Title: From Broadband Absorption to Entangled Emission: Functional Nanogaps for Energy Conversion and Single Molecule Quantum Optics
Abstract: Plasmonic nanogaps offer a unique platform that combines extreme optical confinement with molecular-scale functionality. In this talk, I will present two complementary studies that highlight the powerful capabilities that arise from bridging the length-scales between light and molecules. First, I will introduce electrochemical photovoltage spectroscopy (EC-PVS) as a useful tool to unravel the wavelength-dependent generation and extraction of hot carriers in molecularly functionalized gold nanoparticle films. Through selective harvesting of interband hot holes and intraband hot electrons, we map how Au nanomaterials switch their photochemical capabilities between oxidative and reductive, offering a nanoscale charge-balancing mechanism to allow for stand-alone solar energy conversion. In the second part, I will shift focus to the quantum regime, showcasing the detection of temporally and spectrally correlated Stokes–anti-Stokes photon pairs from single molecules in hybrid plasmonic nanocavities. Through optomechanical pumping and nanolens-enhanced directionality, we achieve room-temperature generation of correlated photon pairs with measurable g²(0) correlations, establishing a new route toward on-chip quantum light sources utilising single molecules. Together, these studies highlight how molecular control and nanophotonic engineering can unlock a wide spectrum of plasmonic functionality, from sustainable energy harvesting to quantum information processing.
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- David de Wiedgebouw - 1.36
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