Unlocking ultrafast spin dynamics in a rare-earth magnet

Abstract

The speed of optically driven magnetization dynamics is fundamentally determined by how efficiently angular momentum can be transferred between electronic, spin and lattice degrees of freedom. In rare-earth magnets, this process is typically slow because optical excitation primarily addresses itinerant electrons, whereas the magnetic moment resides in localized 4f states. Here we show that selective optical excitation of localized magnetic states can overcome this limitation. Using femtosecond pump-probe magneto-optical spectroscopy of ferrimagnetic gadolinium iron garnet, we resonantly excite an intra-4f transition of Gd3+ at 4.65 eV and resolve the ensuing dynamics of the antiferromagnetically coupled Gd and Fe sublattices. Direct excitation of the 4f manifold induces an ultrafast demagnetization of the Gd sublattice with a characteristic time of 38 fs, more than two orders of magnitude faster than in elemental gadolinium and even faster than the response of the Fe sublattice in the same material. By contrast, off-resonant excitation strongly suppresses the acceleration of the Gd dynamics while leaving the Fe response largely unchanged. These results demonstrate that the ultrafast magnetic response of rare-earth systems is governed not only by intrinsic material properties but also by the optical excitation pathway. Selective access to localized magnetic states therefore provides a powerful photonic handle for engineering angular-momentum flow and controlling magnetism far from equilibrium.