A major question in the field of femtosecond laser-induced demagnetization is whereto the angular momentum lost by the electrons is transferred. Recent ultrafast electron diffraction measurements [Tauchert et al., Nature (London) 602, 73 (2022)] suggest that this angular momentum is transferred to the rotational motion of atoms on a sub-picosecond timescale, but a theory confirmation of this proposition has yet to be given. Here, we investigate the coupled electron-nuclear dynamics during ultrafast demagnetization of L10 FePt, using Ehrenfest nuclear dynamics simulations combined with the time-dependent density functional theory (TDDFT) framework. We demonstrate that atomic rotations appear, i.e., the generation of phonons carrying finite angular momentum following ultrafast demagnetization. We further show that both ultrafast demagnetization and the generation of phonons with angular momentum arise from symmetry constraints imposed by the spin-orbit coupling, thus providing insight in spin-phonon interaction at ultrafast timescales.
