Dirac plasmon polaritons in topological insulators (TIs),light coupled to massless Dirac electrons, have been attracting a large amount of attention, both from a fundamental perspective and for potential terahertz (THz) photonic applications. Althoug
h THz polaritons have been observed by far-field THz spectroscopy on TI microstructures, real-space imaging of propagating THz polaritons in unstructured TIs has been elusive so far. Here, we show the very first spectroscopic THz near-field images of thin Bi2Se3 layers (prototypical TIs) revealing polaritons with up to 12 times increased momenta as compared to photons of the same energy and decay times of about 0.24 ps, yet short propagation lengths. From the near-field images we determine the polariton dispersions in layers from 120 to 25 nm thickness and perform a systematic theoretical dispersion analysis, showing that the observed polaritons can be explained only by the simultaneous coupling of THz radiation to Dirac carriers at the TI surfaces, massive bulk carriers and optical phonons. Our work does not only provide critical insights into the nature of THz polaritons in TIs, but also establishes instrumentation of unprecedented sensitivity for imaging of THz polaritons.
Phonon polaritons (PPs) in van der Waals (vdW) materials can strongly enhance light-matter interactions at mid-infrared frequencies, owing to their extreme infrared field confinement and long lifetimes. PPs thus bear potential for achieving vibration
al strong coupling (VSC) with molecules. Although the onset of VSC has recently been observed spectroscopically with PP nanoresonators, no experiments so far have resolved VSC in real space and with propagating modes in unstructured layers. Here, we demonstrate by real-space nanoimaging that VSC can be achieved between propagating PPs in thin vdW crystals (specifically h-BN) and molecular vibrations in adjacent thin molecular layers. To that end, we performed near-field polariton interferometry, showing that VSC leads to the formation of a propagating hybrid mode with a pronounced anti-crossing region in its dispersion, in which propagation with negative group velocity is found. Numerical calculations predict VSC for nanometer-thin molecular layers and PPs in few-layer vdW materials, which could make propagating PPs a promising platform for ultra-sensitive on-chip spectroscopy and strong coupling experiments.
Localized and propagating polaritons allow for highly sensitive analysis of (bio)chemical substances and processes. Nanoimaging of the polaritons evanescent fields allows for critically important experimental mode identification and for studying fiel
d confinement. Here we describe two setups for polariton nanoimaging and spectroscopy in liquid, which is an indispensable environment for (bio)chemical samples. We first demonstrate antenna mapping with a transflection infrared scattering-type scanning near-field optical microscope (s-SNOM), where the tip acts as a near-field scattering probe. We then demonstrate a total internal reflection (TIR) based setup, where the tip is both launching and probing ultra-confined polaritons in van der Waals materials, here phonon polaritons in hexagonal boron nitride (h-BN) flakes. This work lays the foundation for s-SNOM based polariton interferometry in liquid, which has wide application potential for in-situ studies of chemical reactions at the bare or functionalized surface of polaritonic materials, including (bio)chemical recognition analogous to the classical surface plasmon resonance spectroscopy.
