Observation of Transient and Asymptotic Driven Structural States of Tungsten Exposed to Radiation
Not Available
36 MATERIALS SCIENCE↗
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Structural and chemical orders in N i 64.5 Z r 35.5 metallic glass by molecular dynamics simulation
The atomic structure of Ni 64.5 Zr 35.5 metallic glass has been investigated by molecular dynamics (MD) simulations. The calculated structure factors from the MD glassy sample at room temperature agree well with the X-ray diffraction (XRD) and neutron diffraction (ND) experimental data. Using the pairwise cluster alignment and clique analysis methods, we show that there are three types dominant short-range order (SRO) motifs around Ni atoms in the glass sample of Ni 64.5 Zr 35.5 , i.e., Mixed- Icosahedron(ICO)-Cube, Twined-Cube and icosahedron-like clusters. Furthermore, chemical order and medium-range order (MRO) analysis show that the Mixed-ICOCube and Twined-Cube clusters exhibit the characteristics of the crystalline B2 phase. In conclusion, our simulation results suggest that the weak glass-forming ability (GFA) of Ni 64.5 Zr 35.5 can be attributed to the competition between the glass forming ICO SRO and the crystalline Mixed-ICO-Cube and Twined-Cube motifs.
36 MATERIALS SCIENCE↗
An Integrated Study on a Novel High Temperature High Entropy Alloy
This report summarizes our recent works of theoretical modeling, simulation, and experimental validation of the simulation results on the new refractory high entropy alloy (HEA) design and oxide doped refractory HEA research. The simulation of the stability and thermal dynamics simulation on potential thermal stable candidates were performed and related HEA with oxide doped samples were synthesized and characterized. The HEA ab initio density functional theory and molecular dynamics physical property simulation methods and experimental texture validation techniques development, achievements already reached, course work development, students and postdoc training, and future improvement research directions are briefly introduced.
36 MATERIALS SCIENCE↗
Rewritable three-dimensional holographic data storage via optical forces
The development of nanostructures that can be reversibly arranged and assembled into 3D patterns may enable optical tunability. However, current dynamic recording materials such as photorefractive polymers cannot be used to store information permanently while also retaining configurability. Here, we describe the synthesis and optimization of a silver nanoparticle doped poly(2-hydroxyethyl methacrylate-co-methacrylic acid) recording medium for reversibly recording 3D holograms. We theoretically and experimentally demonstrate organizing nanoparticles into 3D assemblies in the recording medium using optical forces produced by the gradients of standing waves. The nanoparticles in the recording medium are organized by multiple nanosecond laser pulses to produce reconfigurable slanted multilayer structures. We demonstrate the capability of producing rewritable optical elements such as multilayer Bragg diffraction gratings, 1D photonic crystals, and 3D multiplexed optical gratings. We also show that 3D virtual holograms can be reversibly recorded. This recording strategy may have applications in reconfigurable optical elements, data storage devices, and dynamic holographic displays.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Elucidating the Atomic Structures of the Gel Layer Formed during Aluminoborosilicate Glass Dissolution: An Integrated Experimental and Simulation Study
The altered glasses produced during aqueous dissolution of silicate and borosilicate glasses are among the most complex structures to understand at the atomic level due to their amorphous nature, random porosity and various levels of hydration. In this study, we gained insights of the complex atomic structures of altered aluminoborosilicate glasses by combining a range of experimental and computational approaches. The altered glasses were prepared by dissolution of three glasses with varying level of alumina in acid for 7 days. A comprehensive set of experimental [elemental analysis, high-energy X-ray diffraction, 29 Si and 27 Al solid-state nuclear magnetic resonance (NMR), and O 1s X-ray photoelectron spectroscopy (XPS)] and modeling (molecular dynamics (MD) simulations using non-reactive and reactive force fields) were used to study the atomic structures of these altered glasses. Elemental analysis showed that most of the B in the pristine glasses was leached into the solution and was not contained in the altered glass. The 29 Si and 27 Al solid-state NMR spectra revealed that the altered glasses have more polymerized silicate network as compared to those in the pristine glasses due to the reformation of linkages among Si and Al oxygen polyhedral in the altered glasses. The bridging and non-bridging (or hydroxyl O) atoms in the altered glasses were also quantified from their O 1s XPS spectra. Atomic structure models of the altered glasses were constructed by using MD simulations using the reactive force field based on the compositional information obtained from experiments. Various pore structures were generated using the charge-scaling (CS) method by using different initial densities and CS temperatures; the best CS parameters of each alternated glass were then determined by comparing with the experimental structure factors obtained from high energy X-ray diffraction. Pore and the atomic structures and vibrational properties around these pore surfaces were analyzed. Furthermore, these results from this comprehensive study thus provides a realistic insight into the pore morphology, atomic structure, and vibrational properties of altered glasses.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Diameter-dependent hydrophobicity in carbon nanotubes
Single-wall carbon nanotubes (SWCNTs) are a good model system that provides atomically smooth nanocavities. It has been reported that water-SWCNTs exhibit hydrophobicity depending on the temperature T and the SWCNT diameter D. SWCNTs adsorb water molecules spontaneously in their cylindrical pores around room temperature, whereas they exhibit a hydrophilic-hydrophobic transition or wet-dry transition (WDT) at a critical temperature T{sub wd} ≈ 220-230 K and above a critical diameter D{sub c} ≈ 1.4-1.6 nm. However, details of the WDT phenomenon and its mechanism remain unknown. Here, we report a systematic experimental study involving X-ray diffraction, optical microscopy, and differential scanning calorimetry. It is found that water molecules inside thick SWCNTs (D > D{sub c}) evaporate and condense into ice Ih outside the SWCNTs at T{sub wd} upon cooling, and the ice Ih evaporates and condenses inside the SWCNTs upon heating. On the other hand, residual water trapped inside the SWCNTs below T{sub wd} freezes. Molecular dynamics simulations indicate that upon lowering T, the hydrophobicity of thick SWCNTs increases without any structural transition, while the water inside thin SWCNTs (D < D{sub c}) exhibits a structural transition, forming an ordered ice. This ice has a well-developed hydrogen bonding network adapting to the cylindrical pores of the SWCNTs. Thus, the unusual diameter dependence of the WDT is attributed to the adaptability of the structure of water to the pore dimension and shape.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Dissolving salt is not equivalent to applying a pressure on water
Abstract Salt water is ubiquitous, playing crucial roles in geological and physiological processes. Despite centuries of investigations, whether or not water’s structure is drastically changed by dissolved ions is still debated. Based on density functional theory, we employ machine learning based molecular dynamics to model sodium chloride, potassium chloride, and sodium bromide solutions at different concentrations. The resulting reciprocal-space structure factors agree quantitatively with neutron diffraction data. Here we provide clear evidence that the ions in salt water do not distort the structure of water in the same way as neat water responds to elevated pressure. Rather, the computed structural changes are restricted to the ionic first solvation shells intruding into the hydrogen bond network, beyond which the oxygen radial-distribution function does not undergo major change relative to neat water. Our findings suggest that the widely cited pressure-like effect on the solvent in Hofmeister series ionic solutions should be carefully revisited.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Dataset of simulated vibrational density of states and X-ray diffraction profiles of mechanically deformed and disordered atomic structures in Gold, Iron, Magnesium, and Silicon
This dataset is comprised of a library of atomistic structure files and corresponding X-ray diffraction (XRD) profiles and vibrational density of states (VDoS) profiles for bulk single crystal silicon (Si), gold (Au), magnesium (Mg), and iron (Fe) with and without disorder introduced into the atomic structure and with and without mechanical loading. Included with the atomistic structure files are descriptor files that measure the stress state, phase fractions, and dislocation content of the microstructures. All data was generated via molecular dynamics or molecular statics simulations using the Large-scale Atomic/Molecular Massively Parallel Simulator (LAMMPS) code. This dataset can inform the understanding of how local or global changes to a materials microstructure can alter their spectroscopic and diffraction behavior across a variety of initial structure types (cubic diamond, face-centered cubic (FCC), hexagonal close-packed (HCP), and body-centered cubic (BCC) for Si, Au, Mg, and Fe, respectively) and overlapping changes to the microstructure (i.e., both disorder insertion and mechanical loading).
96 KNOWLEDGE MANAGEMENT AND PRESERVATION↗
Structural and dynamical trends in alkali-metal silanides characterized by neutron-scattering methods
Structural, vibrational, and dynamical properties of the mono- and mixed-alkali silanides (MSiH 3 , where M = K, Rb, Cs, K 0.5 Rb 0.5 , K 0.5 Cs 0.5 , and Rb 0.5 Cs 0.5 ) were investigated by various neutron experiments, including neutron powder diffraction (NPD), neutron vibrational spectroscopy (NVS), neutron-scattering fixed-window scans (FWSs), and quasielastic neutron scattering (QENS) measurements. Structural characterization showed that the mixed compounds exhibit disordered (α) and ordered (β) phases for temperatures above and below about 200–250 K, respectively, in agreement with their monoalkali correspondents. Vibrational and dynamical properties are strongly influenced by the cation environment; in particular, there is a red shift in the band energies of the librational and bending modes with increasing lattice size as a result of changes in the bond lengths and force constants. Additionally, slightly broader spectral features are observed in the case of the mixed compounds, indicating the presence of structural disorder caused by the random distribution of the alkali-metal cations within the lattice. FWS measurements upon heating showed that there is a large increase in reorientational mobility as the systems go through the order–disorder (β–α) phase transition, and measurements upon cooling of the α-phase revealed the known strong hysteresis for reversion back to the β-phase. Interestingly, at a given temperature, among the different alkali silanide compounds, the relative reorientational mobilities of the SiH 3 – anions in the α- and β-phases tended to decrease and increase, respectively, with increasing alkali-metal mass. Lastly, this dynamical result might provide some insights concerning the enthalpy–entropy compensation effect previously observed for these potentially promising hydrogen storage materials.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Chloride Insertion Enhances the Electrochemical Oxidation of Iron Hydroxide Double-Layer Hydroxide into Oxyhydroxide in Alkaline Iron Batteries
Rechargeable alkaline iron batteries that constitute environmentally benign electrolytes and earth-abundant industrial materials are desirable green solutions for large-scale energy storage. As one of the most abundant metal elements in the earth’s crust, iron (Fe) can satisfy nearly all criteria for low-cost and safe battery electrodes. However, challenges in achieving reversible Fe redox impede their extensive implementation in modern energy supply systems. Here, this study revealed that Cl-anion insertion into Fe(OH) 2 layered double hydroxide (LDH) formed a green rust intermediate phase with the formula [Fe 2 2+ Fe 1 3+ (HO – ) 6 ] + [Cl] – , which assisted a high Fe(OH) 2 /FeOOH conversion reaction (64.7%) and improved cycling stability. This new iron redox chemistry was validated by operando X-ray diffraction, electrochemical testing, X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS) analysis, scanning transmission electron microscopy–energy-dispersive X-ray spectroscopy (STEM-EDS) mapping, and molecular dynamics (MD) simulations. Our study provides new insight into designing LDH materials for high-capacity alkaline iron batteries.
36 MATERIALS SCIENCE↗
Effects of pressure on the structure and lattice dynamics of [alpha]-glycine: a combined experimental and theoretical study
Abstract not provided
Hinton, Jasmine K.↗
Real Space Imaging of Spin Stripe Domain Fluctuations in a Complex Oxide
Understanding the formation and dynamics of charge and spin-ordered states in low-dimensional transition metal oxide materials is crucial to understanding unconventional high-temperature superconductivity. La 2-x Sr x NiO 4+δ (LSNO) has attracted much attention due to its interesting spin dynamics. Recent x-ray photon correlation spectroscopy studies have revealed slow dynamics of the spin order (SO) stripes in LSNO. Here, we applied resonant soft x-ray ptychography to map the spatial distribution of the SO stripe domain inhomogeneity in real space. The reconstructed images show the SO domains are spatially anisotropic, in agreement with previous diffraction studies. For the SO stripe domains, it is found that the correlation lengths along different directions are strongly coupled in space. Surprisingly, fluctuations were observed in the real space amplitude signal, rather than the phase or position. Overall, we attribute the observed slow dynamics of the stripe domains in LSNO to thermal fluctuations of the SO domain boundaries.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Spin Waves in Dirac Semimetal Ca 0.6 Sr 0.4 MnSb 2 Investigated with Neutrons by the Diffraction Method
The tunability of Dirac semimetals with antiferromagnetic Mn layers is of great interest. The observed sign change of interlayer magnetic coupling between CaMnBi 2 and SrMnBi 2 suggests ionic substitution as a potential tuning mechanism. If so, novel behavior near the compensation point could be expected. Here, to explore this, we study a mixed-cation analog, Ca 0.6 Sr 0.4 MnSb 2 , where Bi is replaced by Sb. Conventional inelastic neutron scattering is impractical due to the small crystal size (m ≈ 0.28 g) available for compositional studies; however, we find that using a neutron diffractometer with a wide-angle area detector we can obtain a good quality spin-wave signal, which is shaped by energy-momentum conservation and retains spectroscopic information even without direct energy analysis. Spin-wave modeling reveals an interlayer coupling quantitatively similar to SrMnSb 2 , indicating it is not directly tuned by ionic size and that the sign change in Bi-based compounds likely arises from the observed change in lattice symmetry. Beyond this key insight, our results present an efficient method for parametric and compositional studies of spin dynamics in small crystals.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Ultrafast photochemistry and electron-diffraction spectra in n → (3s) Rydberg excited cyclobutanone resolved at the multireference perturbative level
We study the ultrafast time evolution of cyclobutanone excited to the singlet n → Rydberg state through non-adiabatic surface-hopping simulationsperformed at extended multi-state complete active space second-order perturbation (XMS-CASPT2) level of theory. These dynamics predict relaxation to the ground-state with a timescale of 822 ± 45 fs with minimal involvement of the triplets. The major relaxation path to the ground-state involves a three-state degeneracy region and leads to a variety of fragmented photoproducts. We simulate the resulting time-resolved electron-diffraction spectra, which track the relaxation of the excited state and the formation of various photoproducts in the ground state.
Chemistry↗
Tunable electron beam pulser for picoseconds stroboscopic microscopy in transmission electron microscopes
For two decades, time-resolved transmission electron microscopes (TEM) have relied on pulsed-laser photoemission to generate electron bunches to explore sub-microsecond to sub-picosecond dynamics. Despite the vast successes of photoemission time-resolved TEMs, laser-based systems are inherently complex, thus tend not to be turn-key. In this paper, we report on the successful retrofit of a commercial 200 keV TEM, without an external laser, capable of producing continuously tunable pulsed electron beams with repetition rates from 0.1 GHz up to 12 GHz and a tunable bunch length from tens of nanoseconds down to 10 ps. This innovation enables temporal access into previously inaccessible regimes: i.e., high repetition rate stroboscopic experiments. Combination of a pair of RF-driven traveling wave stripline elements, quadrupole magnets, and a variable beam aperture enables operation of the instrument in (1) continuous waveform (CW) mode as though the instrument was never modified (i.e. convention TEM operation mode, where the electrons from the emission cathode randomly arrive at the sample without resolvable time information), (2) stroboscopic (pump-probe) mode, and (3) pulsed beam mode for dose rate sensitive materials. In order to analyze the effect of a pulsed beam on image quality, we examined Au nanoparticles using bright field, high-resolution TEM imaging and selected area diffraction in both continuous and pulsed-beam mode. Furthermore, in comparison of conventional TEMs, the add-on beam pulser enables the observation of ultrafast dynamic behavior in materials that are reversible under synchronized excitation.
36 MATERIALS SCIENCE↗
Imaging Nanoscale Energy Transport and Conversion with Ultrafast Electron Microscopy (Final Technical Report)
Light-matter interactions are ubiquitous in nature and reside at the heart of innumerable technologies. The cascade of processes that occur when a material absorbs a photon of light are exceedingly complex and are interwoven in both space and time, rendering precise determination of the atomic-scale and ultrafast mechanisms immensely challenging. The advent of methods for generating short pulses of light several decades ago led to major advances in understanding the initial moments of light absorption and the resultant effects, though directly interrogating the response of the atoms within the material continued to prove challenging. More recently, methods for generating ultrashort pulses of X-rays and fast electrons have opened the way to probing photoinduced structural dynamics of a wide range of matter in multiple phases. An especially promising laboratory-scale method is ultrafast electron microscopy (UEM), wherein the modalities of conventional transmission electron microscopes (imaging, diffraction, spectroscopy) are extended into the femtosecond temporal regime. Here, the ultrafast imaging and diffraction modalities of UEM were used to study the transient structural aspects of photoexcitation of semiconducting materials (e.g., spatially-resolved electron-phonon coupling, excitation and emission of acoustic phonons, and discrete nanoscale scattering processes). The project had three main objectives: (1) determination of the excitation mechanisms of dense, hypersonic charge-carrier waves and the spatially mediated means by which they couple to the lattice via coherent phonon emission, especially with UEM imaging, wherein effects of nanoscale structural and morphological features on the coupling and relaxation dynamics are expected to dictate nucleation sites and preferred wave vectors, (2) elucidation of photoinduced acoustic-phonon seeding, emergence, propagation, and decay over nanoscale crystal regions and especially with respect to local strain fields and atomic-scale disruptions in lattice order, and (3) interwoven with the first two were efforts aimed at realizing combined angstrom-femtosecond spatiotemporal imaging with UEM. The outcomes and impacts of this project were the generation of new knowledge with respect to fundamental light-matter interactions and, especially, the spatially-mediated excitation and evolution of the structural response of materials following coherent photoexcitation. Importantly, the spatial and temporal resolutions of the UEM imaging modalities used are well-suited for such studies and enable spatially-resolved mechanisms to be determined as a function of atomic order, structural features, and morphology. In addition, ultrafast crystallographic measurements were used to correlate real- and reciprocal-space dynamics in order to determine atomic-scale preferential wave vectors and ultrafast scattering mechanisms, especially as dictated by specimen boundary conditions. The obtained results, as detailed in peer-reviewed publications and presentations, illustrate the importance of ultrafast, angstrom-scale real-space imaging for developing a comprehensive understanding of energy transport and conversion in materials.
47 OTHER INSTRUMENTATION↗
Subpicosecond Optical Stress Generation in Multiferroic BiFeO 3
We report optical excitation leads to ultrafast stress generation in the prototypical multiferroic BiFeO 3 . The time scales of stress generation are set by the dynamics of the population of excited electronic states and the coupling of the electronic configuration to the structure. X-ray free-electron laser diffraction reveals high-wavevector subpicosecond-time scale stress generation following ultraviolet excitation of a BiFeO 3 thin film. Stress generation includes a fast component with a 1/e rise time with an upper limit of 300 fs and longer-rise time components extending to 1.5 ps. The contributions of the fast and delayed components vary as a function of optical fluence, with a reduced a fast-component contribution at high fluence. The results provide insight into stress-generation mechanisms linked to the population of excited electrons and point to new directions in the application of nanoscale multiferroics and related ferroic complex oxides. The fast component of the stress indicates that structural parameters and properties of ferroelectric thin film materials can be optically modulated with 3 dB bandwidths of at least 0.5 THz.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
Ionic Precursors Transformed Into Vinyl Acetate Synthesis Catalyst via Reaction-Driven Restructuring
Conventional preparation of supported bimetallic catalysts relies on solution-mediated metal salt immobilization and pre-formation of alloy nanoparticles before reaction. Here, we report a fundamentally different synthesis strategy of using a physical mixture of salt precursors to generate an active catalyst during reaction. The catalytic structure is generated in situ from Pd3(OAc)6, Au(OH)3, and KOAc through H2 treatment and reaction-driven restructuring under vinyl acetate monomer (VAM) synthesis conditions. Ascertained from in situ X-ray diffraction and operando infrared spectroscopy analyses, reduction treatment produces segregated Pd and Au domains, and subsequent exposure to a VAM reaction mixture triggers dynamic extraction of Pd from the metal surface. This latter process, mediated by acetate-assisted redox cycles, facilitates Pd migration toward Au domains to form a near-surface localized Pd50Au50 alloy phase. Monometallic Pd domains serve as a reservoir of Pd to the alloy phase, leading to and sustaining a more Pd-enriched active surface and a higher population of accessible Pd sites, compared to a conventionally prepared K-PdAu/SiO2 catalyst. Consequently, this leads to a twofold increase in the VAM formation rate, demonstrating highly active bimetallic catalysts can be generated through the gas-phase treatment of physically mixed ionic precursors.
Cha, Byeong Jun [Rice University]↗