Transient Terahertz Oscillations During Photoinduced Polarization Topology Reconfiguration in Ferroelectric Superlattices

초록

Terahertz resonances embedded in crystalline heterostructures could close a spectral gap between conventional electronics and photonics while opening new windows on phenomena in non-equilibrium lattice dynamics. We show that femtosecond optical screening of the depolarization field in epitaxial PbTiO3/SrTiO3 superlattices launches a collective polar mode that oscillates near 1 THz and coherently spans the entire mini-Brillouin zone. Wave-vector-resolved pump-probe X-ray diffraction resolves a nearly dispersion-less oscillation at 0.87 and 0.94 THz at the zone boundary and zone center, respectively, persisting for similar to 2.5 ps, corresponding to a weakly damped resonance. Dynamical phase-field simulations reveal the origin of the mode to mesoscopic rotation of closure-domain textures during the photoexcited transition from an unscreened to a screened electrostatic state. Varying the PbTiO3 and SrTiO3 ratio tunes the mode frequency continuously from 0.9 to 1.4 THz, providing a quantitative design rule for frequency-selectable THz oscillators in ferroelectric heterostructures. By coupling nanoscale polarization reconfiguration to long-wavelength coherent dynamics, this work establishes depolarization-field engineering to topology-driven THz functionality and expanding the landscape of collective lattice dynamics.

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