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At least 919 records · Page 51

Understanding the evolution of liquid and solid microjets from grooved Sn and Cu samples using radiography

Experiments were performed on grooved Sn and Cu samples to study the temporal evolution of microjets. Jets were generated by the impact of gun-launched flyer plates against the back of grooved targets made from either Cu or Sn (groove depth of ~250 μm). The Hugoniot states in the various Sn targets encompassed conditions where solid phases are maintained throughout (7 and 16 GPa) and also conditions where melting occurs upon the release of compression (25 and 34 GPa); the transition occurs near a Hugoniot pressure of 23 GPa. Cu targets at 27 and 56 GPa provide comparisons in which the jets move at similar speeds but remain solid. In all cases, the spatial distribution of mass within the microjets was measured using high-speed synchrotron radiography. The result is a time history of the jet thickness profile from which quantities like total jet mass and jet velocity can be derived. In both the solid and liquid states, we generally observe that an increase in the shock strength leads to an increase in jet mass. However, this trend breaks down for Hugoniot states near the transition from continuously solid to melted-on-release. This is evidenced by the observation that there was no difference in the rate of mass flow in Sn jets at 16 and 25 GPa, while similar pressure jumps on either side of this range caused substantial changes in the jet mass. This contrasts with the behavior of smaller polishing defects that were present on the same samples (~1 μm deep). From these, no ejecta mass was detected below the melt boundary, but obvious microjets were generated once melting occurred. This indicates that crossing the bulk melt-on-release threshold can alternately promote or inhibit the flow of mass into microjets based on the amplitude of the initial perturbation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Exploration of two surfaces observed in Weyl semimetal BaMnSb 2

Single crystalline BaMnSb 2 is considered as a 3D Weyl semimetal with the 2D electronic structure containing Dirac cones from the Sb sheet. We report experimental investigation of low-temperature cleaved BaMnSb 2 surfaces using scanning tunneling microscopy/spectroscopy and low energy electron diffraction. By natural cleavage, we find two terminations: one is Ba (above the orthorhombically distorted Sb sheet) and another Sb2 (at the surface of the Sb/Mn/Sb sandwich layer). Both terminations show the 2×1 surface reconstructions, with drastically different morphologies and electronic properties, however. The reconstructed structures, defect types and nature of the electronic structures of the two terminations are extensively studied. The quasiparticle interference (QPI) analysis is conducted at the energy range between -2 V and 2 V, although no interesting states are observed near the Fermi level, the surface-projected electronic band structures strongly depend on the surface termination above 1.6 V. The existence of defects can greatly modify the local density of states to create electronic phase separations on the surface in the order of tens of nm scale. Our observation on the atomic structures of the terminations and the corresponding electronic structures provides critical information towards an understanding of topological properties of BaMnSb 2 .

36 MATERIALS SCIENCE↗

Colloquium : Sliding and pinning in structurally lubric 2D material interfaces

A plethora of two-dimensional (2D) materials have been introduced in physics and engineering in the past two decades. Their robust, membranelike sheets permit (mostly require) deposition, giving rise to solid-solid dry interfaces whose mobility, pinning, and general tribological properties under shear stress are currently being understood and controlled, both experimentally and theoretically. Here, in this Colloquium simulated case studies of twisted graphene systems are used as a prototype workhorse tool to demonstrate and discuss the general picture of 2D material interface sliding. First highlighted is the crucial mechanical difference, often overlooked, between small and large incommensurabilities, which corresponds to, for example, small and large twist angles in graphene interfaces. In both cases, focusing on flat, structurally lubric or “superlubric” geometries, the generally separate scalings with the area of static friction in pinned states and of kinetic friction during sliding are elucidated and reviewed, tangled as they are with the effects of velocity, temperature, load, and defects. The roles of island boundaries and elasticity are also discussed, and compared when possible to results in the literature for systems other than graphene. It is proposed that the resulting picture of pinning and sliding should be applicable to interfaces in generic 2D materials that are of importance for the physics and technology of existing and future bilayer and multilayer systems.

2-dimensional systems↗

Point-Defect-Localized Bound States in the Continuum in Photonic Crystals and Structured Fibers

In this work, we show that point defects in two-dimensional photonic crystals can support bound states in the continuum (BICs). The mechanism of confinement is a symmetry mismatch between the defect mode and the Bloch modes of the photonic crystal. These BICs occur in the absence of band gaps and therefore provide an alternative mechanism to confine light. Furthermore, we show that such BICs can propagate in a fiber geometry and exhibit arbitrarily small group velocity which could serve as a platform for enhancing nonlinear effects and light-matter interactions in structured fibers.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Heterogeneous Ice Growth in Micron-Sized Water Droplets Due to Spontaneous Freezing

Understanding how ice nucleates and grows into larger crystals is of crucial importance for many research fields. The purpose of this study was to shed light on the phase and structure of ice once a nucleus is formed inside a metastable water droplet. Wide-angle X-ray scattering (WAXS) was performed on micron-sized droplets evaporatively cooled to temperatures where homogeneous nucleation occurs. We found that for our weak hits ice grows more cubic compared to the strong hits that are completely hexagonal. Due to efficient heat removal caused by evaporation, we propose that the cubicity of ice at the vicinity of the droplet’s surface is higher than for ice formed within the bulk of the droplet. Moreover, the Bragg peaks were classified based on their geometrical shapes and positions in reciprocal space, which showed that ice grows heterogeneously with a significant population of peaks indicative of truncation rods and crystal defects. Frequent occurrences of the (100) reflection with extended in-planar structure suggested that large planar ice crystals form at the droplet surface, then fracture into smaller domains to accommodate to the curvature of the droplets. Planar faulting due to misaligned domains would explain the increased cubicity close to the droplet surface.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Anomalous transport in high-mobility superconducting SrTiO 3 thin films

The study of subtle effects on transport in semiconductors requires high-quality epitaxial structures with low defect density. Using hybrid molecular beam epitaxy (MBE), SrTiO 3 films with a low-temperature mobility exceeding 42,000 cm 2 V -1 s -1 at a low carrier density of 3 × 10 17 cm -3 were achieved. A sudden and sharp decrease in residual resistivity accompanied by an enhancement in the superconducting transition temperature were observed across the second Lifshitz transition where the third band becomes occupied, revealing dominant intraband scattering. These films further revealed an anomalous behavior in the Hall carrier density as a consequence of the antiferrodistortive (AFD) transition and the temperature dependence of the Hall scattering factor. Using hybrid MBE growth, phenomenological modeling, temperature-dependent transport measurements, and scanning superconducting quantum interference device imaging, we provide critical insights into the important role of inter- versus intraband scattering and of AFD domain walls on normal-state and superconducting properties of SrTiO 3 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Resonant interactions involving local vibrational modes in crystals

When an impurity with a light mass is inserted into a crystal, it can undergo a high-frequency oscillation referred to as a local vibrational mode (LVM). A Fermi resonance may occur between the LVM and lower-frequency modes of the defect. The LVM may also interact with phonons or the electromagnetic field. Understanding these interactions can help model and control diffusion, defect reactions, and thermal conductivity. LVMs have been probed in semiconductors using pressure and alloying as experimental parameters, resulting in anticrossing between localized and extended vibrational modes. Furthermore, these types of vibrational interactions could play an important role in the stability and thermal properties of organic–inorganic hybrid semiconductors. The coupling between an LVM and electromagnetic wave yields an “LVM polariton,” an excitation that has significant vibrational and electric-field amplitudes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Materials genome innovation for computational software (magics) center

Functional layered material (LM) architectures will dominate nanomaterials science in this century. We have developed theory, modeling, simulation, and software and data tools that enhance understanding and AI guide synthesis, enable characterization of complex structures, and improve capabilities in the predictive design and growth of LMs. Research at the Center has focused on: Computational synthesis and characterization: AI guided synthesis and experimental synthesis of stacked LMs with tailored properties via optimized chemical vapor deposition (CVD) growth and liquid-phase exfoliation; study defects, edges, grain boundaries, wrinkling of atomic layers and their effects on chemical, mechanical, electrical, and optical properties. Far-from-equilibrium processes: Joint experimental and simulation based probe of electronic processes with NAQMD and ultrafast X-ray free-electron laser (XFEL) and ultrafast electron diffraction (UED) facilities at Stanford. Experimentally validate NAQMD by ultrafast electron diffraction and X-ray spectroscopy studies of structural and excited state dynamics, shape fluctuations, and phonon dynamics. Scalable software: Simulation engines for desktop-to-exascale platforms using low-overhead, linear-scaling QMD algorithms; divide-conquer-recombine NAQMD with electronic excitations; extended-Lagrangian reactive molecular dynamics (RMD), machine learning (ML) based neural-network quantum molecular dynamics (NNQMD), and super-state accelerated molecular dynamics (AMD) and kinetic Monte Carlo codes; thermal and electrical transport software; and design 3D architectures of LMs with desired functionality using scalable software. Distribution of software and data, and training: Software and simulation-experimental data generated within the Center are distributed to the materials science community via Berkeley Materials Project (MP) framework. We have also organized three workshops for software distribution and training at USC (Nov. 2017, Mar. 2018) and Gaithersburg, MD (Nov. 2018) to train researchers, with the last one in focused on underrepresented groups, in collaboration with Howard University which is one of the largest HBCUs. The Center supported a total of 46 personnel and 6 undergraduate students. These include 14 faculty, 11 postdoctoral research associates, 20 graduate research assistants, and mentored 6 undergraduate students. This resulted in the publications of 63 research papers that include 46 publications on Reactive and Quantum Dynamics Simulations, 13 publications on Machine Learning for Quantum Materials, and 4 publications on Quantum Computing.

2D Materials↗

Cross-Cap Defects and Fault-Tolerant Logical Gates in the Surface Code and the Honeycomb Floquet Code

We consider the Z 2 toric code, surface code, and Floquet code defined on a nonorientable surface, which can be considered as families of codes extending Shor’s nine-qubit code. We investigate the fault-tolerant logical gates of the Z 2 toric code in this setup, which corresponds to e ↔ m exchanging symmetry of the underlying Z 2 gauge theory. We find that nonorientable geometry provides a new way for the emergent symmetry to act on the code space, and discover the new realization of the fault-tolerant Hadamard gate of the two-dimensional surface code with a single cross cap connecting the vertices nonlocally along a slit, dubbed a nonorientable surface code. This Hadamard gate can be realized by a constant-depth local unitary circuit modulo nonlocality caused by a cross cap. Via folding, the nonorientable surface code can be turned into a bilayer local quantum code, where the folded cross cap is equivalent to a bilayer twist terminated on a gapped boundary and the logical Hadamard only contains local gates with intralayer couplings when being away from the cross cap, as opposed to the interlayer couplings on each site needed in the case of the folded surface code. We further obtain the complete logical Clifford gate set for a stack of nonorientable surface codes and similarly for codes defined on Klein-bottle geometries. We then construct the honeycomb Floquet code in the presence of a single cross cap, and find that the period of the sequential Pauli measurements acts as a H Z logical gate on the single logical qubit, where the cross cap enriches the dynamics compared with the orientable case. We find that the dynamics of the honeycomb Floquet code is precisely described by a condensation operator of the Z 2 gauge theory, and illustrate the exotic dynamics of our code in terms of a condensation operator supported at a nonorientable surface. Published by the American Physical Society 2024

Physics↗

Visualizing symmetry-breaking electronic orders in epitaxial Kagome magnet FeSn films

Abstract Kagome lattice hosts a plethora of quantum states arising from the interplay of topology, spin-orbit coupling, and electron correlations. Here, we report symmetry-breaking electronic orders tunable by an applied magnetic field in a model Kagome magnet FeSn consisting of alternating stacks of two-dimensional Fe 3 Sn Kagome and Sn 2 honeycomb layers. On the Fe 3 Sn layer terminated FeSn thin films epitaxially grown on SrTiO 3 (111) substrates, we observe trimerization of the Kagome lattice using scanning tunneling microscopy/spectroscopy, breaking its six-fold rotational symmetry while preserving the translational symmetry. Such a trimerized Kagome lattice shows an energy-dependent contrast reversal in dI/dV maps, which is significantly enhanced by bound states induced by Sn vacancy defects. This trimerized Kagome lattice also exhibits stripe modulations that are energy-dependent and tunable by an applied in-plane magnetic field, indicating symmetry-breaking nematicity from the entangled magnetic and charge degrees of freedom in antiferromagnet FeSn.

36 MATERIALS SCIENCE↗

Quantum paramagnetism in a non-Kramers rare-earth oxide: Monoclinic Pr 2 Ti 2 O 7

Little is so far known about the magnetism of the A 2 B 2 O 7 monoclinic layered perovskites that replace the spin-ice supporting pyrochlore structure for r A /r B > 1.78. We show that high quality monoclinic Pr 2 Ti 2 O 7 single crystals with a three-dimensional network of non-Kramers Pr 3+ ions that interact through edge-sharing superexchange interactions, form a singlet ground-state quantum paramagnet that does not undergo any magnetic phase transitions down to, at least, 1.8 K. The chemical phase stability, structure, and magnetic properties of the layered perovskite Pr 2 Ti 2 O 7 were investigated using x-ray diffraction, transmission electron microscopy, and magnetization measurements. Synthesis of polycrystalline samples with the nominal compositions of Pr 2 Ti 2+x O 7 (–0.16 ≤ x ≤ 0.16 ) showed that deviations from the Pr 2 Ti 2 O 7 stoichiometry lead to secondary phases of related structures including the perovskite phase Pr 2/3 TiO 3 and the orthorhombic phases Pr 4 Ti 9 O 24 and Pr 2 TiO 5 . No indications of site disordering (stuffing and antistuffing) or vacancy defects were observed in the Pr 2 Ti 2 O 7 majority phase. A procedure for growth of high-structural-quality stoichiometric single crystals of Pr 2 Ti 2 O 7 by the traveling solvent floating zone method is reported. Thermomagnetic measurements of single-crystalline Pr 2 Ti 2 O 7 reveal an isolated singlet ground state that we associate with the low-symmetry crystal electric-field environments that split the (2J + 1 = 9)-fold degenerate spin-orbital multiplets of the four differently coordinated Pr 3+ ions into 36 isolated singlets resulting in an anisotropic temperature-independent van Vleck susceptibility at low T. Here, a small isotropic Curie term is associated with 0.96(2)% noninteracting Pr 4+ impurities.

36 MATERIALS SCIENCE↗

Atomic-Scale Structural Mapping of Active Sites in Monolayer PGM-Free Catalysts by Low-Voltage 4D-STEM

Two-dimensional (2D) materials have attracted a large amount of attention in both basic and applied fields, and scanning transmission electron microscopy (STEM) is often uniquely well-suited for characterizing the atomic-scale structure of these materials [1-4]. As a result, STEM is poised to significantly impact progress on platinum group metal (PGM)-free catalysts, which are currently under intense development to enable low-cost, commercially viable hydrogen fuel cells [5]. While recent advancements have resulted in fuel cell performance comparable to Pt catalysts by some measures [6], cell durability remains a significant challenge, limiting practical applications [7]. Catalytically active sites in PGM-free materials are proposed to be FeN4 complexes embedded in a graphene lattice (Fig. 1b) within layered or other larger materials, but this is still under debate largely due to the range of potential actives sites predicted by computational methods and lack of methods for directly validating these models [5]. Fundamental insights into the atomic structure and resulting degradation pathways of proposed active sites are therefore needed to fully understand and control cell performance and durability [6].2D materials typically make ideal samples for STEM, but those within PGM-free catalysts present additional challenges since these materials are often defect-rich, with a high density of edges, dopant atoms, etc., which significantly increase susceptibility to beam damage at standard operating voltages. This makes analysis of potential FeN4 active sites particularly challenging, since a large proportion of Fe exists at edge sites where beam-induced atomic displacements can prohibit high-resolution structural characterization [6]. Conventional dark-field imaging compounds this problem by producing less signal for a given dose and being less sensitive to light elements than dose-efficient phase contrast imaging techniques such as those enabled by four-dimensional (4D)-STEM [8-10] (Fig. 1a). Consequently, active site structural analysis is often left to methods such as low-resolution imaging combined with quantum chemical calculations [6], which hinders accurate determination of reaction and degradation mechanisms.Here, we demonstrate direct atomic-scale structural mapping of FeN4 sites by performing low-voltage 4D-STEM on a model PGM-free catalyst system with many exposed monolayer regions. To accomplish this, we pair a 30 keV aberration-corrected probe with a fast pixelated detector that has optimal performance at low beam voltages [11]. This enables us to simultaneously image light and heavy elements with high signal-to-noise by center-of-mass analysis (Fig. 1c) while minimizing beam-induced atomic displacements at sensitive sites. The monolayer nature of these materials additionally allows for experimental validation by direct comparison with multislice simulations [12] of model structures (Fig. 1d-e). This work demonstrates how low-voltage 4D-STEM will provide new insights into the atomic-scale structure and degradation mechanisms of active sites in PGM-free catalysts, facilitating the development of low-cost hydrogen fuel cells and other energy conversion technologies in the future [13].

Zachman, Michael↗

Negative differential resistance observed on the charge density wave of a transition metal dichalcogenide

Charge density waves and negative differential resistance are seemingly unconnected physical phenomena. The former is an ordered quantum fluid of electrons, intensely investigated for its relation with superconductivity, while the latter receives much attention for its potential applications in electronics. Here we show that these two phenomena can not only coexist but also that the localized electronic states of the charge density wave are essential to induce negative differential resistance in a transition metal dichalcogenide, 1T-TaS 2 . Using scanning tunneling microscopy and spectroscopy, we report the observation of negative differential resistance in the commensurate charge density wave state of 1T-TaS 2 . The observed phenomenon is explained by the interplay of interlayer and intra-layer tunneling with the participation of the atomically localized states of the charge density wave maxima and minima. Here, we demonstrate that lattice defects can locally affect the coupling between the layers and are therefore a mechanism to realize NDR in these materials.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

2D Oxides Realized via Confinement Heteroepitaxy

Novel confinement techniques facilitate the formation of non-layered 2D materials. Here it is demonstrated that the formation and properties of 2D oxides (GaO x , InO x , SnO x ) at the epitaxial graphene (EG)/silicon carbide (SiC) interface is dependent on the EG buffer layer properties prior to element intercalation. Using 2D Ga, it is demonstrated that defects in the EG buffer layer lead to Ga transforming to GaO x with non-periodic oxygen in a crystalline Ga matrix via air oxidation at room temperature. However, crystalline monolayer GaO 2 and bilayer Ga 2 O 3 with ferroelectric wurtzite structure(FE-WZ') can then be formed via subsequent high-temperature O 2 annealing. Furthermore, the graphene/X/SiC (X = 2D Ga or Ga 2 O 3 ) junction is tunable from Ohmic to a Schottky or tunnel barrier depending on the interface species. Finally, using vertical transport measurements and electron energy loss spectroscopy analysis, the bandgap of 2D gallium oxide is identified as 6.6 ± 0.6 eV, significantly larger than that of bulk β-Ga 2 O 3 (≈4.8 eV), suggesting strong quantum confinement effects at the 2D limit. Furthermore, the study presented here is foundational for development of atomic-scale, vertical 2D/3D heterostructure for applications requiring short transit times, such as GHz and THz devices.

2D gallium oxides↗

Aging Mechanisms of Broad Area High-Power ~800nm Laser Diodes

Improved lifetime of high-power broad area laser diodes will enhance their utility for manufacturing, scientific, and medical laser systems. However, factors contributing to gradual degradation of diode laser performance are not fully understood. Here we study the aging mechanisms of ~800 nm aluminum-free laser diodes grown by solid-source MBE. Oxygen was intentionally introduced at three different concentration levels into the quantum well (QW) and waveguide (WG) at concentrations <5×10 15 cm -3 . Diode power, slope efficiency (SE th ), threshold current (I th ), and device parameters such as QW and WG lifetimes were measured at discrete time steps throughout the aging run. The data show that lasing characteristics prior to aging are degraded by oxygen introduction, but the gradual power degradation rate of ~5% over 500 hours at current density 1.74 kA/cm 2 does not change with oxygen concentration. Aging-induced changes in nonradiative lifetimes and threshold were observed for shorter aging times, but stabilized after ~100 hrs. and cannot explain the observed power degradation. This suggests that gradual degradation in these devices is not due to nonradiative recombination at low levels of point defects. The data shows that this degradation results primarily from changes in slope efficiency, and simulation of these results suggests that the power degradation arises from increased intracavity absorption (ICA). Efforts to slow ICA growth, instead of efforts to control low levels of nonradiative recombination centers, may be the most fruitful path forward to improve laser diode lifetime.

42 ENGINEERING↗

High-resolution radiation detection using Ni/SiO 2 /n-4H-SiC vertical metal-oxide-semiconductor capacitor

In this article, we demonstrate the radiation detection performance of vertical metal-oxide-semiconductor (MOS) capacitors fabricated on 20 μm thick n-4H-SiC epitaxial layers with the highest energy resolution ever reported. The 100 nm SiO2 layer was achieved on the Si face of n-4H-SiC epilayers using dry oxidation in air. The Ni/SiO2/n-4H-SiC MOS detectors not only demonstrated an excellent energy resolution of 0.42% (ΔE/E 100) for 5.48 MeV alpha particles but also caused a lower enhancement in the electronic noise components of the spectrometer compared with that observed for the best high-resolution Schottky barrier detectors. The MOS detectors also exhibited a high charge collection efficiency (CCE) of 96% at the optimized operating bias despite the presence of the oxide layer. A drift-diffusion model applied to the CCE vs gate bias voltage data revealed a minority (hole) carrier diffusion length of 24 μm. Capacitance mode deep level transient spectroscopy (C-DLTS) scans in the temperature range 84–800 K were carried out to identify the resolution limiting electrically active defects. Interestingly, the C-DLTS spectra revealed both positive and negative peaks, indicating the simultaneous presence of electron (majority) and hole (minority) trap centers. It has been inferred that at the steady-state bias for the C-DLTS measurement, the MOS detector operates in the inversion mode at certain device temperatures, causing holes to populate the minority trap centers and, hence, manifests minority carrier peaks as well.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Detecting impurity-specific effects on structure and radiolytic hydrogen production in aluminum hydroxide

While radiolytic hydrogen (H 2 ) generation is an intrinsic property of aqueous and mineral radiolysis in nuclear waste systems, detection of the sub-ns events leading to H 2 generation is challenging. Interfacial processes involving key mineral phases in the sludge, e.g., gibbsite (α-Al(OH) 3 ), have been implicated, with impurities affecting the amount of H 2 generated. To understand why gibbsite synthesized from nitrate precursors produces less H 2 than gibbsite from chloride precursors, we paired 27 Al multiple quantum magic angle spinning (MQMAS) NMR spectroscopy to determine structural heterogeneity with transverse-field muon spin rotation (TF-μSR) to probe electron availability. MQMAS revealed greater structural disorder in the gibbsite synthesized with nitrate (NO 3 -gibbsite). Correspondingly, TF-μSR showed a larger diamagnetic fraction for NO 3 -gibbsite, indicating reduced persistence of μ + -electron bound states (muonium or other radicals) and thus fewer electrons available for reaction on the sub-ns timescale. This establishes a correlation between impurity-induced disorder and electron loss. The diamagnetic fraction serves as a signature for these sub-ns events, as it provides a key constraint for predictive models without currently resolving whether the electron is lost to direct chemical scavenging or trapping at lattice defects.

Graham, Trent R. [Pacific Northwest National Labor↗

Imprinting a Three-Dimensional Skyrmion in a Bose–Einstein Condensate Via a Raman Process

We describe an experimental protocol for the creation of a three-dimensional topological defect, a skyrmion, in a pseudo-spin-1/2 Bose–Einstein condensate (BEC) confined in a spin-independent harmonic trap. We show that one can imprint the skyrmion on the BEC within a few tens of microseconds using a Raman process with the structured laser fields. We numerically solved the mean-field Gross– Pitaevskii equation to examine our imprinting scheme and found that all parameters we use are experimentally feasible.

3D Skyrmion↗