Ferromagnetic or antiferromagnetic spin ordering is governed by the exchange interaction, the strongest force in magnetism. Understanding spin dynamics in magnetic materials is an issue of crucial importance for progress in information processing and recording technology. Usually the dynamics are studied by observing the collective response of exchange-coupled spins, that is, spin resonances, after an external perturbation by a pulse of magnetic field, current or light. The periods of the corresponding resonances range from one nanosecond for ferromagnets down to one picosecond for antiferromagnets. However, virtually nothing is known about the behaviour of spins in a magnetic material after being excited on a timescale faster than that corresponding to the exchange interaction (10-100 fs), that is, in a non-adiabatic way. Here we use the element-specific technique X-ray magnetic circular dichroism to study spin reversal in GdFeCo that is optically excited on a timescale pertinent to the characteristic time of the exchange interaction between Gd and Fe spins. We unexpectedly find that the ultrafast spin reversal in this material, where spins are coupled antiferromagnetically, occurs by way of a transient ferromagnetic-like state. Following the optical excitation, the net magnetizations of the Gd and Fe sublattices rapidly collapse, switch their direction and rebuild their net magnetic moments at substantially different timescales; the net magnetic moment of the Gd sublattice is found to reverse within 1.5 picoseconds, which is substantially slower than the Fe reversal time of 300 femtoseconds. Consequently, a transient state characterized by a temporary parallel alignment of the net Gd and Fe moments emerges, despite their ground-state antiferromagnetic coupling. These surprising observations, supported by atomistic simulations, provide a concept for the possibility of manipulating magnetic order on the timescale of the exchange interaction.

We experimentally demonstrate that the magnetization can be reversed in a reproducible manner by a single 40 femtosecond circularly polarized laser pulse, without any applied magnetic field. This optically induced ultrafast magnetization reversal previously believed impossible is the combined result of femtosecond laser heating of the magnetic system to just below the Curie point and circularly polarized light simultaneously acting as a magnetic field. The direction of this opto-magnetic switching is determined only by the helicity of light. This finding reveals an ultrafast and efficient pathway for writing magnetic bits at record-breaking speeds.

The question of how, and how fast, magnetization can be reversed is a topic of great practical interest for the manipulation and storage of magnetic information. It is generally accepted that magnetization reversal should be driven by a stimulus represented by time-non-invariant vectors such as a magnetic field, spin-polarized electric current, or cross-product of two oscillating electric fields. However, until now it has been generally assumed that heating alone, not represented as a vector at all, cannot result in a deterministic reversal of magnetization, although it may assist this process. Here we show numerically and demonstrate experimentally a novel mechanism of deterministic magnetization reversal in a ferrimagnet driven by an ultrafast heating of the medium resulting from the absorption of a sub-picosecond laser pulse without the presence of a magnetic field.

Subpicosecond magnetization reversal is experimentally demonstrated by ultrafast heating of a ferrimagnet across its compensation points, under an applied magnetic field. While the reversal is initiated by crossing the magnetization compensation temperature, the short reversal time is related to the angular momentum compensation, where the dynamics of the system is highly accelerated owing to the divergence of the gyromagnetic ratio. These results demonstrate the feasibility of subpicosecond magnetization reversal previously believed impossible.

Using magneto-optical microscopy in combination with ellipsometry measurements, we show that all-optical switching with polarized femtosecond laser pulses in ferrimagnetic GdFeCo is subjected to a threshold fluence absorbed in the magnetic layer, independent of either the excitation wavelength or the polarization of the laser pulse. Furthermore, we present a quantitative explanation of the intensity window in which all-optical helicity-dependent switching (AO-HDS) occurs, based on magnetic circular dichroism. This explanation is consistent with all the experimental findings on AO-HDS so far, varying from single- to multiple-shot experiments. The presented results give a solid understanding of the origin of AO-HDS, and give novel insights into the physics of ultrafast, laser controlled magnetism.