Two-orbital degeneracy lifted local precursor to a metal-insulator transition in MgTi2O4
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99 GENERAL AND MISCELLANEOUS↗
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Results for “atomic ordering”
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Nitride-Oxide-Metal Heterostructure with Self-Assembled Core–Shell Nanopillar Arrays: Effect of Ordering on Magneto-Optical Properties
Magneto-optical (MO) coupling incorporates photon-induced change of magnetic polarization that can be adopted in ultrafast switching, optical isolators, mode convertors, and optical data storage components for advanced optical integrated circuits. However, integrating plasmonic, magnetic, and dielectric properties in one single material system poses challenges since one natural material can hardly possess all these functionalities. Here, co-deposition of a three-phase heterostructure composed of a durable conductive nitride matrix with embedded core–shell vertically aligned nanopillars, is demonstrated. Additionally, the unique coupling between ferromagnetic NiO core and atomically sharp plasmonic Au shell enables strong MO activity out-of-plane at room temperature. Further, a template growth process is applied, which significantly enhances the ordering of the nanopillar array. The ordered nanostructure offers two schemes of spin polarization which result in stronger antisymmetry of Kerr rotation. The presented complex hybrid metamaterial platform with strong magnetic and optical anisotropies is promising for tunable and modulated all-optical-based nanodevices.
36 MATERIALS SCIENCE↗
Enhanced detection limits for radiokrypton analysis
In this paper, we present a method for improving detection limits of Atom Trap Trace Analysis for the krypton radioisotopes 85 Kr and 81 Kr. For the case of 85 Kr this work demonstrates that systematic use of isotopically depleted gas for calibration and extended conditioning of the instrument results in a detection limit of 900 85 Kr atoms per 11 μl of Kr gas, equivalent to a 85 Kr/Kr isotopic abundance of 3 x 10 -15 . This improvement of roughly two orders of magnitude over previously reported limits will help to expand the reach of radiokrypton dating towards longer age ranges where most of the radioisotopes have decayed. Additionally, the method offers an opportunity to investigate radiokrypton production via spontaneous fission within naturally occurring minerals to understand potential underground production of these isotopes.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Nucleon momentum distributions for local chiral interactions [Slides]
We use quantum Monte Carlo methods to calculate single- and two-nucleon momentum distributions in 4 He, 12 C, and 16 O. We use correlated many-body wave functions optimized for local chiral interactions up to next-to-next-to-leading order (N 2 L0).
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
In situ atomic-resolution imaging of water vapor–driven multistep oxidation dynamics in strontium cobaltite
Understanding how water vapor interacts with transition metal oxides (TMOs) is critical for tailoring material properties to improve performance and enable new technologies. Despite extensive research efforts, atomic-scale mechanisms underpinning dynamic reactions and reaction-induced phase transitions remain elusive. Here, we use in situ environmental transmission electron microscopy to investigate how water vapor oxidizes vacancy-ordered SrCoO 2.5 at moderately elevated temperatures, demonstrating that water molecules can initiate oxidation more effectively than oxygen under comparable conditions. We discover a distinct “staging” behavior during the oxidation process: A fully ordered intermediate phase, SrCoO 2.75 , forms before transitioning into a near-perovskite SrCoO 3−δ . In addition, antiphase boundaries, originating at step terraces of SrTiO 3 , alleviate strain by creating reversible nanoscale “gaps” during lattice contraction under oxidation, providing a pathway for preserving structural integrity throughout redox cycling. This work provides atomic-level guidance for engineering TMOs by leveraging water vapor to control their redox behavior and tailor functional properties.
Science & Technology - Other Topics↗
The Origin of Anomalous Density Behavior of Silica Glass
The anomalous density–temperature relationship of vitreous silica with low hydroxyl content is explained by the formation of medium-range ordering structure in the glass transition process. The ordered medium-range structure has the shape of a “nanoflake” and consists of two layers of SiO 4 tetrahedra, bonded by O atoms located in the middle of the structure. The nanoflakes interact with their surrounding structures through both covalent chemical bonds and van der Waals bonds. In the formation of the van der Waals bonds, the orientation of SiO 4 tetrahedra can change, which results in an increase in distance between the nanoflakes and their surrounding structures. Thus, there is a slight volume enlargement associated with the formation of nanoflakes. Since the nanoflakes’ formation starts at a temperature near 1480 °C, and the population of the nanoflakes grows continuously as temperature decreases until about 950 °C, the bulk volume of silica glass increases in the temperature range from about 1480 °C to 950 °C. Therefore, the density anomaly of silica glass can be explained as a byproduct of forming of medium-range ordering structure in the silica glass transition.
36 MATERIALS SCIENCE↗
Atomic-Scale Imaging of Condensed Counterions
Here, the functioning of a wide variety of charged macromolecules, from DNA to fuel cell membranes, is dependent on how the counterions surrounding them are arranged. In order to decrease Coulombic repulsion, some of the fixed charges on these molecules are neutralized by a fraction of the counterions-this phenomenon is called counterion condensation. The nature of counterion condensation can be only be inferred indirectly from traditional experiments such as X-ray scattering and modern experiments such as single molecule electrometry. The prevalent conclusion in the literature, based on both theory and experiment, is that the distribution of counterions is peaked right next to the macromolecule, i.e., condensation results in the formation of contact ion pairs. In this study, cryogenic electron microscopy (cryo-EM) was used to study the arrangement of condensed halide counterions near a positively charged polypeptoid nanofiber. The locations of both condensed and fixed charges were determined directly from atomic-scale images. Our experimentally determined counterion distributions were peaked at distances of about 5 Å away from the fixed positive charge, indicating the presence of a layer of water molecules between condensed ion pairs. We posit that this distribution is driven by the entropy of the condensed ions.
36 MATERIALS SCIENCE↗
Indium segregation in Gd 5 (Si, Ge) 4 magnetocaloric materials
Chemical substitution is one of the most efficient tools to tune and optimize magnetic and magnetocaloric properties of the giant magnetocaloric materials. In particular, Indium substitutions could be useful both for tuning properties of these interesting intermetallic materials and to unveil their local-scale behavior across the magnetostructural transition via hyperfine techniques. Hence, in order to investigate the effect of Indium additions on the crystal structure, micro-structure, magnetic and magnetocaloric properties, a series of In-containing samples derived from the base Gd 5 Si 1.2 Ge 2.8 stoichiometry were prepared. Here, the major findings are that while In is insoluble in the 5:4 phase, it will instead promote the emergence of the impurity 5:3 phase and segregates into this phase. Hence, In leads to major crystallographic changes, which enhance atomic disorder and disrupt the Si to Ge ratio in the 5:4 phase. Subsequently, a higher 5:4 unit cell volume and a lower magnetic ordering temperature are found in the In-substituted samples. Finally, the magnetocaloric properties of the In-substituted samples reveal a detrimental effect on the maximum magnetic entropy change.
36 MATERIALS SCIENCE↗
Property changes induced by the space environment in composite materials on LDEF: Solar array materials passive LDEF experiment A0171 (SAMPLE)
Surface modifications to composite materials induced by long term exposure in low earth orbit (LEO) were dominated by atomic oxygen erosion and micrometeoroid and space debris impacts. As expected, calculated erosion rates were peculiar to material type and within the predicted order of magnitude. Generally, about one ply of the carbon fiber composites was eroded during the 70 month LDEF experiment. Matrix erosion was greater than fiber erosion and was more evident for a polysulfone matrix than for epoxy matrices. Micrometeoroid and space debris impacts resulted in small (less than 1mm) craters and splattered contaminants on all samples. Surfaces became more diffuse and darker with small increases in emissivity and absorption. Tensile strength decreased roughly with thickness loss, and epoxy matrices apparently became slightly embrittled, probably as a result of continued curing under UV and/or electron bombardment. However, changes in the ultimate yield stress of the carbon reinforced epoxy composites correlate neither with weave direction nor fiber type. Unexpected developments were the discovery of new synergistic effects of the space environment in the interaction of atomic oxygen and copious amounts of contamination and in the induced luminescence of many materials.
Source record↗
Low-Light-Shift Cesium Fountain without Mechanical Shutters
A new technique for reducing errors in a laser-cooled cesium fountain frequency standard provides for strong suppression of the light shift without need for mechanical shutters. Because mechanical shutters are typically susceptible to failure after operating times of the order of months, the elimination of mechanical shutters could contribute significantly to the reliability of frequency standards that are required to function continuously for longer time intervals. With respect to the operation of an atomic-fountain frequency standard, the term "light shift" denotes an undesired relative shift in the two energy levels of the atoms (in this case, cesium atoms) in the atomic fountain during interrogation by microwaves. The shift in energy levels translates to a frequency shift that reduces the precision and possibly accuracy of the frequency standard. For reasons too complex to describe within the space available for this article, the light shift is caused by any laser light that reaches the atoms during the microwave- interrogation period, but is strongest for near-resonance light. In the absence of any mitigating design feature, the light shift, expressed as a fraction of the standard fs frequency, could be as large as approx. 2 x 10(exp -11), the largest error in the standard. In a typical prior design, to suppress light shift, the intensity of laser light is reduced during the interrogation period by using a single-pass acoustooptic modulator to deflect the majority of light away from the main optical path. Mechanical shutters are used to block the remaining undeflected light to ensure complete attenuation. Without shutters, this remaining undeflected light could cause a light shift of as much as .10.15, which is unacceptably large in some applications. The new technique implemented here involves additionally shifting the laser wavelength off resonance by a relatively large amount (typically of the order of nanometers) during microwave interrogation. In this design, when microwave interrogation is not underway, the atoms are illuminated by a slave laser locked to the lasing frequency of a lower power master laser.
Enzer, Daphna↗
Noncollinear magnetic configurations and substrate-mediated interactions in Mn trimers on the GaN (000$\bar{1}$) surface
Collinear and noncollinear calculations based on density functional theory are carried out to elucidate the magnetic ordering of Mn trimers on a GaN ($000\bar{1}$) substrate. These trimers had previously been observed in $3a \times 3a$ surface reconstructions through Mn deposition onto the N-polar face of wurtzite GaN($000\bar{1}$). In this work, we start off by studying the effect of spin orbit coupling for the case of monomers and dimers of Mn atoms on top of a GaN surface. Based on an effective spin Hamiltonian, we estimate the magnetic anisotropy energy (MAE) for those cases and found that it is four orders of magnitude weaker than the exchange magnetic coupling between Mn adatoms. In the Mn trimer case, the magnetic ground state has the Mn spins in-plane with the GaN surface in which the relative spin orientation within each trimer is noncollinear due to the competition between the two antiferromagnetic interactions that affect each Mn spin in the trimer, which leads to the found energy minimum with 120 degree angles between the spins. By exploring the nature and fundamental mechanisms for the magnetic interaction among the Mn trimers, we find that the surface states of the substrate play a key role, involving a Ruderman-Kittel-Kasuya-Yosida (RKKY)-type interaction. We report on an electron-mediated long-distance exchange coupling between localized magnetic moments on a GaN($000\bar{1}$) surface.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
A Machine Learning Framework for Modeling Ensemble Properties of Atomically Disordered Materials
Atomic disorder can strongly influence material properties such as charge transport, optical response, and catalytic activity. However, efficiently modeling these disorder effects remains challenging for first-principles methods due to the cost of sampling large configurational spaces and computing complex physical quantities. Recent advances of machine learning techniques, particularly graph neural networks (GNNs), has enabled the efficient and accurate predictions of complex material properties, offering promising tools for studying disordered systems. In this work, we present a general machine-learning-assisted computational framework that integrates equivariant GNNs with Monte Carlo simulations to compute the thermodynamic and ensemble-averaged functional properties of disordered materials. Using the surface-termination-disordered MXene monolayer Ti 3 C 2 T 2–x as a representative system, we find that electrical conductivity exhibits an emergent peak near the order–disorder phase transition temperature due to the interplay between electron scattering and doping. In contrast, optical conductivity remains largely insensitive to local atomic disorder and reflects the global surface chemical composition. These results highlight the role of atomic disorder in affecting material properties and demonstrate the potential of our approach for statistically modeling disorder effects in a wide range of materials such as high-entropy alloys and spin liquids.
MXene↗
Dynamic Structural Change of Plant Epidermal Cell Walls under Strain
Abstract The molecular foundations of epidermal cell wall mechanics are critical for understanding structure–function relationships of primary cell walls in plants and facilitating the design of bioinspired materials. To uncover the molecular mechanisms regulating the high extensibility and strength of the cell wall, the onion epidermal wall is stretched uniaxially to various strains and cell wall structures from mesoscale to atomic scale are characterized. Upon longitudinal stretching to high strain, epidermal walls contract in the transverse direction, resulting in a reduced area. Atomic force microscopy shows that cellulose microfibrils exhibit orientation‐dependent rearrangements at high strains: longitudinal microfibrils are straightened out and become highly ordered, while transverse microfibrils curve and kink. Small‐angle X‐ray scattering detects a 7.4 nm spacing aligned along the stretch direction at high strain, which is attributed to distances between individual cellulose microfibrils. Furthermore, wide‐angle X‐ray scattering reveals a widening of (004) lattice spacing and contraction of (200) lattice spacing in longitudinally aligned cellulose microfibrils at high strain, which implies longitudinal stretching of the cellulose crystal. These findings provide molecular insights into the ability of the wall to bear additional load after yielding: the aggregation of longitudinal microfibrils impedes sliding and enables further stretching of the cellulose to bear increased loads.
59 BASIC BIOLOGICAL SCIENCES↗
Ordering-mediated local nano-clustering results in unusually large Hall-Petch strengthening coefficients in high entropy alloys
This paper reports a dramatic increase in the grain boundary strengthening or Hall-Petch coefficient, K, by systematically investigating the effect of Al addition on tensile yield strength in CoFeNi and CoCrFeNi high entropy alloys (HEAs) or complex concentrated alloys (CCAs). Additionally, detailed atom probe tomography (APT) revealed a high number density of Ni-Al rich nano-clusters in the Al 0.3 CoFeNi and Al 0.3 CoCrFeNi HEAs/CCAs, which can be rationalized based on the strong chemical ordering tendency between these elements. Consequently, the huge increase in K value can be attributed to the additional stress required for overcoming coherency strain fields arising from these nano-clusters.
36 MATERIALS SCIENCE↗
Gravitational redshift space-probe experiment
A Scout D rocket was launched from Wallops Island, Virginia, carrying an atomic hydrogen maser oscillator system as the payload. The frequency of signals from the oscillator was monitored on the ground at Merritt Island, Florida, by using two hydrogen masers as comparison oscillators. The first-order Doppler shift in the signals was eliminated by a go-return transponder link to the payload, and the resulting data, representing the relativistic shifts, were recovered and recorded. The objective was to measure directly the effect of gravitational potential on the frequency of an atomic hydrogen maser assuming it to be a 'proper' clock. A gravitational effect amounting to some 4.5 parts in 10 to the 10th power was measured with an oscillator having a stability better than 1 part in 10 to the 14th power. Therefore, to make the best possible use of the oscillator, all frequency shifts at the 2 to 5 X 10 to the -15 power level in delta f/f in the system must be accounted for. This includes all the phase variations that can cause such a shift to appear. The experiment, the data available and the manner in which they were processed, and the results are described.
Vessot, R. F. C.↗
Spectral quadrature for the first principles study of crystal defects: Application to magnesium
In this work, we present an accurate and efficient finite-difference formulation and parallel implementation of Kohn-Sham Density (Operator) Functional Theory (DFT) for non periodic systems embedded in a bulk environment. Specifically, employing non-local pseudopotentials, local reformulation of electrostatics, and truncation of the spatial Kohn-Sham Hamiltonian, and the Linear Scaling Spectral Quadrature method to solve for the pointwise electronic fields in real-space and the non-local component of the atomic force, we develop a parallel finite difference framework suitable for distributed memory computing architectures to simulate non-periodic systems embedded in a bulk environment. Choosing examples from magnesium-aluminum alloys, we first demonstrate the convergence of energies and forces with respect to spectral quadrature polynomial order, and the width of the spatially truncated Hamiltonian. Next, we demonstrate the parallel scaling of our framework, and show that the computation time and memory scale linearly with respect to the number of atoms. Next, we use the developed framework to simulate isolated point defects and their interactions in magnesium-aluminum alloys. Our findings conclude that the binding energies of divacancies, Al solute-vacancy and two Al solute atoms are anisotropic and are dependent on cell size. Furthermore, the binding is favorable in all three cases.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Atomic Three-Dimensional Investigations of Pd Nanocatalysts for Acetylene Semi-hydrogenation
Deciphering the three-dimensional (3D) insight into nanocatalyst surfaces at the atomic level is crucial to understanding catalytic reaction mechanisms and developing high-performance catalysts. Nevertheless, better understanding the inherent insufficiency of a long-range ordered lattice in nanocatalysts is a big challenge. Here, in this work, we report the local structure of Pd nanocatalysts, which is beneficial for demonstrating the shape-structure-adsorption relationship in acetylene hydrogenation. The 5.27 nm spherical Pd catalyst (Pd sph ) shows an ethylene selectivity of 88% at complete acetylene conversion, which is much higher than those of the Pd octahedron and Pd cube and superior to other reported monometallic Pd nanocatalysts so far. By virtue of the local structure revelation combined with the atomic pair distribution function (PDF) and reverse Monte Carlo (RMC) simulation, the atomic surface distribution of the unique compressed strain of Pd-Pd pairs in Pd sph was revealed. Density functional theory calculations verified the obvious weakening of the ethylene adsorption energy on account of the surface strain of Pd sph . It is the main factor to avoid the over-hydrogenation of acetylene. The present work, entailing shape-induced surface strain manipulation and atomic 3D insight, opens a new path to understand and optimize chemical activity and selectivity in the heterogeneous catalysis process.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Quantum dynamics of cold atomic gas with SU(1,1) symmetry
Motivated by recent advances in quantum dynamics, we investigate the dynamics of the system with SU(1,1) symmetry. Instead of performing the time-ordered integral for the evolution operator of the time-dependent Hamiltonian, we show that the time evolution operator can be expressed as an SU(1,1) group element. Since the SU(1,1) group describes the “rotation” on a hyperbolic surface, the dynamics can be visualized on a Poincaré disk, a stereographic projection of the upper hyperboloid. As an example, we present the trajectory of the revival of Bose-Einstein condensation and that of the scale-invariant Fermi gas on the Poincaré disk. Further considering quantum gases in an oscillating lattice, we also study the dynamics of the system with time-dependent single-particle dispersion.
74 ATOMIC AND MOLECULAR PHYSICS↗