Ultraconfined Plasmons in Atomically Thin Crystalline Silver Nanostructures.

The ability to confine light down to atomic scales is critical for the development of applications in optoelectronics and optical sensing as well as for the exploration of nanoscale quantum phenomena. Plasmons in metallic nanostructures with just a few atomic layers in thickness can achieve this type of confinement, although fabrication imperfections down to the subnanometer scale hinder actual developments. Here, narrow plasmons are demonstrated in atomically thin crystalline silver nanostructures fabricated by prepatterning silicon substrates and epitaxially depositing silver films of just a few atomic layers in thickness. Specifically, a silicon wafer is lithographically patterned to introduce on-demand lateral shapes, chemically process the sample to obtain an atomically flat silicon surface, and epitaxially deposit silver to obtain ultrathin crystalline metal films with the designated morphologies. Structures fabricated by following this procedure allow for an unprecedented control over optical field confinement in the near-infrared spectral region, which is here illustrated by the observation of fundamental and higher-order plasmons featuring extreme spatial confinement and high-quality factors that reflect the crystallinity of the metal. The present study constitutes a substantial improvement in the degree of spatial confinement and quality factor that should facilitate the design and exploitation of atomic-scale nanoplasmonic devices for optoelectronics, sensing, and quantum-physics applications.

Unveiling the Coupling of Single Metallic Nanoparticles to Whispering-Gallery Microcavities.

Whispering-gallery mode resonators host multiple trapped narrow-band circulating optical resonances that find applications in quantum electrodynamics, optomechanics, and sensing. However, the spherical symmetry and low field leakage of dielectric microspheres make it difficult to probe their high-quality optical modes using far-field radiation. Even so, local field enhancement from metallic nanoparticles (MNPs) coupled to the resonators can interface the optical far field and the bounded cavity modes. In this work, we study the interaction between whispering-gallery modes and MNP surface plasmons with nanometric spatial resolution by using electron-beam spectroscopy with a scanning transmission electron microscope. We show that gallery modes are induced over a selective spectral range of the nanoparticle plasmons, and additionally, their polarization can be controlled by the induced dipole moment of the MNP. Our study demonstrates a viable mechanism to effectively excite high-quality-factor whispering-gallery modes and holds potential for applications in optical sensing and light manipulation.

Can Copper Nanostructures Sustain High-Quality Plasmons?

Silver, king among plasmonic materials, features low inelastic absorption in the visible-infrared (vis-IR) spectral region compared to other metals. In contrast, copper is commonly regarded as too lossy for actual applications. Here, we demonstrate vis-IR plasmons with quality factors >60 in long copper nanowires (NWs), as determined by electron energy-loss spectroscopy. We explain this result by noticing that most of the electromagnetic energy in these plasmons lies outside the metal, thus becoming less sensitive to inelastic absorption. Measurements for silver and copper NWs of different diameters allow us to elucidate the relative importance of radiative and nonradiative losses in plasmons spanning a wide spectral range down to <20 meV. Thermal population of such low-energy modes becomes significant and generates electron energy gains associated with plasmon absorption, rendering an experimental determination of the NW temperature. Copper is therefore emerging as an attractive, cheap, abundant material platform for high-quality plasmonics in elongated nanostructures.

Tailored Nanoscale Plasmon-Enhanced Vibrational Electron Spectroscopy.

Atomic vibrations and phonons are an excellent source of information on nanomaterials that we can access through a variety of methods including Raman scattering, infrared spectroscopy, and electron energy-loss spectroscopy (EELS). In the presence of a plasmon local field, vibrations are strongly modified and, in particular, their dipolar strengths are highly enhanced, thus rendering Raman scattering and infrared spectroscopy extremely sensitive techniques. Here, we experimentally demonstrate that the interaction between a relativistic electron and vibrational modes in nanostructures is fundamentally modified in the presence of plasmons. We finely tune the energy of surface plasmons in metallic nanowires in the vicinity of hexagonal boron nitride, making it possible to monitor and disentangle both strong phonon-plasmon coupling and plasmon-driven phonon enhancement at the nanometer scale. Because of the near-field character of the electron beam-phonon interaction, optically inactive phonon modes are also observed. Besides increasing our understanding of phonon physics, our results hold great potential for investigating sensing mechanisms and chemistry in complex nanomaterials down to the molecular level.

Plasmonics in Atomically Thin Crystalline Silver Films.

Light-matter interaction at the atomic scale rules fundamental phenomena such as photoemission and lasing while enabling basic everyday technologies, including photovoltaics and optical communications. In this context, plasmons, the collective electron oscillations in conducting materials, are important because they allow the manipulation of optical fields at the nanoscale. The advent of graphene and other two-dimensional crystals has pushed plasmons down to genuinely atomic dimensions, displaying appealing properties such as a large electrical tunability. However, plasmons in these materials are either too broad or lying at low frequencies, well below the technologically relevant near-infrared regime. Here, we demonstrate sharp near-infrared plasmons in lithographically patterned wafer-scale atomically thin silver crystalline films. Our measured optical spectra reveal narrow plasmons (quality factor of ∼4), further supported by a low sheet resistance comparable to bulk metal in few-atomic-layer silver films down to seven Ag(111) monolayers. Good crystal quality and plasmon narrowness are obtained despite the addition of a thin passivating dielectric, which renders our samples resilient to ambient conditions. The observation of spectrally sharp and strongly confined plasmons in atomically thin silver holds great potential for electro-optical modulation and optical sensing applications.

Lasing and Amplification from Two-Dimensional Atom Arrays.

We explore the ability of two-dimensional periodic atom arrays to produce light amplification and generate laser emission when gain is introduced through external optical pumping. Specifically, we predict that lasing can take place for arbitrarily weak atomic scatterers assisted by cooperative interaction among atoms in a 2D lattice. We base this conclusion on analytical theory for three-level scatterers, which additionally reveals a rich interplay between lattice and atomic resonances. Our results provide a general background to understand light amplification and lasing in periodic atomic arrays, with promising applications in the generation, manipulation, and control of coherent photon states at the nanoscale.

An antireflection transparent conductor with ultralow optical loss (<2 %) and electrical resistance (<6 Ω sq-1).

Transparent conductors are essential in many optoelectronic devices, such as displays, smart windows, light-emitting diodes and solar cells. Here we demonstrate a transparent conductor with optical loss of ∼1.6%, that is, even lower than that of single-layer graphene (2.3%), and transmission higher than 98% over the visible wavelength range. This was possible by an optimized antireflection design consisting in applying Al-doped ZnO and TiO2 layers with precise thicknesses to a highly conductive Ag ultrathin film. The proposed multilayer structure also possesses a low electrical resistance (5.75 Ω sq-1), a figure of merit four times larger than that of indium tin oxide, the most widely used transparent conductor today, and, contrary to it, is mechanically flexible and room temperature deposited. To assess the application potentials, transparent shielding of radiofrequency and microwave interference signals with ∼30 dB attenuation up to 18 GHz was achieved.

Ultrathin transparent conductive polyimide foil embedding silver nanowires.

Metallic nanowires are among the most promising transparent conductor (TC) alternatives to widely used indium tin oxide (ITO) because of their excellent trade-off between electrical and optical properties, together with their mechanical flexibility. However, they tend to suffer from relatively large surface roughness, instability against oxidation, and poor adhesion to the substrate. Embedding in a suitable material can overcome these shortcomings. Here we propose and demonstrate a new TC comprising silver nanowires (AgNWs) in an ultrathin polyimide foil that presents an optical transmission in the visible larger than ITO (>90%), while maintaining similar electrical sheet resistance (15 ohm/sq). The polyimide protects the Ag against environmental agents such as oxygen and water and, thanks to its deformability and very small thickness (5 µm), provides an ideal mechanical support to the NW's network, in this way ensuring extreme flexibility (bending radius as small as at least 1 mm) and straightforwardly removing any adhesion issue. The initial AgNWs' roughness is also reduced by a factor of about 15, reaching RMS values as low as 2.4 nm, suitable for the majority of applications. All these properties together with the simple fabrication technique based on all-solution processing put the developed TC in a competitive position as a lightweight, mechanically flexible and inexpensive substrate for consumer electronic and optoelectronic devices.

Hybrid transparent conductive film on flexible glass formed by hot-pressing graphene on a silver nanowire mesh.

Polycrystalline graphene and metallic nanowires (NWs) have been proposed to replace indium tin oxide (ITO), the most widely used transparent electrode (TE) film on the market. However, the trade-off between optical transparency (Topt) and electrical sheet resistance (Rs) of these materials taken alone makes them difficult to compete with ITO. In this paper, we show that, by hot-press transfer of graphene monolayer on Ag NWs, the resulting combined structure benefits from the synergy of the two materials, giving a Topt-Rs trade-off better than that expected by simply adding the single material contributions Ag NWs bridge any interruption in transferred graphene, while graphene lowers the contact resistance among neighboring NWs and provides local conductivity in the uncovered regions in-between NWs. The hot-pressing not only allows graphene transfer but also compacts the NWs joints, thus reducing contact resistance. The dependence on the initial NW concentration of the effects produced by the hot press process on its own and the graphene transfer using hot press was investigated and indicates that a low concentration is more suitable for the proposed geometry. A TE film with Topt of 90% and Rs of 14 Ω/sq is demonstrated, also on a flexible glass substrate about 140 µm thick, a very attractive platform for efficient flexible electronic and photonic devices.