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The terahertz (THz) frequency range is key to study collective excitations in many crystals and organic molecules. However, due to the large wavelength of THz radiation, the local probing of these excitations in smaller crystalline structures or few-molecular arrangements, requires sophisticated methods to confine THz light down to the nanometer length scale, as well as to manipulate such a confined radiation. For this purpose, in recent years, taking advantage of hyperbolic phonon polaritons (HPhP) in highly anisotropic van der Waals (vdW) materials has emerged as a promising approach, offering a multitude of manipulation options such as control over the wavefront shape and propagation direction. Here, we demonstrate the first THz application of twist-angle-induced HPhP manipulation, designing the propagation of confined THz radiation between 8.39 and 8.98 THz in the vdW material alpha-molybdenum trioxide ($\alpha-MoO_{3}$), hence extending twistoptics to this intriguing frequency range. Our images, recorded by near-field optical microscopy, show the frequency- and twist-angle-dependent change between hyperbolic and elliptic polariton propagation, revealing a polaritonic transition at THz frequencies. As a result, we are able to allocate canalization (highly collimated propagation) of confined THz radiation by carefully adjusting these two parameters, i.e. frequency and twist angle. Specifically, we report polariton canalization in $\alpha-MoO_{3}$ at 8.67 THz for a twist angle of 50{\deg}. Our results demonstrate an unprecedented control and the manipulation of highly-confined collective excitations at THz frequencies, offering novel possibilities for nanophotonic applications., Comment: 25 pages, 4 figures, article, submitted

Terahertz (THz) electromagnetic radiation is key to optically access collective excitations such as magnons (spins), plasmons (electrons), or phonons (atomic vibrations), thus bridging between optics and solid-state physics. Confinement of THz light to the nanometer length scale is desirable for local probing of such excitations in low dimensional systems, thereby inherently circumventing the large footprint and low spectral density of far-field THz optics. For that purpose, phonon polaritons (PhPs, i.e., light coupled to lattice vibrations in polar crystals) in anisotropic van der Waals (vdW) materials have recently emerged as a promising platform for THz nanooptics; yet the amount of explored, viable materials is still exiguous. Hence, there is a demand for the exploration of novel materials that feature not only THz PhPs at different spectral regimes, but also exhibit unique anisotropic (directional) electrical, thermoelectric, and vibronic properties. To that end, we introduce here the semiconducting alpha-germanium(II) sulfide (GeS) as an intriguing candidate. By employing THz nano-spectroscopy supported by theoretical analysis, we provide a thorough characterization of the different in-plane hyperbolic and elliptical PhP modes in GeS. We find not only PhPs with long life times ($\tau$ > 2 ps) and excellent THz light confinement ($\lambda_0/\lambda$ > 45), but also an intrinsic, phonon-induced anomalous dispersion as well as signatures of naturally occurring PhP canalization within one single GeS slab.

Electromagnetic field confinement is crucial for nanophotonic technologies, since it allows for enhancing light-matter interactions, thus enabling light manipulation in deep sub-wavelength scales. In the terahertz (THz) spectral range, radiation confinement is conventionally achieved with specially designed metallic structures - such as antennas or nanoslits - with large footprints due to the rather long wavelengths of THz radiation. In this context, phonon polaritons - light coupled to lattice vibrations - in van der Waals (vdW) crystals have emerged as a promising solution for controlling light beyond the diffraction limit, as they feature extreme field confinements and low optical losses. However, experimental demonstration of nanoscale-confined phonon polaritons at THz frequencies has so far remained elusive. Here, we provide it by employing scattering-type scanning near-field optical microscopy (s-SNOM) combined with a free-electron laser (FEL) to reveal a range of low-loss polaritonic excitations at frequencies from 8 to 12 THz in the vdW semiconductor ${\alpha}-MoO_3$. We visualize THz polaritons with i) in-plane hyperbolic dispersion, ii) extreme nanoscale field confinement (below ${\lambda}_o/75$) and iii) long polariton lifetimes, with a lower limit of > 2 ps.