Broad-temperature-range ultrafast terahertz excitation of collective dynamics in polar skyrmions

Abstract: Ultrafast coherent control of electric dipoles using strong terahertz (THz) pulses provides a means to discover hidden phases of materials and potentially leads to applications in high-speed electro-optic devices. The effectiveness of this means, albeit demonstrated in architype (incipient) ferroelectric systems such as SrTiO3, hinges on a spectral overlapping between their soft phonon modes within the excitation bandwidth of THz pulses. Generally this can only induce an appreciable coupling close to the phase transition temperatures, where the lattice phonons substantially soften. Because of their emergent subterahertz collective dynamics, a fundamentally distinct and effective THz coupling mechanism can be envisaged in topological polar structures recently discovered in PbTiO3/SrTiO3 superlattices. Here, we show that polar skyrmions can be coherently driven into a hidden phase with transient macroscopic polarization, as probed based on THz field-induced second harmonic generation and optical Kerr effects. Such an ultrafast THz-driven phase transition is found to sustain across a broad temperature range of 4-470 K, in accordance with the equilibrium stability field of the skyrmions. Supplemented by dynamical phase-field simulations, we identify the spatial symmetries and relaxation behaviors of the excited collective modes, thereby revealing their correlation with the emergence of the polar phases. Our results unveil the exotic dynamical properties of topological polar structures, which could be technologically exploited given their remarkable flexibility in structure design and tunability under external fields.