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At least 613 records · Page 34

Vacancy-Induced Tunable Kondo Effect in Twisted Bilayer Graphene

In single sheets of graphene, vacancy-induced states have been shown to host an effective spin-1/2 hole that can be Kondo screened at low temperatures. Here, we show how these vacancy-induced impurity states survive in twisted bilayer graphene (TBG), which thus provides a tunable system to probe the critical destruction of the Kondo effect in pseudogap hosts. Ab initio calculations and atomic-scale modeling are used to determine the nature of the vacancy states in the vicinity of the magic angle in TBG, demonstrating that the vacancy can be treated as a quantum impurity. Utilizing this insight, we construct an Anderson impurity model with a TBG host that we solve using the numerical renormalization group combined with the kernel polynomial method. We determine the phase diagram of the model and show how there is a strict dichotomy between vacancies in the AA/BB versus AB/BA tunneling regions. In AB/BA vacancies, the Kondo temperature at the magic angle develops a broad distribution with a tail to vanishing temperatures due to multifractal wave functions at the magic angle. Finally, we argue that scanning tunneling microscopy in the vicinity of the vacancy can act as a probe of both the critical single-particle states and the underlying many-body ground state in magic-angle TBG.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Exploring the relationship between deposition method, microstructure, and performance of Nb/Si-based superconducting coplanar waveguide resonators

Superconducting quantum circuits (SQC) are one of the most promising hardware platforms for quantum computing, yet their performance is currently limited by the presence of various structural defects inside the circuit's structure. Despite impressive progress in the past decade, a precise understanding of the origin of these defects from various fabrication processes and their impact on coherence is still lacking. Here, in this study, we performed a comprehensive investigation on the microstructure, superconductivity, and resonator quality factor of Nb films deposited by high-power impulse magnetron sputtering (HiPIMS) and direct current (DC) magnetron sputtering. A suite of characterization techniques, including electron microscopy with spectroscopy, secondary ion mass spectrometry, magneto-optical microscopy, and pump-probe reflectivity spectroscopy is used. We reveal that niobium (Nb) resonators fabricated using HiPIMS exhibit a smaller average grain size, thicker surface oxide with larger thickness variations (rougher surface), and a thicker amorphous Nb/Si interface layer compared to samples deposited by DC sputtering. We identified that the amorphous Nb oxides (mainly located at the Nb surface and along the grain boundaries) and Nb-Si amorphous layers (at the Nb/Si interface) are major and potential sources of two-level system (TLS), while off-stochiometric oxides and suboxides of Nb close to the surface, crystalline defects (i.e., dislocations at grain boundary, point defects introduced during deposition) are main contributors of non-TLS sources. Our findings clarify the relationship between different defects and coherence loss mechanisms, highlighting the importance of material microstructure control on performance optimization in SQC.

36 MATERIALS SCIENCE↗

Surface magnetism in Fe 3 GeTe 2 van der Waals ferromagnet

The surface magnetization of Fe 3 GeTe 2 was examined by low-energy electron microscopy (LEEM) using an off-normal incidence electron beam. We found that the 180o domain walls are of Bloch type. Temperature-dependent LEEM measurements yield a surface magnetization with a surface critical exponent β1 = 0.79±0.02. This result is consistent with surface magnetism in the 3D semi-infinite Heisenberg (β1 = 0.84±0.01) or Ising (β1 = 0.78±0.02) models, which is distinctly different from the bulk exponent (β = 0.34±0.07). Further, the measurements reveal the power of LEEM with a tilted beam to determine magnetic domain structure in quantum materials, without need for the use of spin-polarized electrons. Single crystal diffraction measurements reveal inversion symmetry-breaking weak peaks and yield space group P-6m2. This Fe site defect-derived loss of inversion symmetry enables the formation of skyrmions in this Fe 3 GeTe 2 crystal.

36 MATERIALS SCIENCE↗

Quantum-Well Bound States in Graphene Heterostructure Interfaces

We present experimental evidence of electronic and optical interlayer resonances in graphene van der Waals heterostructure interfaces. Using the spectroscopic mode of a low-energy electron microscope (LEEM), we characterized these interlayer resonant states up to 10 eV above the vacuum level. Compared with nontwisted, AB-stacked bilayer graphene (AB BLG), an ≈ 0.2 Å increase was found in the interlayer spacing of 30° twisted bilayer graphene (30°-tBLG). In addition, we used Raman spectroscopy to probe the inelastic light-matter interactions. A unique type of Fano resonance was found around the D and G modes of the graphene lattice vibrations. This anomalous, robust Fano resonance is a direct result of quantum confinement and the interplay between discrete phonon states and the excitonic continuum.

36 MATERIALS SCIENCE↗

Spatiotemporal imaging and manipulation of surface plasmons

Abstract Surface plasmon polaritons (SPPs) are travelling surface waves that have shown promise for applications in nanophotonics as they provide a direct route toward photon-mediated electrical signal generation – a central paradigm for speeding up and scaling down photonic elements. SPP waves have also generated fundamental interest due to their high-field strength and sub-wavelength confinement, properties that have enabled the surface-enhanced Raman effect. Over the last decade, photoemission electron microscopy (PEEM) has emerged as a pioneering technique for imaging surface electric fields through ultrashort laser pulse mediated electron emission and has therefore become an indispensable tool for characterizing plasmonic phenomena at interfaces in a variety of materials. PEEM offers nanometer spatial resolution and femtosecond temporal resolution, allowing SPPs to be prepared, monitored, and manipulated on the nanometer-femtosecond scale. Through a brief review of recent reports, we aim to introduce PEEM-based SPP imaging and manipulation modalities and highlight their utility in the context of emerging nanoscale and quantum materials science advancements.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Terahertz magneto-nanoscopy of encapsulated monolayer graphene

This study investigates the nanoscale conductivity of encapsulated monolayer graphene at temperatures down to 5 K and magnetic fields of up to 1 T. We use the scattering-type scanning near-field optical microscopy technique to probe magnetic-field-dependent responses from graphene close to charge neutrality in the terahertz spectral region. We observe the near-perfect high-q reflector behavior of graphene but with subtle changes by the presence of magnetic fields. Measurements align with calculations of the magneto-optical conductivity and the near-field spectroscopic contrast that describes the field-tunable cyclotron resonance of Dirac fermions. Our result provides an initial step toward understanding temperature and magnetic field effects on nanoscale terahertz transport in two-dimensional quantum materials.

Kim, Richard H. J. [Ames Laboratory (AMES), Ames, ↗

Understanding curvature effects on the magnetization reversal of patterned permalloy Archimedean spirals

Geometric curvature in magnetic systems can induce several unique magnetic interactions, the most notable of which are the curvature induced magnetic anisotropy and the curvature introduced Dzyaloshinski-Moria (DM) like interaction. Of the two, the DM-like interaction is particularly interesting as it provides a unique way to control domain wall motion, which is particularly relevant to the field of spintronics. In this work, we study the effect of geometric curvature on magnetization reversal in Permalloy strips patterned into Archimedean spirals with varying widths. Specifically, we simulated the magnetization reversal of Permalloy strips for several widths ranging from microscale to nanoscale to determine a lengthscale at which the curvature effects are strong. Simulations showed that in the microscale spirals, magnetization reversal primarily occurs through the appearance of magnetization ripple in which domains with reversed magnetization nucleate. On the other hand, the nanoscale spirals showed that reversal primarily proceeded through the motion of domain walls into the arms of the spiral. Our experimental in situ Lorentz transmission electron microscopy data of the microscale spirals, however, showed that magnetization reversal occurred with both mechanisms. At the nanoscale, the effect of local variation of curvature leads to hysteresis loops with stepped behavior. This behavior is characteristic of the curvature induced DM-like interaction affecting domain wall motion in the arms of the nanoscale spirals.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Electron-Beam Induced Emergence of Mesoscopic Ordering in Layered MnPS 3

Ordered mesoscale structures in 2D materials induced by small misorientations have allowed for a wide variety of electronic, ferroelectric, and quantum phenomena to be explored. Until now, the only mechanism to induce this periodic ordering was via mechanical rotations between the layers, with the periodicity of the resulting moiré pattern being directly related to twist angle. Here we report a fundamentally distinct mechanism for emergence of mesoscopic periodic patterns in multilayer sulfur-containing metal phosphorus trichalcogenide, MnPS3, induced by the electron beam. The formation under the beam of periodic hexagonal patterns with several characteristic length scales, nucleation and transitions between the phases, and local dynamics are demonstrated. The associated mechanisms are attributed to the relative contraction of the layers caused by beam-induced sulfur vacancy formation with subsequent ordering and lattice parameter change. As a result, the plasmonic response of the system is locally altered, suggesting an element of control over plasmon resonances by electron beam patterning. To conclude, we pose that harnessing this phenomenon provides both insight into fundamental physics of quantum materials and enables device applications by enabling controlled periodic potentials on the atomic scale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Experimental and Theoretical Studies of the Surface Oxidation Process of Rare–Earth Tritellurides

Recent studies have established Van der Waals (vdW) layered and 2D rare-earth tritellurides (RTe 3 ) as superconductors and near room-temperature charge density wave (CDW) materials. Their environmental stability raises natural concern owing to aging/stability effects observed in other tellurium-based layered crystals. Here, the results establish the stability and environmental aging characteristics of these RTe 3 systems involving a variety of metals such as La, Nd, Sm, Gd, Dy, and Ho. The atomic force microscopy (AFM) and scanning electron microscopy (SEM) results show that all the RTe 3 sheets oxidize to form thin TeO x layers that are primarily confined to the surface, edges, and grain boundaries. Time-resolved in situ Raman spectroscopy measurements are used to understand the kinetics of the oxidization process for different lanthanide metal cations and establish their relative stability/resilience to oxidization. Overall results indicate that the vdW layers show higher air stability as the 4f electron number decreases going from Ho to La, resulting in the most stable LaTe 3 compared to the least stable HoTe 3 . Comprehensive quantum mechanical simulations reveal that environmental degradation originates from a strong oxidizing reaction with O 2 molecules, while humidity (H 2 O) plays a negligible role unless Te vacancies are present. Moreover, the simulations explain the effects of 4f electrons on the work function and Te vacancies formation, which directly impact the aging characteristics of RTe 3 layers. Interestingly, optical and electrical measurements show that the CDW response is still observed in aged RTe 3 layers owing to the presence of underlying pristine/nonoxidized RTe 3 layers, except CDW transition temperatures increase due to the thickness effect. Overall results offer the first in-depth environmental aging studies on these materials, which can be applied to engineer and design their chemical stability, surface properties, and overall CDW characteristics.

36 MATERIALS SCIENCE↗

Block copolymer self-assembly derived mesoporous magnetic materials with three-dimensionally (3D) co-continuous gyroid nanostructure

Magnetic nanomaterials are gaining interest for their many applications in technological areas from information science and computing to next-generation quantum energy materials. While magnetic materials have historically been nanostructured through techniques such as lithography and molecular beam epitaxy, there has recently been growing interest in using soft matter self-assembly. In this work, a triblock terpolymer, poly(isoprene-block-styrene-block-ethylene oxide) (ISO), is used as a structure directing agent for aluminosilicate sol nanoparticles and magnetic material precursors to generate organic–inorganic bulk hybrid films with co-continuous morphology. After thermal processing into mesoporous materials, results from a combination of small angle X-ray scattering (SAXS) and scanning electron microscopy (SEM) are consistent with the double gyroid morphology. Nitrogen sorption measurements reveal a type IV isotherm with H1 hysteresis, and yield a specific surface area of around 200 m 2 g −1 and an average pore size of 23 nm. The magnetization of the mesostructured material as a function of applied field shows magnetic hysteresis and coercivity at 300 K and 10 K. Comparison of magnetic measurements between the mesoporous gyroid and an unstructured bulk magnetic material, derived from the identical inorganic precursors, reveals the structured material exhibits a coercivity of 250 Oe, opposed to 148 Oe for the unstructured at 10 K, and presence of remnant magnetic moment not conventionally found in bulk hematite; both of these properties are attributed to the mesostructure. This scalable route to mesoporous magnetic materials with co-continuous morphologies from block copolymer self-assembly may provide a pathway to advanced magnetic nanomaterials with a range of potential applications.

Chemistry↗

Heteroepitaxial Integration of ZnGeN 2 on GaN Buffers Using Molecular Beam Epitaxy

Recently theorized hybrid II-IV-N 2 /III-N heterostructures, based on current commercialized (In,Ga)N devices, are predicted to significantly advance the design space of highly efficient optoelectronics in the visible spectrum, yet there are few epitaxial studies of II-IV-N 2 materials. In this work, we present heteroepitaxial ZnGeN 2 grown on GaN buffers and AlN templates. We demonstrate that a GaN nucleating surface is crucial for increasing the ZnGeN 2 crystallization rate to combat Zn desorption, extending the stoichiometric growth window from 215 degrees C on AlN to 500 degrees C on GaN buffers. Structural characterization reveals well-crystallized films with threading dislocations extending from the GaN buffer. These films have a critical thickness for relaxation of 20-25 nm as determined by reflection high energy electron diffraction (RHEED) and cross-sectional scanning electron microscopy (SEM). The films exhibit a cation-disordered wurtzite structure, with lattice constants a = 3.216 +/- 0.004 A and c = 5.215 +/- 0.005 A determined by RHEED and X-ray diffraction (XRD). This work demonstrates a significant step toward the development of hybrid ZnGeN 2 -GaN integrated devices.

36 MATERIALS SCIENCE↗

Improving Qubit Coherence Time Through Detailed Materials Analysis

This study investigates the defects, imperfections, and variations in Nb thin films deposited on sapphire substrates. Two samples, W114 and W118, were fabricated using DC Magnetron Sputtering and Electron Cyclotron Resonance (ECR), respectively. Each sample was analyzed at five distinct spots to compare elemental homogeneity and variations in oxide layers. Scanning Electron Microscopy (SEM) was employed to examine surface morphology, while Energy Dispersive X-ray Spectroscopy (EDS) and X-ray Photoelectron Spectroscopy (XPS) provided elemental and chemical state analyses. SEM revealed distinct structures in W114 and a uniform surface in W118. EDS showed higher aluminum signals in W118, indicating a thinner film in comparison to W114. XPS detected a higher Nb₂O₅ signal in W118, in comparison to W114, which can be attributed to the presence of a thicker Nb₂O₅ layer in W118. These findings highlight the critical role of precise material characterization in advancing quantum computing technologies.

Rosado Bonilla, Cristy M.↗

Ultrathin epitaxial NbN superconducting films with high upper critical field grown at low temperature

Ultrathin (5–50 nm) epitaxial superconducting niobium nitride (NbN) films were grown on AlN-buffered c-plane Al 2 O 3 by an industrial scale physical vapor deposition technique at 400°C. Both X-ray diffraction and scanning electron microscopy analysis show high crystallinity of the (111)-oriented NbN films, with a narrow full-width-at-half-maximum of the rocking curve down to 0.030°. The lattice constant decreases with decreasing NbN layer thickness, suggesting lattice strain for films with thicknesses below 20 nm. The superconducting transition temperature, the transition width, the upper critical field, the irreversibility line, and the coherence length are closely correlated to the film thickness. This work realized high quality ultrathin epitaxial NbN films by an industry-scale PVD technology at low substrate temperature, which opens up new opportunities for quantum devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Tuning the Curie temperature of a two-dimensional magnet/topological insulator heterostructure to above room temperature by epitaxial growth

Heterostructures of two-dimensional (2D) van der Waals (vdW) magnets and topological insulators (TI) are of substantial interest as candidate materials for efficient spin-torque switching, quantum anomalous Hall effect, and chiral spin textures. However, since many of the vdW magnets have Curie temperatures below room temperature, we want to understand how materials can be modified to stabilize their magnetic ordering to higher temperatures. In this work, we utilize molecular beam epitaxy to systematically tune the Curie temperature (T C ) in thin film Fe 3 GeTe 2 /Bi 2 Te 3 from bulklike values (~220 K) to above room temperature by increasing the growth temperature from 300°C to 375°C. For samples grown at 375°C, cross-sectional scanning transmission electron microscopy (STEM) reveals the spontaneous formation of different Fe m Ge n Te 2 compositions (e.g., Fe 5 Ge 2 Te 2 and Fe 7 Ge 6 Te 2 ) as well as intercalation in the vdW gaps, which are possible origins of the enhanced Curie temperature. Furthermore, this observation paves the way for developing various Fe m Ge n Te 2 /TI heterostructures with novel properties.

36 MATERIALS SCIENCE↗

Strong Structural and Electronic Coupling in Metavalent PbS Moiré Superlattices

Moiré superlattices are twisted bilayer materials in which the tunable interlayer quantum confinement offers access to new physics and novel device functionalities. Previously, moiré superlattices were built exclusively using materials with weak van der Waals interactions, and synthesizing moiré superlattices with strong interlayer chemical bonding was considered to be impractical. Here, in this study, using lead sulfide (PbS) as an example, we report a strategy for synthesizing moiré superlattices coupled by strong chemical bonding. We use water-soluble ligands as a removable template to obtain free-standing ultrathin PbS nanosheets and assemble them into direct-contact bilayers with various twist angles. Atomic-resolution imaging shows the moiré periodic structural reconstruction at the superlattice interface due to the strong metavalent coupling. Electron energy loss spectroscopy and theoretical calculations collectively reveal the twist-angle-dependent electronic structure, especially the emergent separation of flat bands at small twist angles. The localized states of flat bands are similar to well-arranged quantum dots, promising an application in devices. This study opens a new door to the exploration of deep energy modulations within moiré superlattices alternative to van der Waals twistronics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Observation of Topological Chirality Switching Induced Freezing of a Skyrmion Crystal

Magnetic skyrmions are topologically protected quasi-particles with a well-defined chirality. Control over their chirality is proposed as an additional feature for encoding data bits or as qubits in quantum computing due to their high efficiency and stability against achiral magnetic textures. Here it is shown that an in-plane magnetic field can be utilized to reshape the energy barriers between different skyrmionic bubbles (e.g., Bloch type, type-II) enabling spontaneous chirality fluctuations with a frequency that increases with the strength of the in-plane field. The insulating van der Waals ferromagnet CrBr3 is used as an archetypal system for low damping, reduced energy dissipation and a high number of magnetic phases to capture the chirality dynamics in real time through cryo-Lorentz transmission electron microscopy. It is observed that the interplay between the intrinsic Dzyaloshinskii–Moriya interaction and out-of-plane field biased the chirality dynamics, favoring one handedness over the other. A remarkable consequence of the spontaneous chirality switching mechanism is that it induces a freezing (or crystallization) process in the skyrmion lattice. As the bubbles fluctuate between Bloch and type-II they elongate and shrink parallel to the in-plane field. Subsequently, the overall lattice crystallizes along the in-plane field direction, inducing a phase transition from a disordered liquid state to a hexatic phase where skyrmions are highly ordered resembling that of a solid. The results indicate chirality as an active element in the creation of topologically protected skyrmion crystals unveiling pathways toward chiral spintronic device platforms with tunable embedded configuration.

2D Phase Transition↗

Tuning interfacial Dzyaloshinskii-Moriya interactions in thin amorphous ferrimagnetic alloys

Skyrmions can be stabilized in magnetic systems with broken inversion symmetry and chiral interactions, such as Dzyaloshinskii-Moriya interactions (DMI). Further, compensation of magnetic moments in ferrimagnetic materials can significantly reduce magnetic dipolar interactions, which tend to favor large skyrmions. Tuning DMI is essential to control skyrmion properties, with symmetry breaking at interfaces offering the greatest flexibility. However, in contrast to the ferromagnet case, few studies have investigated interfacial DMI in ferrimagnets. Here we present a systematic study of DMI in ferrimagnetic CoGd films by Brillouin light scattering. We demonstrate the ability to control DMI by the CoGd cap layer composition, the stack symmetry and the ferrimagnetic layer thickness. The DMI thickness dependence confirms its interfacial nature. In addition, magnetic force microscopy reveals the ability to tune DMI in a range that stabilizes sub-100 nm skyrmions at room temperature in zero field. Our work opens new paths for controlling interfacial DMI in ferrimagnets to nucleate and manipulate skyrmions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗