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Nanomaterials capable of confining light are desirable for enhancingspectroscopies such as Raman scattering, infrared absorption, and nonlinearoptical processes. Plasmonic superlattices have shown the ability to hostcollective resonances in the mid-infrared, but require stringent fabricationprocesses to create well-ordered structures. Here, we demonstrate howshort-range-ordered Au nanoparticle multilayers on a mirror, self-assembled bya sub-nm molecular spacer, support collective plasmon-polariton resonances inthe visible and infrared, continuously tunable beyond 11 $\mu$m by simplyvarying the nanoparticle size and number of layers. The resultingmolecule-plasmon system approaches vibrational strong coupling, and displaysgiant Fano dip strengths, SEIRA enhancement factors ~10$^6$, light-mattercoupling strengths g~100 cm$^{-1}$, Purcell factors ~10$^6$, and mode volumecompression factors ~10$^8$. The collective plasmon-polariton mode is highlyrobust to nanoparticle vacancy disorder and is sustained by the consistent gapsize defined by the molecular spacer. Structural disorder efficiently coupleslight into the gaps between the multilayers and mirror, enabling Raman andinfrared sensing of sub-picolitre sample volumes.

Giant mid-IR resonant coupling to molecular vibrations in sub-nm gaps of plasmonic multilayer metafilms