arXiv subjects

Vincent H. Crespi

Publications and source records attributed to Vincent H. Crespi.

At least 37 records · Page 2Linked to original sources

arXiv2021

Direct observation of 3D topological spin textures and their interactions using soft x-ray vector ptychography

Magnetic topological defects are energetically stable spin configurations characterized by symmetry breaking. Vortices and skyrmions are two well-known examples of 2D spin textures that have been actively studied for both fundamental interest and practical applications. However, experimental evidence of the 3D spin textures has been largely indirect or qualitative to date, due to the difficulty of quantitively characterizing them within nanoscale volumes. Here, we develop soft x-ray vector ptychography to quantitatively image the 3D magnetization vector field in a frustrated superlattice with 10 nm spatial resolution. By applying homotopy theory to the experimental data, we quantify the topological charge of hedgehogs and anti-hedgehogs as emergent magnetic monopoles and probe their interactions inside the frustrated superlattice. We also directly observe virtual hedgehogs and anti-hedgehogs created by magnetically inert voids. We expect that this new quantitative imaging method will open the door to study 3D topological spin textures in a broad class of magnetic materials. Our work also demonstrates that magnetically frustrated superlattices could be used as a new platform to investigate hedgehog interactions and dynamics and to exploit optimized geometries for information storage and transport applications.

cond-mat.str-el↗

arXiv2021

Field-tunable interactions and frustration in underlayer-mediated artificial spin ice

Artificial spin ice systems have opened experimental windows into a range of model magnetic systems through the control of interactions among nanomagnet moments. This control has previously been enabled by altering the nanomagnet size and the geometry of their placement. Here we demonstrate that the interactions in artificial spin ice can be further controlled by including a soft ferromagnetic underlayer below the moments. Such a substrate also breaks the symmetry in the array when magnetized, introducing a directional component to the correlations. Using spatially resolved magneto-optical Kerr effect microscopy to image the demagnetized ground states, we show that the correlation of the demagnetized states depends on the direction of underlayer magnetization. Further, the relative interaction strength of nearest and next-nearest neighbors varies significantly with the array geometry. We exploit this feature to induce frustration in an inherently unfrustrated square lattice geometry, demonstrating new possibilities for effective geometries in two dimensional nanomagnetic systems.

cond-mat.mes-hall↗

arXiv2020

Atlas of 2D metals epitaxial to SiC: filling-controlled gapping conditions and alloying rules

The realization of air-stable 2D metals epitaxial to SiC and capped by graphene creates a potentially immense chemical space of 2D metals and alloys that could expand the variety of solid-state excitations unique to 2D metals beyond what is known for graphene and niobium/tantalum chalcogenides. We perform a high-throughput computational survey from first-principles predicting the structures and stabilities of all metals in the periodic table when they intercalate graphene/SiC. Our results not only agrees with all experimentally known metal/SiC structures explored so far, but also reveals conspicuous trends related to metal cohesive energies and metal-silicon bonding. For special groups of metals, a small bandgap opens, relying on appropriate electron filling and substrate-induced symmetry breaking. From this gapping stabilization, we derive alloying rules unique to 2D metals.

cond-mat.mtrl-sci↗

arXiv2020

Scanning Transmission Electron Tomography and Electron Energy Loss Spectroscopy of Silicon Metalattices

Transmission electron microscopy, scanning transmission electron tomography, and electron energy loss spectroscopy were used to characterize three-dimensional artificial Si nanostructures called "metalattices", focusing on Si metalattices synthesized by high-pressure confined chemical vapor deposition in 30-nm colloidal silica templates with ~7 and ~12 nm "meta-atoms" and ~2 nm "meta-bonds". The "meta-atoms" closely replicate the shape of the tetrahedral and octahedral interstitial sites of the face-entered cubic colloidal silica template. Composed of either amorphous or nanocrystalline silicon, the metalattice exhibits long-range order and interconnectivity in two-dimensional micrographs and three-dimensional reconstructions. Electron energy loss spectroscopy provides information on local electronic structure. The Si L2,3 core-loss edge is blue-shifted compared to the onset for bulk Si, with the meta-bonds displaying a larger shift (0.55 eV) than the two types of meta-atoms (0.30 and 0.17 eV). Local density of state calculations using an empirical tight binding method are in reasonable agreement.

cond-mat.mtrl-sci↗

arXiv2020

Illuminating Invisible Grain Boundaries in Coalesced Single-Orientation WS2 Monolayer Films

Engineering atomic-scale defects is crucial for realizing wafer-scale, single-crystalline transition metal dichalcogenide monolayers for electronic devices. However, connecting atomic-scale defects to larger morphologies poses a significant challenge. Using electron microscopy and atomistic simulations, we provide insights into WS2 crystal growth mechanisms, providing a direct link between synthetic conditions and the microstructure. Dark-field TEM imaging of coalesced monolayer WS2 films illuminates defect arrays that atomic-resolution STEM imaging identifies as translational grain boundaries. Imaging reveals the films to have nearly a single orientation with imperfectly stitched domains. Through atomic-resolution imaging and ReaxFF reactive force field-based molecular dynamics simulations, we observe two types of translational mismatch and discuss their atomic structures and origin. Our results indicate that the mismatch results from relatively fast growth rates. Through statistical analysis of >1300 facets, we demonstrate that the macrostructural features are constructed from nanometer-scale building blocks, describing the system across sub-Ångstrom to multi-micrometer length scales.

cond-mat.mtrl-sci↗

arXiv2020

Monolayer Vanadium-doped Tungsten Disulfide: A Room-Temperature Dilute Magnetic Semiconductor

Dilute magnetic semiconductors, achieved through substitutional doping of spin-polarized transition metals into semiconducting systems, enable experimental modulation of spin dynamics in ways that hold great promise for novel magneto-electric or magneto-optical devices, especially for two-dimensional systems such as transition metal dichalcogenides that accentuate interactions and activate valley degrees of freedom. Practical applications of 2D magnetism will likely require room-temperature operation, air stability, and (for magnetic semiconductors) the ability to achieve optimal doping levels without dopant aggregation. Here we describe room-temperature ferromagnetic order obtained in semiconducting vanadium-doped tungsten disulfide monolayers produced by a reliable single-step film sulfidation method across an exceptionally wide range of vanadium concentrations, up to 12 at% with minimal dopant aggregation. These monolayers develop p-type transport as a function of vanadium incorporation and rapidly reach ambipolarity. Ferromagnetism peaks at an intermediate vanadium concentration of a few atomic percent and decreases for higher concentrations, which is consistent with quenching due to orbital hybridization at closer vanadium-vanadium spacings, as supported by transmission electron microscopy, magnetometry and first-principles calculations. Room-temperature two-dimensional dilute magnetic semiconductors provide a new component to expand the functional scope of van der Waals heterostructures and bring semiconducting magnetic 2D heterostructures them into the realm of practical application.

cond-mat.mtrl-sci↗

arXiv2020

Achieving Minimal Heat Conductivity by Ballistic Confinement in Phononic Metalattices

Controlling the thermal conductivity of semiconductors is of practical interest in optimizing the performance of thermoelectric and phononic devices. The insertion of inclusions of nanometer size in a semiconductor is an effective means of achieving such control; it has been proposed that the thermal conductivity of silicon could be reduced to 1 W/m/K using this approach and that a minimum in the heat conductivity would be reached for some optimal size of the inclusions. Yet the practical verification of this design rule has been limited. In this work, we address this question by studying the thermal properties of silicon metalattices that consist of a periodic distribution of spherical inclusions with radii from 7 to 30 nm, embedded into silicon. Experimental measurements confirm that the thermal conductivity of silicon metalattices is as low as 1 W/m/K for silica inclusions, and that this value can be further reduced to 0.16 W/m/K for silicon metalattices with empty pores. A detailed model of ballistic phonon transport suggests that this thermal conductivity is close to the lowest achievable by tuning the radius and spacing of the periodic inhomogeneities. This study is a significant step in elucidating the scaling laws that dictate ballistic heat transport at the nanoscale in silicon and other semiconductors.

cond-mat.mtrl-sci↗

arXiv2019

An Air-Stable and Atomically Thin Graphene/Gallium Superconducting Heterostructure

Two-dimensional layered and atomically thin elemental superconductors may be key ingredients in next-generation quantum technologies, if they can be stabilized and integrated into heterostructured devices under ambient conditions. However, atomically thin elemental superconductors are largely unexplored outside ultra-high vacuum due to rapid oxidation, and even 2D layered superconductors require complex encapsulation strategies to maintain material quality. Here we demonstrate environmentally stable, single-crystal, few-atom-thick superconducting gallium, 2D-Ga, produced by confinement heteroepitaxy (CHet) at the interface of epitaxial graphene (EG) and silicon carbide (SiC). 2D-Ga becomes superconducting at 4 K; this elevation over bulk alpha-Ga (Tc~1 K) is primarily attributed to an increased density of states at the Fermi level as the incipient Ga-Ga dimerization seen in alpha-Ga is suppressed by epitaxy to SiC. We also demonstrate the importance of controlling SiC surface morphology (i.e. step height) and defect-engineering in graphene layers prior to intercalation to achieve large-area uniform 2D-Ga layers with isotropic transport properties. This work demonstrates that unique 2D forms of 3D materials can be stabilized at the EG/SiC interface, which represents a scalable route towards air-stable crystalline 2D superconductors as a potential foundation for next-generation quantum technologies.

cond-mat.supr-con↗

arXiv2019

Imaging the stochastic microstructure and dynamic development of correlations in perpendicular artificial spin ice

We use spatially resolved magneto-optical Kerr microscopy to track the complete microstates of arrays of perpendicular anisotropy nanomagnets during magnetization hysteresis cycles. These measurements allow us to disentangle the intertwined effects of nearest neighbor interaction, disorder, and stochasticity on magnetization switching. We find that the nearest neighbor correlations depend on both interaction strength and disorder. We also find that although the global characteristics of the hysteretic switching are repeatable, the exact microstate sampled is stochastic with the behavior of individual islands varying between nonminally identical runs.

cond-mat.mes-hall↗

arXiv2019

Nonlinear dark-field imaging of 1D defects in monolayer dichalcogenides

Extended defects with one dimensionality smaller than that of the host, such as 2D grain boundaries in 3D materials or 1D grain boundaries in 2D materials, can be particularly damaging since they directly impede the transport of charge, spin or heat, and can introduce a metallic character into otherwise semiconducting systems. Unfortunately, a technique to rapidly and non-destructively image 1D defects in 2D materials is lacking. Scanning transmission electron microscopy (STEM), Raman, photoluminescence and nonlinear optical spectroscopies, are all extremely valuable, but current implementations suffer from low throughput and a destructive nature (STEM) or limitations in their unambiguous sensitivity at the nanoscale. Here we demonstrate that dark-field second harmonic generation (SHG) microscopy can rapidly, efficiently, and non-destructively probe grain boundaries and edges in monolayer dichalcogenides (i.e. MoSe2, MoS2 and WS2). Dark-field SHG efficiently separates the spatial components of the emitted light and exploits interference effects from crystal domains of different orientations to localize grain boundaries and edges as very bright 1D patterns through a Cerenkov-type SHG emission. The frequency dependence of this emission in MoSe2 monolayers is explained in terms of plasmon-enhanced SHG related to the defects metallic character. This new technique for nanometer-scale imaging of the grain structure, domain orientation and localized 1D plasmons in 2D different semiconductors, thus enables more rapid progress towards both applications and fundamental materials discoveries.

cond-mat.mes-hall↗

arXiv2018

Triangular Ising antiferromagnet through a fermionic lens, part 2: information-theoretic aspects of zero-temperature states on cylinders

A classical lattice spin model wrapped on a cylinder is profitably viewed as a chain of rings of spins. From that perspective, mutual information between ring configurations plays much the same role as spin-spin correlation functions in simpler settings. We study zero-temperature states of triangular lattice Ising antiferromagnet (TIAFM) systems from this point of view using a fermionic representation presented in a companion paper (Part 1). On infinite cylinders, ring-to-ring mutual information falls off asymptotically at a rate which decreases smoothly with cylinder circumference, but the end-to-end mutual information for finite cylinders depends strongly on the residue class modulo 3 of the circumference as well as on whether spin periodicity or antiperiodicity is imposed in the circumferential direction. In some cases, the falloff is only as the inverse square of the cylinder length. These features, puzzling within the original spin formulation, are easily understood and calculated within the fermionic formulation.

cond-mat.stat-mech↗

arXiv2018

Strong exciton regulation of Raman scattering in monolayer dichalcogenides

The weakly screened electron-hole interactions in an atomically thin semiconductor not only downshift its excitation spectrum from a quasiparticle one, but also redistribute excitation energies and wavefunction characters with profound effects on diverse modes of material response, including the exciton-phonon scattering processes accessible to resonant Raman measurements. Here we develop a first-principles framework to calculate frequency-dependent resonant Raman intensities that includes excitonic effects and goes beyond the Placzek approximation. We show how excitonic effects in MoS2 strongly regulate Raman scattering amplitudes and thereby explain the puzzling near-absence of resonant Raman response around the A and B excitons (which produce very strong signals in optical absorption), and also the pronounced strength of the resonant Raman response from the C exciton. Furthermore, this efficient perturbative approach reduces the number of GW- BSE calculations from two per Raman mode (in finite displacement) to one for all modes and affords natural extension to higher-order resonant Raman processes.

cond-mat.mes-hall↗

arXiv2017

Communicating through a geometrically frustrated channel

We propose an intuitively appealing formulation of the zero-temperature triangular lattice Ising antiferromagnet (TIAFM) on a cylinder as a model of noninteracting fermions hopping on a ring and evolving in imaginary time with pair annihilation events. Among the features of the model which can then be related to local semi-conservation of particle number are: infinite-range influence of boundary conditions, multiple "zero temperature pure phases" in the infinite-length limit differing in entropy density, sensitivity of the asymptotic rate of decay (with respect to length) of mutual information between end configurations to circumference modulo 3, and even the known power-law falloff of the spin-spin correlator on an infinite plane. The ability of boundary conditions to determine the bulk entropy density enables communication between the two far-separated ends of such a cylinder even when all pair-wise spin-spin correlations between the ends are vanishingly small. In the fermionic language, breakdown of these zero-temperature phenomena at positive temperature is understood as passage of the system into a superconducting phase.

cond-mat.stat-mech↗

arXiv2017

Distinguishing Advective and Powered Motion in Self-Propelled Colloids

Self-powered motion in catalytic colloidal particles provides a compelling example of active matter, i.e. systems that engage in single-particle and collective behavior far from equilibrium. The long-time, long-distance behavior of such systems is of particular interest, since it connects their individual micro-scale behavior to macro-scale phenomena. In such analyses, it is important to distinguish motion due to subtle advective effects -- which also has long time scales and length scales -- from phenomena that derive from intrinsically powered motion. Here, we develop a methodology to analyze the statistical properties of the translational and rotational motions of powered colloids to distinguish, for example, active chemotaxis from passive advection by bulk flow.

cond-mat.soft↗

arXiv2016

Bypassing slip velocity: rotational and translational velocities of autophoretic colloids in terms of surface flux

A standard approach to propulsion velocities of autophoretic colloids with thin interaction layers uses a reciprocity relation applied to the slip velocity. But the surface flux (chemical, electrical, thermal, etc.), which is the source of the field driving the slip is often more accessible. We show how, under conditions of low Reynolds number and a field obeying the Laplace equation in the outer region, the slip velocity can be bypassed in velocity calculations. In a sense, the actual slip velocity and a normal field proportional to the flux density are equivalent for this type of calculation. Using known results for surface traction induced by rotating or translating an inert particle in a quiescent fluid, we derive simple and explicit integral formulas for translational and rotational velocities of arbitrary spheroidal and slender-body autophoretic colloids.

cond-mat.soft↗

arXiv2016

Characterization of switching field distributions in Ising-like magnetic arrays

The switching field distribution within arrays of single-domain ferromagnetic islands incorpo- rates both island-island interactions and quenched disorder in island geometry. Separating these two contributions is important for disentangling the effects of disorder and interactions in the magnetization dynamics of island arrays. Using sub-micron, spatially resolved Kerr imaging in an external magnetic field for islands with perpendicular magnetic anisotropy, we map out the evolution of island arrays during hysteresis loops. Resolving and tracking individual islands across four different lattice types and a range of inter-island spacings, we extract the individual switching fields of every island and thereby determine the relative contributions of interactions and quenched disorder in the arrays. The width of the switching field distribution is well explained by a simple model comprising the sum of an array-independent contribution (interpreted as disorder-induced), and a term proportional to the maximum field the fully polarized array could exert on a single island. We conclude that disorder in these arrays is primarily a single-island property.

cond-mat.mes-hall↗

arXiv2015

Microphysics of Neutron Star Outer Envelopes in the Periodized, Magnetic Thomas-Fermi Model

Static and dynamic properties of low density outer envelopes of neutron stars are calculated within the nonlinear magnetic Thomas-Fermi model, assuming degenerate electrons. A novel domain decomposition enables proper description of lattice symmetry and may be seen as a prototype for the general class of problems involving nonlinear charge screening of periodic, quasi-low-dimensionality structures, e.g. liquid crystals. We describe a scalable implementation of the method using Hypre. Phase velocity of long wavelength transverse phonons is found to be a factor of 5-7 larger than in the corresponding Coulomb crystal model, which could have implications for low temperature phonon-mediated thermal conductivity. Other findings include $c'<0$ elastic instabilities for both bcc and fcc lattices, reminiscent of the situation in some light actinides, and suggestive of a symmetry-lowering transition to a tetragonal or orthorhombic lattice.

astro-ph.SR↗

arXiv2014

Kinematic matrix theory and universalities in self-propellers and active swimmers

We describe an efficient and parsimonious matrix-based theory for studying the ensemble behavior of self-propellers and active swimmers, such as nanomotors or motile bacteria, that are typically studied by differential-equation-based Langevin or Fokker-Planck formalisms. The kinematic effects for elementary processes of motion are incorporated into a matrix, called the "kinematrix", from which we immediately obtain correlators and the mean and variance of angular and position variables (and thus effective diffusivity) by simple matrix algebra. The kinematrix formalism enables us recast the behaviors of a diverse range of self-propellers into a unified form, revealing universalities in their ensemble behavior in terms of new emergent time scales. Active fluctuations and hydrodynamic interactions can be expressed as an additive composition of separate self-propellers.

cond-mat.soft↗