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At least 37 records · Page 2

Developments in time-resolved high pressure x-ray diffraction using rapid compression and decompression

Complementary advances in high pressure research apparatus and techniques make it possible to carry out time-resolved high pressure research using what would customarily be considered static high pressure apparatus. This work specifically explores time-resolved high pressure x-ray diffraction with rapid compression and/or decompression of a sample in a diamond anvil cell. Key aspects of the synchrotron beamline and ancillary equipment are presented here, including source considerations, rapid (de)compression apparatus, high frequency imaging detectors, and software suitable for processing large volumes of data. A number of examples are presented, including fast equation of state measurements, compression rate dependent synthesis of metastable states in silicon and germanium, and ultrahigh compression rates using a piezoelectric driven diamond anvil cell.

47 OTHER INSTRUMENTATION↗

Developments in time-resolved x-ray research at APS beamline 7ID

The 7ID beamline of the Advanced Photon Source (APS) is dedicated to time-resolved research using x-ray imaging, scattering, and spectroscopy techniques. Time resolution is achieved via gated detectors and/or mechanical choppers in conjunction with the time structure of the x-ray beam. Three experimental hutches allow for a wide variety of experimental setups. Major areas of research include atomic, molecular, and optical physics; chemistry; condensed matter physics in the bulk, thin film, and surface regimes; and fluid-spray dynamics. Recent developments in facilities at 7ID include a high-power, high-repetition-rate picosecond laser to complement the 1 kHz ultrafast laser. For the ultrafast laser, a newly commissioned optical parametric amplifier provides pump wavelength from 0.2 to 15 µm with energy per pulse up to 200 µJ. A nanodiffraction station has also been commissioned, using Fresnel zone-plate optics to achieve a focused x-ray spot of 300 nm. This nanoprobe is not only used to spatially resolve the evolution of small features in samples after optical excitation, but also has been combined with an intense THz source to study material response under ultrafast electric fields.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Gauge invariance in the theoretical description of time-resolved angle-resolved pump/probe photoemission spectroscopy

Nonequilibrium calculations in the presence of an electric field are usually performed in a gauge, and need to be transformed to reveal the gauge-invariant observables. In this work, we discuss the issue of gauge invariance in the context of time-resolved angle-resolved pump/probe photoemission. If the probe is applied while the pump is still on, one must ensure that the calculations of the observed photocurrent are gauge invariant. We also discuss the requirement of the photoemission signal to be positive and the relationship of this constraint to gauge invariance. Here, we end by discussing some technical details related to the perturbative derivation of the photoemission spectra, which involve processes where the pump pulse photoemits electrons due to nonequilibrium effects.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Time-resolved soft x-ray spectra from laser-produced Cu plasma

The volumetric heating of a thin copper target has been studied with time resolved x-ray spectroscopy. The copper target was heated by a plasma produced using the Lawrence Livermore National Laboratory's Compact Multipulse Terawatt (COMET) laser. A variable spaced grating spectrometer coupled to an x-ray streak camera measured soft x-ray emission (800-1550 eV) from the back of the copper target to characterize the bulk heating of the target. Radiation hydrodynamic simulations were modeled in two-dimensions using the HYDRA code. The target conditions calculated by HYDRA were post-processed with the atomic kinetics code CRETIN to generate synthetic emission spectra. A comparison between the experimental and simulated spectra indicates the presence of specific ionization states of copper and the corresponding electron temperatures and ion densities throughout the laser-heated copper target.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Time-resolved spectra of dense plasma focus using spectrometer, streak camera, and CCD combination

A time-resolving spectrographic instrument has been assembled with the primary components of a spectrometer, image-converting streak camera, and CCD recording camera, for the primary purpose of diagnosing highly dynamic plasmas. A collection lens defines the sampled region and couples light from the plasma into a step index, multimode fiber which leads to the spectrometer. The output spectrum is focused onto the photocathode of the streak camera, the output of which is proximity-coupled to the CCD. The spectrometer configuration is essentially Czerny-Turner, but off-the-shelf Nikon refraction lenses, rather than mirrors, are used for practicality and flexibility. Only recently assembled, the instrument requires significant refinement, but has now taken data on both bridge wire and dense plasma focus experiments.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Quantifying Bulk and Surface Recombination in CdTe Solar Cells Using Time-Resolved Terahertz Spectroscopy

Understanding the nature of recombination mechanisms is essential for higher power conversion efficiency in photovoltaic (PV) devices. Here we use a combination of time-resolved terahertz spectroscopy and numerical modeling to determine the bulk Shockley-Read-Hall lifetime and interface and back surface recombination velocities in CdTe thin film stacks. Furthermore, the measurement was facilitated by fabricating wire-grid device structures using conventional laser scribing. Evaluation of a glass/FTO/SnO2/CdS/CdTe stack treated with CdCl2 allowed separation of the CdTe absorber bulk lifetime, 1.6 ns, from the back surface recombination velocity, ~6x10 4 cm/s, and indicated that CdTe/CdS interface recombination velocity had no significant impact on carrier dynamics.

14 SOLAR ENERGY↗

Femtosecond time-resolved XUV + UV photoelectron imaging of pure helium nanodroplets

Liquid helium nanodroplets, consisting of on average 2 × 10{sup 6} atoms, are examined using femtosecond time-resolved photoelectron imaging. The droplets are excited by an extreme ultraviolet light pulse centered at 23.7 eV photon energy, leading to states within a band that is associated with the 1s3p and 1s4p Rydberg levels of free helium atoms. The initially excited states and subsequent relaxation dynamics are probed by photoionizing transient species with a 3.2 eV pulse and using velocity map imaging to measure time-dependent photoelectron kinetic energy distributions. Significant differences are seen compared to previous studies with a lower energy (1.6 eV) probe pulse. Three distinct time-dependent signals are analyzed by global fitting. A broad intense signal, centered at an electron kinetic energy (eKE) of 2.3 eV, grows in faster than the experimental time resolution and decays in ∼100 fs. This feature is attributed to the initially excited droplet state. A second broad transient feature, with eKE ranging from 0.5 to 4 eV, appears at a rate similar to the decay of the initially excited state and is attributed to rapid atomic reconfiguration resulting in Franck-Condon overlap with a broader range of cation geometries, possibly involving formation of a Rydberg-excited (He{sub n})* core within the droplet. An additional relaxation pathway leads to another short-lived feature with vertical binding energies ≳2.4 eV, which is identified as a transient population within the lower-lying 1s2p Rydberg band. Ionization at 3.2 eV shows an enhanced contribution from electronically excited droplet states compared to ejected Rydberg atoms, which dominate at 1.6 eV. This is possibly the result of increased photoelectron generation from the bulk of the droplet by the more energetic probe photons.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Time-Resolved Synchrotron X-ray Diffraction on Pulse Laser Heated Iron in Diamond Anvil Cell

We present time-resolved synchrotron x-ray diffraction to probe the {epsilon}-{delta} phase transition of iron during pulse-laser heating in a diamond anvil cell. The system utilizes a monochromatic synchrotron x-ray beam, a two-dimensional pixel array x-ray detector and a dual beam, double side laser-heating system. Multiple frames of the diffraction images are obtained in real-time every 22 ms over 500 ms of the entire pulse heating period. The results show the structural evolution of iron phases at 17 GPa, resulting in thermal expansion coefficient 1/V({Delta}V/{Delta}T){sub p} = 7.1 x 10{sup -6}/K for {epsilon}-Fe and 2.4 x 10{sup -5}/K for {gamma}-Fe, as well as the evidence for metastability of {gamma}-Fe at low temperatures below the {epsilon}-{gamma} phase boundary.

36 MATERIALS SCIENCE↗

Time-resolved characterization and energy balance analysis of implosion core in shock-ignition experiments at OMEGA

Time-resolved temperature and density conditions in the core of shock-ignition implosions have been determined for the first time. The diagnostic method relies on the observation, with a streaked crystal spectrometer, of the signature of an Ar tracer added to the deuterium gas fill. The data analysis confirms the importance of the shell attenuation effect previously noted on time-integrated spectroscopic measurements of thick-wall targets [R. Florido et al., Phys. Rev. E 83, 066408 (2011)]. This effect must be taken into account in order to obtain reliable results. The extracted temperature and density time-histories are representative of the state of the core during the implosion deceleration and burning phases. As a consequence of the ignitor shock launched by the sharp intensity spike at the end of the laser pulse, observed average core electron temperature and mass density reach T ~ 1100 eV and ρ ~ 2 g/cm 3 ; then temperature drops to T ~ 920 eV while density rises to ρ ~ 3.4 g/cm 3 about the time of peak compression. Compared to 1D hydrodynamic simulations, the experiment shows similar maximum temperatures and smaller densities. Simulations do not reproduce all observations. Differences are noted in the heating dynamics driven by the ignitor shock and the optical depth time-history of the compressed shell. Time-histories of core conditions extracted from spectroscopy show that the implosion can be interpreted as a two-stage polytropic process. Furthermore, an energy balance analysis of implosion core suggests an increase in total energy greater than what 1D hydrodynamic simulations predict. This new methodology can be implemented in other ICF experiments to look into implosion dynamics and help to understand the underlying physics.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Nonequilibrium lattice-driven dynamics of stripes in nickelates using time-resolved x-ray scattering

Here, we investigate the lattice coupling to the spin and charge orders in the striped nickelate, La 1.75 Sr 0.25 NiO 4 , using time-resolved resonant x-ray scattering. Lattice-driven dynamics of both spin and charge orders are observed when the pump photon energy is tuned to that of an E u bond- stretching phonon. We present a likely scenario for the behavior of the spin and charge order parameters and its implications using a Ginzburg-Landau theory.

36 MATERIALS SCIENCE↗

Quantifying particle-scale 3D granular dynamics during rapid compaction from time-resolved in situ 2D x-ray images

Understanding the particle-scale dynamics of granular materials during rapid compaction and flow is of fundamental importance for manufacturing, planetary science, geology, and defense applications. Time-resolved 2D radiography and static 3D x-ray tomography are powerful in situ tools for studying particle-scale dynamics but provide detail only in 2D or with significant time-scale limitations, respectively. Here, we introduce a new method that uses 2D in situ x-ray imaging for determining time-resolved 3D particle-scale dynamics in rapidly compressed granular materials. The method employs initial particle packing structures obtained from x-ray tomography, a 2D x-ray image generation algorithm, and an optimization algorithm. We first describe and validate the method using finite element simulations. Furthermore, we then apply the technique to x-ray phase-contrast images obtained during rapid compaction of granular materials with varying particle morphology and sample thickness. The depth-resolved particle-scale dynamics reveal complex velocity and porosity fields evolving heterogeneously along and perpendicular to the compaction direction. We characterize these features, their fluctuations near the compaction front, and the compaction front thickness. Our technique can be applied to understanding granular dynamics during rapid compaction events, and rearrangements during slower, but non-quasi-static, flows.

36 MATERIALS SCIENCE↗

Time-resolved dual-comb measurement of number density and temperature in a laser-induced plasma

We demonstrate time-resolved dual-comb spectroscopy of a laser-induced plasma and characterize the temporal evolution of the absorption excitation temperature and population number density for multiple Fe transitions. The spectrum of three excited-state transitions of Fe around 533 nm are simultaneously detected at different time delays following laser ablation of a stainless steel sample. This work probes late-time behavior of laser-induced ablation plumes during plasma cooling, significant for revealing important information on molecule and particle formation. The high spectral resolution and broadband capability of the dual-comb technique, combined with time-resolved measurement capability, will aid in characterization of plasma properties, species identification, and higher resolution spectroscopy including isotopic analysis.

(140.3440) Laser-induced breakdown, (280.5395) Pla↗

Probing Cytochrome c Folding Transitions upon Phototriggered Environmental Perturbations Using Time-Resolved X-ray Scattering

Direct tracking of protein structural dynamics during folding–unfolding processes is important for understanding the roles of hierarchic structural factors in the formation of functional proteins. As such, using cytochrome c (cyt c) as a platform, we investigated its structural dynamics during folding processes triggered by local environmental changes (i.e., pH or heme iron center oxidation/spin/ligation states) with time-resolved X-ray solution scattering measurements. Starting from partially unfolded cyt c, a sudden pH drop initiated by light excitation of a photoacid caused a structural contraction in microseconds, followed by active site restructuring and unfolding in milliseconds. In contrast, the reduction of iron in the heme via photoinduced electron transfer did not affect conformational stability at short timescales (<1 ms), despite active site coordination geometry changes. These results demonstrate how different environmental perturbations can change the nature of interaction between the active site and protein conformation, even within the same metalloprotein, which will subsequently affect the folding structural dynamics.

Rimmerman, Dolev↗