Modulating Polarization in Second Harmonic Generation through Symmetry Evolution in Plasmonic Lattices.

We report a strategy for preparing cost-effective plasmonic square lattices with tunable unit structures of circles, crosses, and circle-cross pairs on a centimeter scale. The asymmetrical electromagnetic (EM) field distribution of the lattice enhances second harmonic generation (SHG) under oblique incidence. The SHG signals are progressively strengthened as the unit symmetry decreases from C∞v (circle) to C4v (cross) to C2v (circle-cross pair). The peak SHG signal is observed from the plasmonic lattice with a circle-cross pair, showcasing a conversion efficiency of 1.0 × 10-2, which is a 7.3-fold enhancement relative to the dielectric lattice comprised of circle units. This notably high conversion efficiency of SHG is on par with that of phase-matched bulk nanostructures under normal incidence, benefiting from the Bloch-surface plasmon polariton (Bloch-SPP) modes associated with the distribution of the photonic local density of states (LDOS). Furthermore, the SHG emission exhibits distinctive directional and polarization characteristics as the unit symmetry is reduced. This work offers valuable insights into a structural symmetry-dependent SHG in plasmonic lattices and the way forward for the design of functional nonlinear plasmonic devices.

Bloch-Surface Plasmon Polariton Enhanced Amplified and Directional Spontaneous Emission from Plasmonic Hexagonal Nanohole Array.

The light-matter interactions at nanoscale can be enhanced by Bloch-surface plasmon polariton (Bloch-SPP) on the plasmonic lattice. An Ag nanohole array in hexagonal arrangement served as an optical cavity to realize the directional and polarized amplified spontaneous emission (ASE) of R6G. A 100-fold enhanced ASE was observed at 15° emission angle under TM polarization when the pump power density exceeded the threshold of 198 W/cm2 based on the degenerated high state density modes. Moreover, a specific polarization dependence of ASE was modulated by the Bloch-SPP modes, and the degree of polarization was enhanced from 1.3 to 2.1 when the pump power density exceeded the threshold of ASE. This work clarifies the interaction between the gain media and plasmonic systems, which lays a foundation for the plasmonic device designing.

Directional amplified spontaneous emissions from Ag nanohole array with high diffraction orders.

Surface plasmon excitations in metallic hole arrays have been extensively studied in the context of light-matter interaction, since the generated Bloch surface plasmon polariton (Bloch-SPP) exhibits unique properties of nanoscale light confinement, near-field enhancements, and long-range metal surface propagation. In this work, we experimentally demonstrate a plasmonic device that exhibits highly directional emission in visible light; using Ag film with a thickness of 100 nm deposited on a subwavelength porous alumina array as a plasmonic cavity, four-level rhodamine 6G (R6G) is selected as the gain material. It is suggested that a Bloch-SPP with high diffraction orders on a Ag nanohole array can generate a strong local electric field and a high Purcell factor at a nanohole edge. Moreover, directional five-fold enhanced amplified spontaneous emission (ASE) with polarization dependence is observed under a low threshold of 199.9 W/cm2 in the visible light region, which comes from the optical feedback provided by the 2D periodic nanohole array. This work opens up a wide range of applications for real-time tunable wavelength, controlled multimode laser, fluorescence detection, etc.

Off-Angle Amplified Spontaneous Emission of Upconversion Nanoparticles by Propagating Lattice Plasmons.

Lanthanide-doped upconversion nanoparticles (UCNPs) are appealing for light emitting applications because their high internal conversion efficiency facilitates the amplified spontaneous emission (ASE) under low pumping. In addition, the integration of photonic crystals and microcavities with optical quantum emitters provides a unique opportunity to manipulate their light emissions and generate coherent light sources for quantum photonics. Here, this work describes a two-dimensional (2D) plasmonic lattice of Al nanocone array (Al NCA), which can confine the light at the tip. Light confinement by the enhancement effect supports narrow linewidth resonances as optical feedback for the ASE of UCNPs doped with sensitizer Yb3+ ions/emitter Ho3+ ions/relaxator Ce3+ ions. An off-angle ASE with an enhancement of 19-fold from UCNPs is achieved by propagating lattice plasmons from the Al NCA. Moreover, this upconverting ASE can be switched on or off by adjusting the polarization state of the incident pump light, and photonic band engineering can be used to manipulate it intentionally. This composite plasmonic system opens prospective applications for the ASE as directional emission, real-time tunable wavelengths, controlled multimode lasing, and optical switches.

Strong coupling between monolayer quantum emitter WS2 and degenerate/non-degenerate surface lattice resonances.

Strong light-matter coupling manifested by Rabi splitting has drawn considerable interest owing to its fundamental significance for impressive interaction enhancement in the fields of ultrafast active plasmonic devices and quantum information. In this paper, we investigate the coherent optical properties of a plasmonic system consisting of periodic metal nanoparticle arrays covered by a WS2 thin film of atomic layer thickness. The coupling factor, energy splitting, and temporal dynamics of this coherent coupling phenomenon are quantitatively revealed by finite-difference time-domain (FDTD) simulation and a full quantum mechanical model proves that the exciton behavior of the fermionic quantum emitter WS2 is carefully modulated by bosonic surface lattice resonances. This work may pave the way for coherent modulation of polariton and plasmon devices and can potentially open up diverse exciting possibilities like nanoscale light sources, single-photon emitters, and all-optical transistors.

Wafer-scale plasmonic metal-dielectric-metal structural color featuring high saturation and low angular dependence.

Structural color has been studied through various methods due to its distinguished features of stability, durability, high information storage density and high integration. However, the artificial structural color samples do not exhibit superior performance in color saturation and low angular dependence. Here, we present an approach to acquire additive reflective color based on a metal-dielectric-metal (MDM) stack. The upper layer composed of Ag particles is perforated in a hexagonal arrangement which profits from the dielectric anodic aluminium oxide (AAO) membrane. The size and shape of the Ag particles are getting inhomogeneous as the deposition thickness of the upper layer increasing, which expands the desired absorption range of surface plasmons. The residual non-anodized Al foil serves as a highly reflective substrate for efficient color presenting through the thin-film interference in this plasmonic MDM system. As a result, the color gamut area of this MDM stack is extended 8 times in CIE chromaticity coordinates. Finally, a wafer-scale (diameter of 83 mm) badge of Harbin Engineering University (HEU) with highly saturated colors and a pattern characterized with low angle-dependent property (up to 60°) are presented, which exhibit promising prospects in commercial coloring and imaging.

Evolution of High Symmetry Points of Photonic Alumina Superlattices in a Lithography-Free Approach.

Ceaselessly increasing demands for elaborate nanostructures prompt advanced structure fabrication with good practicability, especially, subwavelength ordered structures in simple lattices even in superlattices over a large area, namely, large-scale photonic lattices, in which lattice arrangement, geometry, and components of unit cells are key factors for their macroscopic optical properties. Moreover, exciting properties always occur at high symmetry points of the lattice; therefore, straightforward modulation of symmetry points over a large area is very important for the investigation and application of photonic lattices. Here, this work establishes a lithography-free approach of undervoltage oxidation (UVO) for regulating high symmetry points in the reciprocal space of a dielectric alumina superlattice. Embedding subunit cells at high symmetry points Γ (M) result in the degenerate energy changing from 1.34 eV (924.6 nm) to 1.87 eV (662.6 nm) under normal excitation at the Γ point, and the degeneracy lifting under off-normal excitation along the Γ-X high symmetry orientation. Furthermore, systematic characterizations of the alumina membrane are presented to learn its dynamic evolution of the morphology on a centimeter scale, and the pore array changes from a hierarchical period to a form of hexagonal close packing, especially at Γ and M points of the square lattice. Therefore, the reported lithography-free alumina-based nanofabrication offers an ability for varying the spatial structure at high symmetry points of photonic lattices, which is of great significance in the fields of nanomanufacturing and has great potential to bring about preferable performances in nanodevices.