Ultrafast simultaneous manipulation of multiple ferroic orders through nonlinear phonon excitation

TL;DR

This paper demonstrates that nonlinear phonon excitation can simultaneously manipulate ferroelectric and antiferromagnetic orders in BiFeO3, revealing a new ultrafast control method for multiple ferroic properties.

Contribution

It shows for the first time that resonant excitation of a phonon mode can concurrently enhance multiple ferroic orders in a single material, supported by first-principles and phenomenological models.

Findings

Concurrent enhancement of ferroelectric and antiferromagnetic SHG in BiFeO3

Coupling of ferroic orders to lattice distortions via nonlinear phonons

Potential for ultrafast control of multiple ferroic properties

Abstract

Recent experimental studies have demonstrated the possibility of utilizing strong terahertz pulses to manipulate individual ferroic orders on pico- and femtosecond timescales. Here, we extend these findings and showcase the simultaneous manipulation of multiple ferroic orders in BiFeO$_3$, a material that is both ferroelectric and antiferromagnetic at room temperature. We find a concurrent enhancement of ferroelectric and antiferromagnetic second-harmonic generation (SHG) following the resonant excitation of a high-frequency fully-symmetric phonon mode. Based on first-principles calculations and phenomenological modeling, we ascribe this observation to the inherent coupling of the two ferroic orders to the nonequilibrium distortions induced in the crystal lattice by nonlinearly driven phonons. Our finding highlights the potential of nonlinear phononics as a technique for manipulating multiple ferroic order parameters at once. In addition, this approach provides a promising avenue to studying the dynamical magnetization and polarization behavior, as well as their intrinsic coupling, on ultrashort timescales.