Hybrid cavity-antenna architecture for strong and tunable sideband-selective molecular Raman scattering enhancement.

Plasmon resonances at the surface of metallic antennas allow for extreme enhancement of Raman scattering. Intrinsic to plasmonics, however, is that extreme field confinement lacks precise spectral control, which would hold great promise in shaping the optomechanical interaction between light and molecular vibrations. We demonstrate an experimental platform composed of a plasmonic nanocube-on-mirror antenna coupled to an open, tunable Fabry-Perot microcavity for selective addressing of individual vibrational lines of molecules with strong Raman scattering enhancement. Multiple narrow and intense optical resonances arising from the hybridization of the cavity modes and the plasmonic broad resonance are used to simultaneously enhance the laser pump and the local density of optical states, and are characterized using rigorous modal analysis. The versatile bottom-up fabrication approach permits quantitative comparison with the bare nanocube-on-mirror system, both theoretically and experimentally. This shows that the hybrid system allows for similar SERS enhancement ratios with narrow optical modes, paving the way for dynamical backaction effects in molecular optomechanics.

Integrated Sideband-Resolved SERS with a Dimer on a Nanobeam Hybrid.

In analogy to cavity optomechanics, enhancing specific sidebands of a Raman process with narrowband optical resonators would allow for parametric amplification, entanglement of light and molecular vibrations, and reduced transduction noise. We report on the demonstration of waveguide-addressable sideband-resolved surface-enhanced Raman scattering (SERS). We realized a hybrid plasmonic-photonic resonator consisting of a 1D photonic crystal cavity decorated with a sub-20 nm gap dimer nanoantenna. Hybrid resonances in the near-IR provide designer Q factors of 1000, and Q/V=(λ^{3}/10^{6})^{-1}, with SERS signal strength on par with levels found in state-of-the-art purely plasmonic systems. We evidence Fano line shapes in the SERS enhancement of organic molecules, and quantitatively separate out the pump enhancement and optical reservoir contributions.

Integrated Molecular Optomechanics with Hybrid Dielectric-Metallic Resonators.

Molecular optomechanics describes surface-enhanced Raman scattering using the formalism of cavity optomechanics as a parametric coupling of the molecule's vibrational modes to the plasmonic resonance. Most of the predicted applications require intense electric field hotspots but spectrally narrow resonances, out of reach of standard plasmonic resonances. The Fano lineshapes resulting from the hybridization of dielectric-plasmonic resonators with a broad-band plasmon and narrow-band cavity mode allow reaching strong Raman enhancement with high-Q resonances, paving the way for sideband resolved molecular optomechanics. We extend the molecular optomechanics formalism to describe hybrid dielectric-plasmonic resonators with multiple optical resonances and with both free-space and waveguide addressing. We demonstrate how the Raman enhancement depends on the complex response functions of the hybrid system, and we retrieve the expression of Raman enhancement as a product of pump enhancement and the local density of states. The model allows prediction of the Raman emission ratio into different output ports and enables demonstrating a fully integrated high-Q Raman resonator exploiting multiple cavity modes coupled to the same waveguide.

Aberration calibration and correction with nano-scatterers in digital holographic microscopy for semiconductor metrology.

Overlay metrology measures pattern placement between two layers in a semiconductor chip. The continuous shrinking of device dimensions drives the need to explore novel optical overlay metrology concepts that can address many of the existing metrology challenges. We present a compact dark-field digital holographic microscope that uses only a single imaging lens. Our microscope offers several features that are beneficial for overlay metrology, like a large wavelength range. However, imaging with a single lens results in highly aberrated images. In this work, we present an aberration calibration and correction method using nano-sized point scatterers on a silicon substrate. Computational imaging techniques are used to recover the full wavefront error, and we use this to correct for the lens aberrations. We present measured data to verify the calibration method and we discuss potential calibration error sources that must be considered. A comparison with a ZEMAX calculation is also presented to evaluate the performance of the presented method.

Energy-resolved plasmonic chemistry in individual nanoreactors.

Plasmonic resonances can concentrate light into exceptionally small volumes, which approach the molecular scale. The extreme light confinement provides an advantageous pathway to probe molecules at the surface of plasmonic nanostructures with highly sensitive spectroscopies, such as surface-enhanced Raman scattering. Unavoidable energy losses associated with metals, which are usually seen as a nuisance, carry invaluable information on energy transfer to the adsorbed molecules through the resonance linewidth. We measured a thousand single nanocavities with sharp gap plasmon resonances spanning the red to near-infrared spectral range and used changes in their linewidth, peak energy and surface-enhanced Raman scattering spectra to monitor energy transfer and plasmon-driven chemical reactions at their surface. Using methylene blue as a model system, we measured shifts in the absorption spectrum of molecules following surface adsorption and revealed a rich plasmon-driven reactivity landscape that consists of distinct reaction pathways that occur in separate resonance energy windows.

Controlling Optically Driven Atomic Migration Using Crystal-Facet Control in Plasmonic Nanocavities.

Plasmonic nanoconstructs are widely exploited to confine light for applications ranging from quantum emitters to medical imaging and biosensing. However, accessing extreme near-field confinement using the surfaces of metallic nanoparticles often induces permanent structural changes from light, even at low intensities. Here, we report a robust and simple technique to exploit crystal facets and their atomic boundaries to prevent the hopping of atoms along and between facet planes. Avoiding X-ray or electron microscopy techniques that perturb these atomic restructurings, we use elastic and inelastic light scattering to resolve the influence of crystal habit. A clear increase in stability is found for {100} facets with steep inter-facet angles, compared to multiple atomic steps and shallow facet curvature on spherical nanoparticles. Avoiding atomic hopping allows Raman scattering on molecules with low Raman cross-section while circumventing effects of charging and adatom binding, even over long measurement times. These nanoconstructs allow the optical probing of dynamic reconstruction in nanoscale surface science, photocatalysis, and molecular electronics.