Going Green with Nanophotonics Plasmons are optically induced collective electronic excitations tightly confined to the surface of a metal, with silver being the metal of choice. The subwavelength confinement offers the opportunity to shrink optoelectronic circuits to the nanometer scale. However, scattering processes within the metal lead to losses. Lu et al. (p. 450 ) developed a process to produce atomically smooth layers of silver, epitaxially grown on silicon substrates. A cavity in the silver layer is capped with a SiO insulating layer and an AlGaN nanorod was used to produce a low-threshold emission at green wavelengths.

Quantitative surface enhanced Raman spectroscopy (SERS) requires precise control of Raman enhancement factor and detection uniformity across the SERS substrate. Here, we show that alkanethiolate ligand-regulated silver (Ag) nanoparticle films can be used to achieve quantitative SERS measurements down to the single-molecule level. The two-dimensional hexagonal close-packed superlattices of Ag nanoparticles formed in these films allow for SERS detection over a large area with excellent uniformity and high Raman enhancement factor. In particular, the SERS signal from the thiolate ligands on Ag nanoparticle surfaces can be utilized as a stable internal calibration standard for reproducible quantitative measurements. We demonstrate the capability of quantitative SERS by measuring the areal densities of crystal violet molecules embedded in an ultrathin spin-on-glass detection "hot zone", which is a planar and uniformly enhanced region several nanometers above the Ag nanoparticles. The Raman measurement results exhibit a linear response over a wide dynamic range of analyte concentration.

We report on the self-assembly of large-area, highly ordered 2D superlattices of alkanethiolate-stabilized gold nanoparticles ( approximately 10.5 nm in core diameter) onto quartz substrates with varying lattice constants, which can be controlled by the alkyl chain lengths, ranging from C12 (1-dodecanethiolate), C14 (1-tetradecanethiolate), C16 (1-hexadecanethiolate), to C18 (1-octadecanethiolate). These 2D nanoparticle superlattices exhibit strong collective surface plasmon resonance that is tunable via the near-field coupling of adjacent nanoparticles. The approach presented here provides a unique and viable means of building artificial "plasmonic crystals" with precisely designed optical properties, which can be useful for the emerging fields of plasmonics, such as subwavelength integrated optics.

We report on the first demonstration of broadband tunable, single-mode plasmonic nanolasers (spasers) emitting in the full visible spectrum. These nanolasers are based on a single metal-oxide-semiconductor nanostructure platform comprising of InGaN/GaN semiconductor nanorods supported on an Al2O3-capped epitaxial Ag film. In particular, all-color lasing in subdiffraction plasmonic resonators is achieved via a novel mechanism based on a property of weak size dependence inherent in spasers. Moreover, we have successfully reduced the continuous-wave (CW) lasing thresholds to ultrasmall values for all three primary colors and have clearly demonstrated the possibility of "thresholdless" lasing for the blue plasmonic nanolaser.

We apply a nanomanipulation technique to assemble pairs of monodispersed octahedral gold nanocrystals (side length, 150 nm) along their major axes with a varying tip-to-tip separation (25-125 nm). These pairs are immobilized onto indium tin oxide coated silica substrates and studied as plasmonic dimers by polarization-selective total internal reflection (TIR) microscopy and spectroscopy. We confirm that the plasmon coupling modes with the scattering polarization along the incident light direction result from the transverse-magnetic-polarized incident light, which induces two near-field-coupled dipole moments oriented normal to the air-substrate interface. In such cases, both in-phase (antibonding) and antiphase (bonding) plasmon coupling modes can be directly observed with the incident light wave vector perpendicular and parallel to the dimer axis, respectively. The observation of antiphase plasmon coupling modes ("dark" plasmons) is made possible by the unique polarization nature of the TIR-generated evanescent field. Furthermore, with decreasing nanocrystal separation, the plasmon coupling modes shift to shorter wavelengths for the incident light perpendicular to the dimer axis, whereas relatively large red shifts of the plasmonic coupling modes are found for the parallel incident light.

Nanoporous polymers with gyroid nanochannels can be fabricated from the self-assembly of degradable block copolymer, polystyrene-b-poly(l-lactide) (PS-PLLA), followed by the hydrolysis of PLLA blocks. A well-defined nanohybrid material with SiO2 gyroid nanostructure in a PS matrix can be obtained using the nanoporous PS as a template for sol-gel reaction. After subsequent UV degradation of the PS matrix, a highly porous inorganic gyroid network remains, yielding a single-component material with an exceptionally low refractive index (as low as 1.1).

Localized surface plasmon resonances (LSPRs) associated with metallic nanostructures offer unique possibilities for light concentration beyond the diffraction limit, which can lead to strong field confinement and enhancement in deep subwavelength regions. In recent years, many transformative plasmonic applications have emerged, taking advantage of the spectral and spatial tunability of LSPRs enabled by near-field coupling between constituent metallic nanostructures in a variety of plasmonic metastructures (dimers, metamolecules, metasurfaces, metamaterials, etc.). For example, the "hot spot" formed at the interstitial site (gap) between two coupled metallic nanostructures in a plasmonic dimer can be spectrally tuned via the gap size. Capitalizing on these capabilities, there have been significant advances in plasmon enhanced or enabled applications in light-based science and technology, including ultrahigh-sensitivity spectroscopies, light energy harvesting, photocatalysis, biomedical imaging and theranostics, optical sensing, nonlinear optics, ultrahigh-density data storage, as well as plasmonic metamaterials and metasurfaces exhibiting unusual linear and nonlinear optical properties. In this review, we present two complementary approaches for fabricating plasmonic metastructures. We discuss how meta-atoms can be assembled into unique plasmonic metastructures using a variety of nanomanipulation methods based on single- or multiple-probes in an atomic force microscope (AFM) or a scanning electron microscope (SEM), optical tweezers, and focused electron-beam nanomanipulation. We also provide a few examples of nanoparticle metamolecules with designed properties realized in such well-controlled plasmonic metastructures. For the spatial controllability on the mesoscopic and macroscopic scales, we show that controlled self-assembly is the method of choice to realize scalable two-dimensional, and three-dimensional plasmonic metastructures. In the section of applications, we discuss some key examples of plasmonic applications based on individual hot spots or ensembles of hot spots with high uniformity and improved controllability.

The development of ultrasmooth, macroscopic-sized silver (Ag) crystals exhibiting reduced losses is critical to fully characterize the ultimate performance of Ag as a plasmonic material, and to enable cascaded and integrated plasmonic devices. Here we demonstrate the growth of single-crystal Ag plates with millimetre lateral sizes for linear and nonlinear plasmonic applications. Using these Ag crystals, surface plasmon polariton propagation lengths beyond 100 μm in the red wavelength region are measured. These lengths exceed the predicted values using the widely cited Johnson and Christy data. Furthermore, they allow the fabrication of highly reproducible plasmonic nanostructures by focused ion beam milling. We have designed and fabricated double-resonant nanogroove arrays using these crystals for spatially uniform and spectrally tunable second-harmonic generation. In conventional ‘hot-spot'-based nonlinear processes such as surface-enhanced Raman scattering and second-harmonic generation, strong enhancement can only occur in random, localized regions. In contrast, our approach enables uniform nonlinear signal generation over a large area.