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All-optical helicity-independent switching (AO-HIS) is of interest for ultrafast and energy efficient magnetic switching in future magnetic data storage approaches. Yet, to achieve high bit density magnetic recording it is necessary to reduce the size of the magnetic bits addressed by laser pulses at well-controlled positions. Metallic nanostructures that support localized surface plasmons enable spatial electromagnetic confinement well below the diffraction limit and rare-earth transition metal alloys such as GdTbCo have demonstrated nanometre-sized stable domains. Here, we deposit plasmonic gold nanostructures on a GdTbCo film and probe the magnetic state using magnetic force microscopy. We observe localized AO-HIS down to a critical dimension of 240 nm after excitation of the gold nanostructures by a single 370 fs long laser pulse with a centre wavelength of 1030 nm. We demonstrate that the strong localization of optical fields through plasmonic nanostructures enables reproducible localized nanoscale AO-HIS at sub-wavelength length scales. We study the influence of the localized electromagnetic field enhancement by the plasmonic nanostructures on the required fluence to switch the magnetization., Comment: 10 pages, 4 figures

Spin-orbit torques (SOTs) act as efficient drivers for nanoscale magnetic systems, such as in magnetic tunnel junctions, nano-oscillators and racetrack geometries. In particular, in combination with materials exhibiting high Dzyaloshinskii--Moriya interaction, SOTs are considered to result in well-controlled deterministic magnetisation dynamics and are, therefore, used as robust drives to move and create magnetic skyrmions. In contrast to these expectations, we here find unpredictable, transiently chaotic dynamics induced by SOT at an artificial anisotropy-engineered defect in a magnetic racetrack. Based on these controlled conditions, we directly observe the nanoscale dynamics with holography-based, time-resolved x-ray imaging. In concert with micromagnetic simulations, we disclose a regime of violent picosecond fluctuations, including topological instabilities that, remarkably, result in deterministic final configurations. In addition, our images expose previously unseen skyrmion shedding and highlight the potential of transiently chaotic pathways for topological switching. Our approach offers new perspectives for the investigation and application of highly non-linear SOT dynamics in spintronics materials.

Soft x-ray microscopy plays an important role in modern spintronics. However, the achievable resolution of most x-ray magnetic imaging experiments is above 10 nm, limiting access to fundamental and technologically relevant length scales. Here, we demonstrate x-ray magnetic microscopy with 5 nm resolution by combining holography-assisted coherent diffractive imaging with heterodyne amplification of the weak magnetic signal. The gain in resolution and contrast allows direct access to key magnetic properties, including domain wall profiles and the position of pinning sites. The ability to detect and map such properties with photons opens new horizons for element-specific, time-resolved, and in-operando research on magnetic materials and beyond., Comment: 12 pages, 12 figures

Coherent light-matter interactions mediated by opto-magnetic phenomena like the inverse Faraday effect (IFE) are expected to provide a non-thermal pathway for ultrafast manipulation of magnetism on timescales as short as the excitation pulse itself. As the IFE scales with the spin-orbit coupling strength of the involved electronic states, photo-exciting the strongly spin-orbit coupled core-level electrons in magnetic materials appears as an appealing method to transiently generate large opto-magnetic moments. Here, we investigate this scenario in a ferrimagnetic GdFeCo alloy by using intense and circularly polarized pulses of extreme ultraviolet radiation. Our results reveal ultrafast and strong helicity-dependent magnetic effects which are in line with the characteristic fingerprints of an IFE, corroborated by ab initio opto-magnetic IFE theory and atomistic spin dynamics simulations.

The recently discovered topological fluctuation state provides a fascinating new perspective on the ultrafast emergence of topology in condensed matter systems. However, rather little is known about the physics of this state and the origin of the topological fluctuations. Using time-resolved small-angle x-ray scattering, we observe that topological fluctuation states appear after laser excitation even if the final state does not host stable skyrmions. Simulations support these findings and reveal that the fluctuations originate from the competition between spontaneous nucleation and decay of skyrmions, consistent with Arrhenius-like activation over a potential barrier. Stable skyrmions can freeze out of such fluctuations when the effective temperature of the system relaxes faster than the decay time of the skyrmions. Our results reveal a robust scenario for the generation of topological fluctuation states, potentially enabling their study in a wide variety of magnetic systems.

Time-resolved x-ray magnetic circular dichroism (XMCD) enables a unique spectroscopic view on complex spin and charge dynamics in multi-elemental magnetic materials. So far, its application in the soft-x-ray range has been limited to synchrotron-radiation sources and free-electron lasers. By combining a laser-driven plasma source with a magnetic thin-film polarizer, we generate circularly polarized photons in the soft x-ray regime, enabling the first XMCD spectroscopy at the Fe L edges in a laser laboratory. Our approach can be readily adapted to other transition metal L and rare earth M absorption edges and with a temporal resolution of < 10 ps, a wide range of ultrafast magnetization studies can be realized., Comment: 7 pages, 4 figures, supplemental material

We present time-resolved scanning x-ray microscopy measurements with picosecond photo-excitation via a tailored infrared pump laser at a scanning transmission x-ray microscope. Specifically, we image the laser-induced demagnetization and remagnetization of thin ferrimagnetic GdFe films proceeding on a few nanoseconds time scale. Controlling the heat load on the sample via additional reflector and heat-sink layers allows us to conduct destruction-free measurements at a repetition rate of \SI{50}{\mega\hertz}. Near-field enhancement of the photo-excitation and controlled annealing effects lead to laterally heterogeneous magnetization dynamics which we trace with \SI{30}{\nano\meter} spatial resolution. Our work opens new opportunities to study photo-induced dynamics on the nanometer scale, with access to picosecond to nanosecond timescales, which is of technological relevance, especially in the field of magnetism.

In ferromagnetic multilayers, a single laser pulse with a fluence above an optical nucleation threshold can create magnetic skyrmions, which are randomly distributed over the area of the laser spot. However, in order to study the dynamics of skyrmions and for their application in future data technology, a controllable localization of the skyrmion nucleation sites is crucial. Here, it is demonstrated that patterned reflective masks behind a thin magnetic film can be designed to locally tailor the optical excitation amplitudes reached, leading to spatially controlled skyrmion nucleation on the nanometer scale. Using x-ray microscopy, the influence of nanopatterned back-side aluminum masks on the optical excitation is studied in two sample geometries with varying layer sequence of substrate and magnetic Co/Pt multilayer. Surprisingly, the masks' effect on suppressing or enhancing skymion nucleation reverses when changing this sequence. Moreover, optical near-field enhancements additionally affect the spatial arrangement of the nucleated skyrmions. Simulations of the spatial modulation of the laser excitation, and the following heat transfer across the interfaces in the two sample geometries are employed to explain these observations. The results demonstrate a reliable approach to add nanometer-scale spatial control to optically induced magnetization processes on ultrafast timescales.

Ultrafast control of magnetization on the nanometer length scale, in particular all-optical switching, is key to putting ultrafast magnetism on the path towards future technological application in data storage technology. However, magnetization manipulation with light on this length scale is challenging due to the wavelength limitations of optical radiation. Here, we excite transient magnetic gratings in a GdFe alloy with a periodicity of 87 nm by interference of two coherent femtosecond light pulses in the extreme ultraviolet spectral range at the free electron laser facility FERMI. The subsequent ultrafast evolution of the magnetization pattern is probed by diffraction of a third, time-delayed pulse tuned to the Gd N-edge at a wavelength of 8.3 nm. By examining the simultaneously recorded first and second diffraction orders and by performing reference real-space measurements with a wide-field magneto-optical microscope with femtosecond time resolution, we can conclusively demonstrate the ultrafast emergence of all-optical switching on the nanometer length scale., Comment: 6 pages, 5 figures

We report on time- and angle-resolved transverse magneto-optical Kerr effect spectroscopy in the soft x-ray range that, by analysis via polarization-dependent magnetic scattering simulations, allows us to determine the spatio-temporal and element-specific evolution of femtosecond laser-induced spin dynamics in nanostructured magnetic materials. In a ferrimagnetic GdFe thin film system, we correlate a reshaping spectrum of the magneto-optical Kerr signal to depth-dependent magnetization dynamics and disentangle contributions due to non-equilibrium electron transport and nanoscale heat diffusion on their intrinsic time scales. Our work provides a quantitative insight into light-driven spin dynamics occurring at buried interfaces of complex magnetic heterostructures, which can be tailored and functionalized for future opto-spintronic devices.

Ultrafast magnetization dynamics are governed by energy flow between electronic, magnetic, and lattice degrees of freedom. A quantitative understanding of these dynamics must be based on a model that agrees with experimental results for all three subsystems. However, ultrafast dynamics of the lattice remain largely unexplored experimentally. Here, we combine femtosecond electron diffraction experiments of the lattice dynamics with energy-conserving atomistic spin dynamics (ASD) simulations and ab-initio calculations to study the intrinsic energy flow in the 3d ferromagnets cobalt (Co) and iron (Fe). The simulations yield a good description of experimental data, in particular an excellent description of our experimental results for the lattice dynamics. We find that the lattice dynamics are influenced significantly by the magnetization dynamics due to the energy cost of demagnetization. Our results highlight the role of the spin system as the dominant heat sink in the first hundreds of femtoseconds. Together with previous findings for nickel [Zahn et al., Phys. Rev. Research 3, 023032 (2021)], our work demonstrates that energy-conserving ASD simulations provide a general and consistent description of the laser-induced dynamics in all three elemental 3d ferromagnets.

We introduce a wide-field magneto-optical microscope to probe magnetization dynamics with femtosecond temporal and sub-micrometer spatial resolution. We carefully calibrate the non-linear dependency between the magnetization of the sample and the detected light intensity by determining the absolute values of the magneto-optical polarization rotation. With that, an analytical transfer function is defined to directly map the recorded intensity to the corresponding magnetization, which results in significantly reduced acquisition times and relaxed computational requirements. The performance of the instrument is characterized by probing the magnetic all-optical switching dynamics of GdFe in a pump-probe experiment. The high spatial resolution of the microscope allows for accurately subdividing the laser-excited area into different fluence-regions in order to capture the strongly non-linear magnetization dynamics as a function of the optical pump intensity in a single measurement.

At the ultrafast limit of optical spin manipulation is the theoretically predicted phenomena of optical intersite spin transfer (OISTR), in which laser induced charge transfer between the sites of a multi-component material leads to control over magnetic order. A key prediction of this theory is that the demagnetization efficiency is determined by the availability of unoccupied states for intersite charge transfer. Employing state-of-the-art magneto-optical Kerr effect measurements with femtosecond time resolution, we probe this prediction via a systematic comparison of the ultrafast magnetic response between the 3d ferromagnets, Fe, Co, and Ni, and their respective Pt-based alloys and multilayers. We find that (i) the demagnetization efficiency in the elemental magnets increases monotonically from Fe, via Co to Ni and, (ii), that the gain in demagnetization efficiency of the multi-component system over the pure element counterpart scales with the number of empty 3d minority states, exactly as predicted by the OISTR effect. We support these experimental findings with ab initio time-dependent density functional theory calculations that we show to capture the experimental trends very well.

The ultrafast dynamics of magnetic order in a ferromagnet are governed by the interplay between electronic, magnetic and lattice degrees of freedom. In order to obtain a microscopic understanding of ultrafast demagnetization, information on the response of all three subsystems is required. A consistent description of demagnetization and microscopic energy flow, however, is still missing. Here, we combine a femtosecond electron diffraction study of the ultrafast lattice response of nickel to laser excitation with ab initio calculations of the electron-phonon interaction and energy-conserving atomistic spin dynamics simulations. Our model is in agreement with the observed lattice dynamics and previously reported electron and magnetization dynamics. Our approach reveals that the spin system is the dominating heat sink in the initial few hundreds of femtoseconds and implies a transient non-thermal state of the spins. Our results provide a clear picture of the microscopic energy flow between electronic, magnetic and lattice degrees of freedom on ultrafast timescales and constitute a foundation for theoretical descriptions of demagnetization that are consistent with the dynamics of all three subsystems.

Experimental investigations of ultrafast magnetization dynamics increasingly employ resonant magnetic spectroscopy in the ultraviolet spectral range. Besides allowing to disentangle the element-specific transient response of functional magnetic systems, these techniques also promise to access attosecond to few-femtosecond dynamics of spin excitations. Here, we report on a systematic study of transient magnetic circular dichroism (MCD) on the transition metals Fe, Co and Ni as well as on a FeNi and GdFe alloy and reveal a delayed onset between the electronic and magnetic response. Supported by \textit{ab-initio} calculations, we attribute our observation to a transient energy shift of the absorption and MCD spectra at the corresponding elemental resonances due to non-equilibrium changes of electron occupations., Comment: 8 figures

Magnetic skyrmions are currently the most promising option to realize current-driven magnetic shift registers. A variety of concepts to create skyrmions were proposed and demonstrated. However, none of the reported experiments show controlled creation of single skyrmions using integrated designs. Here, we demonstrate that skyrmions can be generated deterministically on subnanosecond timescales in magnetic racetracks at artificial or natural defects using spin orbit torque (SOT) pulses. The mechanism is largely similar to SOT-induced switching of uniformly magnetized elements, but due to the effect of the Dzyaloshinskii-Moriya interaction (DMI), external fields are not required. Our observations provide a simple and reliable means for skyrmion writing that can be readily integrated into racetrack devices.