Topological Magnetic-Spin Textures in Two-Dimensional van der Waals Cr2Ge2Te6.

Two-dimensional (2D) van der Waals (vdW) materials show a range of profound physical properties that can be tailored through their incorporation in heterostructures and manipulated with external forces. The recent discovery of long-range ferromagnetic order down to atomic layers provides an additional degree of freedom in engineering 2D materials and their heterostructure devices for spintronics, valleytronics, and magnetic tunnel junction switches. Here, using direct imaging by cryo-Lorentz transmission electron microscopy we show that topologically nontrivial magnetic-spin states, skyrmionic bubbles, can be realized in exfoliated insulating 2D vdW Cr2Ge2Te6. Due to the competition between dipolar interactions and uniaxial magnetic anisotropy, hexagonally packed nanoscale bubble lattices emerge by field cooling with magnetic field applied along the out-of-plane direction. Despite a range of topological spin textures in stripe domains arising due to pair formation and annihilation of Bloch lines, bubble lattices with single chirality are prevalent. Our observation of topologically nontrivial homochiral skyrmionic bubbles in exfoliated vdW materials provides a new avenue for novel quantum states in atomically thin insulators for magneto-electronic and quantum devices.

Vivid, full-color aluminum plasmonic pixels.

Aluminum is abundant, low in cost, compatible with complementary metal-oxide semiconductor manufacturing methods, and capable of supporting tunable plasmon resonance structures that span the entire visible spectrum. However, the use of Al for color displays has been limited by its intrinsically broad spectral features. Here we show that vivid, highly polarized, and broadly tunable color pixels can be produced from periodic patterns of oriented Al nanorods. Whereas the nanorod longitudinal plasmon resonance is largely responsible for pixel color, far-field diffractive coupling is used to narrow the plasmon linewidth, enabling monochromatic coloration and significantly enhancing the far-field scattering intensity of the individual nanorod elements. The bright coloration can be observed with p-polarized white light excitation, consistent with the use of this approach in display devices. The resulting color pixels are constructed with a simple design, are compatible with scalable fabrication methods, and provide contrast ratios exceeding 100:1.

Aluminum nanocrystals.

We demonstrate the facile synthesis of high purity aluminum nanocrystals over a range of controlled sizes from 70 to 220 nm diameter with size control achieved through a simple modification of solvent ratios in the reaction solution. The monodisperse, icosahedral, and trigonal bipyramidal nanocrystals are air-stable for weeks, due to the formation of a 2-4 nm thick passivating oxide layer on their surfaces. We show that the nanocrystals support size-dependent ultraviolet and visible plasmon modes, providing a far more sustainable alternative to gold and silver nanoparticles currently in widespread use.

Thermoplasmonics: quantifying plasmonic heating in single nanowires.

Plasmonic absorption of light can lead to significant local heating in metallic nanostructures, an effect that defines the subfield of thermoplasmonics and has been leveraged in diverse applications from biomedical technology to optoelectronics. Quantitatively characterizing the resulting local temperature increase can be very challenging in isolated nanostructures. By measuring the optically induced change in resistance of metal nanowires with a transverse plasmon mode, we quantitatively determine the temperature increase in single nanostructures with the dependence on incident polarization clearly revealing the plasmonic heating mechanism. Computational modeling explains the resonant and nonresonant contributions to the optical heating and the dominant pathways for thermal transport. These results, obtained by combining electronic and optical measurements, place a bound on the role of optical heating in prior experiments and suggest design guidelines for engineered structures meant to leverage such effects.

Fluorescence enhancement of molecules inside a gold nanomatryoshka.

Metallic nanoparticles exhibiting plasmonic Fano resonances can provide large enhancements of their internal electric near field. Here we show that nanomatryoshkas, nanoparticles consisting of an Au core, an interstitial nanoscale SiO2 layer, and an Au shell layer, can selectively provide either a strong enhancement or a quenching of the spontaneous emission of fluorophores dispersed within their internal dielectric layer. This behavior can be understood by taking into account the near-field enhancement induced by the Fano resonance of the nanomatryoshka, which is responsible for enhanced absorption of the fluorophores incorporated into the nanocomplex. The combination of compact size and enhanced light emission with internal encapsulation of the fluorophores for increased biocompatibility suggests outstanding potential for this type of nanoparticle complex in biomedical applications.

Orienting nanoantennas in three dimensions to control light scattering across a dielectric interface.

The light scattering properties of hemispherical resonant nanoantennas can be used to redirect normal incidence light to propagate within a thin film or thin film-based device, such as a solar cell, for enhanced efficiency. While planar nanoantennas are typically fabricated as simple nanoparticles or nanostructures in the film plane, here we show that a hemispherical nanoantenna with its symmetry axis tilted out of the plane accomplishes this task with far greater efficacy. The amount of light scattered into an underlying dielectric by the electric and magnetic dipole response of oriented nanocups can be more than three times that achieved using symmetric antenna structures.

Dark plasmons in hot spot generation and polarization in interelectrode nanoscale junctions.

Nanoscale gaps between adjacent metallic nanostructures give rise to extraordinarily large field enhancements, known as "hot spots", upon illumination. Incident light with the electric field polarized across the gap (along the interparticle axis) is generally known to induce the strongest surface enhanced Raman spectroscopy (SERS) enhancements. However, here we show that, for a nanogap located within a nanowire linking extended Au electrodes, the greatest enhancement and resulting SERS emission occurs when the electric field of the incident light is polarized along the gap (transverse to the interelectrode axis). This surprising and counterintuitive polarization dependence results from a strong dipolar plasmon mode that resonates transversely across the nanowire, coupling with dark multipolar modes arising from subtle intrinsic asymmetries in the nanogap. These modes give rise to highly reproducible SERS enhancements at least an order of magnitude larger than the longitudinal modes in these structures.

Embedding plasmonic nanostructure diodes enhances hot electron emission.

When plasmonic nanostructures serve as the metallic counterpart of a metal-semiconductor Schottky interface, hot electrons due to plasmon decay are emitted across the Schottky barrier, generating measurable photocurrents in the semiconductor. When the plasmonic nanostructure is atop the semiconductor, only a small percentage of hot electrons are excited with a wavevector permitting transport across the Schottky barrier. Here we show that embedding plasmonic structures into the semiconductor substantially increases hot electron emission. Responsivities increase by 25× over planar diodes for embedding depths as small as 5 nm. The vertical Schottky barriers created by this geometry make the plasmon-induced hot electron process the dominant contributor to photocurrent in plasmonic nanostructure-diode-based devices.

Three-dimensional plasmonic nanoclusters.

Assembling nanoparticles into well-defined structures is an important way to create and tailor the optical properties of materials. Most advances in metamaterials research to date have been based on structures fabricated in two-dimensional planar geometries. Here, we show an efficient method for assembling noble metal nanoparticles into stable, three-dimensional (3-D) clusters, whose optical properties can be highly sensitive or remarkably independent of cluster orientation, depending on particle number and cluster geometry. Some of the clusters, such as tetrahedra and icosahedra, could serve as the optical kernels for metafluids, imparting metamaterial optical properties into disordered media such as liquids, glasses, or plastics, free from the requirement of nanostructure orientation.

Designing and deconstructing the Fano lineshape in plasmonic nanoclusters.

By varying the relative dimensions of the central and peripheral disks of a plasmonic nanocluster, the depth of its Fano resonance can be systematically modified; spectral windows where the scattering cross section of the nanocluster is negligible can be obtained. In contrast, electron-beam excitation of the plasmon modes at specific locations within the nanocluster yields cathodoluminescence spectra with no Fano resonance. By examining the selection rules for plasmon excitation in the context of a coupled oscillator picture, we provide an intuitive explanation of this behavior based on the plasmon modes observed for optical and electron-beam excitation in this family of nanostructures.