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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 469 records · Page 26
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Imaging Wavepackets in Real-Space & Disentangling Ultrafast Solvation Dynamics with High-Energy Ultrafast X-ray Scattering

The microscopic information of solute and solute-solvent motions can be measured using ultrafast diffuse x-ray scattering, and compared to molecular dynamics simulations, as demonstrated in studies of solvated molecular systems done in X-ray free-electron lasers. However, for the typical photon energies used in these experiments, the photon momentum transfer range was limited to lower Q values where the signals arising from different parts of the studied system overlap significantly. Recently, this limitation was greatly alleviated by extending the photon energy at the Linac Coherent Light-Source (LCLS), significantly increasing the accessible momentum transfer range. This improvement is transformative for ultrafast diffuse x-ray scattering measurements, enabling for the first time to disentangle the solute scattering difference signal, that persists to higher Q values, from the bulk solvent and solute-solvent cross-terms difference signals. In addition, it enhances the prediction ability of modeling and simulation methods such as the hybrid QM/MM approach. The extended Q range also opens the way to resolve in real-space details regarding coherent wavepackets motions beyond their center-of-mass positions. Here, we present the first results on high-energy (18keV) diffuse x-ray scattering in solution, demonstrating high fidelity time-resolved scattering and analysis of the photoexcited model photocatalysts PtPOP ([Pt2(POP)4]4-), and IrDimen ([Ir2(dimen)4]2+) in several solvents. These complexes provide ideal systems for demonstrating the ability of high-Q ultrafast scattering and QM/MM simulations to decompose ultrafast solvation dynamics into specific changes in the solute-solvent pair distribution function with a particular focus on how electronically excited states change the interaction between the solvent and photo-catalytically active metal sites. We introduce an approach to further utilize the high-energy capability and demonstrate a single-shot ultra-wide-angle X-ray Scattering modality using two perpendicular detectors, spanning a scattering angle range of more than 100 degrees, allowing to extend the accessible momentum transfer range up to Q~14 Å-1. We develop a model-free method to invert the x-ray scattering signals and enable the recovery of multiple pair-density motions that happen simultaneously, allowing us to directly measure in real-space nuclear wavepacket motions. . [1] Natan, Adi. "Real-Space Inversion and Super-Resolution of Ultrafast X-ray Scattering using Natural Scattering Kernels." arXiv preprint arXiv:2107.05576 (2021)

Natan, Adi↗
DOE OSTI2024

Graviton detection and the quantization of gravity

We revisit a question asked by Dyson: “Is a graviton detectable?” We demonstrate that in both Dyson’s original sense and in a more modern measurement-theoretic sense, it is possible to construct a detector sensitive to single gravitons, and in fact a variety of existing and near-term gravitational wave detectors can achieve this. However, while such a signal would be consistent with the quantization of the gravitational field, we draw on results from quantum optics to show how the same signal could just as well be explained via classical gravitational waves. We outline the kind of measurements that would be needed to demonstrate quantization of gravitational radiation and explain why these are substantially more difficult than simply counting graviton clicks or observing gravitational noise in an interferometer, and likely impossible to perform in practice. Published by the American Physical Society 2024

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Electrostatic Superlattices Beyond 1:1 Stoichiometry

ABSTRACT Exotic nanoparticle superstructures can be accessed by harnessing nanoparticle softness and charge regulation, features often viewed as obstacles to structural control. Here, we show that regulated charge mismatch in polymer‐grafted nanoparticles enables the assembly of high‐stoichiometry cubic superlattices. By co‐tuning grafting density, particle size, and bulk composition, we realize ionic‐lattice analogues, such as and , as well as single‐component and superlattices without atomic counterparts. The superlattice has recently been identified theoretically as a photonic band‐gap lattice. These phases emerge from a 1:1 “parent” lattice when local charge neutrality cannot be satisfied, driving either progressive interstitial filling or reorganization into a larger basis. For instance, the systematic occupation of ZnS tetrahedral sites yields , while ligand‐swapping symmetry breaking converts CsCl into . Upon heating, the assemblies exhibit reversible lattice contraction and pronounced negative thermal expansion. Furthermore, the energetic penalty for defects increases with nanoparticle size, facilitating the scalable production of high‐quality, open superlattices for photonic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Real-time data processing for serial crystallography experiments

We report the use of streaming data interfaces to perform fully online data processing for serial crystallography experiments, without storing intermediate data on disk. The system produces Bragg reflection intensity measurements suitable for scaling and merging, with a latency of less than 1 s per frame. Our system uses the CrystFEL software in combination with the ASAP::O data framework. In a series of user experiments at PETRA III, frames from a 16 megapixel Dectris EIGER2 X detector were searched for peaks, indexed and integrated at the maximum full-frame readout speed of 133 frames per second. The computational resources required depend on various factors, most significantly the fraction of non-blank frames ('hits'). The average single-thread processing time per frame was 242 ms for blank frames and 455 ms for hits, meaning that a single 96-core computing node was sufficient to keep up with the data, with ample headroom for unexpected throughput reductions. Further significant improvements are expected, for example by binning pixel intensities together to reduce the pixel count. We discuss the implications of real-time data processing on the `data deluge' problem from recent and future photon-science experiments, in particular on calibration requirements, computing access patterns and the need for the preservation of raw data.

47 OTHER INSTRUMENTATION↗
NASA NTRS2016

Application of X-Ray Pulsar Navigation: A Characterization of the Earth Orbit Trade Space

The potential for pulsars as a navigation source has been studied since their discovery in 1967. X-ray pulsar navigation (XNAV) is a celestial navigation system that uses the consistent timing nature of x-ray photons from milli-second pulsars (MSP) to perform space navigation. By comparing the detected arrival of x-ray photons to a reference database of expected pulsar lightcurve timing models, one can infer a range and range rate measurement based on light time delay. Much of the challenge of XNAV comes from the faint signal, availability, and distant nature of pulsars. This is a study of potential pulsar XNAV measurements to measure extended Kalman filter (EKF) tracking performance with a wide trade space of bounded Earth orbits, using a simulation of existing x-ray detector space hardware. An example of an x-ray detector for XNAV is the NASA Station Explorer for X-ray Timing and Navigation (SEXTANT) mission, a technology demonstration of XNAV set to perform on the International Space Station (ISS) in late 2016early 2017. XNAV hardware implementation is driven by trajectory and environmental influences which add noise to the x-ray pulse signal. In a closed Earth orbit, the radiation environment can exponentially increase the signal noise from x-ray pulsar sources, decreasing the quality and frequency of measurements. The SEXTANT mission in particular improves on the signal to noise ratio by focusing an array of 56 x-ray silicon drift detectors at one pulsar target at a time. This reduces timing glitches and other timing noise contributions from ambient x-ray sources to within a 100 nanosecond resolution. This study also considers the SEXTANT scheduling challenges inherent in a single target observation. Finally, as the navigation sources are now relatively inertial targets, XNAV measurements are also subject to periods of occultation from various celestial bodies. This study focuses on the characterization of these drivers in closed Earth orbits and is not a tuning analysis of the EKF. The study shows that the closed Earth orbit for XNAV performance is reliant on the orbit semi-major axis and eccentricity as well as orbit inclination. These parameters are the primary drivers of pulsar measurement availability and significantly influence the natural spacecraft orbit dynamics. Sensitivity to initial orbit determination error growth due to the scarcity of XNAV measurements within an orbital period require appropriate timing of initial XNAV measurements. The orbit angles of argument of perigee and right ascension of the ascending node, alongside the other orbit parameters, complete the initial cadence of XNAV measurements. The performance of initial XNAV measurements then propagates throughout the experimental period. The study provides a basis to missions who wish to consider XNAV as a potential navigation source in a closed Earth orbit design. It provides a family of orbit trajectories as well as other modeling considerations needed to effectively evaluate if XNAV is an effective navigation source for a potential mission. As an EKF is sensitive to a linearized estimated state, this study has a direct benefit of providing effective XNAV measurements to maintain spacecraft tracking, independent of other navigation sources. In the particular use case of the SEXTANT mission, it also provides a novel scheduling algorithm which addresses the need to prioritize and manage pulsar observations for effective navigation.

PULSAR↗
DOE OSTI2025

Diffuse scattering from correlated electron systems

The role of inhomegeneity in determining the properties of correlated electron systems is poorly understood because of the dearth of structural probes of disorder at the nanoscale. Advances in both neutron and x-ray scattering instrumentation now allow comprehensive measurements of diffuse scattering in single crystals over large volumes of reciprocal space, enabling structural correlations to be characterized over a range of length scales from 5 to 200 angstroms or more. When combined with new analysis tools, such as three-dimensional difference pair-distribution functions, these advanced capabilities have produced fresh insights into the interplay of structural fluctuations and electronic properties in a broad range of correlated electron materials. This review describes recent investigations that have demonstrated the importance of understanding structural inhomogeneity pertaining to phenomena as diverse as superconductivity, charge density wave modulations, metal-insulator transitions, and multipolar interactions.

36 MATERIALS SCIENCE↗
NASA NTRS1992

Description of a prototype emission-transmission computed tomography imaging system

We have developed a prototype imaging system that can perform simultaneous x-ray transmission CT and SPECT phantom studies. This system employs a 23-element high-purity-germanium detector array. The detector array is coupled to a collimator with septa angled toward the focal spot of an x-ray tube. During image acquisition, the x-ray fan beam and the detector array move synchronously along an arc pivoted at the x-ray source. Multiple projections are obtained by rotating the object, which is mounted at the center of rotation of the system. The detector array and electronics can count up to 10(6) cps/element with sufficient energy-resolution to discriminate between x-rays at 100-120 kVp and gamma rays from 99mTc. We have used this device to acquire x-ray CT and SPECT images of a three-dimensional Hoffman brain phantom. The emission and transmission images may be superimposed in order to localize the emission image on the transmission map.

NASA Discipline Musculoskeletal↗
NASA NTRS2016

Application of X-Ray Pulsar Navigation: A Characterization of the Earth Orbit Trade Space

The potential for pulsars as a navigation source has been studied since their discovery in 1967. X-ray pulsar navigation (XNAV) is a celestial navigation system that uses the consistent timing nature of x-ray photons from millisecond pulsars (MSP) to perform space navigation. By comparing the detected arrival of x-ray photons to a reference database of expected pulsar light-curve timing models, one can infer a range and range rate measurement based on light time delay. Much of the challenge of XNAV comes from the faint signal, availability, and distant nature of pulsars. This is a study of potential pulsar XNAV measurements to measure extended Kalman filter (EKF) tracking performance with a wide trade space of bounded Earth orbits, using a simulation of existing x-ray detector space hardware. An example of an x-ray detector for XNAV is the NASA Station Explorer for X-ray Timing and Navigation (SEXTANT) mission, a technology demonstration of XNAV set to perform on the International Space Station (ISS) in late 2016early 2017. XNAV hardware implementation is driven by trajectory and environmental influences which add noise to the x-ray pulse signal. In a closed Earth orbit, the radiation environment can exponentially increase the signal noise from x-ray pulsar sources, decreasing the quality and frequency of measurements. The SEXTANT mission in particular improves on the signal to noise ratio by focusing an array of 56 x-ray silicon drift detectors at one pulsar target at a time. This reduces timing glitches and other timing noise contributions from ambient x-ray sources to within a 100 nanosecond resolution. This study also considers the SEXTANT scheduling challenges inherent in a single target observation. Finally, as the navigation sources are now relatively inertial targets, XNAV measurements are also subject to periods of occultation from various celestial bodies. This study focuses on the characterization of these drivers in closed Earth orbits and is not a tuning analysis of the EKF. The study shows that the closed Earth orbit for XNAV performance is reliant on the orbit semi-major axis and eccentricity as well as orbit inclination. These parameters are the primary drivers of pulsar measurement availability and significantly influence the natural spacecraft orbit dynamics. Sensitivity to initial orbit determination error growth due to the scarcity of XNAV measurements within an orbital period require appropriate timing of initial XNAV measurements. The orbit angles of argument of perigee and right ascension of the ascending node, alongside the other orbit parameters, complete the initial cadence of XNAV measurements. The performance of initial XNAV measurements then propagates throughout the experimental period. The study provides a basis to missions who wish to consider XNAV as a potential navigation source in a closed Earth orbit design. It provides a family of orbit trajectories as well as other modeling considerations needed to effectively evaluate if XNAV is an effective navigation source for a potential mission. As an EKF is sensitive to a linearized estimated state, this study has a direct benefit of providing effective XNAV measurements to maintain spacecraft tracking, independent of other navigation sources. In the particular use case of the SEXTANT mission, it also provides a novel scheduling algorithm which addresses the need to prioritize and manage pulsar observations for effective navigation.

x-ray↗
DOE OSTI2025

Imaging Valence Electron Rearrangement in a Chemical Reaction Using Hard X-Ray Scattering

We have observed the signatures of valence electron rearrangement in photoexcited ammonia using ultrafast hard x-ray scattering. Time-resolved x-ray scattering is a powerful tool for imaging structural dynamics in molecules because of the strong scattering from the core electrons localized near each nucleus. Such core-electron contributions generally dominate the differential scattering signal, masking any signatures of rearrangement in the chemically important valence electrons. Ammonia represents an exception to the typically high core-to-valence electron ratio. Here, we measured 9.8 keV x-ray scattering from gas-phase deuterated ammonia following photoexcitation via a 200 nm pump pulse to the 3s Rydberg state. We observed changes in the recorded scattering patterns due to the initial photoexcitation and subsequent deuterium dissociation. Ab initio calculations confirm that the observed signal is sensitive to the rearrangement of the single photoexcited valence electron as well as the interplay between adiabatic and nonadiabatic dissociation channels. The use of ultrafast hard x-ray scattering to image the structural rearrangement of single valence electrons constitutes an important advance in tracking valence electronic structure in photoexcited atoms and molecules.

Gabalski, Ian [SLAC National Accelerator Laborator↗
NASA NTRS1992

The x ray variability of NGC6814: Power spectra

Simulation techniques are used to obtain the X-ray variability power spectrum of unevenly sampled GINGA data from NGC6814. A simple power law is not an adequate description of the power spectrum, with the residuals showing excess power on timescales consistent with the periodicity seen in EXOSAT observations of this object. However the shape of the folded lightcurve is very different, with 3 main peaks, two of which are separated by an extremely sharp dip instead of the single peak and small harmonic structure observed by EXOSAT. Using the dip as a fiducial mark, a second GINGA observation of this source taken one year later is found to be consistent with being completely periodic and phase coherent with this first GINGA observation. Thus the period is consistent with being constant over a period of 6 years, but phase coherence is only maintained on timescales of approximately 1 year. Over 75 percent of the total source variability is due to the periodic component (r.m.s. amplitude of 36 percent). The residual variability can be described as the more usual 'flicker noise' f(exp -1.1) powerlaw. This shows no apparent high frequency break on timescales greater than 300 seconds. Subtle differences in the shape of the folded light curve with energy, and the very large amount of power in the periodic component suggest occultation as its origin, though amplification of variability from an X-ray emitting 'hot spot' at the disk inner radius through gravitational lensing is also possible. The former suffers from the very arbitrary nature of the periodic timescale, while the latter is unattractive as it cannot simply explain the lack of high frequency break in the residual power. That these models probably fail to provide an adequate explanation may be due to the added complexity of anisotropy of the X-ray emission, suggested by the discrepancy between the lack of soft photons implied by the flat spectrum and the copious source of soft photons available from reprocessing in the iron line producing material.

Done, C.↗
DOE OSTI2025

Decision-tree structures utilizing a phase-transition material

The rich internal physics due to competing electronic phases present in phase-transition materials such as VO2 offer the potential for compact building block design for emerging non-von Neumann computing technologies. Here, based on the relaxation dynamics of an insulator-metal phase transition, we demonstrate experimentally a decision-tree classifier embedded within a single volatile resistive switching device. The tree is constructed by the combination of the voltage pulse and relaxation time and can adapt to different tasks. We use machine learning to analyze the relaxation process, enabling a predictive voltage-relaxation time phase diagram for the electrical resistance state. Classification of the etiology of the chronic cough is presented as a proof-of-principle use case. Further, our approach can be generalized to broader classes of solid-state and solid-liquid interfacial systems that demonstrate a variety of phase relaxations.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Cathode Upcycling for Direct Recycling of Lithium‐Ion Batteries Using a Precipitation Approach

With the increased production of electric vehicles to reduce carbon emissions, the lithium-ion battery market to supply those vehicles has grown dramatically. To enhance battery sustainability and circularity, direct recycling methods aim to recover intact cathode materials. However, end-of-life cathode materials are typically 15–20 years old and often have lower energy density compared to current cathode materials. To address this challenge, a rapid precipitation process is developed to boost energy density by converting low Ni-compositions, LiNi 0.33 Co 0.33 Mn 0.33 O 2 (NMC111), into higher Ni-compositions (NMC622). This process forms a Ni-rich coating on cathode particles that diffuses into the core upon high-temperature relithiation, increasing compositional homogeneity. The upcycling process leverages existing infrastructure, offering low capital cost and minimal additional chemical input. Through ex situ tomographic transmission X-ray microscopy (TXM), 3D Ni:Co elemental mixing is quantified, confirming that elemental content evens at the secondary particle level with a mean NMC622 composition upon relithiation. However, elemental gradients remain in the single crystalline primary particles. Ex situ high-resolution and in situ wide-angle X-ray diffraction reveals concurrent structural changes during the relithiation process. These findings provide key insights into the structural and chemical mechanisms of elemental diffusion to obtain further improvements of increased capacity and retention through compositional conversion of cathode materials.

Cathode Upcycling↗
DOE OSTI2025

Securing 3D NAND Without Density Loss via In-Situ Encryption Using a Single Transistor XOR Cell

In this article, we push lightweight XOR-based in-situ encryption to extreme density by proposing a singletransistor XOR memory cell and applying it to 3D NAND, enabling secure data storage without density loss. Using a ferroelectric field-effect transistor (FeFET) as an example technology, we demonstrate that: i) a single-transistor memory can realize the XOR function by exploiting the ability to charge the source and drain separately and control current flow direction, eliminating the need for conventional encrypted cells that rely on complementary devices; ii) with a XOR-based cipher, encryption and decryption can be mapped to in-situ array operations, where ciphertext is stored as the threshold voltage (VTH) states of FeFETs in a NAND string, and decryption is achieved through read operations using key-dependent complementary source/drain bias; iii) the proposed technique is scalable to multi-level cell (MLC) storage by encrypting and decrypting data bit by bit; iv) using an integrated NAND FeFET array, we experimentally demonstrate encryption and decryption operations for both single-level cell (SLC) and MLC storage; v) systemlevel benchmarking shows that the proposed technique achieves 48× and 278× improvements in encryption and decryption throughput, respectively, compared to AES.

36 MATERIALS SCIENCE↗
DOE OSTI2025

DXRD : a user-friendly suite of two- and multiple-beam dynamical X-ray diffraction programs

The DXRD program suite consisting of a series of dynamical theory programs is introduced for computing dynamical X-ray diffraction from single crystals. Its interactive graphical user interfaces (GUIs) allow general users to make complicated calculations with minimal effort. It can calculate plane-wave Darwin curves of single crystals (or multiple crystals) for both the Bragg and Laue cases, including grazing-incidence diffraction and backward diffraction (with Bragg angles approaching 90°). It is also capable of simulating rocking curves for divergent incident X-ray beams with finite bandwidths. A unique feature of DXRD is that it provides a convenient GUI-based multiple-beam diffraction program that can accurately compute arbitrary N-beam diffraction of any geometry using a universal 4N × 4N matrix method. DXRD also provides a mapping program for plotting all the multiple-beam diffraction lines (monochromator glitches) in the azimuth–energy coordinate system. All these functions make DXRD a convenient and powerful software tool for designing crystal-based synchrotron/X-ray optics (monochromators, analyzers, polarizers, phase plates etc.) and for crystal characterization, X-ray spectroscopy and X-ray diffraction teaching.

Bragg reflection↗
DOE OSTI2026

Evaluating multi-slice ptychography tomography for X-ray imaging

X-ray ptychography typically relies on single-slice reconstruction approaches that assume minimal beam propagation through the specimen. However, this approximation breaks down for thick samples or when using high numerical aperture optics, leading to reconstruction artifacts due to multiple scattering. Multi-slice ptychographic tomography (MSPT) addresses this limitation by explicitly modeling beam propagation through the specimen while reducing angular sampling requirements for tomography, but its performance depends critically on reconstruction parameters and experimental conditions. Here, we systematically evaluate MSPT using numerical simulations and experimental X-ray datasets to understand how factors such as object thickness, optical parameters, and initialization strategies affect reconstruction accuracy. We demonstrate that informed object initialization significantly improves depth resolution and enables accurate projection extension, reducing the angular sampling requirements for tomographic reconstruction. Experimental demonstration confirms that MSPT produces reconstructions with reduced artifacts, establishing it as a robust approach for nanoscale imaging at modern synchrotron facilities.

Luktuke, Amey [Argonne National Laboratory (ANL), ↗
NASA NTRS2006

Microwave Oscillators Based on Nonlinear WGM Resonators

Optical oscillators that exploit resonantly enhanced four-wave mixing in nonlinear whispering-gallery-mode (WGM) resonators are under investigation for potential utility as low-power, ultra-miniature sources of stable, spectrally pure microwave signals. There are numerous potential uses for such oscillators in radar systems, communication systems, and scientific instrumentation. The resonator in an oscillator of this type is made of a crystalline material that exhibits cubic Kerr nonlinearity, which supports the four-photon parametric process also known as four-wave mixing. The oscillator can be characterized as all-optical in the sense that the entire process of generation of the microwave signal takes place within the WGM resonator. The resonantly enhanced four-wave mixing yields coherent, phase-modulated optical signals at frequencies governed by the resonator structure. The frequency of the phase-modulation signal, which is in the microwave range, equals the difference between the frequencies of the optical signals; hence, this frequency is also governed by the resonator structure. Hence, further, the microwave signal is stable and can be used as a reference signal. The figure schematically depicts the apparatus used in a proof-of-principle experiment. Linearly polarized pump light was generated by an yttrium aluminum garnet laser at a wavelength of 1.32 microns. By use of a 90:10 fiber-optic splitter and optical fibers, some of the laser light was sent into a delay line and some was transmitted to one face of glass coupling prism, that, in turn, coupled the laser light into a crystalline CaF2 WGM disk resonator that had a resonance quality factor (Q) of 6x10(exp 9). The output light of the resonator was collected via another face of the coupling prism and a single-mode optical fiber, which transmitted the light to a 50:50 fiber-optic splitter. One output of this splitter was sent to a slow photodiode to obtain a DC signal for locking the laser to a particular resonator mode. The other output of this splitter was combined with the delayed laser signal in another 50:50 fiber-optic splitter used as a combiner. The output.of the combiner was fed to a fast photodiode that demodulated light and generated microwave signal. In this optical configuration, the resonator was incorporated into one arm of a Mach-Zehnder interferometer, which was necessary for the following reasons: It was found that when the output of the resonator was sent directly to a fast photodiode, the output of the photodiode did not include a measurable microwave signal. However, when the resonator was placed in an arm of the interferometer and the delay in the other arm was set at the correct value, the microwave signal appeared. Such behavior is distinctly characteristic of phase-modulated light. The phase-modulation signal had a frequency of about 8 GHz, corresponding to the free spectral range of the resonator. The spectral width of this microwave signal was less than 200 Hz. The threshold pump power for generating the microwave signal was about 1 mW. It would be possible to reduce the threshold power by several orders of magnitude if resonators could be made from crystalline materials in dimensions comparable to those of micro-resonators heretofore made from fused silica.

Maleki, Lute↗
DOE OSTI2021

Generation of Bright Soft X-ray Laser Beams (Final Report)

The project goal was to demonstrate new compact soft x-ray lasers emitting high energy ultrashort pulses at shorter wavelengths and increased repetition rates by amplification in atomic transitions in high density laser-created plasmas. To demonstrate these lasers we developed new high power solid state lasers. The project succeeded in demonstrating the shortest wavelength compact soft x-ray laser to date, 6.85 nm wavelength, and the highest repetition rate table-top soft x-ray laser, 400 Hz. We also applied these compact soft x-ray laser sources to determine the composition of materials with nanoscale resolution using a new technique that combines soft x-ray laser ablation with mass spectrometry, and we demonstrated that these lasers are capable of acquiring nanoscale resolution holograms with picosecond time resolution. The combination of an increased pumping efficiency with increased repetition rates can yield soft x-ray laser beams with an unprecedented average power on a table-top for applications demanding a high photon flux. We have demonstrated that the efficiency of plasma-based laser-pumped soft x-ray lasers can be significantly increased by detailed pulse shaping of the pump laser using a new pulse synthesizer. Results include the demonstration of 18.9 nm wavelength laser operation at a record 400 Hz repetition rate, and the extension of repetitive gain-saturated plasma-based table-top x-ray lasers to the shortest wavelength to date, 6.85 nm. Laser amplification was also observed at wavelengths as short at 5.8 nm by isolectronic scaling in Ni-like lanthanide ions. We have also conducted simulations to explore the possibility of demonstrating gain saturated atomic x-ray lasers near the carbon K-edge, in the “carbon window” for the first time. The work conducted under this program also includes the use of compact soft x-ray lasers in applications to problems of chemical interest, such as isotopic composition mapping of micron-size uranium particles with nanoscale resolution, and nanoscale resolution depth profiling analysis of CoNCN-coated electrodes for water oxidation catalysis. We also demonstrated single-shot high resolution soft x-ray Fourier transform holography over a broad 7 µm diameter field of view with ~ 5 ps temporal resolution.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Single-atom molybdenum doping induces nickel oxide-to-hydroxide transformation for enhanced alkaline hydrogen evolution

NiMoO x compounds are widely regarded as among the most efficient non-noble metal catalysts for the hydrogen evolution reaction (HER). Nevertheless, understanding the structural evolution under in situ conditions and further enhancing their performance remain key challenges. Herein, we report that single-atom Mo doping in NiO significantly enhances its HER activity, reducing the overpotential to 131 mV at 10 mA cm −2 compared to undoped NiO. In situ X-ray absorption spectroscopy and Raman spectroscopy reveal that under catalytic conditions, Mo single atoms remain structurally stable, while Ni 2+ species in NiO are converted to Ni(OH) 2 in alkaline media under the applied working potential for HER. Notably, this transformation is absent in undoped NiO, indicating that Mo doping promotes the formation of active Ni(OH) 2 sites, which, in turn, accelerate the rate-limiting water dissociation step. These findings provide critical mechanistic insights into the structural evolution of NiMoO x during alkaline HER and highlight the importance of in situ studies in the development of highly efficient catalysts.

58 GEOSCIENCES↗