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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. 

Hyperbolic phonon polaritons (HPhPs) enable strong confinements, low losses, and intrinsic beam steering capabilities determined by the refractive index anisotropy—providing opportunities from hyperlensing to flat optics and other applications. Here, two scanning-probe techniques, photothermal induced resonance (PTIR) and scattering-type scanning near-field optical microscopy (s-SNOM), are used to map infrared (6.4–7.4 µm) HPhPs in large (up to 120 × 250 µm2) near-monoisotopic (>99% 10B) hexagonal boron nitride (hBN) flakes. Wide (≈40 µm) PTIR and s-SNOM scans on such large flakes avoid interference from polaritons launched from different asperities (edges, folds, surface defects, etc.) and together with Fourier analyses (0.05 µm−1 resolution) enable precise measurements of HPhP lifetimes (up to ≈4.2 ps) and propagation lengths (up to ≈25 and ≈17 µm for the first- and second-order branches, respectively). With respect to naturally abundant hBN, we report an eightfold improved, record-high (for hBN) propagating figure of merit (i.e., with both high confinement and long lifetime) in ≈99% 10B hBN, achieving, finally, theoretically predicted values. We show that wide near-field scans critically enable accurate estimates of the polaritons’ lifetimes and propagation lengths and that the incidence angle of light, with respect to both the sample plane and the flake edge, needs to be considered to extract correctly the dispersion relation from the near-field polaritons maps. Overall, the measurements and data analyses employed here elucidate details pertaining to polaritons’ propagation in isotopically enriched hBN and pave the way for developing high-performance HPhP-based devices. 

Abstract As the length scales of materials decrease, the heterogeneities associated with interfaces become almost as important as the surrounding materials. This has led to extensive studies of emergent electronic and magnetic interface properties in superlattices 1–9 . However, the interfacial vibrations that affect the phonon-mediated properties, such as thermal conductivity 10,11 , are measured using macroscopic techniques that lack spatial resolution. Although it is accepted that intrinsic phonons change near boundaries 12,13 , the physical mechanisms and length scales through which interfacial effects influence materials remain unclear. Here we demonstrate the localized vibrational response of interfaces in strontium titanate–calcium titanate superlattices by combining advanced scanning transmission electron microscopy imaging and spectroscopy, density functional theory calculations and ultrafast optical spectroscopy. Structurally diffuse interfaces that bridge the bounding materials are observed and this local structure creates phonon modes that determine the global response of the superlattice once the spacing of the interfaces approaches the phonon spatial extent. Our results provide direct visualization of the progression of the local atomic structure and interface vibrations as they come to determine the vibrational response of an entire superlattice. Direct observation of such local atomic and vibrational phenomena demonstrates that their spatial extent needs to be quantified to understand macroscopic behaviour. Tailoring interfaces, and knowing their local vibrational response, provides a means of pursuing designer solids with emergent infrared and thermal responses. 

Abstract The anisotropy of hexagonal boron nitride (hBN) gives rise to hyperbolic phonon-polaritons (HPhPs), notable for their volumetric frequency-dependent propagation and strong confinement. For frustum (truncated nanocone) structures, theory predicts five, high-order HPhPs, sets, but only one set was observed previously with far-field reflectance and scattering-type scanning near-field optical microscopy. In contrast, the photothermal induced resonance (PTIR) technique has recently permitted sampling of the full HPhP dispersion and observing such elusive predicted modes; however, the mechanism underlying PTIR sensitivity to these weakly-scattering modes, while critical to their understanding, has not yet been clarified. Here, by comparing conventional contact- and newly developed tapping-mode PTIR, we show that the PTIR sensitivity to those weakly-scattering, high-Q (up to ≈280) modes is, contrary to a previous hypothesis, unrelated to the probe operation (contact or tapping) and is instead linked to PTIR ability to detect tip-launched dark, volumetrically-confined polaritons, rather than nanostructure-launched HPhPs modes observed by other techniques. Furthermore, we show that in contrast with plasmons and surface phonon-polaritons, whose Q -factors and optical cross-sections are typically degraded by the proximity of other nanostructures, the high- Q HPhP resonances are preserved even in high-density hBN frustum arrays, which is useful in sensing and quantum emission applications.