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Phonon polaritons (PhPs) are hybrid photon-phonon waves which enable strong light-matter interactions and subdiffractional confinement, potentially empowering applications in sensing, nonlinear optics and nanoscale energy manipulation. In this work, we use confocal Raman microscopy to investigate the coupling between bulk phonon modes and localized surface phonon polariton (SPhP) modes in indium phosphide (InP) nanopillars and 4H-silicon carbide (4H-SiC) gratings. The Raman intensity within the nanostructures is described in terms of the SPhP eigenmodes and used to reconstruct the field intensity, providing a method to map SPhP eigenmodes using visible and near-IR light. Our results indicate that, contrary to expectation, all Raman-active bulk phonon modes of InP and 4H-SiC couple to the localized SPhP modes. Further, we confirm that polarizability selection rules form the predominant coupling mechanism between phonons and SPhP modes, with electron-phonon coupling playing a role for certain phonon modes (A1(LO) and E1(TO) in 4H-SiC). These observations provide a method for extending Raman studies of PhP modes to achieve full 3D reconstruction of the PhP eigenmodes and visualize light-matter interactions within nanostructures, thus advancing Raman scattering as a technique for understanding PhP modes.

Metal-Insulator-Metal (MIM) plasmonic structures can confine electromagnetic waves to a deep subwavelength regime, enabling strong light-matter interactions with potential applications in nonlinear optics and on-chip photonic circuitry. In addition, strong coupling of mid-infrared (mid-IR) vibrational transitions to optical cavities provides a way to modify and control a material's chemical reactivity and may also allow for highly sensitive chemical detection technology. Here, we experimentally and theoretically investigate the mid-IR optical properties of 3D-printed, nanoscale, anisotropic, L-shaped MIM plasmonic cavities. We observe strong vibrational-plasmon coupling between the two dipolar modes of the L-cavity and the polymer dielectric. The resulting three polariton modes are well described by a multimode coupled oscillator model, which we employ to predict the polariton behavior as a function of cavity arm length. The 3D printing technique offers time and cost reduction advantages over typical electron beam lithography and represents a highly accessible and versatile means of printing arbitrary-shaped nanometer-sized mid-IR plasmonic cavities capable of producing strong light-matter interactions for a variety of photonic or photochemical applications.

We demonstrate how to exploit long-cell polytypes of silicon carbide to achieve strong coupling between transverse phonon polaritons and zone folded longitudinal optical phonons. The resulting quasiparticles possess hybrid longitudinal and transverse nature, allowing them to be generated through electric currents while emitting radiation to the far field. We develop a microscopic theory predicting the existence of the hybrid longitudinal-transverse excitations. We then provide their first experimental observation by tuning the monopolar resonance of a nanopillar array through the folded longitudinal optical mode, obtaining a clear spectral anti-crossing. This represents an important first step in the development of electrically pumped mid-infrared emitters., Comment: 9 pages, 4 figures

Surface phonon polaritons (SPhPs) - the surface-bound electromagnetic modes of a polar material resulting from the coupling of light with optic phonons - offer immense technological opportunities for nanophotonics in the infrared (IR) spectral region. Here, we present a novel approach to overcome the major limitation of SPhPs, namely the narrow, material-specific spectral range where SPhPs can be supported, called the Reststrahlen band. We use an atomic-scale superlattice (SL) of two polar semiconductors, GaN and AlN, to create a hybrid material featuring layer thickness-tunable optic phonon modes. As the IR dielectric function is governed by the optic phonon behavior, such control provides a means to create a new dielectric function distinct from either constituent material and to tune the range over which SPhPs can be supported. This work offers the first glimpse of the guiding principles governing the degree to which the dielectric function can be designed using this approach.

Conventional optical components are limited to size-scales much larger than the wavelength of light, as changes in the amplitude, phase and polarization of the electromagnetic fields are accrued gradually along an optical path. However, advances in nanophotonics have produced ultra-thin, co-called "flat" optical components that beget abrupt changes in these properties over distances significantly shorter than the free space wavelength. While high optical losses still plague many approaches, phonon polariton (PhP) materials have demonstrated long lifetimes for sub-diffractional modes in comparison to plasmon-polariton-based nanophotonics. We experimentally observe a three-fold improvement in polariton lifetime through isotopic enrichment of hexagonal boron nitride (hBN). Commensurate increases in the polariton propagation length are demonstrated via direct imaging of polaritonic standing waves by means of infrared nano-optics. Our results provide the foundation for a materials-growth-directed approach towards realizing the loss control necessary for the development of PhP-based nanophotonic devices.

Surface-phonon polaritons (SPhPs) are attractive alternatives to far-infrared plasmonics for sub-diffractional confinement of light. Localized SPhP resonances in semiconductor nanoresonators are very narrow, but that linewidth and the limited extent of the Reststrahlen band inherently limit spectral coverage. To address this limitation, we report active tuning of SPhP resonances in InP and 4H-SiC by photoinjecting free carriers into the nanoresonators, taking advantage of the coupling between the carrier plasma and optical phonons to blue-shift SPhP resonances. We demonstrate state-of-the-art tuning figures of merit upon continuous-wave (CW) excitation (in InP) or pulsed excitation (in 4H-SiC). Lifetime effects cause the tuning to saturate in InP, and carrier-redistribution leads to rapid (<50 ps) recovery of the tuning in 4H-SiC. This work opens the path toward actively tuned nanophotonic devices, such as modulators and beacons, in the infrared and identifies important implications of coupling between electronic and photonic excitations.

We use scanning near-field optical microscopy to study the response of hexagonal boron nitride nanocones at infrared frequencies, where this material behaves as a hyperbolic medium. The obtained images are dominated by a series of hot rings that occur on the sloped sidewalls of the nanocones. The ring positions depend on the incident laser frequency and the nanocone shape. Both dependences are consistent with directional propagation of hyperbolic phonon polariton rays that are launched at the edges and zigzag through the interior of the nanocones, sustaining multiple internal reflections off the sidewalls. Additionally, we observe a strong overall enhancement of the near-field signal at discrete resonance frequencies. These resonances attest to low dielectric losses that permit coherent standing waves of the sub-diffractional polaritons to form. We comment on potential applications of such shape-dependent resonances and the field concentration at the hot rings., Comment: Accepted for publication in Nano Letters

Strongly anisotropic media where the principal components of the dielectric tensor have opposite signs are called hyperbolic. Such materials length exhibit unique nanophotonic properties enabled by the highly directional propagation of slow-light modes localized at deeply sub-diffractional scales. While artificial hyperbolic metamaterials have been demonstrated, they suffer from high plasmonic losses and require complex nanofabrication, which in turn induces the size-dependent limitations on optical confinement. The low-loss, mid-infrared, natural hyperbolic material, hexagonal boron nitride is an attractive alternative. We observe four series of multiple (up to seven) 'hyperbolic polariton' modes in boron nitride nanocones in two spectral bands. The resonant modes obey the predicted aspect ratio dependence and exhibit record-high quality factors (Q up to 283) in the strong confinement regime (lambda/86 in the smallest structures). These observations assert hexagonal boron nitride as a promising platform for studying novel regimes of light-matter interactions and nanophotonic device engineering.