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Experimental Verification of the Spectral Shift between Near- and Far-Field Peak Intensities of Plasmonic Nanoantennas

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 Publication date 2013
  fields Physics
and research's language is English




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Theory predicts a distinct spectral shift between the near- and far-field optical responses of plasmonic antennas. Here we combine near-field optical microscopy and far-field spectroscopy of individual infrared-resonant nanoantennas to verify experimentally this spectral shift. Numerical calculations corroborate our experimental results. We furthermore discuss the implications of this effect in surface-enhanced infrared spectroscopy (SEIRS).



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In the past decade, advances in nanotechnology have led to the development of plasmonic nanocavities which facilitate light-matter strong coupling in ambient conditions. The most robust example is the nanoparticle-on-mirror (NPoM) structure whose geometry is controlled with subnanometer precision. The excited plasmons in such nanocavities are extremely sensitive to the exact morphology of the nanocavity, giving rise to unexpected optical behaviors. So far, most theoretical and experimental studies on such nanocavities have been based solely on their scattering and absorption properties. However, these methods do not provide a complete optical description of a NPoM. Here, the NPoM is treated as an open non-conservative system supporting a set of photonic quasinormal modes (QNMs). By investigating the morphology-dependent optical properties of nanocavities, we propose a simple yet comprehensive nomenclature based on spherical harmonics and report spectrally overlapping bright and dark nanogap eigenmodes. The near-field and far-field optical properties of NPoMs are explored and reveal intricate multi-modal interactions.
Asymmetric metal-dielectric nanostructures are demonstrated superior optical properties arise from the combination of strong enhancement of their near fields and controllable scattering characteristics which originate from plasmonic and high-index dielectric components. Here, being inspired by the recent experimental work [Dmitry~Zuev, textit{et al.}, Adv. Mater. textbf{28}, 3087 (2016)] on a new technique for fabrication of asymmetric hybrid nanoparticles via femtosecond laser melting at the nanoscale, we suggest and study numerically a novel type of hybrid dimer nanoantennas. The nanoantennas consist of asymmetric metal-dielectric (Au/Si) nanoparticles and can allow tuning of the near- and far-field properties via laser melting of the metal part. We demonstrate a modification of scattering properties, near electric field distribution, normalized local density of states, and power patters of radiation of the nanoantennas upon laser reshaping. The parameters used to investigate these effects correspond to experimentally demonstrated values in the recent work.
We describe an efficient near-field to far-field transformation for optical quasinormal modes, which are the dissipative modes of open cavities and plasmonic resonators with complex eigenfrequencies. As an application of the theory, we show how one can compute the reservoir modes (or regularized quasinormal modes) outside the resonator, which are essential to use in both classical and quantum optics. We subsequently demonstrate how to efficiently compute the quantum optical parameters necessary in the theory of quantized quasinormal modes [Franke et al., Phys. Rev. Lett. 122, 213901 (2019)]. To confirm the accuracy of our technique, we directly compare with a Dyson equation approach currently used in the literature (in regimes where this is possible), and demonstrate several order of magnitude improvement for the calculation run times. We also introduce an efficient pole approximation for computing the quantized quasinormal mode parameters, since they require an integration over a range of frequencies. Using this approach, we show how to compute regularized quasinormal modes and quantum optical parameters for a full 3D metal dimer in under one minute on a standard desktop computer. Our technique is exemplified by studying the quasinormal modes of metal dimers and a hybrid structure consisting of a gold dimer on top of a photonic crystal beam. In the latter example, we show how to compute the quantum optical parameters that describe a pronounced Fano resonance, using structural geometries that cannot practically be solved using a Dyson equation approach. All calculations for the spontaneous emission rates are confirmed with full-dipole calculations in Maxwells equations and are shown to be in excellent agreement.
Scattering-type scanning near-field optical microscopy (s-SNOM) is instrumental in exploring polaritonic behaviors of two-dimensional (2D) materials at the nanoscale. A sharp s-SNOM tip couples momenta into 2D materials through phase matching to excite phonon polaritons, which manifest as nanoscale interference fringes in raster images. However, s-SNOM lacks the ability to detect the progression of near-field property along the perpendicular axis to the surface. Here, we perform near-field analysis of a micro-disk and a reflective edge made of isotopically pure hexagonal boron nitride (h-11BN), by using three-dimensional near-field response cubes obtained by peak force scattering-type near-field optical microscopy (PF-SNOM). Momentum quantization of polaritons from the confinement of the circular structure is revealed in situ. Moreover, tip-sample distance is found to be capable of fine-tuning the momentum of polaritons and modifying the superposition of quantized polaritonic modes. The PF-SNOM-based three-dimensional near-field analysis provides detailed characterization capability with a high spatial resolution to fully map three-dimensional near-fields of nano-photonics and polaritonic structures.
A core process in many quantum tasks is the generation of entanglement. It is being actively studied in a variety of physical settings - from simple bipartite systems to complex multipartite systems. In this work we experimentally study the generation of bipartite entanglement in a nanophotonic system. Entanglement is generated via the quantum interference of two surface plasmon polaritons in a beamsplitter structure, i.e. utilising the Hong-Ou-Mandel (HOM) effect, and its presence is verified using quantum state tomography. The amount of entanglement is quantified by the concurrence and we find values of up to 0.77 +/- 0.04. Verifying entanglement in the output state from HOM interference is a nontrivial task and cannot be inferred from the visibility alone. The techniques we use to verify entanglement could be applied to other types of photonic system and therefore may be useful for the characterisation of a range of different nanophotonic quantum devices.
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