Engineering photonic-plasmonic devices for spectroscopy and sensing applications

Abstract

The control of light on the nano-scale has driven the development of novel optical devices such as biosensors, antennas and guiding elements. These applications benefit from the distinctive resonant properties of noble metal thin films and nanoparticles. Many optimization parameters exist in order to engineer nanoparticle properties for spectroscopy and sensing applications: for example, the choice of metal, the particle morphology, and the array geometry. By utilizing various designs from simple monomer gratings to more complex engineered arrays, we model and characterize plasmonic arrays for sensing applications. In this thesis, I have focused on the novel paradigm of photonic-plasmonic coupling to design, fabricate, and characterize optimized nanosensors. In particular, nanoplasmonic necklaces, which consist of circular loops of closely spaced gold nanoparticles, are designed using 3D finite-difference time-domain (FDTD) simulations, fabricated with electron-beam lithography, and characterized using dark-field scattering and surface-enhanced Raman spectroscopy (SERS) of p-mercaptoaniline (pMA) monolayers. I show that such necklaces are able to support hybridized dipolar scattering resonances and polarization-controlled electromagnetic hot-spots. In addition, necklaces exhibit strong intensity enhancement when the necklace diameter leads to coupling between the broadband plasmonic resonance and the circular resonator structure of the necklace. Hence, these necklaces lead to stronger field intensity enhancement than nanoparticle monomers and dimers, which are also carefully studied. Furthermore, by embedding a dimer into one or more concentric necklace resonators, I am able to efficiently couple radiation into the dimer hot-spot by utilizing first- and second-order far-field coupling. This nanolensing leads to an order of 6-18 times improvement in Raman enhancement over isolated dimers, which is a promising platform for compact on-chip sensors. Additionally, I have fabricated and experimentally characterized devices that were designed in my group for SERS of pMA using an optimization algorithm. The algorithm confirms that the best arrangement of nanoparticles to increase near-field intensity enhancement in a single hot-spot is to embed a dimer into particles that couple light into the hot-spot via far-field photonic radiation. These genetically optimized nanoantennas show improvement in Raman enhancement 10 times that of nanoparticle dimers, and 100 times the enhancement of optimized two-dimensional monomer diffraction gratings.