Large-Area Intercalated Two-Dimensional Pb/Graphene Heterostructure as a Platform for Generating Spin-Orbit Torque.

A scalable platform to synthesize ultrathin heavy metals may enable high-efficiency charge-to-spin conversion for next-generation spintronics. Here, we report the synthesis of air-stable, epitaxially registered monolayer Pb underneath graphene on SiC (0001) by confinement heteroepitaxy (CHet). Diffraction, spectroscopy, and microscopy reveal that CHet-based Pb intercalation predominantly exhibits a mottled hexagonal superstructure due to an ordered network of Frenkel-Kontorova-like domain walls.

Prediction of a Novel Electromechanical Response in Polar Polymers with Rigid Backbones: Contrasting Furan-Derived Nanothreads to Poly(Vinylidene Fluoride).

furan nanothreads have all oxygen atoms arranged on one side of the thread backbone; these polar threads present intriguing opportunities in electromechanical response owing to their rigid ladder-like backbone. We retrained a C/H/O reactive force field to simulate their response to external electric field for both end-anchored individual threads and bulk nanothread crystals, contrasting the results to those for poly(vinylidene fluoride) (PVDF) polymer. Whereas the field induces a length-independent torque in PVDF through backbone rotation about σ bonds, furan-derived nanothreads generate a length-dependent torque by progressively twisting their rigid backbone.

Emergence of inertia in the low-Reynolds regime of self-diffusiophoretic motion.

For isotropic swimming particles driven by self-diffusiophoresis at zero Reynolds number (where particle velocity responds instantaneously to applied force), the diffusive timescale of emitted solute can produce an emergent quasi-inertial behavior. These particles can orbit in a central potential and reorient under second-order dynamics, not the first-order dynamics of classical zero-Reynolds motion. They are described by a simple effective model that embeds their history-dependent behavior as an effective inertia, this being the most primitive expression of memory.

Strain-Induced 2H to 1T' Phase Transition in Suspended MoTe Using Electric Double Layer Gating.

MoTe can be converted from the semiconducting (2H) phase to the semimetallic (1T') phase by several stimuli including heat, electrochemical doping, and strain. This type of phase transition, if reversible and gate-controlled, could be useful for low-power memory and logic. In this work, a gate-controlled and fully reversible 2H to 1T' phase transition is demonstrated via strain in few-layer suspended MoTe field effect transistors.

Step engineering for nucleation and domain orientation control in WSe epitaxy on c-plane sapphire.

Epitaxial growth of two-dimensional transition metal dichalcogenides on sapphire has emerged as a promising route to wafer-scale single-crystal films. Steps on the sapphire act as sites for transition metal dichalcogenide nucleation and can impart a preferred domain orientation, resulting in a substantial reduction in mirror twins. Here we demonstrate control of both the nucleation site and unidirectional growth direction of WSe on c-plane sapphire by metal-organic chemical vapour deposition.

Three-dimensional topological magnetic monopoles and their interactions in a ferromagnetic meta-lattice.

Topological magnetic monopoles (TMMs), also known as hedgehogs or Bloch points, are three-dimensional (3D) non-local spin textures that are robust to thermal and quantum fluctuations due to the topology protection. Although TMMs have been observed in skyrmion lattices, spinor Bose-Einstein condensates, chiral magnets, vortex rings and vortex cores, it has been difficult to directly measure the 3D magnetization vector field of TMMs and probe their interactions at the nanoscale. Here we report the creation of 138 stable TMMs at the specific sites of a ferromagnetic meta-lattice at room temperature.

Nonstoichiometric Salt Intercalation as a Means to Stabilize Alkali Doping of 2D Materials.

Although doping with alkali atoms is a powerful technique for introducing charge carriers into physical systems, the resulting charge-transfer systems are generally not air stable. Here we describe computationally a strategy towards increasing the stability of alkali-doped materials that employs stoichiometrically unbalanced salt crystals with excess cations (which could be deposited during, e.g.

Photochemically Mediated Polymerization of Molecular Furan and Pyridine: Synthesis of Nanothreads at Reduced Pressures.

Nanothreads are emerging one-dimensional sp-hybridized materials with high predicted tensile strength and a tunable band gap. They can be synthesized by compressing aromatic or nonaromatic small molecules to pressures ranging from 15-30 GPa. Recently, new avenues are being sought that reduce the pressure required to afford nanothreads; the focus has been placed on the polymerization of molecules with reduced aromaticity, favorable stacking, and/or the use of higher reaction temperatures.

Theory of Borazine-Derived Nanothreads: Enumeration, Reaction Pathways, and Piezoelectricity.

Nanothreads are one-dimensional macromolecules formed by pressure-induced polymerization along stacks of multiply unsaturated (or highly strained) molecules such as benzene (or cubane). Borazine is isoelectronic to benzene yet with substantial bond polarity, thus motivating a theoretical examination of borazine-derived nanothreads with degrees of saturation of 2, 4, and 6 (defined as the number of four-coordinated boron and nitrogen atoms per borazine formula unit). The energy increases upon going from molecular borazine to degree-2 borazine-derived threads and then decreases for degree-4 and degree-6 nanothreads as more σ bonds are formed.

Confined Monolayer Ag As a Large Gap 2D Semiconductor and Its Momentum Resolved Excited States.

2D materials have intriguing quantum phenomena that are distinctively different from their bulk counterparts. Recently, epitaxially synthesized wafer-scale 2D metals, composed of elemental atoms, are attracting attention not only for their potential applications but also for exotic quantum effects such as superconductivity. By mapping momentum-resolved electronic states using time-resolved and angle-resolved photoemission spectroscopy (ARPES), we reveal that monolayer Ag confined between bilayer graphene and SiC is a large gap (>1 eV) 2D semiconductor, consistent with ab initio GW calculations.

Shape Entropy of a Reconfigurable Ising Surface.

Disclinations in a 2D sheet create regions of Gaussian curvature whose inversion produces a reconfigurable surface with many distinct metastable shapes, as shown by molecular dynamics of a disclinated graphene monolayer. This material has a near-Gaussian "density of shapes" and an effectively antiferromagnetic interaction between adjacent cones. A∼10  nm patch has hundreds of distinct metastable shapes with tunable stability and topography on the size scale of biomolecules.

ZrTe/CrTe: an epitaxial van der Waals platform for spintronics.

The rapid discovery of two-dimensional (2D) van der Waals (vdW) quantum materials has led to heterostructures that integrate diverse quantum functionalities such as topological phases, magnetism, and superconductivity. In this context, the epitaxial synthesis of vdW heterostructures with well-controlled interfaces is an attractive route towards wafer-scale platforms for systematically exploring fundamental properties and fashioning proof-of-concept devices. Here, we use molecular beam epitaxy to synthesize a vdW heterostructure that interfaces two material systems of contemporary interest: a 2D ferromagnet (1T-CrTe) and a topological semimetal (ZrTe).

Mutual information and breakdown of the Perron-Frobenius scenario in zero-temperature triangular Ising antiferromagnets on cylinders.

A nominally two-dimensional spin model wrapped onto a cylinder can profitably be viewed, especially for long cylinders, as a one-dimensional chain. Each site of such a chain is a ring of spins with a complex state space. Traditional correlation functions are inadequate for the study of correlations in such a system and need to be replaced with something like mutual information.

Theoretical Studies of Furan and Thiophene Nanothreads: Structures, Cycloaddition Barriers, and Activation Volumes.

This theoretical study examines the formation, structure, and stability of two of the most ordered nanothreads produced yet, those derived from furan and thiophene. The energetic consequences and activation barriers of the first two steps of oligomerization via a Diels-Alder mechanism were examined. The ca.

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.

Tunable 2D Group-III Metal Alloys.

Chemically stable quantum-confined 2D metals are of interest in next-generation nanoscale quantum devices. Bottom-up design and synthesis of such metals could enable the creation of materials with tailored, on-demand, electronic and optical properties for applications that utilize tunable plasmonic coupling, optical nonlinearity, epsilon-near-zero behavior, or wavelength-specific light trapping. In this work, it is demonstrated that the electronic, superconducting, and optical properties of air-stable 2D metals can be controllably tuned by the formation of alloys.

Illuminating Invisible Grain Boundaries in Coalesced Single-Orientation WS 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 ReaxFF reactive force field-based molecular dynamics simulations, we provide insights into WS crystal growth mechanisms, providing a direct link between synthetic conditions and microstructure.

Perfect and Defective C-Furan-Derived Nanothreads from Modest-Pressure Synthesis Analyzed by C NMR.

The molecular structure of nanothreads produced by the slow compression of C-furan was studied by advanced solid-state NMR. Spectral editing showed that >95% of carbon atoms were bonded to one hydrogen (C-H) and that there were 2-4% CH, 0.6% C═O, and <0.

'Sacrificial' supramolecular assembly and pressure-induced polymerization: toward sequence-defined functionalized nanothreads.

Limited supramolecular strategies have been utilized to synthesize sequence-defined polymers, despite the prominence of noncovalent interactions in materials design. Herein, we illustrate the utility of 'sacrificial' aryl-perfluoroaryl supramolecular synthons to synthesize sp-hybridized nanothreads from sp-enriched reactants. Our strategy features A-B reactant pairs in the form of a phenol:pentafluorophenol co-crystal that is preorganized for an electronically-biased and sequence-defined polymerization.

Scalable Synthesis of Crystalline One-Dimensional Carbon Nanothreads through Modest-Pressure Polymerization of Furan.

Carbon nanothreads, which are one-dimensional sp-rich polymers, combine high tensile strength with flexibility owing to subnanometer widths and diamond-like cores. These extended carbon solids are constructed through pressure-induced polymerization of sp molecules such as benzene. Whereas a few examples of carbon nanothreads have been reported, the need for high onset pressures (≥17 GPa) to synthesize them precludes scalability and limits scope.

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

Dilute magnetic semiconductors (DMS), 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 (2D) 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, 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, is described.

Unexpected Near-Infrared to Visible Nonlinear Optical Properties from 2-D Polar Metals.

Near-infrared-to-visible second harmonic generation from air-stable two-dimensional polar gallium and indium metals is described. The photonic properties of 2D metals, including the largest second-order susceptibilities reported for metals (approaching 10 nm/V), are determined by the atomic-level structure and bonding of two-to-three-atom-thick crystalline films. The bond character evolved from covalent to metallic over a few atomic layers, changing the out-of-plane metal-metal bond distances by approximately ten percent (0.

Nondestructive Measurements of the Mechanical and Structural Properties of Nanostructured Metalattices.

Metalattices are artificial 3D solids, periodic on sub-100 nm length scales, that enable the functional properties of materials to be tuned. However, because of their complex structure, predicting and characterizing their properties is challenging. Here we demonstrate the first nondestructive measurements of the mechanical and structural properties of metalattices with feature sizes down to 14 nm.

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 experimental verification of this design rule has been limited.

Atomically thin half-van der Waals metals enabled by confinement heteroepitaxy.

Atomically thin two-dimensional (2D) metals may be key ingredients in next-generation quantum and optoelectronic devices. However, 2D metals must be stabilized against environmental degradation and integrated into heterostructure devices at the wafer scale. The high-energy interface between silicon carbide and epitaxial graphene provides an intriguing framework for stabilizing a diverse range of 2D metals.