- Chen, F;
- Zhu, Y;
- Liu, S;
- Qi, Y;
- Hwang, HY;
- Brandt, NC;
- Lu, J;
- Quirin, F;
- Enquist, H;
- Zalden, P;
- Hu, T;
- Goodfellow, J;
- Sher, M-J;
- Hoffmann, MC;
- Zhu, D;
- Lemke, H;
- Glownia, J;
- Chollet, M;
- Damodaran, AR;
- Park, J;
- Cai, Z;
- Jung, IW;
- Highland, MJ;
- Walko, DA;
- Freeland, JW;
- Evans, PG;
- Vailionis, A;
- Larsson, J;
- Nelson, KA;
- Rappe, AM;
- Sokolowski-Tinten, K;
- Martin, LW;
- Wen, H;
- Lindenberg, AM
The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here we apply subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO3 ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray-scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large-amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent across unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond time scales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables a direct comparison with first-principles-based molecular-dynamics simulations, with good agreement obtained.