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Unveiling the key mechanisms that determine optically driven spin dynamics is essential both to probe the fundamental nature of ultrafast light-matter interactions, but also to drive future technologies of smaller, faster, and more energy efficient devices. Essential to this task is the ability to use experimental spectroscopic tools to evidence the underlying energy- and spin-resolved dynamics of non-equilibrium electron occupations. In this joint theory and experimental work, we demonstrate that ultrafast helicity-dependent soft X-ray absorption spectroscopy (HXAS) allows access to spin-, time- and energy specific state occupation after optical excitation. We apply this method to the prototype transition metal ferromagnet cobalt and find convincing agreement between theory and experiment. The richly structured energy-resolved spin dynamics unveil the subtle interplay and characteristic time scales of optical excitation and spin-orbit induced spin-flip transitions in this material: the spin moment integrated in an energy window below the Fermi level first exhibits an ultrafast increase as minority carriers are excited by the laser pulse, before it is reduced as spin-flip process in highly localized, low energy states start to dominate. The results of this study demonstrate the power of element specific transient HXAS, placing it as a potential new tool for identifying and determining the role of fundamental processes in optically driven spin dynamics in magnetic materials.

Ultrafast manipulation of the magnetic state of matter bears great potential for future information technologies. While demagnetisation in ferromagnets is governed by dissipation of angular momentum, materials with multiple spin sublattices, e.g. antiferromagnets, can allow direct angular momentum transfer between opposing spins, promising faster functionality. In lanthanides, 4$\it{f}$ magnetic exchange is mediated indirectly through the conduction electrons (the Ruderman-Kittel-Kasuya-Yosida interaction, RKKY), and the effect of such conditions on direct spin transfer processes is largely unexplored. Here, we investigate ultrafast magnetization dynamics in 4f antiferromagnets, and systematically vary the 4$\it{f}$ occupation, thereby altering the magnitude of RKKY. By combining time-resolved soft x-ray diffraction with ab-initio calculations, we find that the rate of direct transfer between opposing moments is directly determined by the magnitude of RKKY. Given the high sensitivity of RKKY to the conduction electrons, our results offer a novel approach for fine-tuning the speed of magnetic devices.

A change of orbital state alters the coupling between ions and their surroundings drastically. Orbital excitations are hence key to understand and control interaction of ions. Rare-earth (RE) elements with strong magneto-crystalline anisotropy (MCA) are important ingredients for magnetic devices. Thus, control of their localized 4f magnetic moments and anisotropy is one major challenge in ultrafast spin physics. With time-resolved X-ray absorption and resonant inelastic scattering experiments, we show for Tb metal that 4f-electronic excitations out of the ground state multiplet occur after optical pumping. These excitations are driven by inelastic 5d-4f-electron scattering, alter the 4f-orbital state and consequently the MCA with important implications for magnetization dynamics in 4f-metals, and more general for the excitation of localized electronic states in correlated materials., Comment: Manuscript (23 pages, 5 figures) and Supplementary Information (32 pages, 10 figures)

We present evidence for an ultrafast optically induced ferromagnetic alignment of antiferromagnetic Mn in Co/Mn multilayers. We observe the transient ferromagnetic signal at the arrival of the pump pulse at the Mn L$_3$ resonance using x-ray magnetic circular dichroism in reflectivity. The timescale of the effect is comparable to the duration of the excitation and occurs before the magnetization in Co is quenched. Theoretical calculations point to the imbalanced population of Mn unoccupied states caused by the Co interface for the emergence of this transient ferromagnetic state., Comment: 6 pages, 3 figures

A central prospect of antiferromagnetic spintronics is to exploit magnetic properties that are unavailable with ferromagnets. However, this poses the challenge of accessing such properties for readout and control. To this end, light-induced manipulation of the transient ground state, e.g. by changing the magnetic anisotropy potential, opens promising pathways towards ultrafast deterministic control of antiferromagnetism. Here, we use this approach to trigger a $\it{coherent}$ rotation of the entire long-range antiferromagnetic spin arrangement about a crystalline axis in $GdRh_2Si_2$ and demonstrate $\it{deterministic}$ control of this rotation upon ultrafast optical excitation. Our observations can be explained by a displacive excitation of the Gd spins$'$ local anisotropy potential by the optical excitation, allowing for a full description of this transient magnetic anisotropy potential.

Femtosecond laser induced ultrafast magnetization dynamics have been studied in multisublattice CoxDy1-x alloys. By performing element and time-resolved X-ray spectroscopy, we distinguish the ultrafast quenching of Co3d and Dy4f magnetic order when the initial temperatures are below (T=150K) or above (T=270K) the temperature of magnetic compensation (Tcomp). In accordance with former element-resolved investigations and theoretical calculations, we observe different dynamics for Co3d and Dy4f spins. In addition we observe that, for a given laser fluence, the demagnetization amplitudes and demagnetization times are not affected by the existence of a temperature of magnetic compensation. However, our experiment reveals a twofold increase of the ultrafast demagnetization rates for the Dy sublattice at low temperature. In parallel, we measure a constant demagnetization rate of the Co3d sublattice above and below Tcomp. This intriguing difference between the Dy4f and Co3d sublattices calls for further theoretical and experimental investigations., Comment: 6 Figure, 2 Tables

Using femtosecond time-resolved resonant magnetic x-ray diffraction at the Ho L3 absorption edge, we investigate the demagnetization dynamics in antiferromagnetically ordered metallic Ho after femtosecond optical excitation. Tuning the x-ray energy to the electric dipole (E1, 2p -> 5d) or quadrupole (E2, 2p -> 4f) transition allows us to selectively and independently study the spin dynamics of the itinerant 5d and localized 4f electronic subsystems via the suppression of the magnetic (2 1 3-tau ) satellite peak. We find demagnetization timescales very similar to ferromagnetic 4f systems, suggesting that the loss of magnetic order occurs via a similar spin-flip process in both cases. The simultaneous demagnetization of both subsystems demonstrates strong intra-atomic 4f-5d exchange coupling. In addition, an ultrafast lattice contraction due to the release of magnetostriction leads to a transient shift of the magnetic satellite peak.

We studied the electronic and magnetic dynamics of ferromagnetic insulating BaFeO3 thin films by using pump-probe time-resolved resonant x-ray reflectivity at the Fe 2p edge. By changing the excitation density, we found two distinctly different types of demagnetization with a clear threshold behavior. We assigned the demagnetization change from slow (~ 150 ps) to fast (< 70 ps) to a transition into a metallic state induced by laser excitation. These results provide a novel approach for locally tuning magnetic dynamics. In analogy to heat assisted magnetic recording, metallization can locally tune the susceptibility for magnetic manipulation, allowing to spatially encode magnetic information., Comment: 5 pages, 4 figures

Ultrafast magnetization dynamics induced by femtosecond laser pulses have been measured in ferrimagnetic Co0.8Gd0.2, Co.74Tb.26 and Co.86Tb.14 alloys. Using element sensitivity of X-ray magnetic circular dichroism at the Co L3, Tb M5 and Gd M5 edges we evidence that the demagnetization dynamics is element dependent. We show that a thermalization time as fast as 280 fs is observed for the rare-earth in the alloy, when the laser excited state temperature is below the compensation temperature. It is limited to 500 fs when the laser excited state temperature is below the Curie temperature (Tc). We propose critical spin fluctuations in the vicinity of TC as the mechanism which reduces the demagnetization rates of the 4f electrons in transition-metal rare-earth alloys whereas at any different temperature the limited demagnetization rates could be avoided., Comment: 11 pages, 4 figures

We follow for the first time the evolution of the spin and orbital angular momentum of a thin Ni film during ultrafast demagnetization, by means of x-ray magnetic circular dichroism. Both components decrease with a 130 +/- 40 fs time constant upon excitation with a femtosecond laser pulse. Additional x-ray absorption measurements reveal an increase in the spin-orbit interaction by 6 +/- 2 % during this process. This is the experimental demonstration quantifying the importance of spin-orbit mediated processes during the demagnetization.