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DNA nanotechnology for light-emitting plasmonic applications https://doi.org/10.17863/CAM.115406 Rocchetti, Sara 0009000977660465 Baumberg, Jeremy Keyser, Ulrich DNA nanotechnology for light-emitting plasmonic applications - Sara Rocchetti. The development of plasmonic nanocavities allows for the direct observation of light-matter interactions at the nanoscale. Collective oscillations of electrons (SPPs) at a metal-dielectric interface confine light into nanometric spaces, sustaining an optical resonance. This resonance can be carefully tuned by changing the geometry and material of the gap. In this work, I use the NanoParticle-on-Mirror (NPoM) geometry to fabricate plasmonic cavities in a bottom-up fashion by simply drop casting gold nanoparticles on thin gold films. The existence of tightly confined optical modes enhances both electronic and vibrational transitions of the molecules present in the gap. To accurately position single molecules within these plasmonic cavities, I utilise DNA nanotechnology. This bottom-up, self-assembly technique facilitates the creation of molecular platforms at the nanoscale. By developing pro tocols to fabricate NPoM constructs where DNA nanostructures serve as molecular frameworks, I can precisely place single emitters within plasmonic gaps. This allows for the investigation of the emission properties of individual molecules and their interaction with metals at a sub-nanometric scale. By combining DNA nanotechnol ogy with NPoMs, I demonstrate that utilising various DNA constructs as scaffolds results in different regimes of light-matter interaction. This leads to the observation of amplified optical forces at the nanoscale and strongly coupled systems. University of Cambridge 2024-05-21 Thesis Doctoral Doctor of Philosophy (PhD) eng https://www.repository.cam.ac.uk/handle/1810/379253 https://www.repository.cam.ac.uk/bitstreams/665260d9-0d05-4fe7-ad8e-71525d2e6e4d/download e0cfe424efa273dcaccda1ba6db26b3a https://www.repository.cam.ac.uk/bitstreams/26d2e145-8e0f-426f-96fb-93da966426d7/download 87eda9de84448d1f82354d60eee3eb5f http://purl.org/NET/rdflicense/allrightsreserved DNA nanotechnology picocavities plasmonic nanocavity quantum emitters surface enhanced Raman spectroscopy