Ultrafast Chiral Precession of Spin and Orbital Angular Momentum Induced by Circularly Polarized Laser Pulse in...

Despite spin (SAM) and orbital (OAM) angular momentum dynamics being well-studied in demagnetization processes, their components receive less focus. Here, we utilize real-time time-dependent density functional theory (rt-TDDFT) to unveil significant x and y components of SAM and OAM induced by circularly left (σ⁺) and right (σ^-) polarized laser pulses in ferromagnetic Fe, Co, and Ni. Our results show that the magnitude of the OAM is an order of magnitude larger than that of the SAM, highlighting a stronger optical response from the orbital degrees of freedom of electrons. Intriguingly, σ⁺ and σ^- pulses induce chirality in the precession of SAM and OAM, respectively, with clear associations with laser frequency and duration. Finally, we demonstrate the time scale of the OAM and SAM precession occurs even earlier than that of the demagnetization process and the OISTR effect. Our results provide detailed insight into the dynamics of SAM and OAM during and shortly after a polarized laser pulse.