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At least 523 records · Page 29
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Excitation and detection of coherent nanoscale spin waves via extreme ultraviolet transient gratings

The advent of free electron lasers has opened the opportunity to explore interactions between extreme ultraviolet (EUV) photons and collective excitations in solids. While EUV transient grating spectroscopy, a noncollinear four-wave mixing technique, has already been applied to probe coherent phonons, the potential of EUV radiation for studying nanoscale spin waves has not been harnessed. Here we report EUV transient grating experiments with coherent magnons in Fe/Gd ferrimagnetic multilayers. Magnons with tens of nanometers wavelengths are excited by a pair of femtosecond EUV pulses and detected via diffraction of a probe pulse tuned to an absorption edge of Gd. The results unlock the potential of nonlinear EUV spectroscopy for studying magnons and provide a tool for exploring spin waves in a wave vector range not accessible by established inelastic scattering techniques.

Science & Technology - Other Topics↗
DOE OSTI2024

Sulfur speciation in dacitic melts using X-ray absorption near-edge structure spectroscopy of the S K -edge (S-XANES): Consideration of radiation-induced changes and the implications for sulfur in natural arc systems

Abstract The synchrotron technique of micro X-ray absorption near-edge structure spectroscopy at the sulfur K-edge (S-XANES) provides a unique opportunity to measure the proportion of different oxidation states of sulfur (S) in silicate glasses. Although applied extensively in the analysis of basaltic silicate glasses, few S-XANES studies have investigated variations in S oxidation states with fO2 in felsic silicate glasses. In addition, no study has systematically compared the S-XANES results obtained from the same samples at different photon flux densities to quantify the relationship between exposure time and changes in S speciation in silicate glass, as has been done for Fe and V. This study evaluates observed differences in S speciation measured in experimentally produced H2O-saturated dacitic glasses over a range of reducing to oxidizing conditions (from log fO2 = ΔFMQ-0.7 to ΔFMQ+3.3; FMQ is the fayalite-magnetite-quartz mineral redox buffer) and equilibrated at 1000 °C and 300 MPa. S-XANES spectra were collected at three different photon flux densities using three microspectroscopy beamlines. As is observed in S-XANES analyses of basaltic silicate glasses, beam-induced changes to the S6+/ΣS are observed as a function of photon flux density and beam exposure time. Our results demonstrate that silicate glasses of dacitic composition undergo beam-induced photo-reduction in samples equilibrated at ΔFMQ > +1.75 and photo-oxidation if equilibrated at ΔFMQ < +1. The time required to observe beam-induced changes in the spectra varies as a function of flux density, and our study establishes an upper photon density limit at ~1.0 × 1012 photons/µm2. The S6+/ΣS calculated from spectra collected below this absorbed photon limit at intermediate flux densities (~1–4 × 109 photons/s per µm2) are affected by beam damage, as no conditions were found to be completely free of beam-induced changes. However, the S6+/ΣS ratios calculated below the limit at intermediate flux densities are consistent with thermodynamic constraints, demonstrating that S6+/ΣS ratios calculated from S-XANES spectra can be considered reliable for estimating the oxygen fugacity. Our results carry important implications for the S budget of felsic magmas and dissolution mechanisms in evolved melts. While our results from all three flux densities show the presence of S4+ dissolved in relatively oxidized (ΔFMQ > +1.75) dacitic glass, even in the spectra exposed to the lowest photon densities, we are unable to rule out the possibility that the S4+ signal is the result of instantaneous X-ray irradiation induced beam damage using S-XANES alone. When our spectra are compared to S-XANES spectra from basaltic silicate glasses, important differences exist in the solubility of S2– and S6+ between dacitic silicate melts, pointing to differences in solubility mechanisms as melt composition changes. This study highlights the need for further investigation into beam damage systematics, presence of S4+, and the solubility mechanisms of different oxidation states of S as silicate melt composition changes.

Geochemistry & Geophysics↗
DOE OSTI2023

The multiwavelength view of shocks in the fastest nova V1674 Her

Classical novae are shock-powered multiwavelength transients triggered by a thermonuclear runaway on an accreting white dwarf. V1674 Her is the fastest nova ever recorded (time to declined by two magnitudes is t 2 = 1.1 d) that challenges our understanding of shock formation in novae. We investigate the physical mechanisms behind nova emission from GeV γ-rays to cm-band radio using coordinated Fermi-LAT, NuSTAR, Swift, and VLA observations supported by optical photometry. Fermi-LAT detected short-lived (18 h) 0.1–100 GeV emission from V1674 Her that appeared 6 h after the eruption began; this was at a level of (1.6 ± 0.4) × 10 −6 photons cm −2 s −1 . Eleven days later, simultaneous NuSTAR and Swift X-ray observations revealed optically thin thermal plasma shock-heated to k $T$ shock = 4 keV. The lack of a detectable 6.7 keV Fe Kα emission suggests super-solar CNO abundances. The radio emission from V1674 Her was consistent with thermal emission at early times and synchrotron at late times. The radio spectrum steeply rising with frequency may be a result of either free-free absorption of synchrotron and thermal emission by unshocked outer regions of the nova shell or the Razin–Tsytovich effect attenuating synchrotron emission in dense plasma. The development of the shock inside the ejecta is unaffected by the extraordinarily rapid evolution and the intermediate polar host of this nova.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Coupled Charge and Radiation Transport Processes in Thermophotovoltaic and Thermoradiative Cells

Accurate modeling of charge transport and both thermal and luminescent radiation is crucial to the understanding and design of radiative thermal energy converters. Charge-carrier dynamics in semiconductors are well-described by the Poisson-drift-diffusion equations, and thermal radiation in emitter-absorber structures can be computed using multilayer fluctuational electrodynamics. These two types of energy flows interact through radiation absorption or luminescence and charge-carrier generation or recombination. However, past research has typically only assumed limited interaction, with thermal radiation absorption as an input for charge-carrier models to predict device performance. To examine this assumption, we develop a fully coupled iterative model of charge and radiation transport in semiconductor devices, and we use our model to analyze near-field and far-field GaSb thermophotovoltaic and thermoradiative systems. By comparing our results with past methods that do not consider cross-influences between charge and radiation transport, we find that a fully coupled approach is necessary to accurately model photon recycling and near-field enhancement of external luminescence. As these effects can substantially alter device performance, our modeling approach can aid in the design of efficient thermophotovoltaic and thermoradiative systems.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2023

Engineering Band Gap and Photoconduction in Semiconducting Metal Organic Frameworks: Metal Node Effect

We report a systematic study on the correlation of the metal nodes in M-THQ conducting MOFs (M = Fe, Ni, Cu and Zn; THQ = tetra-hydroxybenzoquinone) with their structure, photophysical property, and photoconductivity. We found that structural preference in these MOFs is controlled by metal node identity where Cu prefers a square planar coordination which leads to a 2D Kagome type structure. Fe, Ni and Zn prefer an octahedral sphere which leads to a 3D structure. Fe-THQ has the smallest band gap and highest photoconduction as well as a long-lived ligand to metal charge transfer state due to the mixed valence state revealed by time resolved optical and X-ray absorption and tera hertz spectroscopy. Furthermore, these results demonstrate the importance of the metal node in tuning the photophysical and photocatalytic properties of MOFs.

14 SOLAR ENERGY↗
DOE OSTI2024

Nanometer-Scale Acoustic Wave Packets Generated by Stochastic Core-Level Photoionization Events

We demonstrate that the absorption of femtosecond hard x-ray pulses excites quasispherical, high-amplitude, and high-wave-vector coherent acoustic phonon wave packets using an all hard-x-ray pump-probe scattering experiment. The time- and momentum-resolved diffuse scattering signal is consistent with an ensemble of 3D strain wave packets induced by the rapid electron cascade dynamics following photoionization at uncorrelated excitation centers. We quantify key parameters of this process, including the localization size of the stress field and the photon energy conversion efficiency into elastic energy. The parameters are determined by the photoelectron and Auger electron cascade dynamics, as well as the electron-phonon interaction. In particular, we obtain the localization size of the observed strain wave packet to be 1.5 and 2.5 nm for bulk SrTiO 3 and KTaO 3 single crystals, respectively. The results provide crucial information on the mechanism of x-ray energy deposition into matter and shed light on the shortest collective length scales accessible to coherent acoustic phonon generation using x-ray excitation. Published by the American Physical Society 2024

36 MATERIALS SCIENCE↗
DOE OSTI2020

Redox Mechanism in Na-Ion Battery Cathodes Probed by Advanced Soft X-Ray Spectroscopy

A Na-ion battery (NIB) device is a promising solution for mid-/large-scale energy storage, with the advantages of material abundance, low cost, and environmental benignity. To improve the NIB capacity and retainability, extensive efforts have been put into the developments of NIB electrode materials. The redox activities of the transition metal (TM)-based NIB electrodes are critical in defining the capacity and stability. Here, we provide a comprehensive review on recent studies of the redox mechanisms of NIB cathodes through synchrotron-based soft X-ray absorption spectroscopy (sXAS) and mapping of resonant inelastic X-ray scattering (mRIXS). These soft X-ray techniques are direct and effective tools to fingerprint the TM-3d and O-p states with both bulk and surface sensitivities. Particularly, 3d TM L-edge sXAS has been used to quantify the cationic redox contributions to the electrochemical property; however, it suffers from lineshape distortion for the bulk sensitive signals in some scenarios. With the new dimension of information along the emitted photon energy, mRIXS can address the distortion issue of in TM-L sXAS; moreover, it also breaks through the limitation of conventional sXAS on detecting unconventional TM and O states, e.g., Mn(I) in NIB anode and oxidized oxygen in NIB cathodes. The mRIXS fingerprint of the oxidized oxygen state enables the detection of the reversibility of the oxygen redox reaction through the evolution of feature intensity upon electrochemical cycling and thus clarifies various misunderstandings in our conventional wisdom. We conclude that, with mRIXS established as a powerful tool, its potential and power will continue to be explored for characterizing novel chemical states in NIB electrodes.

25 ENERGY STORAGE↗
DOE OSTI2025

Hydrodynamic expansion and near-infrared absorption of x-ray heated aluminum plasmas

We use x-ray pulses from dense argon plasmas at the Z Machine (Sandia National Laboratories) to generate hypersonic aluminum plasmas akin to material ejecta during proposed planetary defense missions, fusion reactor wall excursions, and other high-energy density processes. Near-infrared absorption is used to diagnose the controlled expansion of the plasmas through cylindrical cavities following their generation from x-ray heating of solid aluminum 7075 alloy. The data are compared to multidimensional radiation hydrodynamics simulations utilizing the ALEGRA multiphysics code, accounting for the dynamics of radiation scattering, material phase change, plasma expansion, thermal re-irradiation, and interactions with the cavity and with the infrared beams. To allow for accurate simulation, density functional theory is used to apply the Hagen–Rubens relation for the far-infrared and is adjoined with a detailed configuration accounting model using the Propaceos code, producing opacities spanning 10 −1 –10 4 eV photon energy for aluminum 7075 alloy, and in comparison with pure aluminum. The model is found to agree with experimental data in the higher-fluence regime when the Hagen–Rubens relation is applied. The ejected material, which is observed to travel up to 55 km/s, is comprised of a strongly ionized, non-LTE plasma front at ∼10 eV temperature followed by a weakly ionized LTE gas at higher density. The present findings lend some confidence to the broad-range equation of state and infrared opacity models for weakly ionized aluminum plasmas while demonstrating an approach to their future refinement, with potential application to astrophysical plasmas and other extreme processes.

Adiabatic process↗
DOE OSTI2024

Development and characterization of the flight model spectrometer onboard LuSEE-Night

The Lunar Surface Electromagnetics Experiment - Night, LuSEE-Night, is a low-frequency radio astronomy experiment that will explore the cosmic Dark Ages signal on the radio-quiet far side of the Moon. Here, the LuSEE-Night carries a radio frequency spectrometer consisting of a set of antennas, analog and digital processing electronics, and will be launched by NASA’s Commercial Lunar Payload Services in 2025. The spectrometer is designed to observe the spectrum of the radio sky in the 0.5-50MHz band. The flight model (FM) of the four-channel spectrometer has been developed. The FM has been characterized for linearity, gain, noise, and their temperature dependence, confirming that the FM meets all the requirements for LuSEE-Night.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Ultrafast Collective Excited-State Dynamics of a Virus-Supported Fluorophore Antenna

Radiation brightening was recently observed in a multifluorophore-conjugated brome mosaic virus (BMV) particle at room temperature under pulsed excitation. On the basis of its nonlinear dependence on the number of chromophores, the origins of the phenomenon were attributed to a collective relaxation. However, the mechanism remains unknown. Here, we present ultrafast transient absorption and fluorescence spectroscopic studies which shed new light on the collective nature of the relaxation dynamics in such radiation-brightened, multifluorophore particles. Our findings indicate that the emission dynamics is consistent with a superradiance mechanism. The ratio between the rates of competing radiative and nonradiative relaxation pathways depends on the number of chromophores per virus. The findings suggest that small icosahedral virus shells provide a unique biological scaffold for developing nonclassical, deep subwavelength light sources and may open new avenues for the development of photonic probes for medical imaging applications.

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

Harvesting electrons and holes from photodriven symmetry-breaking charge separation within a perylenediimide photosynthetic model dimer

Understanding how to utilize symmetry-breaking charge separation (SB-CS) offers a path toward increasingly efficient light-harvesting technologies. This process plays a central role in the first step of photosynthesis, in which the dimeric “special pair” of the photosynthetic reaction center enters a coherent SB-CS state after photoexcitation. Previous research on SB-CS in both biological and synthetic chromophore dimers has focused on increasing the efficiency of light-driven processes. In a chromophore dimer undergoing SB-CS, the energy of the radical ion pair product is nearly isoenergetic with that of the lowest excited singlet (S 1 ) state of the dimer. This means that very little energy is lost from the absorbed photon. In principle, the relatively high energy electron and hole generated by SB-CS within the chromophore dimer can each be transferred to adjacent charge acceptors to extend the lifetime of the electron–hole pair, which can increase the efficiency of solar energy conversion. To investigate this possibility, we have designed a bis-perylenediimide cyclophane (mPDI 2 ) covalently linked to a secondary electron donor, peri-xanthenoxanthene (PXX) and a secondary electron acceptor, partially fluorinated naphthalenediimide (FNDI). Upon selective photoexcitation of mPDI 2 , transient absorption spectroscopy shows that mPDI 2 undergoes SB-CS, followed by two secondary charge transfer reactions to generate a PXX •+ -mPDI 2 -FNDI •– radical ion pair having a nearly 3 µs lifetime. In conclusion, this strategy has the potential to increase the efficiency of molecular systems for artificial photosynthesis and photovoltaics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Ultrafast One-Dimensional Peierls-Distortion Dynamics in 1⁢T′−Re⁢S 2 Revealed by 4D Electron Microscopy

Rhenium disulfide (ReS 2 ), a prototypical 2D semiconductor with an anisotropic 1⁢T′ structure due to the pronounced Peierls distortion, has demonstrated great potential for polarization-dependent optoelectronics and photonics. Here, we report an ultrafast phase transition occurring within 1 ps, accompanied by a one-dimensional Peierls-distortion relaxation in 1⁢T′−ReS 2 revealed with combined 4D electron microscopy and time-dependent density functional theory calculations. Upon femtosecond laser pulse excitation, the Re-Re dimerization morphology rapidly transforms from a diamond cluster to zigzag chains and persists for several nanoseconds. Here, this ultrafast Peierls-distortion relaxation is further verified by transient changes in optical anisotropy via polarization-dependent transient absorption spectroscopy. Time-dependent density functional theory calculations attribute this novel phase transition to strong correlation between Peierls distortion and impulsive photoexcited carrier doping, predicting a transient band-gap collapse. This Letter opens up an exciting avenue for ultrafast control of Peierls-distortion-induced anisotropy and the metal-insulator transition in 1⁢T′−ReS 2 .

1T’-ReS2↗
DOE OSTI2025

Updating the MCNP neutron guide extension for supermirror absorption, gamma production, and neutron polarization

As supermirror technology has developed, there is a trend towards higher m-values for supermirrors which propagate more neutrons with higher divergence to experimental areas. These supermirrors have thousands of alternating layers of typically nickel and titanium with varying thicknesses deposited on the surface. Neutrons of grazing incidence are reflected from these layers with a probability dependent on the angle of incidence and the wavelength of the neutron. Those neutrons that are not reflected may be captured in the supermirror layers and produce high energy gamma rays that require shielding. The supermirror extension for MCNP has been updated to estimate the capture of neutrons in the supermirror layers of a neutron guide through the banking of photons in a virtual supermirror layer and the reduction of the weight of the neutrons transmitted into the substrate. A new functionality has been added to simulate neutron polarization specifically in the context of a supermirror polarizer for neutron beamlines. In conclusion, the underlying theory, code implementation in MCNP, and examples of gamma production and a V-cavity polarizer will be discussed.

Gamma production↗
DOE OSTI2025

Autocorrelation and Multifractal Detrended Fluctuation Analyses Reveal Superdiffusive Mass Transport in Solvent-Filled Nanoporous Media

Fluorescence fluctuation spectroscopy experiments were conducted to better understand the complex mass transport dynamics of organic molecules in liquid-filled nanoporous media. Anodic aluminum oxide (AAO) membranes incorporating 10 and 20 nm diameter cylindrical pores were employed as model materials. Nile red (NR) dye was used as a fluorescent tracer. The dye was dissolved separately in ethanol and toluene at a concentration of 20 nM and used to fill the membrane nanopores. Confocal fluorescence microscopy was employed to capture photon intensity time series data reflecting apparent diffusion of the dye within the pores. Autocorrelation of these data revealed that NR diffusion within the membranes occurred over a broad range of time scales. The autocorrelation decays were fit to a model for one-dimensional diffusion incorporating both fast and slow components having apparent diffusion coefficients, D f and D s , differing by a factor of ∼100. The fast mechanism was attributed to hindered bulk-like diffusion in the central pore cavity, while slow diffusion likely involved absorption of the dye to the pore surfaces. Unfortunately, important evidence of diffusion anomalies is lost in the broad autocorrelation decays obtained. The method of multifractal detrended fluctuation analysis (MF-DFA) was applied to the same data as a means to overcome this limitation. MF-DFA revealed that time series acquired from within the nanopores were multifractal and exhibited evidence of anomalous superdiffusion, likely resulting from the participation of a desorption-mediated diffusion mechanism. Monte Carlo simulations of time series modeling desorption-mediated diffusion in cylindrical nanopores provided support for this assignment. Here, the new knowledge gained affords an improved understanding of hydrocarbon dynamics within nanoporous oil and gas shales.

Diffusion↗
DOE OSTI2024

Machine learning enhanced characterization and optimization of photonic cured MAPbI 3 for efficient perovskite solar cells

Photonic curing (PC) can facilitate high-speed perovskite solar cell (PSC) manufacturing because it uses high-intensity light pulses to crystallize perovskite films in milliseconds. However, optimizing PC conditions is challenging due to its many variables, and using power conversion efficiency (PCE) as the optimization metric is both time-consuming and labor-intensive. This work presents a machine learning (ML) approach to optimize PC conditions for fabricating methylammonium lead iodide (MAPbI 3 ) films by quantitatively comparing their ultraviolet-visible (UV-vis) absorbance spectra to thermal annealed (TA) films using four similarity metrics. We perform Bayesian optimization coupled with Gaussian process regression (BO-GP) to minimize the similarity metrics. Refining PC conditions using active learning based on BO-GP models, we achieve a PC MAPbI3 film with an absorbance spectrum closely matching a TA reference film, which is further verified by its crystalline and morphological properties. Thus, we demonstrate that the UV-vis absorption spectrum can accurately proxy film quality. Additionally, we use an AI-based segmentation model for a more efficient grain size analysis. However, when we use the optimized PC condition to fabricate PSCs, we find that interaction between MAPbI 3 and the hole transport layer (HTL) during PC critically degrades the PSC performance. By adding a buffer layer between the HTL and MAPbI 3 , the optimized PC PSCs produce a champion PCE of 11.8%, comparable to the TA reference of 11.7%. Using UV-vis similarity metrics instead of device PCE as the objective in our BO-GP method accelerates the optimization of PC processing conditions for MAPbI 3 films.

14 SOLAR ENERGY↗
DOE OSTI2024

Abstract for CRADA between National Energy Technology Laboratory and TOPTICA Photonics, Inc.

The National Energy Technology Laboratory (NETL) and Toptica Photonics (Participant) will collaborate to demonstrate the application of a frequency-comb laser (dual-comb spectroscopy) in an optically accessible rotating detonation engine (RDE). RDEs are a next-generation energy conversion technology which are well-suited to hydrogen usage and have the potential to significantly increase the efficiency of gas turbine engine power cycles. However, critical information is needed about the high temperature and pressure detonation wave, which represents an extremely challenging diagnostic environment. Dual-comb spectroscopy can be used to characterize the pressure-broadened IR absorption features at MHz rates, providing information not possible with conventional tunable diode laser (TDL) technologies. This collaboration will, for the first time, demonstrate application of dual-comb spectroscopy within the combustion annulus of a hydrogen-air RDE. If successful, the data generated will help to accelerate commercialization of RDE technologies in support of decarbonizing our nation’s energy sector.

08 HYDROGEN↗
DOE OSTI2025

Excited State Covalency, Dynamics, and Photochemistry of Square Planar Ni-Thiolate Complexes Revealed by Ultrafast X-ray Absorption

Highly covalent Ni bis(dithiolene) and related complexes provide an ideal platform for investigating the effects of metal–ligand orbital hybridization on excited state character and dynamics. In particular, we focus on the ligand field excited states that dominate the photophysics of first-row transition metal complexes. Here, we investigate if they can be significantly delocalized off the metal center, possibly yielding photochemical reactivity more similar to charge transfer excited states than metal-centered ligand field excited states. Here [Ni(mpo) 2 ] (mpo = 2-mercaptopyridine- N-oxide) provides a representative example for the larger chemical class and is an active electro- and photo-catalyst for proton reduction. A detailed characterization of the excited state electronic structure, dynamics, and photochemistry of [Ni(mpo) 2 ] is presented based on ultrafast transient X- ray absorption spectroscopy at the Ni and S 1s core absorption K-edges. By comparing the ultrafast Ni K-edge absorption to ab initio calculations, we identify an excited state relaxation mechanism where an initial ligand-to-metal charge transfer excitation results in both excited state electron transfer (generating a catalytically relevant reduced photoproduct [Ni(mpo) 2 ] − ) and relaxation to a pseudo-tetrahedral triplet ligand field excited state. From the ultrafast S K-edge absorption, the ligand field excited state is found to be highly delocalized onto the thiolate ligands and a tetrahedral structural distortion is shown to substantially influence the degree of delocalization. The results identify a significant structural coordinate to target when aiming to control the excited state covalency in square planar complexes.

Lim, Hyeongtaek [SLAC National Accelerator Laborat↗