Polaritons, which are quasiparticles composed of a photon coupled to an electric or magnetic dipole, are a major focus in nanophotonic research of van der Waals (vdW) crystals and their derived 2D materials. For the variety of existing vdW materials, polaritons can be active in a broad range of the electromagnetic spectrum (meVs to eVs) and exhibit momenta much higher than the corresponding free-space radiation. Hence, the use of high momentum broadband sources or probes is imperative to excite those quasiparticles and measure the frequency-momentum dispersion relations, which provide insights into polariton dynamics. Synchrotron infrared nanospectroscopy (SINS) is a technique that combines the nanoscale spatial resolution of scattering-type scanning near-field optical microscopy with ultrabroadband synchrotron infrared radiation, making it highly suitable to probe and characterize a variety of vdW polaritons. Here, the advances enabled by SINS on the study of key photonic attributes of far- and mid-infrared plasmon- and phonon-polaritons in vdW and 2D crystals are reviewed. In that context the SINS technique is comprehensively described and it is demonstrated how fundamental polaritonic properties are retrieved for a range of atomically thin systems including hBN, MoS2, graphene and 2D heterostructures.

Talc is an insulating layered material that is stable at ambient conditions and has high-quality basal cleavage, which is a major advantage for its use in van der Waals heterostructures. Here, we use near-field synchrotron infrared nanospectroscopy, Raman spectroscopy, and first-principles calculations to investigate the structural and vibrational properties of talc crystals, ranging from monolayer to bulk, in the 300-750 and <60 cm-1 spectral windows. We observe a symmetry crossover from mono to bilayer talc samples, attributed to the stacking of adjacent layers. The in-plane lattice parameters and frequencies of intralayer modes of talc display weak dependence on the number of layers, consistent with a weak interlayer interaction. On the other hand, the low-frequency (<60 cm-1) rigid-layer (interlayer) modes of talc are suitable to identify the number of layers in ultrathin talc samples, besides revealing strong in-plane and out-of-plane anisotropy in the interlayer force constants and related elastic stiffnesses of single crystals. The shear and breathing force constants of talc are found to be 66 and 28%, respectively, lower than those of graphite, making talc an excellent lubricant that can be easily exfoliated. Our results broaden the understanding of the structural and vibrational properties of talc at the nanoscale regime and serve as a guide for future ultrathin heterostructures applications.

The exploitation of phonon-polaritons in nanostructured materials offers a pathway to manipulate infrared (IR) light for nanophotonic applications. Notably, hyperbolic phonon-polaritons (HP2) in polar bidimensional crystals have been used to demonstrate strong electromagnetic field confinement, ultraslow group velocities, and long lifetimes (up to ∼12 ps). Here we present nanobelts of α-phase molybdenum trioxide (α-MoO3) as a low-dimensional medium supporting HP2 modes in the mid- and far-IR ranges. Through real-space nanoimaging techniques with synchrotron and tunable laser IR light, we observe HP2 Fabry-Perot resonances that demonstrate distinct anisotropic propagation and frequency dependence. We remark an anisotropic propagation that critically depends on the frequency range. Our findings are supported by the convergence of experiment, theory, and numerical simulations. Our work shows that the low dimensionality of natural nanostructured crystals, like α-MoO3 nanobelts, provides an attractive platform to study polaritonic light-matter interactions and offers appealing cavity properties that could be harnessed in future designs of compact nanophotonic devices.

Hyperbolic phonon polaritons have recently attracted considerable attention in nanophotonics mostly due to their intrinsic strong electromagnetic field confinement, ultraslow polariton group velocities, and long lifetimes. Here we introduce tin oxide (SnO₂) nanobelts as a photonic platform for the transport of surface and volume phonon polaritons in the mid- to far-infrared frequency range. This report brings a comprehensive description of the polaritonic properties of SnO₂ as a nanometer-sized dielectric and also as an engineered material in the form of a waveguide. By combining accelerator-based IR-THz sources (synchrotron and free-electron laser) with s-SNOM, we employed nanoscale far-infrared hyper-spectral-imaging to uncover a Fabry-Perot cavity mechanism in SnO₂ nanobelts via direct detection of phonon-polariton standing waves. Our experimental findings are accurately supported by notable convergence between theory and numerical simulations. Thus, the SnO₂ is confirmed as a natural hyperbolic material with unique photonic properties essential for future applications involving subdiffractional light traffic and detection in the far-infrared range.

Polaritons, i.e., hybrid quasi-particles of light and matter resonances, have been extensively investigated due to their potential to enhance light-matter interactions. Although polaritonic applications thrive in the mid-infrared range, their extension to the terahertz (THz) range remains limited. Here, we present paratellurite (α-TeO2) nanowires, a versatile material acting as a platform for different types of phonon polaritons. Utilizing synchrotron infrared nanospectroscopy from 10 to 24 THz, we uncover the polaritonic properties of α-TeO2 nanowires, showcasing their dual functionality as both a Fabry-Pérot cavity and a waveguide for surface phonon polaritons. Furthermore, near-field measurements with a free-electron laser as a THz source reveal a localized optical contrast down to 5.5 THz, an indication of hyperbolic bands. Our findings complement the repertoire of polaritonic materials, with significant implications for advancing THz technologies.