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At least 1,477 records · Page 82

Attosecond light science and its application for probing quantum materials

In this paper, we review the development and application of coherent short wavelength light sources implemented using the high harmonic generation (HHG) process. The physics underlying HHG brought quantum physics into the domain of attosecond time-scales for the first time. Here, the observation and manipulation of electron dynamics on such short time-scales—a capability not conceived—of just a few decades ago—is becoming both more-and-more sophisticated and useful as a route to achieve exquisite control over short wavelength light. New experimental techniques are enabling HHG light sources to provide new insights into fundamental quantum interactions in materials, making it possible for the first time to capture the fastest charge, spin, photon and phonon interactions and to achieve diffraction-limited imaging at short wavelengths.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Structural imaging of nanoscale phonon transport in ferroelectrics excited by metamaterial-enhanced terahertz fields

Nanoscale phonon transport is a key process that governs thermal conduction in a wide range of materials and devices. Creating controlled phonon populations by resonant excitation at terahertz (THz) frequencies can drastically change the characteristics of nanoscale thermal transport and allow a direct real-space characterization of phonon mean-free paths. Using metamaterial-enhanced terahertz excitation, we tailored a phononic excitation by selectively populating low-frequency phonons within a nanoscale volume in a ferroelectric BaTiO 3 thin film. Real-space time-resolved x-ray diffraction microscopy following THz excitation reveals ballistic phonon transport over a distance of hundreds of nm, two orders of magnitude longer than the averaged phonon mean-free path in BaTiO 3 . On longer length scales, diffusive phonon transport dominates the recovery of the transient strain response, largely due to heat conduction into the substrate. The measured real-space phonon transport can be directly compared with the phonon mean-free path as predicted by molecular dynamics modeling. In conclusion, this time-resolved real-space visualization of THz-matter interactions opens up opportunities to engineer and image nanoscale transient structural states with new functionalities.

36 MATERIALS SCIENCE↗

VTXO: the Virtual Telescope for X-ray Observations

The Virtual Telescope for X-ray Observations (VTXO) will use lightweight Phase Frensel Lenses (PFLs) in a virtual X-ray telescope with 1 km focal length and with nearly 50 milli-arcsecond angular resolution. Laboratory characterization of PFLs have demonstrated near diffraction-limited angular resolution in the X-ray band, but they require long focal lengths to achieve this quality of imaging. VTXO is formed by using precision formation flying of two SmallSats: a smaller, 6U OpticsSat that houses the PFLs and navigation beacons while a larger, ESPA-class DetectorSat contains an X-ray camera, a charged-particle radiation monitor, a precision star tracker, and the propulsion for the formation flying. The baseline flight dynamics uses a highly-elliptical supersynchronous geostationary transfer orbit to allow the inertial formation to form and hold around the 90,000 km apogee for 10 hours of the 32.5-hour orbit with nearly a year mission lifetime. The guidance, navigation, and control (GN&C) for the formation flying uses standard CubeSat avionics packages, a precision star tracker, imaging beacons on the Optics Sat, and a radio ranging system that also serves as an inter-satellite communication link. VTXO’s fine angular resolution enables measuring the environments nearly an order of magnitude closer to the central engines of bright compact X-ray sources compared to the current state of the art. This X-ray imaging capability allows for the study of the effects of dust scattering nearer to the central objects such as Cyg X-3 and GX 5-1, for the search for jet structure nearer to the compact object in X-ray novae such as Cyg X-1and GRS 1915+105, and for the search for structure in the termination shock of in the Crab pulsar wind nebula. The In this paper, the VTXO science performance, SmallSat and instrument designs,and mission description is be described. The VTXO development was supported as one of the selected 2018 NASA Astrophysics SmallSat Study (AS3) missions.

John Krizmanic↗

Atomic-Level Structural Dynamics of Polyoxoniobates during DMMP Decomposition

Ambient pressure in situ synchrotron-based spectroscopic techniques have been correlated to illuminate atomic-level details of bond breaking and formation during the hydrolysis of a chemical warfare nerve agent simulant over a polyoxometalate catalyst. Specifically, a Cs 8 [Nb 6 O 19 ] polyoxoniobate catalyst has been shown to react readily with dimethyl methylphosphonate (DMMP). The atomic-level transformations of all reactant moieties, the [Nb 6 O 19 ] 8- polyanion, its Cs + counterions, and the DMMP substrate, were tracked under ambient conditions by a combination of X-ray absorption fine structure spectroscopy, Raman spectroscopy, and X-ray diffraction. Results reveal that the reaction mechanism follows general base (in contrast to specific base) hydrolysis. Together with computational results, the work demonstrates that the ultimate fate of DMMP hydrolysis at the Cs 8 [Nb 6 O 19 ] catalyst is strong binding of the (methyl) methylphosphonic acid ((M)MPA) product to the polyanions, which ultimately inhibits catalytic turnover.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Probing Hydrogen-Bond Anharmonicity in Cocrystals with Colossal Thermal Expansion

Organic cocrystals with sizable anisotropic thermal expansion (TE) are attractive building blocks for thermally responsive soft actuators. Such materials often display intermolecular H-bonding, whose thermal strength fluctuations are frequently overlooked if displacements and/or conformational changes are visible during TE. In this work, we employed variable-temperature single-crystal synchrotron diffraction to investigate the linear expansion coefficients of two organic cocrystals, 1 and 2, which exhibit colossal thermal expansivity exceeding 140 MK –1 . Despite such pronounced TE, solid-state 2 H and 13 C NMR experiments show no evidence of fast internal reorientations or large-amplitude molecular displacement during expansion. Although nondirectional π–π stacking dominates the colossal TE, our results indicate that hydrogen bonds play a non-negligible role in the anisotropic response. Molecular dynamics simulations reveal a temperature-dependent broadening of H-bond length distributions, which arises from the increased thermal sampling of an anharmonic potential energy surface. Our data support an expansion mechanism based on cooperativity in π-π interactions, accompanied by thermal softening and fluctuation-driven stretching of directional hydrogen bonds in these molecular solids. This mechanism underscores the significance of directional interactions in organic cocrystals, which is a key factor in the design of organic thermoresponsive crystalline materials.

Hernández-Morales, Ernesto A. [Univ. Nacional Auto↗

Structural evolution of liquid silicates under conditions in Super-Earth interiors

Molten silicates at depth are crucial for planetary evolution, yet their local structure and physical properties under extreme conditions remain elusive due to experimental challenges. In this study, we utilize in situ X-ray diffraction (XRD) at the Matter in Extreme Conditions (MEC) end-station of the Linear Coherent Linac Source (LCLS) at SLAC National Accelerator Laboratory to investigate liquid silicates. Using an ultrabright X-ray source and a high-power optical laser, we probed the local atomic arrangement of shock-compressed liquid (Mg,Fe)SiO 3 with varying Fe content, at pressures from 81(9) to 385(40) GPa. We compared these findings to ab initio molecular dynamics simulations under similar conditions. Results indicate continuous densification of theO-O and Mg-Si networks beyond Earth’s interior pressure range, potentially altering melt properties at extreme conditions. This could have significant implications for early planetary evolution, leading to notable differences in differentiation processes between smaller rocky planets, such as Earth and Venus, and super-Earths, which are exoplanets withmasses nearly three times that of Earth.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

In situ TEM observation of alpha-particle induced annealing of radiation damage in Durango apatite

A major issue in thermochronology and U-Th-Pb dating is the effect of radiation damage, created by α-recoils from α-decay events, on the diffusion of radiogenic elements (e.g., He and Pb) in host mineral. Up until now, thermal events have been considered as the only source of energy for the recovery of radiation-damage. However, irradiation, such as from the α-particle of the α-decay event, can itself induce damage recovery. Quantification of radiation-induced recovery caused by α-particles during α-decay events has not been possible, as the recovery process at the atomic-scale has been difficult to observe. Here we present details of the dynamics of the amorphous-to-crystalline transition process during α-particle irradiations using in situ transmission electron microscopy (TEM) and consecutive ion-irradiations: 1 MeV Kr 2+ (simulating α-recoil damage), followed by 400 keV He+ (simulating α-particle annealing). Upon the He + irradiation, partial recrystallization of the original, fully-amorphous Durango apatite was clearly evident and quantified based on the gradual appearance of new crystalline domains in TEM images and new diffraction maxima in selected area electron diffraction patterns. Thus, α-particle induced annealing occurs and must be considered in models of α-decay event damage and its effect on the diffusion of radiogenic elements in geochronology and thermochronology.

58 GEOSCIENCES↗

Two-Dimensional CsAg 5 Te 3– x S x Semiconductors: Multi-anion Chalcogenides with Dynamic Disorder and Ultralow Thermal Conductivity

Metal chalcogenides underpin a wide variety of energyrelated applications and are ideal systems for probing lattice dynamics and fundamental transport phenomena. Here we describe the synthesis and transport properties of CsAg 5 TeS 2 and its solid solution CsAg 5 Te 3-x S x (x = 1-2), new semiconductors with tunable band gaps ranging from 0.17 to 0.30 eV. CsAg 5 TeS 2 has a fully ordered two-dimensional structure that includes a group of Ag atoms in a heteroleptic tetrahedral coordination geometry (AgTe 2 S 2 ). Single-crystal X-ray diffraction indicates that the compounds crystallize in the tetragonal space group P 4/ mmm , while pair distribution function (PDF) analysis reveals off-centering at the heteroleptic Ag sites, signifying the lower-symmetry I4/ mcm space group. The underlying disorder as a phonon-blocking mechanism that helps facilitate an ultralow lattice thermal conductivity below 0.40 Wm -1 • K -1 at , ~ 300 K , highlighting the importance of local disorder in thermal transport. In conclusion, density functional theory provides additional insight into the electronic and thermal properties of the materials, which are good candidates for p-type thermoelectrics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Polymorphism of feldspars above 10 GPa

Feldspars are rock-forming minerals that make up most of the Earth’s crust. Along the mantle geotherm, feldspars are stable at pressures up to 3 GPa and may persist metastably at higher pressures under cold conditions. Previous structural studies of feldspars are limited to ~10 GPa, and have shown that the dominant mechanism of pressure-induced deformation is the tilting of AlO 4 and SiO 4 tetrahedra in a tetrahedral framework. Herein, based on results of in situ single-crystal X-ray diffraction studies up to 27 GPa, we report the discovery of new high-pressure polymorphs of the feldspars anorthite (CaSi 2 Al 2 O 8 ), albite (NaAlSi 3 O 8 ) , and microcline (KAlSi 3 O 8 ). The phase transitions are induced by severe tetrahedral distortions, resulting in an increase in the Al and/or Si coordination number. High-pressure phases derived from feldspars could persist at depths corresponding to the Earth upper mantle and could possibly influence the dynamics and fate of cold subducting slabs.

58 GEOSCIENCES↗

Phase transformation pathways of ultrafast-laser-irradiated Ln 2 O 3 ( Ln = Er – Lu )

Ultrafast laser irradiation causes intense electronic excitations in materials, leading to transient high temperatures and pressures. Here, we show that ultrafast laser irradiation drives an irreversible cubic-to-monoclinic phase transformation in Ln 2 O 3 ( Ln = Er – Lu ) , and explore the mechanism by which the phase transformation occurs. A combination of grazing incidence x-ray diffraction and transmission electron microscopy are used to determine the magnitude and depth-dependence of the phase transformation, respectively. Although all compositions undergo the same transformation, their transformation mechanisms differ. The transformation is pressure-driven for Ln = Tm – Lu , consistent with the material's phase behavior under equilibrium conditions. However, the transformation is thermally driven for Ln = Er , revealing that the nonequilibrium conditions of ultrafast laser irradiation can lead to novel transformation pathways. Ab initio molecular-dynamics simulations are used to examine the atomic-scale effects of electronic excitation, showing the production of oxygen Frenkel pairs and the migration of interstitial oxygen to tetrahedrally coordinated constitutional vacancy sites, the first step in a defect-driven phase transformation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Experimental and theoretical study of topology and electronic correlations in PuB 4

We synthesize single crystals of PuB 4 using an Al-flux technique. Single-crystal diffraction data provide structural parameters for first-principles density functional theory (DFT) calculations. By computing the density of states, the Z 2 topological invariant using the Wilson loop method, and the surface electronic structure from slab calculations, we find that PuB 4 is a nonmagnetic strong topological insulator with a band gap of 254 meV. Our magnetic susceptibility, heat capacity, and resistivity measurements are consistent with this analysis, albeit with a smaller gap of 35 meV. DFT plus dynamical mean-field theory calculations show that electronic correlations reduce the size of the band gap, and provide better agreement with the value determined by resistivity. Furthermore, these results demonstrate that PuB 4 is a promising actinide material to investigate the interplay of electronic correlations and nontrivial topology.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Correlating Nanoscopic Energy Transfer and Far-Field Emission to Unravel Lasing Dynamics in Plasmonic Nanocavity Arrays

Excited-state interactions between nanoscale cavities and photoactive molecules are critical in plasmonic nanolasing, although the underlying details are less-resolved. This paper reports direct visualization of the energy-transfer dynamics between two-dimensional arrays of plasmonic gold bowtie nanocavities and dye molecules. Transient absorption microscopy measurements of single bowties within the array surrounded by gain molecules showed fast excited-state quenching (2.6 ± 1 ps) characteristic of individual nanocavities. Upon optical pumping at powers above threshold, lasing action emerged depending on the spacing of the array. By correlating ultrafast microscopy and far-field light emission characteristics, we found that bowtie nanoparticles acted as isolated cavities when the diffractive modes of the array did not couple to the plasmonic gap mode. These results demonstrate how ultrafast microscopy can provide insight into energy relaxation pathways and, specifically, how nanocavities in arrays can show single-unit nanolaser properties.

14 SOLAR ENERGY↗

Nonisentropic Release of a Shocked Solid

Here, we introduce molecular dynamics simulations of shock and release in micron-scale tantalum crystals that exhibit postbreakout temperatures far exceeding those expected under the standard assumption of isentropic release. We illustrate via an energy-budget analysis that this is due to plastic-work heating from material strength that largely counters thermoelastic cooling. The simulations are corroborated by experiments where the release temperatures of laser-shocked tantalum foils are deduced from their thermal strains via in situ x-ray diffraction and are found to be close to those behind the shock.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Luciola Hypertelescope Space Observatory

Luciola is a large (one kilometer) "multi-aperture densified-pupil imaging interferometer", or "hypertelescope" employing many small apertures, rather than a few large ones, for obtaining direct snapshot images with a high information content. A diluted collector mirror, deployed in space as a flotilla of small mirrors, focuses a sky image which is exploited by several beam-combiner spaceships. Each contains a pupil densifier micro-lens array to avoid the diffractive spread and image attenuation caused by the small sub-apertures. The elucidation of hypertelescope imaging properties during the last decade has shown that many small apertures tend to be far more efficient, regarding the science yield, than a few large ones providing a comparable collecting area. For similar underlying physical reasons, radio-astronomy has also evolved in the direction of many-antenna systems such as the proposed Low Frequency Array having hundreds of thousands of individual receivers . With its high limiting magnitude, reaching the mv=30 limit of HST when 100 collectors of 25cm will match its collecting area, high-resolution direct imaging in multiple channels, broad spectral coverage from the 1200 Angstrom ultra-violet to the 20 micron infra-red, apodization, coronagraphic and spectroscopic capabilities, the proposed hypertelescope observatory addresses very broad and innovative science covering different areas of ESA s Cosmic Vision program. In the initial phase, a focal spacecraft covering the UV to near IR spectral range of EMCCD photon-counting cameras ( currently 200 to 1000nm), will image details on the surface of many stars, as well as their environment, including multiple stars and clusters. Spectra will be obtained for each resel. It will also image neutron star, black-hole and micro-quasar candidates, as well as active galactic nuclei, quasars, gravitational lenses, and other Cosmic Vision targets observable with the initial modest crowding limit. With subsequent upgrade missions, the spectral coverage can be extended from 120nm to 20 microns, using four detectors carried by two to four focal spacecraft. The number of collector mirrors in the flotilla can also be increased from 12 to 100 and possibly 1,000. The imaging and spectroscopy of habitable exoplanets in the mid infra-red then becomes feasible once the collecting area reaches 6m2 , using a specialized mid infra-red focal spacecraft. Calculations ( Boccaletti et al., 2000) have shown that hypertelescope coronagraphy has unequalled sensitivity for detecting, at mid infra-red wavelengths, faint exoplanets within the exo-zodiacal glare. Later upgrades will enable the more difficult imaging and spectroscopy of these faint objects at visible wavelengths, using refined techniques of adaptive coronagraphy (Labeyrie. & Le Coroller, 2004). Together, the infra-red and visible spectral data carry rich information on the possible presence of life. The close environment of the central black-hole in the Milky Way will be imageable with unprecedented detail in the near infra-red . Cosmological imaging of remote galaxies at the limit of the known universe is also expected, from the ultra-violet to the near infra-red, following the first upgrade, and with greatly increasing sensitivity through successive upgrades. These areas will indeed greatly benefit from the upgrades, in terms of dynamic range, limiting complexity of the objects to be imaged, size of the elementary Direct Imaging Field , and limiting magnitude, approaching that of an 8-meter space telescope when 1000 apertures of 25cm are installed. Similar gains will occur for addressing fundamental problems in physics and cosmology, particularly when observing neutron stars and black holes, single or binary, including the giant black holes, with accretion disks and jets, in active galactic nuclei beyond the Milky Way. Gravitational lensing and micro-lensing patterns, including time-variable patterns and perhaps millisecond lensing flasheshich may be beamed by diffraction from sub-stellar masses at sub-parsec distances (Labeyrie, 1994) , will also be observable initially in the favourable cases, and upgrades will greatly improve the number of observable objects. The observability of gravitational waves emitted by binary lensing masses, in the form of modulated lensing patterns, is a debated issue ( Ragazzoni et al., 2003) but will also become addressable observationally. The technology readiness of Luciola approaches levels where low-orbit testing and stepwise implementation will become feasible in the 2015-2025 time frame. For the following decades beyond 2020, once accurate formation flying techniques will be mastered, much larger hypertelescopes such as the proposed 100km Exo-Earth Imager and the 100,000 km Neutron Star Imager should also become feasible. Luciola is therefore also seen as a precursor toward such very powerful instruments.

Labeyrie, Antoine↗

Effect of solution chemistry on the iodine release from iodoapatite in aqueous environments

To ensure the safe disposal of nuclear waste, understanding the release process of radionuclides retained in the nuclear waste forms is of vital importance. Iodoapatite Pb 9.85 (VO 4 ) 6 I 1.7 , a potential waste form for iodine-129, was selected as a model system for ceramic waste forms in this study to understand the effect of aqueous species on iodine release. Semi-dynamic leaching tests were conducted on bulk samples in cap-sealed Teflon vessels with 0.1 mol/L NaCl, Na 2 CO 3 , Na 3 PO 4 , and Na 2 SO 4 solutions under 90 °C, fixed sample surface area to solution volume ratio of 5/m, and periodic replacement of leaching solutions. The reacted solutions were then analyzed by Inductively Coupled Plasma-Mass Spectrometry and Inductively Coupled Plasma-Optical Emission Spectrometry; the leached surfaces were characterized by X-ray diffraction, scanning electron microscopy, and infrared spectroscopy. The finding shows that, compared to deionized water, the ion-rich solutions enhanced the iodine release as a result of the increased ionic strength, reduced activity coefficient of dissolved species, and increased solution pH. Surface reactions can lead to the formations of secondary phases by ion-exchange and precipitation. These findings indicate that an ion-rich environment in the geological repository can be detrimental to the disposal safety of the nuclear waste form.

36 MATERIALS SCIENCE↗

Synthesis of magnesiowüstite nanocrystallites embedded in an amorphous silicate matrix via low energy multiple ion implantations

The synthesis process is presented for experimentally simulating modifications in cosmic dust grains using sequential ion implantations or irradiations followed by thermal annealing. Cosmic silicate dust analogues were prepared via implantation of 20–80 keV Fe - , Mg - , and O - ions into commercially available p-type silicon (100)wafers. The as-implanted analogues are amorphous with a Mg/(Fe+Mg) ratio of 0.5 tailored to match theoretical abundances in circumstellar dusts. Before the ion implantations were performed, Monte-Carlo-based ion-solid interaction codes were used to model the dynamic redistribution of the implanted atoms in the silicon substrate. 600 keV helium ion irradiation was performed on one of the samples before thermal annealing. Two samples were thermally annealed at a temperature appropriate for an M-class stellar wind, 1000 K, for 8.3 h in a vacuum chamber with a pressure of 1 x 10 -7 torr. The elemental depth profiles were extracted utilizing Rutherford Backscattering Spectrometry (RBS) in the samples before and after thermal annealing. X-ray diffraction (XRD)analysis was employed for the identification of various phases in crystalline minerals in the annealed analogues. Transmission electron microscopy (TEM) analysis was utilized to identify specific crystal structures. RBS analysis shows redistribution of the implanted Fe, Mg, and O after thermal annealing due to incorporation into the crystal structures for each sample type. XRD patterns along with TEM analysis showed nanocrystalline Mg and Fe oxides with possible incorporation of additional silicate minerals.

79 ASTRONOMY AND ASTROPHYSICS↗

Pressure-tuned quantum criticality in the large-D antiferromagnet DTN

Strongly correlated spin systems can be driven to quantum critical points via various routes. In particular, gapped quantum antiferromagnets can undergo phase transitions into a magnetically ordered state with applied pressure or magnetic field, acting as tuning parameters. These transitions are characterized by z = 1 or z = 2 dynamical critical exponents, determined by the linear and quadratic low-energy dispersion of spin excitations, respectively. Employing high-frequency susceptibility and ultrasound techniques, we demonstrate that the tetragonal easy-plane quantum antiferromagnet NiCl 2 · 4SC(NH 2 ) 2 (aka DTN) undergoes a spin-gap closure transition at about 4.2 kbar, resulting in a pressure-induced magnetic ordering. The studies are complemented by high-pressure-electron spin-resonance measurements confirming the proposed scenario. Powder neutron diffraction measurements revealed that no lattice distortion occurs at this pressure and the high spin symmetry is preserved, establishing DTN as a perfect platform to investigate z = 1 quantum critical phenomena. The experimental observations are supported by DMRG calculations, allowing us to quantitatively describe the pressure-driven evolution of critical fields and spin-Hamiltonian parameters in DTN.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

High-resolution high-throughput spatiotemporal strain imaging reveals loss mechanisms in a surface acoustic wave device

Surface acoustic wave devices are key components for processing radio frequency signals in wireless communication because these devices offer simultaneously high performance, compact size and low cost. The optimization of the device structure requires a quantitative understanding of energy conversion and loss mechanisms. Here we use stroboscopic full-field diffraction x-ray microscopy to reveal an unanticipated acoustic loss in a prototypical one-port resonator device. A non-uniform acoustic excitation in the active area was responsible for the substantial end and side leakages observed at the design frequency. Quantitative analysis of the strain amplitude using a wave decomposition method allowed the determination of several key device parameters. This high-resolution high-throughput spatiotemporal strain imaging technique is more generally applicable to the study of dynamic strain modulation in nanoscale acoustic, electronic, optical and quantum devices. The high sensitivity allows precise measurement of the strain modulation with picometer-scale amplitude.

Zhou, Tao [ESRF - The European Synchrotron, Grenob↗