Frequency renormalization and its effects in nonlinear phononics with $Q_RQ_{IR}^{2}$-type coupling

Abstract

A two-phonon system with lowest-order coupling of form $Q_RQ_{IR}^2$ is studied by perturbation method, and analytic results for both phonon displacements and frequencies are obtained. The frequency renormalization of infrared (IR) active mode brings the rectification of Raman mode to saturate at high pump field. For degenerate IR mode with coupling of form $Q_R(Q_{IR,x}^2-Q_{IR,y}^2)$, the frequency of IR mode will split when resonantly pumped by elliptically or linearly polarized ultrashort mid-IR pulse, realizing Raman rectification and magnetization simultaneously. Our results reveal a dynamical effect of nonlinear phononics not captured by first-principles calculation, extend the dynamical multiferroicity to systems with coupling $Q_R(Q_{IR,x}^2-Q_{IR,y}^2)$, and the method can be readily applied to higher-order couplings. The amplitude saturation under strong pump field stimulates future researches to overcome this nonlinear effect.