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.
Highlights
Strong vibrational excitations of solids are able to modify electronic correlations in a material and induce emergent states of matter that do not exist in equilibrium [1,2]
We synthesize the physics of nonlinear phononics and strong light-matter coupling to overcome frequency mismatches in phononic scattering processes
We show the response of the phonon modes to an excitation by a terahertz pulse with E0 = 7 MV/cm and τ = 500 fs in Fig. 3, which is structured analogously to Fig. 2
Summary
Strong vibrational excitations of solids are able to modify electronic correlations in a material and induce emergent states of matter that do not exist in equilibrium [1,2]. This polaritonic engineering has been used to modify electronic excitations, such as plasmons and excitons [34,35,36] and to modulate the chemical landscape of molecules [37,38,39,40,41], and various studies suggest an influence of strong light-matter coupling on superconductivity [42,43,44,45]. The coefficient d is nonzero only in noncentrosymmetric (e.g., ferroelectric or polar) materials
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