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We show that light drives large-amplitude structural changes in thin films of the prototypical ferroelectric PbTiO[subscript 3] via direct coupling to its intrinsic photovoltaic response. Using time-resolved x-ray scattering to visualize atomic displacements on femtosecond time scales, photoinduced changes in the unit-cell tetragonality are observed. These are driven by the motion of photogenerated free charges within the ferroelectric and can be simply explained by a model including both shift and screening currents, associated with the displacement of electrons first antiparallel to and then parallel to the ferroelectric polarization direction.United States. Dept. of Energy (contract DE-FG02-07ER46431)United States. Office of Naval Research (grant N00014-06-1- 0459

Ultrafast Photovoltaic Response in Ferroelectric Nanolayers