Cavity control of nonlinear phononics

Abstract: Nonlinear interactions between phonon modes govern the behavior of vibrationally highly excited solids and molecules. Here, we demonstrate theoretically that optical cavities can be used to control the redistribution of energy from a highly excited coherent infrared-active phonon state into the other vibrational degrees of freedom of the system. The hybridization of the infrared-active phonon mode with the fundamental mode of the cavity induces a polaritonic splitting that we use to tune the nonlinear interactions with other vibrational modes in and out of resonance. We show that not only can the efficiency of the redistribution of energy be enhanced or decreased, but also the underlying scattering mechanisms may be changed. This work introduces the concept of cavity control to the field of nonlinear phononics, enabling nonequilibrium quantum optical engineering of new states of matter.