Multistate control of nonlinear photocurrents in ferroelectric IV-monochalcogenide monolayers via phase manipulation of the light field

Abstract

Ultrafast optical control of ferroelectricity using short, intense light pulses enables precise manipulation of ferroelectric materials, offering potential breakthroughs in nonvolatile memory technologies. We demonstrate that phase manipulation of electric fields in the strong-field sub-cycle regime induces nonlinear injection currents that couple efficiently with band topology, dynamically reversing both current and polarization. Time-dependent first-principles calculations show that tuning the phase of linearly or circularly polarized light-via chirp or carrier-envelope phase-breaks time-reversal symmetry, allowing control over multi-ferroelectric states. In SnTe monolayers, nonlinear coupling between current and band topology enables dynamic ferroelectric manipulation. Time- and momentum-resolved transverse current analysis highlights the role of Berry curvature multipoles, linking odd/even orders to pseudo-harmonics that drive polarization reversal. These phase manipulations of short pulse waveforms may lead to control of nonlinear photocurrents and polarization states, paving the way for precise ultrafast opto-ferroelectric devices.