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Results for “time-resolved diffraction”

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 505 records · Page 28
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Measurement of carbon condensates using small-angle x-ray scattering during detonation of the high explosive hexanitrostilbene

The dynamics of carbon condensation in detonating high explosives remains controversial. Detonation model validation requires data for processes occurring at nanometer length scales on time scales ranging from nanoseconds to microseconds. A new detonation endstation has been commissioned to acquire and provide time-resolved small-angle x-ray scattering (SAXS) from detonating explosives. Hexanitrostilbene (HNS) was selected as the first to investigate due to its ease of initiation using exploding foils and flyers, vacuum compatibility, high thermal stability, and stoichiometric carbon abundance that produces high carbon condensate yields. The SAXS data during detonation, collected with 300 ns time resolution, provide unprecedented signal fidelity over a broad q-range. This fidelity permits the first analysis of both the Guinier and Porod/power-law regions of the scattering profile during detonation, which contains information about the size and morphology of the resultant carbon condensate nanoparticles. To bolster confidence in these data, the scattering angle and intensity were additionally cross-referenced with a separate, highly calibrated SAXS beamline. The data show that HNS produces carbon particles with a radius of gyration of 2.7 nm in less than 400 ns after the detonation front has passed, and this size and morphology are constant over the next several microseconds. These data directly contradict previous pioneering work on RDX/TNT mixtures and TATB, where observations indicate significant particle growth (50% or more) continues over several microseconds. The power-law slope is about −3, which is consistent with a complex disordered, irregular, or folded sp{sup 2} sub-arrangement within a relatively monodisperse structure possessing radius of gyration of 2.7 nm after the detonation of HNS.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Demonstration of a time-resolved x-ray scattering instrument utilizing the full-repetition rate of x-ray pulses at the Pohang Light Source

We report on the development of a new experimental instrument for time-resolved x-ray scattering (TRXS) at the Pohang Light Source (PLS-II). It operates with a photon energy ranging from 5 to 18 keV. It is equipped with an amplified Ti:sappahire femtosecond laser, optical diagnostics, and laser beam delivery for pump-probe experiments. A high-speed single-element detector and high trigger-rate oscilloscope are used for rapid data acquisition. While this instrument is capable of measuring sub-nanosecond dynamics using standard laser pump/x-ray probe techniques, it also takes advantage of the dense 500 MHz standard fill pattern in the PLS-II storage ring to efficiently record nano-to-micro-second dynamics simultaneously. We demonstrate this capability by measuring both the (fast) impulsive strain and (slower) thermal recovery dynamics of a crystalline InSb sample following intense ultrafast laser excitation. Exploiting the full repetition rate of the storage ring results in a significant improvement in data collection rates compared to conventional bunch-tagging methods.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

Si-APD linear-array x-ray detector with 10-100 μm spatial and sub-nanosecond time resolution

We developed a silicon avalanche photodiode (Si-APD) linear-array detector to be used for time-resolved X-ray scattering experiments using synchrotron X-rays. The Si-APD linear array consists of 64 pixels (pixel size: 100 × 200 μm{sup 2}) with a pixel pitch of 150 μm and a depletion depth of 10 μm. The multichannel scaler counted X-ray pulses over continuous 2046 time bins for every 0.5 ns and recorded a time spectrum at each pixel with a time resolution of 0.5 ns (FWHM) for 8.0 keV X-rays. Using the detector system, we were able to observe X-ray peaks clearly separated with 2 ns interval in the multibunch-mode operation of the Photon Factory ring. The small-angle X-ray scattering for polyvinylidene fluoride film was also observed with the detector.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

A pulse-front-tilt–compensated streaked optical spectrometer with high throughput and picosecond time resolution

A high-throughput, broadband optical spectrometer coupled to the Rochester optical streak system equipped with a Photonis P820 streak tube was designed to record time-resolved spectra with 1-ps time resolution. Spectral resolution of 0.8 nm is achieved over a wavelength coverage range of 480 to 580 nm, using a 300-groove/mm diffraction grating in conjunction with a pair of 225-mm-focal-length doublets operating at an f/2.9 aperture. Overall pulse-front tilt across the beam diameter generated by the diffraction grating is reduced by preferentially delaying discrete segments of the collimated input beam using a 34-element reflective echelon optic. The introduced delay temporally aligns the beam segments and the net pulse-front tilt is limited to the accumulation across an individual sub-element. The resulting spectrometer design balances resolving power and pulse-front tilt while maintaining high throughput.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

Liquid-phase mega-electron-volt ultrafast electron diffraction

The conversion of light into usable chemical and mechanical energy is pivotal to several biological and chemical processes, many of which occur in solution. To understand the structure–function relationships mediating these processes, a technique with high spatial and temporal resolutions is required. Here, we report on the design and commissioning of a liquid-phase mega-electron-volt (MeV) ultrafast electron diffraction instrument for the study of structural dynamics in solution. Limitations posed by the shallow penetration depth of electrons and the resulting information loss due to multiple scattering and the technical challenge of delivering liquids to vacuum were overcome through the use of MeV electrons and a gas-accelerated thin liquid sheet jet. To demonstrate the capabilities of this instrument, the structure of water and its network were resolved up to the 3rd hydration shell with a spatial resolution of 0.6 Å; preliminary time-resolved experiments demonstrated a temporal resolution of 200 fs.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Improved temporal resolution in ultrafast electron diffraction measurements through THz compression and time-stamping

We present an experimental demonstration of ultrafast electron diffraction (UED) with THz-driven electron bunch compression and time-stamping that enables UED probes with improved temporal resolution. Through THz-driven longitudinal bunch compression, a compression factor of approximately four is achieved. Moreover, the time-of-arrival jitter between the compressed electron bunch and a pump laser pulse is suppressed by a factor of three. Simultaneously, the THz interaction imparts a transverse spatiotemporal correlation on the electron distribution, which we utilize to further enhance the precision of time-resolved UED measurements. We use this technique to probe single-crystal gold nanofilms and reveal transient oscillations in the THz near fields with a temporal resolution down to 50 fs. These oscillations were previously beyond reach in the absence of THz compression and time-stamping.

43 PARTICLE ACCELERATORS↗
DOE OSTI2025

Filling data analysis gaps in time-resolved crystallography by machine learning

There is a growing understanding of the structural dynamics of biological molecules fueled by x-ray crystallography experiments. Time-resolved serial femtosecond crystallography (TR-SFX) with x-ray Free Electron Lasers allows the measurement of ultrafast structural changes in proteins. Nevertheless, this technique comes with some limitations. One major challenge is the quality of data from TR-SFX measurements, which often faces issues like data sparsity, partial recording of Bragg reflections, timing errors, and pixel noise. To overcome these difficulties, conventionally, large volumes of data are collected and grouped into a few temporal bins. The data in each bin are then averaged and paired with the mean of their corresponding jittered timestamps. This procedure provides one structure per bin, resulting in a limited number of averaged structures for the entire time interval spanned by the experiment. Therefore, the information on ultrafast structural dynamics at high temporal resolution is lost. This has initiated research for advanced methods of analyzing experimental TR-SFX data beyond the standard binning and averaging method. To address this problem, we use a machine learning algorithm called Nonlinear Laplacian Spectral Analysis (NLSA), which has emerged as a promising technique for studying the dynamics of complex systems. In this work, we demonstrate the power of this algorithm using synthetic x-ray diffraction snapshots from a protein with significant data incompleteness, timing uncertainties, and noise. Our study confirms that NLSA is a suitable approach that effectively mitigates the effects of these artifacts in TR-SFX data and recovers accurate structural dynamics information hidden in such data.

Trujillo, Justin (ORCID:0000000285505360)↗
DOE OSTI2021

Suppression of the vacuum space-charge effect in fs-photoemission by a retarding electrostatic front lens

The performance of time-resolved photoemission experiments at fs-pulsed photon sources is ultimately limited by the e–e Coulomb interaction, downgrading energy and momentum resolution. Here, we present an approach to effectively suppress space-charge artifacts in momentum microscopes and photoemission microscopes. A retarding electrostatic field generated by a special objective lens repels slow electrons, retaining the k-image of the fast photoelectrons. The suppression of space-charge effects scales with the ratio of the photoelectron velocities of fast and slow electrons. Fields in the range from -20 to 01100 V/mm for E kin = 100 eV to 4 keV direct secondaries and pump-induced slow electrons back to the sample surface. Ray tracing simulations reveal that this happens within the first 40 to 3 μm above the sample surface for E kin = 100 eV to 4 keV. An optimized front-lens design allows switching between the conventional accelerating and the new retarding mode. Time-resolved experiments at E kin = 107 eV using fs extreme ultraviolet probe pulses from the free-electron laser FLASH reveal that the width of the Fermi edge increases by just 30 meV at an incident pump fluence of 22 mJ/cm2 (retarding field -21 V/mm). For an accelerating field of +2 kV/mm and a pump fluence of only 5 mJ/cm 2 , it increases by 0.5 eV (pump wavelength 1030 nm). At the given conditions, the suppression mode permits increasing the slow-electron yield by three to four orders of magnitude. The feasibility of the method at high energies is demonstrated without a pump beam at E kin = 3830 eV using hard x rays from the storage ring PETRA III. The approach opens up a previously inaccessible regime of pump fluences for photoemission experiments.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Near-field imaging of plasmonic nanopatch antennas with integrated semiconductor quantum dots

Plasmonic nanopatch antennas that incorporate dielectric gaps hundreds of picometers to several nanometers thick have drawn increasing attention over the past decade because they confine electromagnetic fields to grossly sub-diffraction-limited volumes. Substantial control over the optical properties of excitons and color centers confined within these plasmonic cavities has already been demonstrated with far-field optical spectroscopies, but near-field optical spectroscopies are essential for an improved understanding of the plasmon–emitter interaction at the nanoscale. Here, we characterize the intensity and phase-resolved plasmonic response of isolated nanopatch antennas by cathodoluminescence microscopy. Furthermore, we explore the distinction between optical and electron beam spectroscopies of coupled plasmon–exciton heterostructures to identify constraints and opportunities for future nanoscale characterization and control of hybrid nanophotonic structures. While we observe substantial Purcell enhancement in time-resolved photoluminescence spectroscopies, negligible Purcell enhancement is observed in cathodoluminescence spectroscopies of hybrid nanophotonic structures. The substantial differences in measured Purcell enhancement for electron beam and laser excitation can be understood as a result of the different selection rules for these complementary experiments. Overall, these results provide a fundamentally new understanding of near-field plasmon–exciton interactions in nanopatch antennas, which is essential for myriad emerging quantum photonic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2013

MULTIBAND STUDIES OF THE OPTICAL PERIODIC MODULATION IN THE X-RAY BINARY SAX J1808.4-3658 DURING ITS QUIESCENCE AND 2008 OUTBURST

We report on time-resolved optical imaging of the X-ray binary SAX J1808.4-3658 during its quiescent state and 2008 outburst. The binary, containing an accretion-powered millisecond pulsar, has a large sinusoidal-like modulation in its quiescent optical emission. We employ a Markov chain Monte Carlo technique to fit our multi-band light curve data in quiescence with an irradiated star model, and derive a tight constraint of 50{sup +6}{sub -5} deg on the inclination angle i of the binary system. The pulsar and its companion are constrained to have masses of 0.97{sub -0.22}{sup +0.31} M{sub Sun} and 0.04{sub -0.01}{sup +0.02} M{sub Sun} (both 1{sigma} ranges), respectively. The dependence of these results on the measurements of the companion's projected radial velocity is discussed. We also find that the accretion disk had nearly constant optical fluxes over a {approx}500 day period in the quiescent state our data covered, but started brightening 1.5 months before the 2008 outburst. Variations in modulation during the outburst were detected in our four observations made 7-12 days after the start of the outburst, and a sinusoidal-like modulation with 0.2 mag amplitude changed to have a smaller amplitude of 0.1 mag. The modulation variations are discussed. We estimate the albedo of the companion during its quiescence and the outburst, which was approximately 0 and 0.8 (for isotropic emission), respectively. This large difference probably provides additional evidence that the neutron star in the binary turns on as a radio pulsar in quiescence.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2013

THE MASS AND THE RADIUS OF THE NEUTRON STAR IN THE TRANSIENT LOW-MASS X-RAY BINARY SAX J1748.9-2021

We use time-resolved spectroscopy of thermonuclear X-ray bursts observed from SAX J1748.9-2021 to infer the mass and the radius of the neutron star in the binary. Four X-ray bursts observed from the source with the Rossi X-ray Timing Explorer enable us to measure the angular size and the Eddington limit on the neutron star surface. Combined with a distance measurement to the globular cluster NGC 6440, in which SAX J1748.9-2021 resides, we obtain two solutions for the neutron star radius and mass, R = 8.18 {+-} 1.62 km and M = 1.78 {+-} 0.3 M{sub Sun} or R = 10.93 {+-} 2.09 km and M = 1.33 {+-} 0.33 M{sub Sun }.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2018

Deciphering mineralogical changes and carbonation development during hydration and ageing of a consolidated ternary blended cement paste

To understand the main properties of cement, a ubiquitous material, a sound description of its chemistry and mineralogy, including its reactivity in aggressive environments and its mechanical properties, is vital. In particular, the porosity distribution and associated sample carbonation, both of which affect cement's properties and durability, should be quantified accurately, and their kinetics and mechanisms of formation known both in detail and in situ . However, traditional methods of cement mineralogy analysis ( e.g. chemical mapping) involve sample preparation ( e.g. slicing) that can be destructive and/or expose cement to the atmosphere, leading to preparation artefacts ( e.g. dehydration). In addition, the kinetics of mineralogical development during hydration, and associated porosity development, cannot be examined. To circumvent these issues, X-ray diffraction computed tomography (XRD-CT) has been used. This allowed the mineralogy of ternary blended cement composed of clinker, fly ash and blast furnace slag to be deciphered. Consistent with previous results obtained for both powdered samples and dilute systems, it was possible, using a consolidated cement paste (with a water-to-solid ratio akin to that used in civil engineering), to determine that the mineralogy consists of alite (only detected in the in situ hydration experiment), calcite, calcium silicate hydrates (C-S-H), ettringite, mullite, portlandite, and an amorphous fraction of unreacted slag and fly ash. Mineralogical evolution during the first hydration steps indicated fast ferrite reactivity. Insights were also gained into how the cement porosity evolves over time and into associated spatially and time-resolved carbonation mechanisms. It was observed that macroporosity developed in less than 30 h of hydration, with pore sizes reaching about 100–150 µm in width. Carbonation was not observed for this time scale, but was found to affect the first 100 µm of cement located around macropores in a sample cured for six months. Regarding this carbonation, the only mineral detected was calcite.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Complementarity of neutron, XFEL and synchrotron crystallography for defining the structures of metalloenzymes at room temperature

Room-temperature macromolecular crystallography allows protein structures to be determined under close-to-physiological conditions, permits dynamic freedom in protein motions and enables time-resolved studies. In the case of metalloenzymes that are highly sensitive to radiation damage, such room-temperature experiments can present challenges, including increased rates of X-ray reduction of metal centres and site-specific radiation-damage artefacts, as well as in devising appropriate sample-delivery and data-collection methods. It can also be problematic to compare structures measured using different crystal sizes and light sources. In this study, structures of a multifunctional globin, dehaloperoxidase B (DHP-B), obtained using several methods of room-temperature crystallographic structure determination are described and compared. Here, data were measured from large single crystals and multiple microcrystals using neutrons, X-ray free-electron laser pulses, monochromatic synchrotron radiation and polychromatic (Laue) radiation light sources. These approaches span a range of 18 orders of magnitude in measurement time per diffraction pattern and four orders of magnitude in crystal volume. The first room-temperature neutron structures of DHP-B are also presented, allowing the explicit identification of the hydrogen positions. The neutron data proved to be complementary to the serial femtosecond crystallography data, with both methods providing structures free of the effects of X-ray radiation damage when compared with standard cryo-crystallography. Comparison of these room-temperature methods demonstrated the large differences in sample requirements, data-collection time and the potential for radiation damage between them. With regard to the structure and function of DHP-B, despite the results being partly limited by differences in the underlying structures, new information was gained on the protonation states of active-site residues which may guide future studies of DHP-B.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Direct imaging of ultrafast lattice dynamics

Under rapid high-temperature, high-pressure loading, lattices exhibit complex elastic-inelastic responses. The dynamics of these responses are challenging to measure experimentally because of high sample density and extremely small relevant spatial and temporal scales. In this work, we use an x-ray free-electron laser providing simultaneous in situ direct imaging and x-ray diffraction to spatially resolve lattice dynamics of silicon under high–strain rate conditions. We present the first imaging of a new intermediate elastic feature modulating compression along the axis of applied stress, and we identify the structure, compression, and density behind each observed wave. The ultrafast probe x-rays enabled time-resolved characterization of the intermediate elastic feature, which is leveraged to constrain kinetic inhibition of the phase transformation between 2 and 4 ns. These results not only address long-standing questions about the response of silicon under extreme environments but also demonstrate the potential for ultrafast direct measurements to illuminate new lattice dynamics.

47 OTHER INSTRUMENTATION↗
DOE OSTI2017

Terahertz-radiation generation in low-temperature InGaAs epitaxial films on (100) and (411) InP substrates

The spectrum and waveforms of broadband terahertz-radiation pulses generated by low-temperature In{sub 0.53}Ga{sub 0.47}As epitaxial films under femtosecond laser pumping are investigated by terahertz time-resolved spectroscopy. The In{sub 0.53}Ga{sub 0.47}As films are fabricated by molecular-beam epitaxy at a temperature of 200°C under different arsenic pressures on (100)-oriented InP substrates and, for the first time, on (411)A InP substrates. The surface morphology of the samples is studied by atomic-force microscopy and the structural quality is established by high-resolution X-ray diffraction analysis. It is found that the amplitude of terahertz radiation from the LT-InGaAs layers on the (411)A InP substrates exceeds that from similar layers formed on the (100) InP substrates by a factor of 3–5.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Time-resolved chemical imaging based on stimulated TERS (Final Scientific-Technical Report-Phase-II-DE-SC0013172)

This is the Final Scientific/Technical Report for the DOE FastTrack SBIR Grant from Fiscal Year 2015. The report details the work pursued to scientifically demonstrate ultrahigh spatial resolution in ultrafast spectroscopy and commercially develop a product offering that provides the similar capability to other researchers. Chemical and electronic information associated with molecular-scale processes can be interrogated via optical spectroscopy. By utilizing two ultrafast lasers, one to “pump” and the other to “probe” with time delay between them, researchers are able to study various molecular and electronic dynamics with time resolution in femtosecond range. Due to the diffraction limit associated with these optical techniques, these techniques measure average behavior of ensemble of molecules since individual molecules are typically much smaller than the wavelengths of the lasers being utilized. This report presents the successful demonstration of ultrafast spectroscopy (temporal resolution of 150 femtosecond limited by the laser pulse width) of electronic recovery in carbon nanotubes, revealing different recovery dynamics for individual carbon nanotubes with spatial resolution of ~ 10 nm, more than 50X smaller than the wavelengths used to study them. The report also details the required instrumentation for such measurements and how it plans to offer a turnkey solution to the research community to provide such capability in a user-friendly and low maintenance package.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Long-time variation in magnetic structure of CeIr 3 Si 2 : Observation of a nucleation-and-growth process of magnetic domains

CeIr 3 Si 2 is the first three-dimensional uniform magnet in which the long-time variation in magnetic structure was observed. To clarify the microscopic mechanism of this magnetic structural change, time-resolved neutron scattering measurements have been reinvestigated. Clear time variations in the line widths as well as the amplitudes of magnetic Bragg diffractions have been observed in this improved instrumentation. On the notion of this observation, a nucleation-and-growth model of magnetic structural change has been presented. The numerical calculation with this model reproduces well the observation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗