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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 217 records · Page 12
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Dark-field X-ray microscopy with structured illumination for three-dimensional imaging

Dark-field X-ray microscopy is a lens-based technique that enables real-space imaging of heterogeneous micro- and meso-scale ordered materials. However, achieving accurate three-dimensional (3D) reconstruction often requires meticulous sample alignment or rastering, requiring complex rotational setups and extended acquisition times. To address these challenges, we introduce a structured illumination technique optimized for 3D imaging of ordered materials at sub-micrometer length scales. Our approach employs a coded aperture to spatially modulate the incident X-ray beam, enabling 3D structural reconstruction from images captured at various aperture positions. Unlike current 3D imaging approaches, which often rely on rotational or rastering methods, our technique uses scanning X-ray silhouettes of the coded aperture for depth resolution along the diffraction axis. This eliminates the need for sample rotation or rastering, resulting in a highly stable and efficient imaging modality. We validated the efficacy of this approach through experimental imaging of an isolated twin domain within a bulk single crystal of an iron pnictide using a dark-field X-ray microscope. This advancement aligns with the enhanced brightness upgrades of modern synchrotron radiation facilities, unlocking new possibilities for high-resolution imaging of ordered materials.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

New reflections on hard X-ray photon-in/photon-out spectroscopy

Analysis of the electronic structure and local coordination of an element is an important aspect in the study of the chemical and physical properties of materials. This is particularly relevant at the nanoscale where new phases of matter may emerge below a critical size. X-ray emission spectroscopy (XES) at synchrotron radiation sources and free electron lasers has enriched the field of X-ray spectroscopy. Additionally, the spectroscopic techniques derived from the combination of X-ray absorption and emission spectroscopy (XAS–XES), such as resonant inelastic X-ray scattering (RIXS) and high energy resolution fluorescence detected (HERFD) XAS, are an ideal tool for the study of nanomaterials. New installations and beamline upgrades now often include wavelength dispersive instruments for the analysis of the emitted X-rays. With the growing use of XAS–XES, scientists are learning about the possibilities and pitfalls. We discuss some experimental aspects, assess the feasibility of measuring weak fluorescence lines in dilute, radiation sensitive samples, and present new experimental approaches for studying magnetic properties of colloidal nanoparticles directly in the liquid phase.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Tailoring the cavities of hydrogen-bonded amphidynamic crystals using weak contacts: towards faster molecular machines

This work describes the use of C–H∙∙∙F–C contacts in the solid-state from the stator towards the rotator to fine-tune their internal motion, by constructing a set of interactions that generate close-fitting cavities in three supramolecular rotors 1–3I. The crystal structures of these rotors, determined by synchrotron radiation experiments at different temperatures, show the presence of such C–H∙∙∙F–C contacts between extended carbazole stators featuring fluorinated phenyl rings and the 1,4-diazabicyclo[2.2.2]octane (DABCO) rotator. According to the 2 H NMR results, using deuterated samples, and periodic density functional theory computations, the rotators experience fast angular displacements (preferentially 120° jumps) due to their low rotational activation energies (E a = 0.8–2.0 kcal mol -1 ). The higher rotational barrier for 1 (2.0 kcal mol -1 ) is associated with a larger number of weak C–H∙∙∙F–C contacts generated by the stators. This strategy offers the possibility to explore the correlation among weak intermolecular forces, cavity shape, and internal dynamics, which has strong implications in the design of future fine-tuned amphidynamic crystals.

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

The O K -2 V spectrum of CO: the influence of the second core-hole

Using synchrotron radiation in the tender X-ray regime, a photoelectron spectrum showing the formation of single site double-core-hole pre-edge states, involving the K shell of the O atom in CO, has been recorded by means of high-resolution electron spectroscopy. The experimentally observed structures have been simulated, interpreted and assigned, employing state-of-the-art ab initio quantum chemical calculations, on the basis of a theoretical model, accounting for their so-called direct or conjugate character. Features appearing above the double ionization threshold have been reproduced by taking into account the strong mixing between multi-excited and continuum states. The shift of the σ* resonance below the double ionization threshold, in combination with the non-negligible contributions of multi-excited configurations in the final states reached, gives rise to a series of avoided crossings between the different potential energy curves.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Theoretical and experimental study on the O( 3 P) + 2,5-dimethylfuran reaction in the gas phase

In this work we report a joint experimental and computational study on the 2,5-dimethylfuran oxidation reaction in the gas phase initiated by atomic oxygen O( 3 P). The experiments have been performed by using vacuum-ultraviolet synchrotron radiation at the Advanced Light Source (ALS) of the Lawrence Berkeley National Laboratory (LBNL), at a temperature of 550 K and a pressure of 8 Torr. The experimental data were supported by quantum-chemical calculations along with a kinetic model, also taking into account the possible involvement of different magnetic states, performed in the framework of the RRKM theory. Propyne, acetaldehyde, methylglyoxal, dimethylglyoxal, 3-penten-2-one, 2,5-dimethylfuran-3(2 H )-one, and 1,2-diacetyl ethylene have been identified as the main primary products arising under the conditions of the experiment. Our computational model suggests that these species can be formed at the concentration and branching ratio experimentally observed only in the presence of a non-negligible fraction of non-thermalized intermediates.

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

Auger electron angular distributions following excitation or ionization from the Xe 3d and F 1s levels in xenon difluoride

Linearly polarized synchrotron radiation has been used to record polarization dependent, non-resonant Auger electron spectra of XeF 2 , encompassing the bands due to the xenon M 45 N 1 N 45 , M 45 N 23 N 45 , M 45 N 45 N 45 and M 45 N 45 V and fluorine KVV transitions. Resonantly excited Auger spectra have been measured at photon energies coinciding with the Xe 3d 5/2 → σ* and the overlapped Xe 3d 3/2 /F 1s → σ* excitations in XeF 2 . The non-resonant and resonantly excited spectra have enabled the Auger electron angular distributions, as characterized by the β A parameter, to be determined for the M 45 N 45 N 45 transitions. In the photon energy range over which the Auger electron angular distributions were measured, theoretical results indicate that transitions into the εf continuum channel dominate the Xe 3d photoionization in XeF 2 . In this limit, the theoretical value of the atomic alignment parameter (A 20 ) characterizing the core ionized state becomes constant. This theoretical value has been used to obtain the Auger electron intrinsic anisotropy parameters (α 2 ) from the β A parameters extracted from our non-resonant Auger spectra. For a particular Auger transition, the electron kinetic energy measured in the resonantly excited spectrum is higher than that in the directly ionized spectrum, due to the screening provided by the electron promoted into the σ* orbital. The interpretation of the F KVV Auger band in XeF 2 has been discussed in relation to previously published one-site populations of the doubly charged ions (XeF 2 2+ ). Here, the experimental results show that the ionization energies of the doubly charged states predominantly populated in the decay of a vacancy in the F 1s orbital in XeF 2 tend to be higher than those populated in the decay of a vacancy in the Xe 4d level in XeF 2 .

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

BioCARS: Synchrotron facility for probing structural dynamics of biological macromolecules

A major goal in biomedical science is to move beyond static images of proteins and other biological macromolecules to the internal dynamics underlying their function. This level of study is necessary to understand how these molecules work and to engineer new functions and modulators of function. Stemming from a visionary commitment to this problem by Keith Moffat decades ago, a community of structural biologists has now enabled a set of x-ray scattering technologies for observing intramolecular dynamics in biological macromolecules at atomic resolution and over the broad range of timescales over which motions are functionally relevant. Many of these techniques are provided by BioCARS, a cutting-edge synchrotron radiation facility built under Moffat leadership and located at the Advanced Photon Source at Argonne National Laboratory. BioCARS enables experimental studies of molecular dynamics with time resolutions spanning from 100 ps to seconds and provides both time-resolved x-ray crystallography and small- and wide-angle x-ray scattering. Structural changes can be initiated by several methods—UV/Vis pumping with tunable picosecond and nanosecond laser pulses, substrate diffusion, and global perturbations, such as electric field and temperature jumps. Studies of dynamics typically involve subtle perturbations to molecular structures, requiring specialized computational techniques for data processing and interpretation. In this review, we present the challenges in experimental macromolecular dynamics and describe the current state of experimental capabilities at this facility. As Moffat imagined years ago, BioCARS is now positioned to catalyze the scientific community to make fundamental advances in understanding proteins and other complex biological macromolecules.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

Valence shell photoelectron angular distributions and vibrationally resolved spectra of imidazole: A combined experimental–theoretical study

Linearly polarized synchrotron radiation has been used to record polarization dependent valence shell photoelectron spectra of imidazole in the photon energy range 21–100 eV. These have allowed the photoelectron angular distributions, as characterized by the anisotropy parameter β, and the electronic state intensity branching ratios to be determined. Complementing these experimental data, theoretical photoionization partial cross sections and β-parameters have been calculated for the outer valence shell orbitals. The assignment of the structure appearing in the experimental photoelectron spectra has been guided by vertical ionization energies and spectral intensities calculated by various theoretical methods that incorporate electron correlation and orbital relaxation. Strong orbital relaxation effects have been found for the 15a', nitrogen lone-pair orbital. The calculations also predict that configuration mixing leads to the formation of several low-lying satellite states. The vibrational structure associated with ionization out of a particular orbital has been simulated within the Franck–Condon model using harmonic vibrational modes. The adiabatic approximation appears to be valid for the X 2A" state, with the β-parameter for this state being independent of the level of vibrational excitation. However, for all the other outer valence ionic states, a disparity occurs between the observed and the simulated vibrational structure, and the measured β-parameters are at variance with the behavior expected at the level of the Franck–Condon approximation. Furthermore, these inconsistencies suggest that the excited electronic states may be interacting vibronically such that the nuclear dynamics occur over coupled potential energy surfaces.

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

Optimal deformation procedure for hybrid adaptive x-ray mirror based on mechanical and piezo-driven bending system

Here, a hybrid deformable x-ray mirror consisting of a mechanical bender and a bimorph deformable mirror has been developed to realize adaptive optical systems, such as zoom condenser optics, for synchrotron-radiation-based x-ray microscopy. In the developed system, both bending mechanisms comprehensively contribute to the formation of the target mirror shape and can narrow the role of piezoelectric actuators, thereby enabling a more stable operation. In this study, the behavior of the bimorph mirror under the clamped condition was investigated, and the sharing of the deformation amount for each bending mechanism was optimized to minimize the amplitude of the voltage distribution of the bimorph mirror.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Work function lowering of LaB 6 by monolayer hexagonal boron nitride coating for improved photo- and thermionic-cathodes

We report a lowering of work function for lanthanum hexaboride (LaB 6 ) by monolayer hexagonal boron nitride (hBN) coating. Photoemission electron microcopy (PEEM) and thermionic emission electron microscopy (TEEM) both revealed that the hBN coated region of a LaB 6 (100) single crystal has a lower work function compared to the bare (i.e., non-coated) and graphene coated regions. A broad and uniform brighter image of the hBN coated region in PEEM was quantitatively supported by a 0.4 eV decrease in the work function in photoelectron spectra compared to the bare region. TEEM results were consistent in that the hBN coated region exhibited thermionic emission at 905 °C, whereas the bare and graphene coated regions did not. A larger decrease in the work function for hBN coated LaB 6 (100) compared to graphene coated LaB 6 (100) was qualitatively supported by our density functional theory calculations. Adding an oxide layer in the calculations improved consistency between the calculation and experimental results. We followed up our calculations with synchrotron-radiation x-ray photoelectron spectroscopy and confirmed the presence of an oxide layer on our LaB 6 .

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

Multi frame radiography of supersonic water jets interacting with a foil target

Pulsed-power-driven underwater electrical explosion of cylindrical or conical wire arrays produces supersonic water jets that emerge from a bath, propagating through the air above it. Interaction of these jets with solid targets may represent a new platform for attaining materials at high pressure (>1010 Pa) conditions in a university-scale laboratory. However, measurements of the internal structure of such jets and how they interact with targets are difficult optically due to large densities and density contrasts involved. We utilized multi-frame x-ray radiographic imaging capabilities of the ID19 beamline at the European Synchrotron Radiation Facility to explore the water jet and its interaction with a 50 μm thick copper foil placed a few mm from the surface of water. The jet was generated with a ∼130 kA-amplitude current pulse of ∼450 ns rise time applied to a conical wire array. X-ray imaging revealed a droplet-type structure of the jet with an average density of <400 kg/m3 propagating with a velocity of ∼1400 m/s. Measurements of deformation and subsequent perforation of the target by the jet suggested pressures at the jet–target interface of ∼5 × 109 Pa. The results were compared to hydrodynamic simulations for better understanding of the jet parameters and their interaction with the foil target. These results can be used in future research to optimize the platform, and extend it to larger jet velocities in the case of higher driving currents supplied to the wire array.

Physics↗
DOE OSTI2024

Valence shell electronically excited states of norbornadiene and quadricyclane

The absolute photoabsorption cross sections of norbornadiene (NBD) and quadricyclane (QC), two isomers with chemical formula C 7 H 8 that are attracting much interest for solar energy storage applications, have been measured from threshold up to 10.8 eV using the Fourier transform spectrometer at the SOLEIL synchrotron radiation facility. The absorption spectrum of NBD exhibits some sharp structure associated with transitions into Rydberg states, superimposed on several broad bands attributable to valence excitations. Sharp structure, although less pronounced, also appears in the absorption spectrum of QC. Assignments have been proposed for some of the absorption bands using calculated vertical transition energies and oscillator strengths for the electronically excited states of NBD and QC. Natural transition orbitals indicate that some of the electronically excited states in NBD have a mixed Rydberg/valence character, whereas the first ten excited singlet states in QC are all predominantly Rydberg in the vertical region. In NBD, a comparison between the vibrational structure observed in the experimental 1 1 B 1 –1 1 A 1 (3sa 1 ← 5b 1 ) band and that predicted by Franck–Condon and Herzberg–Teller modeling has necessitated a revision of the band origin and of the vibrational assignments proposed previously. Similar comparisons have encouraged a revision of the adiabatic first ionization energy of NBD. Simulations of the vibrational structure due to excitation from the 5b 2 orbital in QC into 3p and 3d Rydberg states have allowed tentative assignments to be proposed for the complex structure observed in the absorption bands between ~5.4 and 7.0 eV.

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

Tracking ultrafast non-adiabatic dissociation dynamics of the deuterated water dication molecule

Here, we applied reaction microscopy to elucidate fast non-adiabatic dissociation dynamics of deuterated water molecules after direct photo-double ionization at 61 eV with synchrotron radiation. For the very rare D + + O + + D breakup channel, the particle momenta, angular, and energy distributions of electrons and ions, measured in coincidence, reveal distinct electronic dication states and their dissociation pathways via spin–orbit coupling and charge transfer at crossings and seams on the potential energy surfaces. Notably, we could distinguish between direct and fast sequential dissociation scenarios. For the latter case, our measurements reveal the geometry and orientation of the deuterated water molecule with respect to the polarization vector that leads to this rare 3-body molecular breakup channel. Aided by multi-reference configuration-interaction calculations, the dissociation dynamics could be traced on the relevant potential energy surfaces and particularly their crossings and seams. This approach also unraveled the ultrafast time scales governing these processes.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Multi-Analytical Investigation of Arsenical Transfer and Remediation on Nineteenth-Century Green Books

Books containing heavy metals, specifically nineteenth-century green arsenical books, have been identified at Northwestern University Libraries, raising health and safety concerns related to handling. Copper acetoarsenite pigments, such as emerald green, were detected on book covers, decorative page edges, labels, and other components using noninvasive analytical techniques including X-ray fluorescence (XRF), Raman spectroscopy, and Fourier-transform infrared (FTIR) spectroscopy. Further examination of selected volumes using synchrotron radiation (SR) techniques revealed pigment migration, degradation, and arsenic transfer to adjacent books. This paper expands on initial findings through two related experiments. The first explored the transfer of arsenic using mechanical friction; Staedtler Mars® white vinyl erasers rubbed on arsenical books generated crumbs which were analyzed via scanning electron microscopy–energy-dispersive X-ray spectroscopy (SEM-EDX). Results confirmed the transfer of arsenic, copper, and lead, with decorative page edges being particularly prone to shedding arsenic onto other materials. The second experiment tested remediation methods on a book contaminated by prolonged exposure to an arsenical neighbor. Surface cleaning using erasers and a vacuum removed flecks of pigment but did not eliminate non-chromophoric arsenic as confirmed by SR analyses, which highlights its presence either as a degradation product embedded within the paper or present in the paper as part of its production process. Findings demonstrate the acute toxicity risk posed by arsenical books and support the need for safe handling protocols. However, materials with only trace levels of arsenic embedded during production may pose a lower risk of transfer. Cross contamination beyond prolonged direct contact appears limited. These results highlight critical considerations for library preservation practices and future research on arsenic in historical materials.

arsenic↗
DOE OSTI2020

Element- and Time-Resolved Measurements of Spin Dynamics Using X-ray Detected Ferromagnetic Resonance

Although XFMR experiments have been carried out at a number of synchrotron radiation facilities since 2004, only a few facilities currently have XFMR setups available for user operation. Here in this review, we mainly focus on recent developments and work that has been carried out using time-resolved XFMR at beamline 4.0.2 of the Advanced Light Source and at beamline I10 of the Diamond Light Source. The experimental setup and the sample holder used at beamline I10 and beamline 4.0.2, respectively, are shown in Figure 1. We will first introduce the working principle of XFMR and then provide examples of the capabilities of this technique. Finally, we will briefly describe an outlook for the future development of and new opportunities for XFMR.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Guest Editorial

The design of X-ray optical systems is very different from that of conventional optical systems, whether it be for the peculiarities of synchrotron radiation or the grazing incidence operation of most X-ray optical components. Further, specific simulation tools are thus required to ensure that designs work as expected, and there is now a vibrant landscape of open-source, freely available software that can be used to that end, and explore new design concepts.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Photoionization of the I 4d and valence orbitals of methyl iodide

Here, the photoabsorption and photoionization dynamics of the I 4d and valence orbitals in methyl iodide have been studied both experimentally and theoretically. Synchrotron radiation has been employed to measure the total ion yield in the vicinity of the I 4d ionization thresholds. The observed structure, due to excitations into Rydberg or valence states, has been assigned using transition energies and relative intensities computed with time-dependent density functional theory within the Tamm–Dancoff approximation. Photoelectron spectra, recorded with plane polarized radiation in two polarization geometries, have allowed the effect of autoionization on the valence electron angular distributions to be investigated. The spectra obtained at photon energies of 50.62 and 52.34 eV, coinciding respectively with the I 4d 5/2 → σ* and 4d 3/2 → σ* transitions, reveal, in addition to valence shell photoelectron bands, features not associated with simple photoionization of the parent molecule. High resolution photoelectron spectra of the I 4d main-lines display structure resulting from spin–orbit coupling and molecular field splitting. The binding energies of the five states contributing to the (I 4d) -1 ionization have been determined. The iodine (in CH 3 I) N 45 VV Auger spectrum has been measured and the observed structure has been assigned using the core hole binding energies derived in the present work together with established ionization energies of the doubly charged ion. The experimentally determined Auger electron angular distributions have been discussed in relation to the theoretical angular distribution parameter characterizing the spatial alignment of molecular axes in the (I 4d) -1 state.

74 ATOMIC AND MOLECULAR PHYSICS↗