Multistate Control of Nonlinear Photocurrents in Optoferroelectrics via phase manipulation of light field

TL;DR

This paper demonstrates that phase manipulation of ultrafast light pulses can control nonlinear photocurrents and polarization states in optoferroelectrics, enabling dynamic switching of ferroelectric states for advanced ultrafast optoelectronic devices.

Contribution

It introduces a novel method of controlling ferroelectric polarization via phase manipulation of light in the strong field regime, revealing new mechanisms involving Berry curvature multipoles.

Findings

Phase manipulation induces nonlinear injection currents.

Time-reversal symmetry breaking enables polarization reversal.

Berry curvature multipoles are key to polarization dynamics.

Abstract

Ultrafast optical control of ferroelectricity based on short and intense light can be utilized to achieve accurate manipulations of ferroelectric materials, which may pave a basis for future breakthrough in nonvolatile memories. Here, we demonstrate that phase manipulation of electric field in the strong field sub-cycle regime induces a nonlinear injection current, efficiently coupling with the topology of band structure and enabling dynamic reversal of both current and polarization. Our time-dependent first-principles calculations reveal that tuning the phase of linearly or circularly polarized light through time-varying chirp, or constant carrier envelop phases within sub-laser-cycle dynamics effectively breaks the time-reversal symmetry, allowing the control over current and electronic polarization reversal over multi-ferroelectric states. Our time- and momentum-resolved transverse current analysis reveal the significance of Berry curvature higher order poles in the apparent association between the odd (even) orders of Berry curvature multipoles to odd (even) pseudo-harmonics in driving polarization dynamics reversal. We suggest that these phase manipulations of short pulse waveform may lead to unprecedented accurate control of nonlinear photocurrents and polarization states, which facilitate the development of precise ultrafast opto-ferroelectric devices.