Multiresonant Plasmonics with Spatial Mode Overlap

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Virginia Tech


Plasmonic nanostructures can enhance light-matter interactions in the subwavelength domain, which is useful for photodetection, light emission, optical biosensing, and spectroscopy. However, conventional plasmonic devices are optimized to operate in a single wavelength band, which is not efficient for wavelength-multiplexed operations and quantum optical applications involving multi-photon nonlinear processes at multiple wavelength bands. Overcoming the limitations of single-resonant plasmonics requires development of plasmonic devices that can enhance the optical interactions at the same locations but at different resonance wavelengths. This dissertation comprehensively studies the theory, design, and applications of such devices, called "multiresonant plasmonic systems with spatial mode overlap". We start by a literature review to elucidate the importance of this topic as well as its current and potential applications. Then, we briefly discuss the fundamentals of plasmonic resonances and mode hybridization to thoroughly explore, classify, and compare the different architectures of the multiresonant plasmonic systems with spatial mode overlap. Also, we establish the black-box coupled mode theory to quantify the coupling of optical modes and analyze the complicated dynamics of optical interactions in multiresonant plasmonic systems. Next, we introduce the nanolaminate plasmonic crystals (NPCs), wafer-scale metamaterials structures that support many (>10) highly-excitable plasmonic modes with spatial overlap across the visible and near-infrared optical bands. The enabling factors behind the NPC's superior performance as multiresonant systems are also theoretically and experimentally investigated. After that, we experimentally demonstrate the NPCs application in simultaneous second harmonic generation and anti-Stokes photoluminescence (ASPL) with controllable nonlinear emission properties. By designing specific non-linear optical experiments and developing advanced ASPL models, this work addresses some important but previously unresolved questions on the ASPL mechanism as well. Finally, we conclude the dissertation by discussing the potential applications of out-of-plane plasmonic systems with spatial mode overlap in wavelength-multiplexed devices and presenting some preliminary results.



Multiresonant plasmonics, Spatial overlap, Mode hybridization, Black-box coupled-mode theory, Nanolaminate plasmonic crystal, Plasmonic Photoluminescence, Second harmonic generation