Strong light‐matter coupling between a molecular vibrational mode in a PMMA film and a low‐loss mid‐IR microcavity

Microcavity devices exhibiting strong light‐matter coupling in the mid‐infrared spectral range offer the potential to explore exciting open physical questions pertaining to energy transfer between heat and light and can lead to a new generation of efficient wavelength tunable mid‐infrared sources of coherent light based on polariton Bose‐Einstein Condensation. Vibrational transitions of organic molecules, which often have strong absorption peaks in the infrared and considerably narrower linewidths than organic excitonic resonances, can generate polaritonic states in the mid‐infrared spectral range using microcavity devices. Here, narrow linewidth polaritonic resonances are exhibited in the mid‐infrared by coupling the carbonyl stretch vibrational transition of a polymethyl methacrylate film to the photonic resonance of a low optical‐loss mid‐infrared microcavity, which consisted of two Ge/ZnS dielectric Bragg reflectors. Rabi‐splitting of 14.3 meV is observed, with a 4.4 meV polariton linewidth at anti‐crossing. The large Rabi‐splitting relative to linewidth indicates efficient impedance‐matching between the bare vibrational and photonic states, and suggests molecular‐vibration polaritons incorporated in dielectric microcavities can be an enabling step towards realizing polariton optical switching and polariton condensation in the mid‐infrared spectral range.