Hybrid THz architectures for molecular polaritonics

Nature Communications 15, 4427 (2024) Physical and chemical properties of materials can be modified by a resonant optical mode. Such recent demonstrations have mostly relied on a planar cavity geometry, others have relied on a plasmonic resonator. However, the combination of these two device architectures have remained largely unexplored, especially in the context of maximizing light-matter interactions. Here, we investigate several schemes of electromagnetic field confinement aimed at facilitating the collective coupling of a localized photonic mode to molecular vibrations in the terahertz region. The key aspects are the use of metasurface plasmonic structures combined with standard Fabry-Perot configurations and the deposition of a thin layer of glucose, via a spray coating technique, within a tightly focused electromagnetic mode volume. More importantly, we demonstrate enhanced vacuum Rabi splittings reaching up to 200 GHz when combining plasmonic resonances, photonic cavity modes and low-energy molecular resonances. Furthermore, we demonstrate how a cavity mode can be utilized to enhance the zero-point electric field amplitude of a plasmonic resonator. Our study provides key insight into the design of polaritonic platforms with organic molecules to harvest the unique properties of hybrid light-matter states.