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Register a new userShape and Size Resonances in Second Harmonic Generation from Plasmonic Nano-Cavities
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The nonlinear response of sub wavelength nano-cavities in thin metal films is investigated. We report the resonant dependence of the Second Harmonic Generation by individual triangular and square holes on shape, size and wavelength. For cavities with internal nano-corrugations, giant field enhancements are observed, making them excellent candidates for high sensitivity spectroscopy.
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We predict plasmonic mediated nucleation of pancake shaped resonant nano-cavities in metallic layers that are penetrable to laser fields. The underlying physics is that the cavity provides a narrow plasmonic resonance that maximizes its polarizability in an external field. The resonance yields a significant energy gain making the formation of such cavities highly favorable. Possible implications include nano-optics and generation of the dielectric bits in conductive films that underlie the existing optical recording phase change technology.
A hallmark of wave-matter duality is the emergence of quantum-interference phenomena when an electronic transition follows different trajectories. Such interference results in asymmetric absorption lines such as Fano resonances, and gives rise to secondary effects like electromagnetically induced transparency (EIT) when multiple optical transitions are pumped. Few solid-state systems show quantum interference and EIT, with quantum-well intersubband transitions in the IR offering the most promising avenue to date to devices exploiting optical gain without inversion. Quantum interference is usually hampered by inhomogeneous broadening of electronic transitions, making it challenging to achieve in solids at visible wavelengths and elevated temperatures. However, disorder effects can be mitigated by raising the oscillator strength of atom-like electronic transitions - excitons - which arise in monolayers of transition-metal dichalcogenides (TMDCs). Quantum interference, probed by second-harmonic generation (SHG), emerges in monolayer WSe2, without a cavity, splitting the SHG spectrum. The splitting exhibits spectral anticrossing behaviour, and is related to the number of Rabi flops the strongly driven system undergoes. The SHG power-law exponent deviates strongly from the canonical value of 2, showing a Fano-like wavelength dependence which is retained at room temperature. The work opens opportunities in solid-state quantum-nonlinear optics for optical mixing, gain without inversion and quantum-information processing.
Hyperbolic plasmonic metamaterials provide numerous opportunities for designing unusual linear and nonlinear optical properties. We show that the modal overlap of fundamental and second-harmonic light in an anisotropic plasmonic metamaterial slab results in the broadband enhancement of radiated second-harmonic intensity by up to 2 orders of magnitudes for TM- and TE-polarized fundamental light, compared to a smooth Au film under TM-polarised illumination. The results open up possibilities to design tuneable frequency-doubling metamaterial with the goal to overcome limitations associated with classical phase matching conditions in thick nonlinear crystals.
The second-order nonlinear optical susceptibility $Pi^{(2)}$ for second harmonic generation is calculated for gapped graphene. The linear and second-order nonlinear plasmon excitations are investigated in context of second harmonic generation (SHG). We report a red shift and an order of magnitude enhancement of the SHG resonance with growing gap, or alternatively, reduced electro-chemical potential.
Efficient frequency conversion techniques are crucial to the development of plasmonic metasurfaces for information processing and signal modulation. In principle, nanoscale electric-field confinement in nonlinear materials enables higher harmonic conversion efficiencies per unit volume than those attainable in bulk materials. Here we demonstrate efficient second-harmonic generation (SHG) in a serrated nanogap plasmonic geometry that generates steep electric field gradients on a dielectric metasurface. An ultrafast pump is used to control plasmon-induced electric fields in a thin-film material with inversion symmetry that, without plasmonic enhancement, does not exhibit an an even-order nonlinear optical response. The temporal evolution of the plasmonic near-field is characterized with ~100as resolution using a novel nonlinear interferometric technique. The ability to manipulate nonlinear signals in a metamaterial geometry as demonstrated here is indispensable both to understanding the ultrafast nonlinear response of nanoscale materials, and to producing active, optically reconfigurable plasmonic devices
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