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Manipulating Light-Matter Interactions with Plasmonic Nanoparticle Lattices

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Rationally assembled nanostructures exhibit distinct physical and chemical properties beyond their individual units. The development of nanofabrication tools enables precise structural defining of nanomaterials scalable to large areas. This dissertation focuses on plasmonic nanoparticle arrays that show unique diffractive coupling with lattice spacings engineered close to the wavelength of light. Collectively coupled plasmonic nanoparticles induce sharp, intense lattice plasmon resonances upon optical excitations compared to the broad resonances of individual nanoparticles, and the electromagnetic fields are strongly enhanced and localized near the sub-wavelength vicinity of the nanoparticles. By harnessing different lattice structural designs and materials systems, various light-matter interactions can be engineered including nanoscale lasing, nonlinear optics, and quantum optics. The structured plasmonic nanoparticle lattices can serve as a versatile, scalable platform for enhanced photochemistry, large-scale quantum optics and nontrivial topological photonics. The first half of the thesis describes the structural engineering of plasmonic nanocavity arrays for various functionalities in nanoscale lasing. Integrated with organic dye molecules, high-quality band-edge lattice plasmons (quality factor > 200) can contribute to single-mode lasing at room-temperature with directional emission. Beyond the dipolar lattice plasmons, Chapter 2 discusses a robust, stretchable nanolaser platform that can preserve its high mode quality under strain based on hybrid quadrupole lattice plasmons as a new lasing feedback mechanism. Chapter 3 describes multi-scale plasmonic superlattices can support multiple band-edge modes capable of multi-modal nanolasing at programmed emission wavelengths and with large mode spacings. Chapter 4 introduces the scaling behaviors for lasing from plasmonic nanocavity arrays, where the number of nanoparticles in plasmonic nanocavity arrays plays a critical role in lasing action in terms of ultrafast dynamics and lasing thresholds. In the final two chapters, we discussed the light-matter interactions between plasmonic nanocavities and photo-active materials systems beyond dye molecules. Chapter 5 covers continuous-wave upconverting lasing at room temperature with record-low thresholds and high photostability by integrating Yb3+/Er3+-co-doped upconverting nanoparticles with Ag nanopillar arrays. Chapter 6 discusses the emerging applications of plasmonic nanocavity arrays in nonlinear optics, quantum optics and topological photonics. Second harmonic generation signal was greatly increased up to 450 times by the propagating lattice plasmons. Quantum emitters in 2D hexagonal boron nitride can be deterministically coupled to plasmonic nanocavity arrays with preserved single photon emission. The delocalized lattice plasmons can also serve a versatile platform for long-range quantum entanglement and parity-time symmetric nanophotonics.

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