomotive force does not lead to charge separation but to density depletion. Second, for astrophysically relevant plasmas of pulsar magnetospheres [and possible loci of fast radio bursts (FRBs)], where the cyclotron frequency $ω_B$ dominates over the plasma frequency $ω_p$ and the frequency of the electromagnetic wave $ω_B \gg ω_p, ω$, we show that (i) there is virtually no nonlinearity due to changing effective mass in the field of the wave; (ii) the ponderomotive force is $F^{(B)}_p = –m_ec^2/4B^2_0∇E^2$, which is reduced by a factor $(ω/ω_B)^2$ if compared to the unmagnetized case ($B_0$ is the external magnetic field and $\textit{E}$ is the electric field of the wave); and (iii) for a radiation beam propagating along a constant magnetic field in the pair plasma with density $n_±$, the ponderomotive force leads to the appearance of circular currents that lead to a decrease of the field within the beam by a factor $ΔB/B_0 = 2πn_±m_ec^2E^2 /B^4_0$. Applications to the physics of FRBs are discussed; we conclude that for the parameters of FRBs, the dominant magnetic field completely suppresses nonlinear self-focusing or filamentation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Extreme-ultraviolet spatiotemporal vortices via high harmonic generation

Spatiotemporal optical vortices (STOVs) are space–time structured light pulses with a unique topology that couples spatial and temporal domains and carry transverse orbital angular momentum (OAM). Up to now, their generation has been limited to the visible and infrared regions of the spectrum. During the last decade, it was shown that through the process of high-order harmonic generation, it is possible to upconvert spatial optical vortices that carry longitudinal OAM from the near-infrared into the extreme-ultraviolet (EUV), thereby producing vortices with distinct femtosecond and attosecond structure. In this work, we demonstrate theoretically and experimentally the generation of EUV spatiotemporal and spatiospectral vortices using near-infrared STOV driving laser pulses. Here, we use analytical expressions for focused STOVs to perform macroscopic calculations of high-order harmonic generation that are directly compared to the experimental results. As STOV beams are not eigenmodes of propagation, we characterize the highly charged EUV STOVs in both the near and far fields to show that they represent conjugated spatiotemporal and spatiospectral vortex pairs. Our work provides high-frequency light beams topologically coupled at the nanometre/attosecond scales domains with transverse OAM that could be suitable to explore electronic dynamics in magnetic materials, chiral media and nanostructures.

High-harmonic generation↗
DOE OSTI2021

Crystal structure of silver pentazolates AgN 5 and AgN 6

Silver pentazolate, a high energy density compound containing the cyclo-N 5 – anion, has recently been synthesized under ambient conditions. However, due to high sensitivity to irradiation, its crystal structure has not been determined. In this work, silver–nitrogen crystalline compounds under ambient conditions and at high pressures, up to 100 GPa, are predicted and characterized by performing first-principles evolutionary crystal structure searching with variable stoichiometry. It is found that newly discovered AgN 5 and AgN 6 are the only thermodynamically stable silver–nitrogen compounds at pressures between 42 and 80 GPa. In contrast to AgN 5 , the pentazolate AgN 6 compound contains N 2 diatomic molecules in addition to cyclo-N 5 – . These AgN 5 and AgN 6 crystals are metastable under ambient conditions with positive formation enthalpies of 54.95 kJ mol –1 and 46.24 kJ mol –1 , respectively. Here, the underlying cause of the stability of cyclo-N 5 – silver pentazolates is the enhanced aromaticity enabled by the charge transfer from silver atoms to nitrogen rings. To aid in the experimental identification of these materials, calculated Raman spectra are reported at ambient pressure: the frequencies of N 5 – vibrational modes of AgN 5 are in good agreement with those measured in the experiment.

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

Harvesting Wave Energy to Power Acoustic Transmitters Using Triboelectric Nanogenerator

Wave energy has the largest reserves and widest distribution among blue energy sources. However, the conversion and utilization of ocean wave energy are challenging. In this work, we developed a contact-separation mode triboelectric nanogenerator (TENG) with a simple structure for harvesting wave energy and powering marine sensors and transmitters and performed detailed electrical characterization under controlled laboratory conditions. A prototype power management circuit (PMC) was implemented to improve the output performance of the TENG. The output from the PMC could charge up a storage capacitor for powering sensors and electronics. Eventually, the TENG was integrated within a water-proof enclosure and tested using a custom-built wave simulator to evaluate the device performance in a more representative scenario. The device sustainably powered up an array of 27 LEDs and was able to charge up a capacitor up to 1.8 V for driving an acoustic transmitter. The results demonstrate that TENG technology shows great promise in harvesting low-frequency ocean wave energy.

Yang, Yang↗
DOE OSTI2024

Space Charge Dominated Momentum Spread and Compensation Strategies in the Post-Linac Section of Proton Improvement Plan-II at Fermilab

The upcoming Proton Improvement Plan-II (PIP-II), designated for enhancements to the Fermilab accelerator complex, features a Beam Transfer Line (BTL) that channels the beam from the linac exit to the booster. In the absence of longitudinal focusing beyond the superconducting linac, the beam experiences an elevated momentum spread, primarily due to nonlinear space-charge forces, surpassing the allowable limit of 2.1e-4. This study presents a detailed examination of the space-charge-induced momentum spread and outlines mitigative strategies. The investigation includes the fine-tuning of a de-buncher cavity, analyzed in terms of operating frequency, longitudinal location, and gap voltage, under both standard and perturbed beam conditions—specifically accounting for momentum jitter and energy variation. The impact of buncher cavity misalignments on the beam's longitudinal phase space is also assessed. The paper concludes by recommending an optimized cavity configuration to effectively mitigate the observed increase in momentum spread along the BTL.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2019

Broad band tunable energy electron beam pulser

An electromagnetic mechanical pulser implements a transverse wave metallic comb stripline TWMCS kicker having inwardly opposing teeth structured to retard a phase velocity of an RF traveling wave propagated therethrough to match the kinetic velocity of a continuous electron beam simultaneously propagated therethrough. The kicker imposes transverse oscillations onto the beam, which is subsequently chopped into pulses by an aperture. The RF phase velocity is substantially independent of RF frequency and amplitude, thereby enabling independent tuning of the electron pulse widths and repetition rate. The exterior surface of the kicker is conductive, thereby avoiding electron charging. In embodiments, various elements of the kicker and/or aperture can be mechanically varied to provide further tuning of the pulsed electron beam. A divergence suppression section can include a mirror TWMCS and/or magnetic quadrupoles. RF can be applied to a down-selecting TWMCS downstream of the aperture to reduce the pulse repetition rate.

Jing, Chunguang↗
DOE OSTI2021

Evidence for a thermally driven charge-density-wave transition in 1T-TaS 2 thin-film devices: Prospects for GHz switching speed

We report on the room-temperature switching of 1T-TaS 2 thin-film charge-density-wave devices, using nanosecond-duration electrical pulsing to construct their time-resolved current–voltage characteristics. The switching action is based upon the nearly commensurate to incommensurate charge-density-wave phase transition in this material, which has a characteristic temperature of 350 K at thermal equilibrium. For sufficiently short pulses, with rise times in the nanosecond range, self-heating of the devices is suppressed, and their current–voltage characteristics are weakly nonlinear and free of hysteresis. This changes as the pulse duration is increased to ~200 ns, where the current develops pronounced hysteresis that evolves nonmonotonically with the pulse duration. By combining the results of our experiments with a numerical analysis of transient heat diffusion in these devices, we clearly reveal the thermal origins of their switching. In spite of this thermal character, our modeling suggests that suitable reduction of the size of these devices should allow their operation at GHz frequencies.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Unexpected Giant Microwave Conductivity in a Nominally Silent BiFeO 3 Domain Wall

Nanoelectronic devices based on ferroelectric domain walls (DWs), such as memories, transistors, and rectifiers, have been shown in recent years. Practical high-speed electronics, on the other hand, usually demand operation frequencies in the gigahertz (GHz) regime, where the effect of dipolar oscillation is important. Herein, an unexpected giant GHz conductivity on the order of 10 3 S m -1 is observed in certain BiFeO 3 DWs, which is about 100 000 times greater than the carrier-induced direct current (dc) conductivity of the same walls. Surprisingly, the nominal configuration of the DWs precludes the alternating current (ac) conduction under an excitation electric field perpendicular to the surface. Theoretical analysis reflects that the inclined DWs are stressed asymmetrically near the film surface, whereas the vertical walls in a control sample are not. The resultant imbalanced polarization profile can then couple to the out-of-plane microwave fields and induce power dissipation, which is confirmed by the phase-field modeling. Since the contributions from mobile-carrier conduction and bound-charge oscillation to the ac conductivity are equivalent in a microwave circuit, the research on local structural dynamics may open a new avenue to implement DW nano-devices for radio-frequency applications.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Structural, Morphological, Electrical and Magnetic Properties of Yttrium-Substituted Co-Zn Ferrites Synthesized by Double Sintering Technique

A series of rare earth Y{sup 3+} ion substituted Co-Zn ferrites Co{sub 0.5}Zn{sub 0.5}Y{sub x}Fe{sub 2-x}O{sub 4} (x = 0.00 to 0.08 in step of 0.02) have been synthesized by conventional double sintering technique from the oxide powders of Co, Zn, Fe, and Y. The XRD, FESEM, EDS, DC resistivity, dielectric measurements, VSM, and Curie temperature (T{sub c}) analysis have been used to investigate structural, morphological, electrical, and magnetic properties. Single phase of cubic spinel structure has been confirmed up to x < 0.06, and a small amount of secondary phase YFeO{sub 3} has also been detected for x > 0.06. The lattice parameter initially decreases than increases with yttrium concentrations. The FESEM image shows that the grains and grain boundaries are distinct and uniformly distributed and the purity has also been endorsed from the EDS spectra. The average grain size decreases at x = 0.02 and then increases with Y substitution. The long range mobility of charge carriers and presence of localized charge carriers with retreat from the Debye-like behavior in the compositions have been explored using electric modulus and impedance. The magnetic strength diminishes owing to existence of magnetic dilution in the A-B interactions subsequent to the T{sub c} declines with the x contents. The value of saturation magnetization decreases with increasing Y{sup 3+} contents that indicates that the domain wall motion become tougher due to substitution of foreign ions Y{sup 3+} that possess larger ionic radius. Therefore, the Y{sup 3+} substituted Co{sub 0.5}Zn{sub 0.5}Y{sub x}Fe{sub 2-x}O{sub 4} (x = 0.00 to 0.08 in step of 0.02) ferrites with high resistivity and low losses has implications to be used in high frequency and power supply devices applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Light-Induced Charge Separation in Photosystem I from Different Biological Species Characterized by Multifrequency Electron Paramagnetic Resonance Spectroscopy

Photosystem I (PSI) serves as a model system for studying fundamental processes such as electron transfer (ET) and energy conversion, which are not only central to photosynthesis but also have broader implications for bioenergy production and biomimetic device design. In this study, we employed electron paramagnetic resonance (EPR) spectroscopy to investigate key light-induced charge separation steps in PSI isolated from several green algal and cyanobacterial species. Following photoexcitation, rapid sequential ET occurs through either of two quasi-symmetric branches of donor/acceptor cofactors embedded within the protein core, termed the A and B branches. Using high-frequency (130 GHz) time-resolved EPR (TR-EPR) and deuteration techniques to enhance spectral resolution, we observed that at low temperatures prokaryotic PSI exhibits reversible ET in the A branch and irreversible ET in the B branch, while PSI from eukaryotic counterparts displays either reversible ET in both branches or exclusively in the B branch. Furthermore, we observed a notable correlation between low-temperature charge separation to the terminal [4Fe-4S] clusters of PSI, termed F A and F B , as reflected in the measured F A /F B ratio. These findings enhance our understanding of the mechanistic diversity of PSI’s ET across different species and underscore the importance of experimental design in resolving these differences. Though further research is necessary to elucidate the underlying mechanisms and the evolutionary significance of these variations in PSI charge separation, this study sets the stage for future investigations into the complex interplay between protein structure, ET pathways, and the environmental adaptations of photosynthetic organisms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Effect of the Chemical Composition of TlIn{sub 1 –} {sub x}Er{sub x}S{sub 2} (0 ≤ x ≤ 0.01) Crystals on Their Dielectric Characteristics and the Parameters of Localized States

The frequency dependences of the real (ε') and imaginary (ε'') parts of the complex dielectric permittivity, the dielectric loss tangent (tanδ), and the ac conductivity (σ{sub ac}) in the frequency range f = 5 × 10{sup 4}–3.5 × 10{sup 7} Hz have been studied in the TlIn{sub 1 –} {sub x}Er{sub x}S{sub 2} (0 ≤ x ≤ 0.01) crystals synthesized in this work. It is found that, in TlIn{sub 1 –} {sub x}Er{sub x}S{sub 2}, the relaxation dispersions of ε' and ε'' take place. The effect of the erbium concentration (Er) in the TlIn{sub 1 –} {sub x}Er{sub x}S{sub 2} crystals on their dielectric coefficients has been studied. At high frequencies, the ac conductivity of the TlIn{sub 1 –} {sub x}Er{sub x}S{sub 2} crystals obeys the relationship σ{sub ac} ~ f {sup 0.8}, which is characteristic of the hopping mechanism of the charge transfer over states localized near the Fermi level. The parameters of the states localized in the forbidden band of TlIn{sub 1 –} {sub x}Er{sub x}S{sub 2} and the influence of the chemical composition of the crystals on these parameters are estimated.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Predicting battery capacity from impedance at varying temperature and state of charge using machine learning

Prediction of battery health from electrochemical impedance spectroscopy (EIS) data can enable rapid measurement of battery state in real-world applications without using additional sensors or time-consuming performance measurements. However, deconvoluting the effect of capacity, state of charge, and temperature on EIS response is complicated analytically. Here, various machine-learning models, such as linear, Gaussian process, random forest, and artificial neural network regression, are utilized to predict capacity from EIS using hundreds of capacity, direct current (DC) resistance, and EIS measurements recorded under varying conditions of health, temperature, and state of charge (SOC). Several feature extraction and selection methods from traditional electrochemical analysis and statistical modeling are explored using machine-learning pipelines. EIS data from just two frequencies can accurately predict capacity, and interrogation shows that the optimal set of frequencies is not usually intuitive. Best results are achieved with an ensemble model, which predicts battery capacity with a mean absolute error of 1.9% on data from unobserved cells.

25 ENERGY STORAGE↗
DOE OSTI2020

New Insights into the Charge-Transfer-to-Solvent Spectrum of Aqueous Iodide: Surface versus Bulk

Liquid phase charge-transfer-to-solvent (CTTS) transitions are important, as they serve as photochemical routes to solvated electrons. Here in this work, broadband deep-ultraviolet electronic sum frequency generation (DUV-ESFG) and two-photon absorption (2PA) spectroscopic techniques were used to assign and compare the nature of the aqueous iodide CTTS excitations at the air/water interface and in bulk solution. In the one-photon absorption (1PA) spectrum, excitation to the 6s Rydberg-like orbital (5p → 6s) gives rise to a pair of spin–orbit split iodine states, 2 P 3/2 and 2 P 1/2 . In the 2PA spectra, the lower-energy 2 P 3/2 peak is absent and the observed 2PA peak, which is ~0.14 eV blue-shifted relative to the upper 2 P 1/2 CTTS peak seen in 1PA, arises from 5p → 6p electronic promotion. The band observed in the ESFG spectrum is attributed to mixing of excited states involving 5p → 6p and 5p → 6s promotions caused by both vibronic coupling and the external electric field generated by asymmetric interfacial solvation.

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

Picosecond Ultrasonics in Magnetic Topological Insulator MnBi 2 Te 4

MnBi 2 Te 4 is a magnetic topological insulator with layered A-type antiferromagnetic order. It exhibits a rich layer- and magnetic-state dependent topological phase diagram; however, much about the coupling between spin, charge, and lattice remains to be explored. Here, in this work, we report that MnBi 2 Te 4 is an excellent acoustic phonon cavity by realizing phonon frequency combs using picosecond ultrasonics. With the generated acoustic phonon wavepackets, we demonstrate that the timing and phase of acoustic echoes can be used to detect the presence of stacking faults between van der Waals layers buried deep within the crystal. Furthermore, by implementing this nondestructive ultrafast optical measurement in conjunction with time-resolved magneto-optical Kerr effect experiments, we uncover that out-of-plane vibrations in MnBi 2 Te 4 do not couple to the magnetic order, i.e. there is no appreciable magnetostriction. Our work points out how a well-developed technique can probe the structural defects and phonon pulse engineering in layered topological insulators.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Morphological Degradation of Oxygen Evolution Reaction-Electrocatalyzing Nickel Selenides at Industrially Relevant Current Densities

We investigated electrodeposited nanoparticulate nickel selenide (pre)catalysts that transform into nickel oxides/ oxyhydroxides under oxygen evolution reaction conditions in alkaline solutions. Previous studies of this transformation were conducted at lower current densities than those of industrial relevance (≥1 A cm −2 ). We used ultramicroelectrodes (UMEs) to achieve such current densities, benefiting from their small size, ensuring low absolute currents and low ohmic drop but high current densities. Morphological degradation of the catalyst material was only observed at current densities exceeding 1 A cm −2 but not for smaller ones. Using X-ray absorption, Xray photoemission spectroscopy, and X-ray diffraction, we confirmed that the degradation was accompanied by the literature-known transformation of nanoparticulate Ni 3 Se 2 (bulk)/NiSe (surface) into nickel oxyhydroxide. The transformation of the precatalyst goes along with a significant improvement in the charge transfer kinetics observed by decreasing Tafel slopes with ongoing experimental time extracted from cyclic voltammetry (CV) experiments and electrochemical impedance spectroscopy (EIS) in the high-frequency range. However, these kinetic improvements are accompanied by limitations in mass transport concluded from decreasing current responses at high overpotentials in CVs and increasing impedance in the low-frequency range of the EIS spectra after extended CV cycling. These mass transport limitations originated from morphological degradations at the UME exceeding 1 A cm −2 which we proved by applying identical location scanning electron microscopy. This has not been reported in studies that have been limited to lower current densities before. Our findings showcase how UMEs can be used to study (pre)catalysts (herein nickel selenides) under current densities of industrial relevance in the absence of ohmic drop-related ambiguities, combined with in-depth materials characterization studies, e.g., identical location microscopy and advanced spectroscopic methods. This approach enables direct evaluation and comparison of catalyst materials and thus demonstrates how to overcome long-standing limitations of electrocatalyst design and testing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗