Tunable SERS Enhancement via Sub-nanometer Gap Metasurfaces.

Raman sensing is a powerful technique for detecting chemical signatures, especially when combined with optical enhancement techniques such as using substrates containing plasmonic nanostructures. In this work, we successfully demonstrated surface-enhanced Raman spectroscopy (SERS) of two analytes adsorbed onto gold nanosphere metasurfaces with tunable subnanometer gap widths. These metasurfaces, which push the bounds of previously studied SERS nanostructure feature sizes, were fabricated with precise control of the intersphere gap width to within 1 nm for gaps close to and below 1 nm. Analyte Raman spectra were measured for samples for a range of gap widths, and the surface-affected signal enhancement was found to increase with decreasing gap width, as expected and corroborated via electromagnetic field modeling. Interestingly, an enhancement quenching effect was observed below gaps of around 1 nm. We believe this to be one of the few studies of gap-width-dependent SERS for the subnanometer range, and the results suggest the potential of such methods as a probe of subnanometer scale effects at the interface between plasmonic nanostructures. With further study, we believe that tunable sub-nanometer gap metasurfaces could be a useful tool for the study of nonlocal and quantum enhancement-quenching effects. This could aid the development of optimized Raman-based sensors for a variety of applications.

The Role of Rayleigh-Wood Anomalies and Surface Plasmons in Optical Enhancement for Nano-Gratings.

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.

Plasmonic Au Array SERS Substrate with Optimized Thin Film Oxide Substrate Layer.

This work studies the effect of a plasmonic array structure coupled with thin film oxide substrate layers on optical surface enhancement using a finite element method. Previous results have shown that as the nanowire spacing increases in the sub-100 nm range, enhancement decreases; however, this work improves upon previous results by extending the range above 100 nm. It also averages optical enhancement across the entire device surface rather than localized regions, which gives a more practical estimate of the sensor response. A significant finding is that in higher ranges, optical enhancement does not always decrease but instead has additional plasmonic modes at greater nanowire and spacing dimensions resonant with the period of the structure and the incident light wavelength, making it possible to optimize enhancement in more accessibly fabricated nanowire array structures. This work also studies surface enhancement to optimize the geometries of plasmonic wires and oxide substrate thickness. Periodic oscillations of surface enhancement are observed at specific oxide thicknesses. These results will help improve future research by providing optimized geometries for SERS molecular sensors.

Substrate Oxide Layer Thickness Optimization for a Dual-Width Plasmonic Grating for Surface-Enhanced Raman Spectroscopy (SERS) Biosensor Applications.

This work investigates a new design for a plasmonic SERS biosensor via computational electromagnetic models. It utilizes a dual-width plasmonic grating design, which has two different metallic widths per grating period. These types of plasmonic gratings have shown larger optical enhancement than standard single-width gratings. The new structures have additional increased enhancement when the spacing between the metal decreases to sub-10 nm dimensions. This work integrates an oxide layer to improve the enhancement even further by carefully studying the effects of the substrate oxide thickness on the enhancement and reports ideal substrate parameters. The combined effects of varying the substrate and the grating geometry are studied to fully optimize the device's enhancement for SERS biosensing and other plasmonic applications. The work reports the ideal widths and substrate thickness for both a standard and a dual-width plasmonic grating SERS biosensor. The ideal geometry, comprising a dual-width grating structure atop an optimal SiO2 layer thickness, improves the enhancement by 800%, as compared to non-optimized structures with a single-width grating and a non-optimal oxide thickness.