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At least 217 records · Page 12

Mechanisms of Skyrmion and Skyrmion Crystal Formation from the Conical Phase

Real-space topological magnetic structures such as skyrmions and merons are promising candidates for information storage and transport. However, the microscopic mechanisms that control their formation and evolution are still unclear. In this work, using in situ Lorentz transmission electron microscopy, we demonstrate that skyrmion crystals (SkXs) can nucleate, grow, and evolve from the conical phase in the same ways that real nanocrystals form from vapors or solutions. More intriguingly, individual skyrmions can also “reproduce” by division in a mitosis-like process that allows them to annihilate SkX lattice imperfections, which is not available to crystals made of mass-conserving particles. Combined string method and micromagnetic calculations show that competition between repulsive and attractive interactions between skyrmions governs particle-like SkX growth, but nonconservative SkX growth appears to be defect mediated. Our results provide insights toward manipulating magnetic topological states by applying established crystal growth theory, adapted to account for the new process of skyrmion mitosis.

36 MATERIALS SCIENCE↗

Precision redshift-space galaxy power spectra using Zel'dovich control variates

Numerical simulations in cosmology require trade-offs between volume, resolution and run-time that limit the volume of the Universe that can be simulated, leading to sample variance in predictions of ensemble-average quantities such as the power spectrum or correlation function(s). Sample variance is particularly acute at large scales, which is also where analytic techniques can be highly reliable. This provides an opportunity to combine analytic and numerical techniques in a principled way to improve the dynamic range and reliability of predictions for clustering statistics. In this paper we extend the technique of Zel'dovich control variates, previously demonstrated for 2-point functions in real space, to reduce the sample variance in measurements of 2-point statistics of biased tracers in redshift space. We demonstrate that with this technique, we can reduce the sample variance of these statistics down to their shot-noise limit out to k ~ 0.2 h Mpc -1 . This allows a better matching with perturbative models and improved predictions for the clustering of e.g. quasars, galaxies and neutral Hydrogen measured in spectroscopic redshift surveys at very modest computational expense. We discuss the implementation of ZCV, give some examples and provide forecasts for the efficacy of the method under various conditions.

79 ASTRONOMY AND ASTROPHYSICS↗

FLAMES─Fast, Low-Storage, Accurate, and Memory-Efficient Adaptive Sampling─Approach to Resolve Spatially Dependent Dynamics of Molecular Liquids

Many critical phenomena in soft matter occur at large length scales, necessitating the resolution of their structure and dynamics at low wavenumbers. However, resolving wavenumber-dependent dynamics computationally via molecular dynamics simulations presents significant challenges, as these phenomena span several orders of magnitude in both time and length scales, resulting in high computational costs and memory demands. Here, this work highlights the computational and memory challenges associated with analyzing molecular trajectories in reciprocal space and demonstrates a method to address them. We introduce FLAMESFast, Low-storage, Accurate, and Memory-Efficient adaptive Sampling, which is a direct method for calculation of structure factors, allowing us to select only the required number of wavevectors for binning. We also use wavenumber-dependent time steps to extract dynamics. Our FLAMES approach effectively mitigates computational and memory/storage bottlenecks. We demonstrate the method using simulations of a model system, liquid octane, at various temperatures. Comparisons with experimental data and real space computation show that the FLAMES technique achieves high accuracy in resolving temperature- and spatially dependent dynamics while being significantly more computationally efficient and requiring less memory and storage than methods based on a uniform wavevector grid and fixed temporal spacing.

Chen, Guang [Argonne National Laboratory (ANL), Ar↗

CP2 skyrmions and skyrmion crystals in realistic quantum magnets

Abstract Magnetic skyrmions are nanoscale topological textures that have been recently observed in different families of quantum magnets. These objects are called CP 1 skyrmions because they are built from dipoles—the target manifold is the 1D complex projective space, CP 1 ≅ S 2 . Here we report the emergence of magnetic CP 2 skyrmions in a realistic spin-1 model, which includes both dipole and quadrupole moments. Unlike CP 1 skyrmions, CP 2 skyrmions can also arise as metastable textures of quantum paramagnets, opening a new road to discover emergent topological solitons in non-magnetic materials. The quantum phase diagram of the spin-1 model also includes magnetic field-induced CP 2 skyrmion crystals that can be detected with regular momentum- (diffraction) and real-space (Lorentz transmission electron microscopy) experimental techniques.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Investigating Quantum Materials with Half-Polarized Diffraction and magnetic PDF analysis at the HB-2A Neutron Powder Diffractometer

Local magnetic ordering and anisotropy is often central to the emergent behavior and subsequent functional properties in quantum materials and beyond. Neutron powder diffraction provides a straightforward yet extremely powerful technique for quantitative measurements of microscopic magnetic properties. The HB-2A powder diffractometer located at the High Flux Isotope Reactor in ORNL is traditionally utilized for long-range magnetic structure determination. Recently these capabilities have been extended to include methods aimed at accessing local magnetism: Half- polarized neutron powder diffraction (pNPD) and magnetic pair distribution function (mPDF) analysis. These two distinct techniques are possible on HB-2A due to the versatility of the instrument’s reciprocal space coverage, resolution and novel ultra-low temperature multi-sample changers that operate down to dilution refrigerator temperatures. This provides unique capabilities not found on any powder diffraction instrument and is particularly well suited to investigations of magnetic quantum materials. The development and implementation of these techniques will be discussed with a series of science case examples ranging from geometric frustrated magnets to magnetic metal-organic frameworks. Data reduction and analysis tools will be presented that enable the extraction of the local site susceptibility tensor and local spin-spin correlations in real space. Finally, potential combinations of these techniques in the form of half-polarized magnetic pair distribution function (pmPDF) analysis will be considered. Looking forward, HB-2A is undergoing a detector upgrade that will be in the user program by 2026. This will offer an order of magnitude increase in count rates to further aid the development of these often low signal measurements and provide new scientific capabilities.

Neutron Scattering↗

Møller–Plesset and Density-Fixed Adiabatic Connections for a Model Diatomic System at Different Correlation Regimes

In recent years, adiabatic connection (AC) interpolations developed within density functional theory (DFT) have been found to provide good performances in the calculation of interaction energies when used with Hartree–Fock (HF) ingredients. The physical and mathematical reasons for such unanticipated performance have been clarified, to some extent, by studying the strong-interaction limit of the Møller–Plesset (MP) AC. In this work, we calculate both the MP and the DFT AC integrand for the asymmetric Hubbard dimer, which allows for a systematic investigation of different correlation regimes by varying two simple parameters in the Hamiltonian: the external potential, Δv, and the interaction strength, U. Notably, we find that, while the DFT AC integrand appears to be convex in the full parameter space, the MP integrand may change curvature twice. Furthermore, we discuss different aspects of the second-order expansion of the correlation energy in each AC, and we demonstrate why the derivative of the λ-dependent density in the MP AC at λ = 0 (i.e., at the HF density) is zero in the model. Concerning the strong-interaction limit of both ACs in the Hubbard dimer setting, we show that the asymptotic value of the MP AC, W ∞ HF , is lower than (or equal to) its DFT analogue, W ∞ KS , if the two are compared at a given density, just like in real space. Furthermore, we also show that this is not always the case if the two quantities are compared at a given external potential.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Establishing coherent momentum-space electronic states in locally ordered materials

Rich momentum-dependent electronic structure naturally arises in solids with long-range crystalline symmetry. Reliable and scalable quantum technologies rely on materials that are either not perfect crystals or non-crystalline, breaking translational symmetry. This poses the fundamental questions of whether coherent momentum-dependent electronic states can arise without long-range order, and how they can be characterized. Here we investigate Bi 2 Se 3 , which exists in crystalline, nanocrystalline, and amorphous forms, allowing direct comparisons between varying degrees of spatial ordering. Through angle-resolved photoemission spectroscopy, we show for the first time momentum-dependent band structure with Fermi surface repetitions in an amorphous solid. The experimental data is complemented by a model that accurately reproduces the vertical, dispersive features as well as the replication at higher momenta in the amorphous form. These results reveal that well-defined real-space length scales are sufficient to produce dispersive band structures, and that photoemission can expose the imprint of these length scales on the electronic structure.

36 MATERIALS SCIENCE↗

AI-enabled Lorentz microscopy for quantitative imaging of nanoscale magnetic spin textures

The manipulation and control of nanoscale magnetic spin textures are of rising interest as they are potential foundational units in next-generation computing paradigms. Achieving this requires a quantitative understanding of the spin texture behavior under external stimuli using in situ experiments. Lorentz transmission electron microscopy (LTEM) enables real-space imaging of spin textures at the nanoscale, but quantitative characterization of in situ data is extremely challenging. Here, we present an AI-enabled phase-retrieval method based on integrating a generative deep image prior with an image formation forward model for LTEM. Our approach uses a single out-of-focus image for phase retrieval and achieves significantly higher accuracy and robustness to noise compared to existing methods. Furthermore, our method is capable of isolating sample heterogeneities from magnetic contrast, as shown by application to simulated and experimental data. This approach allows quantitative phase reconstruction of in situ data and can also enable near real-time quantitative magnetic imaging.

36 MATERIALS SCIENCE↗

End-to-End Automated Segmentation Framework for Four-Dimensional Scanning Transmission Electron Microscopy Data

Four-dimensional scanning transmission electron microscopy (4D-STEM) is powerful for rapidly characterizing arrays of nanoparticles produced via high-throughput synthesis. However, such 4D-STEM datasets typically contain thousands of nanoparticles, each characterized by thousands of diffraction patterns spatially distributed across the nanoparticle, necessitating efficient and comprehensive analysis. We propose an end-to-end segmentation framework to automatically segment each nanoparticle into regions with distinct composition/orientation of crystal grains, using only the 4D-STEM data. Bragg disk information is extracted in a physics-informed manner from the diffraction patterns at each spatial location and combined with the real space coordinates to form feature vectors. These feature vectors are then used as inputs to a Gaussian mixture model (GMM) to segment the nanoparticle into distinct regions. We also develop two visualization tools based on the GMM outputs to infer the interface transition and the degree of superposition. Our framework comprehensively integrates machine learning tools and physics knowledge, and provides a basis for substantially compressing enormous 4D-STEM datasets, e.g., by replacing the full 4D-STEM dataset for each nanoparticle with only a single set of Bragg disk features for each distinct crystal grain identified in the nanoparticle. In this article, we demonstrate the power of our framework by presenting results for real, complex datasets.

47 OTHER INSTRUMENTATION↗

Topological Nernst effect, anomalous Nernst effect, and anomalous thermal Hall effect in the Dirac semimetal Fe 3 Sn 2

Topological semimetals have been a focal point of research in recent years. One of the salient characters of topological semimetals is the anomalous Hall effect arising from the nontrivial momentum-space Berry phase. In contrast, anomalous transverse thermoelectric coefficient and thermal Hall effect are much less explored up to date. In this paper, we report thermoelectric and thermal transport properties of Fe 3 Sn 2 , a prototypical Dirac semimetal. We find that Fe 3 Sn 2 exhibits large topological Nernst effect which is associated with the non-zero spin chirality of the skyrmion bubble phase. Furthermore, Fe 3 Sn 2 shows prominent anomalous thermal Hall effect and anomalous Nernst effect with features similar to the anomalous Hall effect. The anomalous Nernst signal is about 2.1 μV/K at room temperature, which is comparable to the largest value reported thus far. These results highlight the synergic effects of Berry phase in both real space and momentum space of Fe 3 Sn 2 , and this study demonstrates an effective strategy of investigating topological materials by measuring their transverse thermal and thermoelectric responses.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Review: knots and other new topological effects in liquid crystals and colloids

Abstract Humankind has been obsessed with knots in religion, culture and daily life for millennia, while physicists like Gauss, Kelvin and Maxwell already involved them in models centuries ago. Nowadays, colloidal particles can be fabricated to have shapes of knots and links with arbitrary complexity. In liquid crystals, closed loops of singular vortex lines can be knotted by using colloidal particles and laser tweezers, as well as by confining nematic fluids into micrometer-sized droplets with complex topology. Knotted and linked colloidal particles induce knots and links of singular defects, which can be interlinked (or not) with colloidal particle knots, revealing the diversity of interactions between topologies of knotted fields and topologically nontrivial surfaces of colloidal objects. Even more diverse knotted structures emerge in nonsingular molecular alignment and magnetization fields in liquid crystals and colloidal ferromagnets. The topological solitons include hopfions, skyrmions, heliknotons, torons and other spatially localized continuous structures, which are classified based on homotopy theory, characterized by integer-valued topological invariants and often contain knotted or linked preimages, nonsingular regions of space corresponding to single points of the order parameter space. A zoo of topological solitons in liquid crystals, colloids and ferromagnets promises new breeds of information displays and a plethora of data storage, electro-optic and photonic applications. Their particle-like collective dynamics echoes coherent motions in active matter, ranging from crowds of people to schools of fish. This review discusses the state of the art in the field, as well as highlights recent developments and open questions in physics of knotted soft matter. We systematically overview knotted field configurations, the allowed transformations between them, their physical stability and how one can use one form of knotted fields to model, create and imprint other forms. The large variety of symmetries accessible to liquid crystals and colloids offer insights into stability, transformation and emergent dynamics of fully nonsingular and singular knotted fields of fundamental and applied importance. The common thread of this review is the ability to experimentally visualize these knots in real space. The review concludes with a discussion of how the studies of knots in liquid crystals and colloids can offer insights into topologically related structures in other branches of physics, with answers to many open questions, as well as how these experimentally observable knots hold a strong potential for providing new inspirations to the mathematical knot theory.

Physics↗

First-Principles Simulation of Beam-Induced Processes Underlying Atomic Manipulation in Electron Microscopes

The development of experimental methods and apparatuses capable of promoting atomically precise material manipulations holds great promise for realizing the ultimate limit of feature miniaturization in materials and devices. The ability to modify materials atom by atom is anticipated to usher in new technologies in areas as diverse as separation science, medicine, and quantum information science. Historically, scanning probe-based techniques have been the most prominent approaches in this space. However, these methods are best suited for the manipulation of surface-exposed regions of materials, as the strong perturbations required for bond scission are delivered most effectively to atoms in the near-proximity to the scanning probe. In contrast, convergent electron beams with energies tuned slightly below the threshold for inducing irreversible knock-on damage have recently been employed (within scanning transmission electron microscopy) to promote atomic-scale bond rearrangements in various beam-stable solids. Currently, however, the efficiency and selectivity of beam-induced atomic manipulation processes with focused electron beams are such that long irradiation times are required to induce a desired atomic rearrangement. With a better understanding of the underlying physics dictating the outcome of a given irradiation event, methods can be devised to improve the efficiency of these techniques so that their promise can be fully realized through widespread adoption.To this end, this Account details our recent efforts to develop and apply tractable first-principles simulation approaches for studying the response of materials to electric beam-like external electric potentials applied in real space. We briefly review the concepts and capabilities in the area of atomically precise materials manipulation and review the early demonstrations of accomplishments in this area, focusing on studies using scanned convergent electron beam probes in particular. We expound upon the depth of the challenge and identify critical shortcomings of theoretical methods that have previously been employed in the simulation of beam-induced processes. We then describe the computational methods that we have generalized from the concepts and tools most commonly applied to the study of molecular photochemistry and how our adaptations of these methods can be employed to capture the relevant dynamical phenomena for beam-induced processes ranging from the initial electron scattering to the ensuing multistate reactions. Here, we contextualize these methods within the current state of the art in this area, which has historically focused primarily on the simulation of inelastic image formation in the electron microscope for the purpose of interpreting the results of quantitative electron microscopy experiments. We demonstrate that the spatial distribution of state-specific excitation rates due to the presence of an external (probe) electric charge is inhomogeneous, such that irradiation at particular locations in materials can favor specific electronic transitions (and disallow others). In addition to the potential for excited-state reaction pathways to be accessed through the initial inelastic scattering of the tightly focused electron beam from the targeted atoms, we also identify favorable conditions for the electronically nonadiabatic evolution of the highly vibrationally excited system to open complex multistate reaction pathways. Implications of the early results for understanding the mechanisms and potential routes to improved efficiency and selectivity in beam-induced reactions are discussed. We conclude with a summary of the current state of theory and modeling capabilities in this area and provide our perspective on future directions for theoretical and experimental developments that we view as crucial to advancing the use of convergent electron beams in mode-specific, atomically precise platforms for direct-write materials modifications.

36 MATERIALS SCIENCE↗

Unravelling Magnetic Nanochain Formation in Dispersion for In Vivo Applications

Self-assembly of iron oxide nanoparticles (IONPs) into 1D chains is appealing, because of their biocompatibility and higher mobility compared to 2D/3D assemblies while traversing the circulatory passages and blood vessels for in vivo biomedical applications. In this work, parameters such as size, concentration, composition, and magnetic field, responsible for chain formation of IONPs in a dispersion as opposed to spatially confining substrates, are examined. In particular, the monodisperse 27 nm IONPs synthesized by an extended LaMer mechanism are shown to form chains at 4 mT, which are lengthened with applied field reaching 270 nm at 2.2 T. The chain lengths are completely reversible in field. Using a combination of scattering methods and reverse Monte Carlo simulations the formation of chains is directly visualized. The visualization of real-space IONPs assemblies formed in dispersions presents a novel tool for biomedical researchers. This allows for rapid exploration of the behavior of IONPs in solution in a broad parameter space and unambiguous extraction of the parameters of the equilibrium structures. Additionally, it can be extended to study novel assemblies formed by more complex geometries of IONPs.

36 MATERIALS SCIENCE↗

Distinguishing Elements at the Sub‐Nanometer Scale on the Surface of a High Entropy Alloy

Materials in crystalline form possess translational symmetry (TS) when the unit cell is repeated in real space with long- and short-range orders. The periodic potential in the crystal regulates the electron wave function and results in unique band structures, which further define the physical properties of the materials. Amorphous materials lack TS due to the randomization of distances and arrangements between atoms, causing the electron wave function to lack a well-defined momentum. High entropy materials provide another way to break the TS by randomizing the potential strength at periodic atomic sites. The local elemental distribution has a great impact on physical properties in high entropy materials. It is critical to distinguish elements at the sub-nanometer scale to uncover the correlations between the elemental distribution and the material properties. Here, the use of synchrotron X-ray scanning tunneling microscopy (SX-STM) with sub-nm scale resolution in identifying elements on a high entropy alloy (HEA) surface is demonstrated. By examining the elementally sensitive X-ray absorption spectra with an STM tip to enhance the spatial resolution, the elemental distribution on an HEA's surface at a sub-nm scale is extracted. In conclusion, these results open a pathway towards quantitatively understanding high entropy materials and their material properties.

36 MATERIALS SCIENCE↗

Optical Control of Adaptive Nanoscale Domain Networks

Adaptive networks can sense and adjust to dynamic environments to optimize their performance. Understanding their nanoscale responses to external stimuli is essential for applications in nanodevices and neuromorphic computing. However, it is challenging to image such responses on the nanoscale with crystallographic sensitivity. Here, the evolution of nanodomain networks in (PbTiO 3 ) n /(SrTiO 3 ) n superlattices (SLs) is directly visualized in real space as the system adapts to ultrafast repetitive optical excitations that emulate controlled neural inputs. The adaptive response allows the system to explore a wealth of metastable states that are previously inaccessible. Their reconfiguration and competition are quantitatively measured by scanning x-ray nanodiffraction as a function of the number of applied pulses, in which crystallographic characteristics are quantitatively assessed by assorted diffraction patterns using unsupervised machine-learning methods. The corresponding domain boundaries and their connectivity are drastically altered by light, holding promise for light-programable nanocircuits in analogy to neuroplasticity. Phase-field simulations elucidate that the reconfiguration of the domain networks is a result of the interplay between photocarriers and transient lattice temperature. The demonstrated optical control scheme and the uncovered nanoscopic insights open opportunities for the remote control of adaptive nanoscale domain networks.

36 MATERIALS SCIENCE↗

Adaptive Scalpel Scanning Probe Microscopy for Enhanced Volumetric Sensing in Tomographic Analysis

Controlling nanoscale tip‐induced material removal is crucial for achieving atomic‐level precision in tomographic sensing with atomic force microscopy (AFM). While advances have enabled volumetric probing of conductive features with nanometer accuracy in solid‐state devices, materials, and photovoltaics, limitations in spatial resolution and volumetric sensitivity persist. This work identifies and addresses in‐plane and vertical tip‐sample junction leakage as sources of parasitic contrast in tomographic AFM, hindering real‐space 3D reconstructions. Novel strategies are proposed to overcome these limitations. First, the contrast mechanisms analyzing nanosized conductive features are explored when confining current collection purely to in‐plane transport, thus allowing reconstruction with a reduction in the overestimation of the lateral dimensions. Furthermore, an adaptive tip‐sample biasing scheme is demonstrated for the mitigation of a class of artefacts induced by the high electric field inside the thin oxide when volumetrically reduced. This significantly enhances vertical sensitivity by approaching the intrinsic limits set by quantum tunneling processes, allowing detailed depth analysis in thin dielectrics. The effectiveness of these methods is showcased in tomographic reconstructions of conductive filaments in valence change memory, highlighting the potential for application in nanoelectronics devices and bulk materials and unlocking new limits for tomographic AFM.

36 MATERIALS SCIENCE↗

Tunable, Homoepitaxial Hyperbolic Metamaterials Enabled by High Mobility CdO

We report propagating light exhibits hyperbolicity in strongly anisotropic materials where the principal components of the dielectric tensor are opposite in sign. While hyperbolicity occurs naturally in anisotropic polar dielectrics, wherein optical phonons along orthogonal crystal axes are nondegenerate, such optical anisotropy can also be engineered in hyperbolic metamaterials (HMMs): thin film superlattices of alternating dielectric and metallic layers. Contrasted with the severely limited tunability of natural hyperbolic materials, the hyperbolic behavior of HMMs can be tailored significantly both through superlattice design and material selection. However, so far HMMs have suffered from high optical losses, hindering their performance. In this report, broadly tunable (λ = 2–5 µm) Type I and II hyperbolic modes with low losses (quality (Q)-factors up to 19.7) are observed through attenuated total reflectance measurements of monolithic, homoepitaxial superlattices of high- and low-doped cadmium oxide (CdO). Further, the low losses offered by CdO enable the first demonstration of real-space imaging of hyperbolic plasmon polaritons in nanoresonators by scattering-type scanning near-field optical microscopy—previously only possible for hyperbolic phonon polariton materials. Tunable, low-loss CdO HMMs promise designability for applications such as on-chip photonics, super-resolution imaging (hyperlensing), enhanced emission, novel emitter designs, and possibly quantum nanophotonic and time variant metasurfaces.

36 MATERIALS SCIENCE↗

Effect of Stoichiometry on the Structure and Polarization of BaTiO 3

Barium titanate (BaTiO 3 ) is a material of interest for photonic device applications due to its strong optical non-linearity. However, BaTiO 3 -based devices have not found widespread adoption, in part due to the challenges associated with synthesizing high quality thin-films. Here, high-resolution scanning transmission electron microscope (STEM) imaging is used to investigate the atomic structure of both on- and off-stoichiometric BaTiO 3 synthesized by molecular beam epitaxy (MBE). Here, this investigation reveals an asymmetry in the way the BaTiO 3 atomic lattice accommodates off-stoichiometry growth and unveils features beyond what is expected from diffraction or surface characterization techniques. Excess titanium incorporates into the BaTiO 3 lattice to form pervasive defects despite titanium-rich films having a low surface roughness and high-quality appearance in diffraction. Excess barium forms a rough, water-soluble surface layer but does not significantly impact the quality of the BaTiO 3 lattice. STEM is used to map titanium atom displacement in real-space. The average displacement distance is 30–60 pm in the strained thin-films, higher than the <20 pm displacement in bulk BaTiO 3 . Additionally, the titanium atom displacement direction deviates from the c-axis of the unit cell, which may have implications for the material's electro-optic tensor and thus for electro-optic device design.

Cavanagh, Ashley E. [Harvard Univ., Cambridge, MA ↗