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            Abstract The topological features of optical vortices have been opening opportunities for free-space and on-chip photonic technologies, e.g., for multiplexed optical communications and robust information transport. In a parallel but disjoint effort, polar anisotropic van der Waals nanomaterials supporting hyperbolic phonon polaritons (HP 2 s) have been leveraged to drastically boost light-matter interactions. So far HP 2 studies have been mainly focusing on the control of their amplitude and scale features. Here we report the generation and observation of mid-infrared hyperbolic polariton vortices (HP 2 Vs) associated with reconfigurable topological charges. Spiral-shaped gold disks coated with a flake of hexagonal boron nitride are exploited to tailor spin–orbit interactions and realise deeply subwavelength HP 2 Vs. The complex interplay between excitation spin, spiral geometry and HP 2 dispersion enables robust reconfigurability of the associated topological charges. Our results reveal unique opportunities to extend the application of HP 2 s into topological photonics, quantum information processing by integrating these phenomena with single-photon emitters, robust on-chip optical applications, sensing and nanoparticle manipulation.more » « less
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            Abstract The lattice symmetry of a crystal is one of the most important factors in determining its physical properties. Particularly, low-symmetry crystals offer powerful opportunities to control light propagation, polarization and phase 1–4 . Materials featuring extreme optical anisotropy can support a hyperbolic response, enabling coupled light–matter interactions, also known as polaritons, with highly directional propagation and compression of light to deeply sub-wavelength scales 5 . Here we show that monoclinic crystals can support hyperbolic shear polaritons, a new polariton class arising in the mid-infrared to far-infrared due to shear phenomena in the dielectric response. This feature emerges in materials in which the dielectric tensor cannot be diagonalized, that is, in low-symmetry monoclinic and triclinic crystals in which several oscillators with non-orthogonal relative orientations contribute to the optical response 6,7 . Hyperbolic shear polaritons complement previous observations of hyperbolic phonon polaritons in orthorhombic 1,3,4 and hexagonal 8,9 crystal systems, unveiling new features, such as the continuous evolution of their propagation direction with frequency, tilted wavefronts and asymmetric responses. The interplay between diagonal loss and off-diagonal shear phenomena in the dielectric response of these materials has implications for new forms of non-Hermitian and topological photonic states. We anticipate that our results will motivate new directions for polariton physics in low-symmetry materials, which include geological minerals 10 , many common oxides 11 and organic crystals 12 , greatly expanding the material base and extending design opportunities for compact photonic devices.more » « less
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            null (Ed.)Abstract All-dielectric nanostructures have recently opened exciting opportunities for functional nanophotonics, owing to their strong optical resonances along with low material loss in the near-infrared range. Pushing these concepts to the visible range is hindered by their larger absorption coefficient, thus encouraging the search for alternative dielectrics for nanophotonics. Here, we employ bandgap engineering to synthesize hydrogenated amorphous Si nanoparticles (a-Si:H NPs) offering ideal features for functional nanophotonics. We observe significant material loss suppression in a-Si:H NPs in the visible range caused by hydrogenation-induced bandgap renormalization, producing strong higher-order resonant modes in single NPs with Q factors up to ~100 in the visible and near-IR range. We also realize highly tunable all-dielectric meta-atoms by coupling a-Si:H NPs to photochromic spiropyran molecules. ~70% reversible all-optical tuning of light scattering at the higher-order resonant mode under a low incident light intensity is demonstrated. Our results promote the development of high-efficiency visible nanophotonic devices.more » « less
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            Abstract Phonon polaritons, the hybrid quasiparticles resulting from the coupling of photons and lattice vibrations, have gained significant attention in the field of layered van der Waals heterostructures. Particular interest has been paid to hetero‐bicrystals composed of molybdenum oxide (MoO3) and hexagonal boron nitride (hBN), which feature polariton dispersion tailorable via avoided polariton mode crossings. In this work, the polariton eigenmodes in MoO3‐hBN hetero‐bicrystals self‐assembled on ultrasmooth gold are systematically studied using synchrotron infrared nanospectroscopy. It is experimentally demonstrated that the spectral gap in bicrystal dispersion and corresponding regimes of negative refraction can be tuned by material layer thickness, and these results are quantitatively matched with a simple analytic model. Polaritonic cavity modes and polariton propagation along “forbidden” directions are also investigated in microscale bicrystals, which arise from the finite in‐plane dimension of the synthesized MoO3micro‐ribbons. The findings shed light on the unique dispersion properties of polaritons in van der Waals heterostructures and pave the way for applications leveraging deeply sub‐wavelength mid‐infrared light‐matter interactions.more » « less
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