Quantum nonlinear phononics route towards nonequilibrium materials engineering: Melting dynamics of a ferrielectric charge density wave

Abstract

Negative nonlinear electron-phonon coupling involving an infrared-active phonon mode can lead to an instability towards the formation of a polar lattice distortion with ferrielectric (FE) moments accompanied by an electronic charge-density wave (CDW). Analyzing a small model system in and out of thermal equilibrium, we investigate the FE-CDW and its melting dynamics following an ultrashort laser pulse that drives the ionic dipoles. We observe nonequilibrium coherent phonon amplitude mode oscillations that soften towards the transition to the normal phase. Our case study serves as a first step towards a microscopic understanding of quantum nonlinear phononics as a basis for nonequilibrium control in quantum materials.