Optical nanoimaging of highly-confined phonon polaritons in atomically-thin nanoribbons of α-MoO₃

Phonon polaritons (PhPs), collective modes hybridizing photons with lattice vibrations in polar insulators, enable nanoscale control of light. In recent years, the exploration of in-plane anisotropic PhPs has yielded new levels of confinement and directional manipulation of nano-light. However, the investigation of in-plane anisotropic PhPs at the atomic layer limit is still elusive. Here, we report the optical nanoimaging of highly-confined phonon polaritons in atomically-thin nanoribbons of α-MoO₃ (5 atomic layers). We show that narrow α-MoO₃ nanoribbons as thin as a few atomic layers can support anisotropic PhPs modes with a high confinement ratio (∼133 times smaller wavelength than that of light). The anisotropic PhPs interference fringe patterns in atomic layers are tunable depending on the PhP wavelength via changing the illumination frequency. Moreover, spatial control over the PhPs interference patterns is also achieved by varying the nanostructures' shape or nanoribbon width of atomically-thin α-MoO₃. Our work may serve as an empirical reference point for other anisotropic PhPs that approach the thickness limit and pave the way for applications such as atomically integrated nano-photonics and sensing.