LAUSR

Vibrational strong coupling (VSC), the strong coupling between optical resonances and the dipolar absorption of molecular vibrations at mid‐infrared frequencies, holds the great potential for the development of ultrasensitive infrared spectroscopy, the modification of chemical properties of molecules, and the control of chemical reactions. In the realm of ultracompact VSC, there is a need to scale down the size of mid‐infrared optical resonators and to elevate their optical field strength. Herein, by using single quartz micropillars as mid‐infrared optical resonators, the strong coupling is demonstrated between surface phonon polariton (SPhP) resonances and molecular vibrations from far‐field observation. The single quartz micropillars support sharp SPhP resonances with an ultrasmall mode volume, which strongly couples with the molecular vibrations of 4‐nitrobenzyl alcohol (C7H7NO3) molecules featuring pronounced mode splitting and anticrossing dispersion. The coupling strength depends on the molecular concentration and reaches the strong coupling regime with only 7300 molecules. The findings pave the way for promoting the VSC sensitivity, miniaturing the VSC devices, and will boost the development of ultracompact mid‐infrared spectroscopy and chemical reaction control devices.