Tensile Control of Vibrational Strong Light‐Matter Coupling with Flexible Polyester Films

Abstract Polaritons are generated by strong interaction between photons and matter, with the hybridization fundamentally changing the energy landscape of the system. Future exploitation of polaritons will benefit from implementing low‐cost, flexible, and easily tuneable configurations, as electronics have before. Here, coherent coupling of the carbonyl stretch vibrations of polyester (poly(ethylene terephthalate), PET) films to the optical modes of a Fabry–Perot (FP) cavity is presented, in which the FP cavity is directly formed on flexible, free‐standing, and commercially available PET films. For 2‐µm thick PET films, the carbonyl stretch vibration of the PET overlaps with the half‐wavelength FP cavity mode, leading to the coupling of the two modes, a Rabi splitting above 160 cm⁻¹, and associated anticrossing in angular dispersion measurements. The study demonstrates dynamic control of light‐matter interaction strength by modulating film thickness under tension, finding that a 25% tensile stretch can tune the light‐matter interaction from 20:80 mixing to near‐perfect 50:50 hybridization at normal incidence. These findings are discussed in the context of future foldable/twistable/wearable polaritonic devices.