Light-Driven Ultrafast Control of Time-Reversal Symmetry in SrTiO3

Abstract

Light-driven control of material symmetry enables the engineering of phenomena forbidden in equilibrium. Although electromagnetic fields have been used to break time-reversal symmetry, its dynamic control on ultrafast timescales in nonmagnetic insulating oxides remains virtually unexplored. Here, we demonstrate simultaneous magnetic symmetry lowering and timereversal-symmetry breaking in cubic SrTiO3 driven by an off-resonant, elliptically polarized THz pulse. Second harmonic generation (SHG) polarimetry reveals emergent SHG circular dichroism inconsistent with third-order nonlinear processes under cubic m3m symmetry. The SHG polar patterns exhibit mirror-symmetry breaking, indicating a transient reduction to tetragonal 4/mm'm' magnetic symmetry. Furthermore, the SHG response scales linearly with the angular momentum of THz pulse, providing direct evidence for THz-field-induced timereversal-symmetry breaking. These results establish a direct pathway for ultrafast symmetry control in non-magnetic oxides, enabling dynamic manipulation of emergent phases on ultrafast timescales.