Optically Helicity-Dependent Orbital and Spin Dynamics in Two-Dimensional Ferromagnets

Abstract: Disentangling orbital (OAM) and spin (SAM) angular momenta in the ultrafast spin dynamics of two-dimensional (2D) ferromagnets on subfemtoseconds is a challenge in the field of ultrafast magnetism. Herein, we employed non-collinear spin version of real-time time-dependent density functional theory to investigate the orbital and spin dynamics of 2D ferromagnets Fe3GeTe2 (FGT) induced by circularly polarized light. Our results show the demagnetization of Fe sublattice in FGT is accompanied by helicity-dependent precession of OAM and SAM excited by circularly polarized lasers. We further identify that precession of OAM and SAM in FGT is faster than the demagnetization within a few femtoseconds. Remarkably, circularly polarized lasers can significantly induce a periodically transverse response of OAM and SAM on very ultrafast timescales of ~250 attoseconds. Our finding suggests a powerful new route for attosecond regimes of the angular momentum manipulation to coherently control helicity-dependent orbital and spin dynamics in 2D limits.