Characterisation of Single Biomolecules With Optoplasmonic Resonators
Vincent, S
Date: 19 October 2020
Publisher
University of Exeter
Degree Title
PhD in Physics
Abstract
Biomolecules can be detected through induced changes in the optical whispering-gallery mode (WGM) resonance in a circularly symmetric dielectric. The spatial and temporal confinement of light in a WGM is further complemented by coupling to the localised surface plasmons (LSPs) of metallic nanoparticles attached to the WGM resonator. ...
Biomolecules can be detected through induced changes in the optical whispering-gallery mode (WGM) resonance in a circularly symmetric dielectric. The spatial and temporal confinement of light in a WGM is further complemented by coupling to the localised surface plasmons (LSPs) of metallic nanoparticles attached to the WGM resonator. LSP-WGM hybridisation allows for the optical readout of single-molecule surface reactions on gold nanoantennae, the mechanisms for which are not yet fully understood from a theoretical perspective. The specificity of this modality is, moreover, a subject of intense research. In this thesis, we propose three strategies for characterising molecules with light. The first strategy is a prototype polarimeter that differentiates chirality based on a signal-reversible Faraday effect in a magneto-optical WGM microcavity. Thermal tuning integrated into the resonator minimises geometrical birefringence, in turn maximising Faraday rotation to optimise chiral sensitivity. There we endeavour to resolve single-molecule chirality. Without engineering reconsiderations, however, the polarimeter is found to be limited to bulk chiral analysis. The second strategy is an (optoplasmonic) LSP-WGM resonator with chiral gold nanoantennae. Signals from the molecules conjointly show a correlation with the molecular weight and diffusivity of detected DL-cysteine and poly-DL-lysine. Aside from these features, the sensing site heterogeneity on the chiral gold nanoparticles impedes chiral discrimination. The third strategy is a novel reaction scheme adapted to the optoplasmonic sensor. Aminothiol linkers functionalise the gold surface via amine-gold anchoring, setting up cyclical interactions with thiolated analytes by thiol/disulfide exchange. Unexpected perturbations in the LSP-WGM resonance are observed, such as linewidth oscillation without resonance shift attributed to optomechanical coupling between LSPs and the vibrational modes in a given analyte. This offers a new form of spectroscopy wherein single biomolecules could be characterised by their mass, size, and composition through monitoring secondary parameters of the optoplasmonic resonance.
Doctoral Theses
Doctoral College
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