Effects on nuclear structure in mu-atomic spectra
Nuclear structure effects in muon-meson atomic spectral analyses
NUCLEAR STRUCTURE↗
SEARCH · Engineering Papers
Results for “atomic structure”
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In situ synchrotron pair distribution function analysis to monitor synthetic pathways under electromagnetic excitation
Electromagnetic (EM) fields, specifically microwave radiation (MWR), can significantly influence the synthesis of ceramic oxide materials and promote rapid, low-temperature growth. However, the mechanisms by which EM fields affect the phase formation process are not well understood. A major limitation to increasing this understanding has been the lack of information regarding dynamic changes in local atomic structure during MWR exposure compared to conventional hydrothermal synthesis routes. Here, we utilize in situ synchrotron X-ray pair distribution function (PDF) analysis to monitor MWR-assisted SnO 2 nanoparticle synthesis. A clear impact of the EM field is demonstrated, with MWR inducing changes in nearest neighbor distances and peaks in oxygen atomic displacement that do not occur during synthesis without MWR exposure. The observed local structural disorder serves as a precursor to rapid rutile SnO 2 nanoparticle crystallization, suggesting that EM field-assisted growth is mediated by changes to the oxygen sublattice. These findings further our understanding of the mechanisms underlying MWR-assisted synthesis and represent a step towards utilizing EM fields to engineer tailored atomic structures for a broad range of applications.
36 MATERIALS SCIENCE↗
Structure and vibrations of different charge Ge impurity in α-quartz
Atomic structure and localized vibrations of α‐SiO{sub 2}:Ge are studied using computer modeling techniques. The simulation was carried out by the lattice dynamics calculation of the local density of vibrational states. Local structures parameters are calculated, localized symmetrized vibrations frequency caused by Ge impurity in different charge states are defined. The movements of atoms located near Ge impurity are analyzed and their contribution into localized vibrations of different type is evaluated.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
One- and two-photon ionization of hydrogen atom embedded in Debye plasmas
We present a detailed analysis of the plasma-induced resonance-like atomic structures near the ionization threshold in one- and two-photon ionization of hydrogen atom. Such resonance-like structures result from the migration of the upper bound excited states of bound-bound atomic transitions into the continuum due to the less attractive screened Coulomb potential which simulates the external environmental effect for an atom embedded in Debye plasma. The change from the resonance-like narrow structures into broad continuous spectra as the plasma effect increases could be accounted for by the overlap between the respective wavefunctions of the atomic electron in the initial state and its corresponding outgoing ionized state in the continuum.
74 ATOMIC AND MOLECULAR PHYSICS↗
Identification and correction of temporal and spatial distortions in scanning transmission electron microscopy
Scanning transmission electron microscopy (STEM) has become the technique of choice for quantitative characterization of atomic structure of materials, where the minute displacements of atomic columns from high-symmetry positions can be used to map strain, polarization, octahedra tilts, and other physical and chemical order parameter fields. The latter can be used as inputs into mesoscopic and atomistic models, providing insight into the correlative relationships and generative physics of materials on the atomic level. However, these quantitative applications of STEM necessitate understanding the microscope induced image distortions and developing the pathways to compensate them both as part of a rapid calibration procedure for in situ imaging, and the post-experimental data analysis stage. Here, we explore the spatiotemporal structure of the microscopic distortions in STEM using multivariate analysis of the atomic trajectories in the image stacks. Based on the behavior of principal component analysis (PCA), we develop the Gaussian process (GP)-based regression method for quantification of the distortion function. The limitations of such an approach and possible strategies for implementation as a part of in-line data acquisition in STEM are discussed. Here, the analysis workflow is summarized in a Jupyter notebook that can be used to retrace the analysis and analyze the reader's data.
36 MATERIALS SCIENCE↗
Single crystalline thin films as a novel class of electrocatalysts
The ubiquitous use of single crystal metal electrodes has garnered invaluable insight into the relationship between surface atomic structure and functional electrochemical properties. But, the sensitivity of their electrochemical response to surface orientation and the amount of precious metal required can limit their use. We present here a generally applicable procedure for producing thin metal films with a large proportion of atomically flat (111) terraces without the use of an epitaxial template. Thermal annealing in a controlled atmosphere induces long-range ordering of magnetron sputtered thin metal films deposited on an amorphous substrate. The ordering transition in these thin metal films yields characteristic (111) electrochemical signatures with minimal amount of material and provides an adequate replacement for oriented bulk single crystals. Our procedure can be generalized towards a novel class of practical multimetallic thin film based electrocatalysts with tunable near-surface compositional profile and morphology. Annealing of atomically corrugated sputtered thin film Pt-alloy catalysts yields an atomically smooth structure with highly crystalline, (111)-like ordered and Pt segregated surface that displays superior functional properties, bridging the gap between extended/bulk surfaces and nanoscale systems.
36 MATERIALS SCIENCE↗
Activity of N-coordinated multi-metal-atom active site structures for Pt-free oxygen reduction reaction catalysis: Role of *OH ligands
We report calculated oxygen reduction reaction energy pathways on multi-metal-atom structures that have previously been shown to be thermodynamically favorable. We predict that such sites have the ability to spontaneously cleave the O₂ bond and then will proceed to over-bind reaction intermediates. In particular, the *OH bound state has lower energy than the final 2 H₂O state at positive potentials. Contrary to traditional surface catalysts, this *OH binding does not poison the multi-metal-atom site but acts as a modifying ligand that will spontaneously form in aqueous environments leading to new active sites that have higher catalytic activities. These *OH bound structures have the highest calculated activity to date.
30 DIRECT ENERGY CONVERSION↗
X-ray absorption spectroscopy elucidates the impact of structural disorder on electron mobility in amorphous zinc-tin-oxide thin films
Abstract not provided
Siah, Sin Cheng↗
Structural Properties of Nanometer‐Sized Gold Nanoparticles on a Silicon Substrate
Properties of gold nanoparticles (Au NPs) supported on Si substrates, which have been the focus of recent attention, depend sensitively on the size, structure, and coordination of Au NPs as well as on the processes of interdiffusion and chemical bonding at the Au–Si interface. There is a great need, therefore, for developing structural techniques capable of imaging such nanosystems in atomic detail. Here, it is discussed how the atomic structure of nanometer‐sized Au NPs deposited on a silicon surface can be determined by using high‐energy X‐ray diffraction measurements in combination with an analysis based on atomic‐pair‐distribution functions and advanced reverse Monte Carlo methods. This approach delivers simple and incisive pictures of the structure of Au clusters on Si and reveals direct structural evidence for the emergence of a Au‐silicide interface following room temperature deposition of Au NPs on Si. This study will contribute to designing Au/Si nanostructures with desirable properties.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Electrically driven photon emission from individual atomic defects in monolayer WS 2
Quantum dot–like single-photon sources in transition metal dichalcogenides (TMDs) exhibit appealing quantum optical properties but lack a well-defined atomic structure and are subject to large spectral variability. Here, we demonstrate electrically stimulated photon emission from individual atomic defects in monolayer WS 2 and directly correlate the emission with the local atomic and electronic structure. Radiative transitions are locally excited by sequential inelastic electron tunneling from a metallic tip into selected discrete defect states in the WS 2 bandgap. Coupling to the optical far field is mediated by tip plasmons, which transduce the excess energy into a single photon. The applied tip-sample voltage determines the transition energy. Atomically resolved emission maps of individual point defects closely resemble electronic defect orbitals, the final states of the optical transitions. Inelastic charge carrier injection into localized defect states of two-dimensional materials provides a powerful platform for electrically driven, broadly tunable, atomic-scale single-photon sources.
74 ATOMIC AND MOLECULAR PHYSICS↗
Replication Data for: Atomic-Scale Surface Structure and CO Tolerance of NiCu Single-Atom Alloys
The data underlying this published work have been made publicly available in this repository as part of the IMASC Data Management Plan. This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0012573.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
The RNA synthesis machinery of negative-stranded RNA viruses
The group of Negative-Stranded RNA Viruses (NSVs) includes many human pathogens, like the influenza, measles, mumps, respiratory syncytial or Ebola viruses, which produce frequent epidemics of disease and occasional, high mortality outbreaks by transmission from animal reservoirs. The genome of NSVs consists of one to several single-stranded, negative-polarity RNA molecules that are always assembled into mega Dalton-sized complexes by association to many nucleoprotein monomers. These RNA-protein complexes or ribonucleoproteins function as templates for transcription and replication by action of the viral RNA polymerase and accessory proteins. Here we review our knowledge on these large RNA-synthesis machines, including the structure of their components, the interactions among them and their enzymatic activities, and we discuss models showing how they perform the virus transcription and replication programmes. - Highlights: • Overall organisation of NSV RNA synthesis machines. • Structure and function of the ribonucleoprotein components: Atomic structure of the RNA polymerase complex. • Commonalities and differences between segmented- and non-segmented NSVs. • Transcription versus replication programmes.
60 APPLIED LIFE SCIENCES↗
Bulk Stoichiometry-Controlled Surface Reconstruction of Nanosized Ni−In Intermetallic Catalysts Steers Methanol Selectivity in CO2 Hydrogenation
Intermetallic compounds (IMCs) are attractive platforms for elucidating structure−catalysis relationships due to their ordered atomic structure and well-defined bulk composition. Yet, how their surfaces reconstruct under reaction conditions and how such reconstruction is governed by bulk stoichiometry remain poorly understood. Here, we show that SiO2-supported Ni−In IMCs undergo reaction-driven surface reconstruction during CO2 hydrogenation and that bulk stoichiometry can be used to steer this evolution toward methanol formation. Among the compositions examined (Ni2In1, Ni1In1, Ni2In3, and Ni1In2), Ni2In3/SiO2 exhibits the highest methanol selectivity (∼70%) and a methanol space-time yield of 652 mg·gmetal−1·h−1 at 250 °C and 30 bar. Combined structural, surface characterization, and kinetic analyses suggest that the intermetallic bulk remains largely preserved, whereas the surface departs from the stoichiometric bulk and evolves toward InOx-enriched surface domains coupled to an electron-rich Ni−In intermetallic phase. The extent of this evolution depends strongly on the bulk Ni:In stoichiometry and is most pronounced for Ni2In3/SiO2. These findings identify bulk stoichiometry as a handle for tuning the working-state surface of intermetallic catalysts and provide a basis for designing methanol synthesis catalysts through controlled surface reconstruction.
Wang, Caiqi [ORNL] (ORCID:0000000198849990)↗
Defect graph neural networks for materials discovery in high-temperature clean-energy applications
We present a graph neural network approach that fully automates the prediction of defect formation enthalpies for any crystallographic site from the ideal crystal structure, without the need to create defected atomic structure models as input. Here we used density functional theory reference data for vacancy defects in oxides, to train a defect graph neural network (dGNN) model that replaces the density functional theory supercell relaxations otherwise required for each symmetrically unique crystal site. Interfaced with thermodynamic calculations of reduction entropies and associated free energies, the dGNN model is applied to the screening of oxides in the Materials Project database, connecting the zero-kelvin defect enthalpies to high-temperature process conditions relevant for solar thermochemical hydrogen production and other energy applications. The dGNN approach is applicable to arbitrary structures with an accuracy limited principally by the amount and diversity of the training data, and it is generalizable to other defect types and advanced graph convolution architectures. In conclusion, it will help to tackle future materials discovery problems in clean energy and beyond.
97 MATHEMATICS AND COMPUTING↗
Amorphous zinc–molybdenum–sulfide chalcogel as a long-cycle, high-capacity electrode for lithium-ion batteries
The inherent limitations of intercalation-based electrodes in lithium-ion batteries have prompted the search for alternative materials with higher specific capacities and robust electrochemical stability. Sulfur-based electrodes, despite their high theoretical capacities (1672 mAh g −1 ), typically suffer from poor cycling performance. In this work, zinc molybdenum polysulfide (Zn x Mo 3 S 13 , 0.5 ≤ x), an amorphous semiconductor chalcogel, exhibits high specific capacity and excellent cycling stability. Synchrotron X-ray pair distribution function and extended X-ray absorption fine structure analyses reveal a short-range atomic structure comprising Mo–Mo, M–S (M = Mo, Zn), and S–S bonding motifs. The coordination environment of Mo and S closely resembles that of Mo 3 S 13 clusters, interconnected via S–S bridges and Zn 2+ cations. The Li/Zn x Mo 3 S 13 cell delivers an initial discharge capacity of 844 mAh g −1 at C/3, and retains 386.2 mAh g −1 after 1000 cycles with an average coulombic efficiency of 99.99%. The distribution of relaxation times analysis confirms the formation of a stable solid electrolyte interphase, which underpins the cell's long-term stability. In conclusion, this outstanding performance is attributed to the synergistic effects of the chalcogel's unique amorphous framework, semiconductive character, Zn-mediated polysulfide anchoring, and structural resilience, positioning Zn x Mo 3 S 13 chalcogel among the most durable pure metal sulfide cathodes reported for next-generation LIBs.
36 MATERIALS SCIENCE↗
Simulated structure and thermodynamics of decagonal Al-Co-Cu quasicrystals
Atomic structures of Al-Co-Cu decagonal quasicrystals (dQCs) are investigated using empirical oscillating pair potentials (EOPP) in molecular dynamic (MD) simulations that we enhance by Monte Carlo (MC) swapping of chemical species and replica exchange. Predicted structures exhibit planar decagonal tiling patterns and are periodic along the perpendicular direction. We then recalculate the energies of promising structures using first-principles density functional theory (DFT), along with energies of competing phases. We find that our τ -inflated sequence of QC approximants (QCAs) are energetically unstable at low temperature by at least 3 meV/atom. Extending our study to finite temperatures by calculating harmonic vibrational entropy, as well as anharmonic contributions that include chemical species swaps and tile flips, our results suggest that the quasicrystal phase is entropically stabilized at temperatures in the range 600-800 K and above. It decomposes into ordinary (though complex) crystal phases at low temperatures, including a partially disordered B2-type phase. We discuss the influence of density and composition on QC phase stability; we compare the structural differences between Co-rich and Cu-rich quasicrystals; and we analyze the role of entropy in stabilizing the quasicrystal, concluding with a discussion of the possible existence of “high entropy” quasicrystals. Published by the American Physical Society 2024
Huang, Yang (ORCID:0009000045917347)↗
Cryogenic X-ray crystallographic studies of biomacromolecules at Turkish Light Source " Turkish DeLight "
X-ray crystallography is a robust and powerful structural biology technique that provides high-resolution atomic structures of biomacromolecules. Scientists use this technique to unravel mechanistic and structural details of biological macromolecules (e.g., proteins, nucleic acids, protein complexes, protein-nucleic acid complexes, or large biological compartments). Since its inception, single-crystal cryocrystallography has never been performed in Türkiye due to the lack of a single-crystal X-ray diffractometer. The X-ray diffraction facility recently established at the University of Health Sciences, Istanbul, Türkiye will enable Turkish and international researchers to easily perform high-resolution structural analysis of biomacromolecules from single crystals. Here, we describe the technical and practical outlook of a state-of-the-art home-source X-ray, using lysozyme as a model protein. The methods and practice described in this article can be applied to any biological sample for structural studies. Therefore, this article will be a valuable practical guide from sample preparation to data analysis.
59 BASIC BIOLOGICAL SCIENCES↗
Medium-range order and compositional correlation in metallic glasses
The compositional atomic ordering in metallic glasses was studied by simulation focusing on the medium-range order (MRO). Many metallic alloy liquids and glasses show MRO characterized by the oscillations in the atomic pair-distribution function (PDF) beyond the first peak, which decay exponentially with distance. To study the effects of the local chemical order on MRO, we examine the compositionally resolved PDF and its MRO for models of various binary metallic alloy glasses. We show that compositional ordering is limited mostly to the nearest-neighbor atoms and the MRO is largely independent of the compositional order. For some elements that strongly repel each other in the alloy, a second MRO periodicity is observed owing to the distinct correlations among them. These results are discussed in light of the idea that the MRO oscillations in the PDF describe the correlations in the atomic density fluctuations, rather than the detailed local atomic structure.
Atomic structure↗