Displacive lattice excitation through nonlinear phononics viewed by femtosecond X-ray diffraction

The nonlinear lattice dynamics of La_0.7Sr_0.3MnO₃, as initiated by strong mid-infrared femtosecond pulses made resonant with a specific lattice vibration, are measured with ultrafast X-ray diffraction at the LCLS free electron laser. Our experiments show that large amplitude excitation of an infrared-active stretching mode leads also to a displacive motion along the coordinate of a second, anharmonically coupled, Raman mode. This rectification of the vibrational field is described within the framework of the Ionic Raman Scattering theory and explains how direct lattice excitation in the nonlinear regime can induce a structural phase transition.