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We theoretically investigate several types of plasmonic slot waveguides for enhancing the measured signal in Raman spectroscopy, which is a consequence of electric field and Purcell factor enhancements, as well as an increase in light-matter interaction volume and the Raman signal collection efficiency. An intuitive methodology is presented for calculating the accumulated Raman enhancement factor of an ensemble of molecules in waveguide sensing, which exploits an analytical photon Green function expansion in terms of the waveguide normal modes, and we combine this with a quantum optics formalism of the molecule-waveguide interaction to model Raman scattering. We subsequently show how integrated plasmonic slot waveguides can attain significantly higher Raman enhancement factors: $\sim$5.3$\times$ compared to optofluidic fibers and $\sim$3.7$\times$ compared to planar integrated dielectric waveguides, with a device size and thus analyte volume of at least three-orders of magnitude less. We also provide a comprehensive comparison between the different types of plasmonic slot waveguides based on the important figures-of-merit, and determine the optimal approaches to maximize Raman enhancement., Comment: 24 pages, 21 figures

We theoretically investigate the enhancement of surface enhanced Raman spectroscopy (SERS) using hyperbolic stratified nanostructures and compare to metal nanoresonators. The photon Green function of each nanostructure within its environment is first obtained from a semi-analytical modal theory, which is used in a quantum optics formalism of the molecule-nanostructure interaction to model the SERS spectrum. An intuitive methodology is presented for calculating the single molecule enhancement factor (SMEF), which is also able to predict known experimental SERS enhancement factors of an example gold nano-dimer. We elucidate the important figures-of-merit of the enhancement and explore these for different designs. We find that the use of hyperbolic stratified materials can enhance the photonic local density of states (LDOS) by close to 2 times in comparison to pure metal nanostructures, when both designed to work at the same operating wavelengths. However, the increased LDOS is accompanied by higher electric field concentration within the lossy hyperbolic material, which leads to increased quenching that serves to reduce the overall detected SERS enhancement in the far field. For nanoresonators with resonant localized surface plasmon wavelengths in the near-infrared, the SMEF for the hyperbolic stratified nanostructure is approximately an order of magnitude lower than the pure metal counterpart. Conversely, we show that by detecting the Raman signal using a near-field probe, hyperbolic materials can provide an improvement in SERS enhancement compared to using pure metal nanostructures when the probe is sufficiently close (<50 nm) to the Raman active molecule at the plasmonic hotspot., Comment: 18 pages, 9 figures

We study the optical properties of quantum dipole emitters coupled to hyperbolic metamaterial nano-resonators using a semi-analytical quasinormal mode approach. We show that coupling to metamaterial nano-resonators can lead to significant Purcell enhancements that are nearly an order of magnitude larger than those of plasmonic resonators with comparable geometry. However, the associated single photon output $\beta$-factors are extremely low (around 10$\%$), far smaller than those of comparable sized metallic resonators (70$\%$). Using a quasinormal mode expansion of the photon Green function, we describe how the low $\beta$-factors are due to increased Ohmic quenching arising from redshifted resonances, larger quality factors, and stronger confinement of light within the metal. In contrast to current wisdom, these results suggest that hyperbolic metamaterial nano-structures make poor choices for single photon sources.