Theory of nonlinear phononics for coherent light control of solids

We present a microscopic theory for ultrafast control of solids with high-intensity terahertz frequency optical pulses. When resonant with selected infrared-active vibrations, these pulses transiently modify the crystal structure and lead to new collective electronic properties. The theory predicts the dynamical path taken by the crystal lattice using first-principles calculations of the energy surface and classical equations of motion, as well as symmetry considerations. Two classes of dynamics are identified. In the perturbative regime, displacements along the normal mode coordinate of symmetry-preserving Raman active modes can be achieved by cubic anharmonicities. This explains the light-induced insulator-to-metal transition reported experimentally in manganites. We predict a regime in which ultrafast instabilities that break crystal symmetry can be induced. This nonperturbative effect involves a quartic anharmonic coupling and occurs above a critical threshold, below which the nonlinear dynamics of the driven mode displays softening and dynamical stabilization.