Optical phase control induced by molecular vibrations in strongly driven infrared nanoresonators

Recent experimental advances on quantum control with mid-IR nanoresonators have stimulated the development of quantum theory that can accurately describe driven-dissipative light-matter physics in the quantum few-photon regime. We propose a semi-empirical quantum optics approach to describe light-matter interaction between nanoconfined resonant fields with ensembles of molecular vibrations in the mid-IR, subject to ultrafast laser driving with femtosecond pulses. For strong pulses that moderately deplete the vacuum field level, the model predicts the ability to implement coherent intensity-dependent phase shifts on the scattered output pulse at room temperature, which rely on a dynamical blockade effect that occurs naturally for weak light-matter coupling due to the anharmonicity of the vibrational potential [1]. The scaling of the proposed phase shifts with molecule number is also discussed. Our results suggest novel applications of vibration-nanoantenna systems for quantum control and quantum information processing in the mid-infrared regime.