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Optical coupling effects between plasmon resonances in disordered metal nanostructures and a nanocavityÖqvist, Elin January 2024 (has links)
Ultra-thin solar cells that incorporate earth-abundant and non-toxic materials are promising candidates in the endeavor toward sustainable energy harvesting. Methods to counteract the inevitable low absorption of thinner semiconductor layers are of high interest and have raised considerable attention in the research society. In an attempt to increase the absorption of these types of assemblies, optical coupling effects between the localized surface plasmon resonances (LSPR) of disordered Au nanostructures and a Fabry-Pérot cavity were studied using a previously established absorber/spacer/reflector stack. The disordered Au array was fabricated by evaporating a thin Au film on a substrate with a 55 nm SiO2 dielectric spacer and a 100 nm Al reflecting film, followed by thermal annealing. Nominal Au film thicknesses in the range of 5-25 Å and annealing temperatures of 200-500 oC were investigated. In situ spectroscopic ellipsometry measurements during the subsequent atomic layer deposition (ALD) of tin monosulfide (SnS) allowed analysis of how the optical properties of the SnS/Au absorber layer changed as a function of the growing SnS layer thickness. By employing the Transfer Matrix Method with the estimated optical properties from the in situ analysis, the absorptance of the absorber/spacer/reflector stacks was simulated as a function of the spacer thickness, revealing any signs of the characteristic anti-crossing behavior. It was discovered that a nominal Au film thickness of 25 Å, annealed at 450 oC, and coated with a SnS film of ∼13 nm primed toward the π-phase, resulted in strong optical coupling between the cavity mode and the LSPR. The energy difference at the avoided crossing in the specular reflectance measurement gave an estimated Rabi-splitting energy of 537 meV. This corresponded to about 40% of the original LSPR energy, placing itself within the ultra-strong coupling regime. To evaluate the relevance of the thin-layered structure in photovoltaic applications, more advanced computational methods are required to estimate the useful absorption that occurs in the SnS layer. Nevertheless, these results elucidate the realization of strong optical coupling effects between disordered Au nanostructures and a Fabry-Pérot cavity, and further the possibility of using scalable fabrication methods for this type of ultra-thin absorber/spacer/reflector stack.
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