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.

Surface-enhanced Raman spectroscopy (SERS) is an experimental tool for accessing vibrational and chemical information, down to the single molecule level. SERS typically relies on plasmon excitations in metal nanostructures to concentrate the incident radiation and to provide an enhanced photon density of states to couple emitted radiation to the far field. Many common SERS platforms involve metal nanoparticles to generate the required electromagnetic enhancements. Here we concentrate on an alternative approach, in which the relevant plasmon excitations are supported at a truly nanoscale gap between extended electrodes, rather than discrete subwavelength nanoparticles. The ability to fabricate precise gaps on demand, and in some cases to tune the gap size in situ, combined with the additional capability of simultaneous electronic transport measurements of the nanogap, provides access to information not previously available in standard SERS. We summarize the rich plasmonic physics at work in these extended systems and highlight the recent state of the art including tip-enhanced Raman spectroscopy (TERS) and the application of mechanical break junctions and electromigrated junctions. We describe in detail how we have performed in situ gap-enhanced Raman measurements of molecular-scale junctions while simultaneously subjecting these structures to electronic transport. These extended electrode structures allow us to study the pumping of vibrational modes by the flow of tunneling electrons, as well as the shifting of vibrational energies due to the applied bias. These experiments extend SERS into a tool for examining fundamental processes of dissipation, and provide insight into the mechanisms behind SERS spectral diffusion. We conclude with a brief discussion of future directions.

We propose and report on the design of a 1-D metallo-dielectric nano-grating on a GaAs substrate. We numerically study the impact of grating period, slit and wire widths, and irradiating angle of incidence on the optical response. The optimal wire width, w = 160 nm, was chosen based on previous results from investigations into the influence of wire width and nano-slit dimensions on optical and electrical enhancements in metal-semiconductor-metal photodetectors. In this present project, resonant absorption and reflection modes were observed while varying the wire and nano-slit widths to study the unique optical modes generated by Rayleigh-Wood anomalies and surface plasmon polaritons. We observed sharp and diffuse changes in optical response to these anomalies, which may potentially be useful in applications such as photo-sensing and photodetectors. Additionally, we found that varying the slit width produced sharper, more intense anomalies in the optical spectrum than varying the wire width.

We report on the tunable edge-plasmon-enhanced absorption of phosphorene nanoribbons supported on a dielectric substrate. Monolayer anisotropic black phosphorous (phosphorene) nanoribbons are explored for light trapping and absorption enhancement on different dielectric substrates. We show that these phosphorene ribbons support infrared surface plasmons with high spatial confinement. The peak position and bandwidth of the calculated phosphorene absorption spectra are tunable with low loss over a wide wavelength range via the surrounding dielectric environment of the periodic nanoribbons. Simulation results show strong edge plasmon modes and enhanced absorption as well as a red-shift of the peak resonance wavelength. The periodic Fabry-Perot grating model was used to analytically evaluate the absorption resonance arising from the edge of the ribbons for comparison with the simulation. The results show promise for the promotion of phosphorene plasmons for both fundamental studies and potential applications in the infrared spectral range.

The adhesion layer used in nanofabrication process of metallic nanostructures affects the surface plasmon modes. We characterize the localized surface plasmon resonances (SPRs) of gold nanodisks of various diameters and heights while varying the thickness of the Ti adhesion layers. Scattering, absorption, and extinction coefficient calculations show a significant dependence of the SPR on the size of nanostructures and the adhesion layer thickness. Comparisons of peak resonance wavelengths of different Ti adhesion layer thicknesses indicate a significant red shift and a reduction in amplitude as the Ti thickness increases. A comparison of spectral broadening of the plasmon mode indicates a linear increase with Ti thickness and percentage. In addition, the decay time of the plasmon mode decreased significantly as the adhesion layer size increases. These observations aid in understanding size dependent adhesion layer effects and optimized fabrication of single nanoplasmonic structures.