Polarisation-dependent single-pulse ultrafast optical switching of an elementary ferromagnet

The ultimate control of magnetic states of matter at femtosecond (or even faster) timescales defines one of the most pursued paradigm shifts for future information technology. In this context, ultrafast laser pulses developed into extremely valuable stimuli for the all-optical magnetization reversal in ferrimagnetic and ferromagnetic alloys and multilayers, while this remains elusive in elementary ferromagnets. Here we demonstrate that a single laser pulse with sub-picosecond duration can lead to the reversal of the magnetization of bulk nickel, in tandem with the expected demagnetization. As revealed by realistic time-dependent electronic structure simulations, the central mechanism involves ultrafast light-induced torques that act on the magnetization. They are only effective if the laser pulse is circularly polarized on a plane that contains the initial orientation of the magnetization. We map the laser pulse parameter space enabling the magnetization switching and unveil rich intra-atomic orbital-dependent magnetization dynamics featuring transient inter-orbital non-collinear states. Our findings open further perspectives for the efficient implementation of optically-based spintronic devices. Laser pulses can be used not only to investigate the ultrafast dynamics of a magnetic system but also to manipulate their magnetization states with potential applications in information storage. To this end, using time-dependent electronic structure simulations, the authors investigate the underlying physics of the laser-induced ultrafast magnetization dynamics in bulk nickel and predict magnetization reversal with a single pulse.