Terahertz field-induced giant symmetry modulations in a van der Waals antiferromagnet

Abstract

Strong-field terahertz (THz) excitations enable dynamic control over electronic, lattice and symmetry degrees of freedom in quantum materials. Here, we uncover pronounced terahertz-induced symmetry modulations and coherent phonon dynamics in the van der Waals antiferromagnet MnPS3, in which inversion symmetry is broken by its antiferromagnetic spin configuration. Time-resolved second harmonic generation measurements reveal long-lived giant oscillations in the antiferromagnetic phase, with amplitudes comparable to the equilibrium signal, driven by phonons involving percent-level atomic displacements relative to the equilibrium bond lengths. The temporal evolution of the rotational anisotropy patterns indicate a dynamic breaking of mirror symmetry, modulated by two vibrational modes at 1.7 THz and 4.5 THz, with the former corresponding to a hidden mode not observed in equilibrium spectroscopy. We show that these effects arise in part from a field-induced charge rearrangement mechanism that lowers the local crystal symmetry, and couples to the phonon modes. A long-lived field-driven response was uncovered with a complex THz polarization dependence which, in comparison to theory, indicates evidence for an antiferromagnetic-to-ferrimagnetic transition. Our results establish an effective field-tunable pathway for driving excitations otherwise weak in equilibrium, and for manipulating magnetism in low-dimensional materials via dynamical modulation of symmetry.