Strong coupling (SC) between light and matter excitations
bears
intriguing potential for manipulating material properties. Typically,
SC has been achieved between mid-infrared (mid-IR) light and molecular
vibrations or between visible light and excitons. However, simultaneously
achieving SC in both frequency bands remains unexplored. Here, we
introduce polaritonic nanoresonators (formed by h-BN layers on Al
ribbons) hosting surface plasmon polaritons (SPPs) at visible frequencies
and phonon polaritons (PhPs) at mid-IR frequencies, which simultaneously
couple to excitons and molecular vibrations in an adjacent layer of
CoPc molecules, respectively. Employing near-field optical nanoscopy,
we demonstrate the colocalization of near fields at both visible and
mid-IR frequencies. Far-field transmission spectroscopy of the nanoresonator
structure covered with a layer of CoPc molecules shows clear mode
splittings in both frequency ranges, revealing simultaneous SPP–exciton
and PhP–vibron coupling. Dual-band SC may offer potential for
manipulating coupling between exciton and molecular vibration in future
optoelectronics, nanophotonics, and quantum information applications.