Ultrafast reversal of the ferroelectric polarization by a midinfrared pulse

TL;DR

This paper models the ultrafast reversal of ferroelectric polarization in LiNbO₃ induced by a midinfrared pulse, explaining experimental observations through nonlinear phonon coupling and depolarizing fields.

Contribution

It provides a theoretical framework for understanding polarization reversal dynamics driven by midinfrared pulses, incorporating symmetry-invariant thermodynamic potential and numerical solutions.

Findings

Transient polarization reversal explained by depolarizing electric field

Estimate of depolarizing field magnitude consistent with experiments

Polarization reversal could be achieved with effective screening

Abstract

We calculate the ferroelectric polarization dynamics induced by a femtosecond midinfrared pulse as measured in the recent experiment by R. Mankowsky et al., Phys. Rev. Lett. 118, 197601 (2017). It is due to the nonlinear coupling of the excited infrared-active phonon with the ferroelectric mode or to the excitation of the ferroelectric mode itself depending on the pulse frequency. To begin with, we write the LiNbO$_3$ crystal symmetry invariant thermodynamic potential including electric field and nonlinear phonon coupling terms. We solve the equations of motion determined by this potential for phonon coordinates numerically in classical approximation. We explain the transient polarization reversal observed in the experiment by action of the depolarizing electric field which is due to bound charges at the polarization domain boundaries and give a reasonable estimate for its value. We argue that the polarization could be ultimately reversed when this field is screened.