Swept coded aperture real-time femtophotography.

Single-shot real-time femtophotography is indispensable for imaging ultrafast dynamics during their times of occurrence. Despite their advantages over conventional multi-shot approaches, existing techniques confront restricted imaging speed or degraded data quality by the deployed optoelectronic devices and face challenges in the application scope and acquisition accuracy. They are also hindered by the limitations in the acquirable information imposed by the sensing models. Here, we overcome these challenges by developing swept coded aperture real-time femtophotography (SCARF). This computational imaging modality enables all-optical ultrafast sweeping of a static coded aperture during the recording of an ultrafast event, bringing full-sequence encoding of up to 156.3 THz to every pixel on a CCD camera. We demonstrate SCARF's single-shot ultrafast imaging ability at tunable frame rates and spatial scales in both reflection and transmission modes. Using SCARF, we image ultrafast absorption in a semiconductor and ultrafast demagnetization of a metal alloy.

Single-Shot Laser-Induced Switching of an Exchange Biased Antiferromagnet.

Ultrafast manipulation of magnetic order has challenged the understanding of the fundamental and dynamic properties of magnetic materials. So far single-shot magnetic switching has been limited to ferrimagnetic alloys, multilayers, and designed ferromagnetic (FM) heterostructures. In FM/antiferromagnetic (AFM) bilayers, exchange bias (He) arises from the interfacial exchange coupling between the two layers and reflects the microscopic orientation of the antiferromagnet. Here the possibility of single-shot switching of the antiferromagnet (change of the sign and amplitude of He) with a single femtosecond laser pulse in IrMn/CoGd bilayers is demonstrated. The manipulation is demonstrated in a wide range of fluences for different layer thicknesses and compositions. Atomistic simulations predict ultrafast switching and recovery of the AFM magnetization on a timescale of 2 ps. The results provide the fastest and the most energy-efficient method to set the exchange bias and pave the way to potential applications for ultrafast spintronic devices.

Optically induced ultrafast magnetization switching in ferromagnetic spin valves.

The discovery of spin-transfer torque (STT) enabled the control of the magnetization direction in magnetic devices in nanoseconds using an electrical current. Ultrashort optical pulses have also been used to manipulate the magnetization of ferrimagnets at picosecond timescales by bringing the system out of equilibrium. So far, these methods of magnetization manipulation have mostly been developed independently within the fields of spintronics and ultrafast magnetism. Here we show optically induced ultrafast magnetization reversal taking place within less than a picosecond in rare-earth-free archetypal spin valves of [Pt/Co]/Cu/[Co/Pt] commonly used for current-induced STT switching. We find that the magnetization of the free layer can be switched from a parallel to an antiparallel alignment, as in STT, indicating the presence of an unexpected, intense and ultrafast source of opposite angular momentum in our structures. Our findings provide a route to ultrafast magnetization control by bridging concepts from spintronics and ultrafast magnetism.

Accelerating ultrafast magnetization reversal by non-local spin transfer.

When exciting a magnetic material with a femtosecond laser pulse, the amplitude of magnetization is no longer constant and can decrease within a time scale comparable to the duration of the optical excitation. This ultrafast demagnetization can even trigger an ultrafast, out of equilibrium, phase transition to a paramagnetic state. The reciprocal effect, namely an ultrafast remagnetization from the zero magnetization state, is a necessary ingredient to achieve a complete ultrafast reversal. However, the speed of remagnetization is limited by the universal critical slowing down which appears close to a phase transition. Here we demonstrate that magnetization can be reversed in a few hundreds of femtoseconds by overcoming the critical slowing down thanks to ultrafast spin cooling and spin heating mechanisms. We foresee that these results outline the potential of ultrafast spintronics for future ultrafast and energy efficient magnetic memory and storage devices. Furthermore, this should motivate further theoretical works in the field of femtosecond magnetization reversal.

Optical Creation of Skyrmions by Spin Reorientation Transition in Ferrimagnetic CoHo Alloys.

Manipulating magnetic skyrmions by means of a femtosecond (fs) laser pulse has attracted great interest due to their promising applications in efficient information-storage devices with ultralow energy consumption. However, the mechanism underlying the creation of skyrmions induced by an fs laser is still lacking. As a result, a key challenge is to reveal the pathway for the massive reorientation of magnetization from trivial to nontrivial topological states. Here, we studied a series of ferrimagnetic CoHo alloys and investigated the effect of a single laser pulse on the magnetic states. Thanks to the time-resolved magneto-optical Kerr effect and imaging techniques, we demonstrate that the laser-induced phase transitions from single domains into a topological skyrmion phase are mediated by the transient in-plane magnetization state, in real time and space domains, respectively. Combining experiments and micromagnetic simulations, we propose a two-step process for creating skyrmions through laser pulse irradiation: (i) the electron temperature enhancement induces a spin reorientation transition on a picosecond (ps) timescale due to the suppression of perpendicular magnetic anisotropy (PMA) and (ii) the PMA slowly restores, accompanied by out-of-plane magnetization recovery, leading to the generation of skyrmions with the help of spin fluctuations. This work provides a route to control skyrmion patterns using an fs laser, thereby establishing the foundation for further exploration of topological magnetism at ultrafast timescales.

Energy Efficient Single Pulse Switching of [Co/Gd/Pt]N Nanodisks Using Surface Lattice Resonances.

The impact of plasmonic surface lattice resonances on the magneto-optical properties and energy absorption efficiency has been studied in arrays of [Co/Gd/Pt]N multilayer nanodisks. Varying the light wavelength, the disk diameter, and the period of the array, it is demonstrated that surface lattice resonances allow all-optical single pulse switching of [Co/Gd/Pt]N nanodisk arrays with an energy 400% smaller than the energy needed to switch a continuous [Co/Gd/Pt]N film. Moreover, the magneto-optical Faraday effect is enhanced at the resonance condition by up to 5,000%. The influence of the disk diameter and array period on the amplitude, width and position of the surface lattice resonances is in qualitative agreement with theoretical calculations and opens the way to designing magnetic metasurfaces for all-optical magnetization switching applications.

Ab Initio Study of Helicity-Dependent Light-Induced Demagnetization: From the Optical Regime to the Extreme Ultraviolet Regime.

We use ab initio real-time time-dependent density functional theory to investigate the effect of optical and extreme ultraviolet (XUV) circularly polarized femtosecond pulses on the magnetization dynamics of ferromagnetic materials. We demonstrate that the light induces a helicity-dependent reduction of the magnitude of the magnetization. In the XUV regime, where the 3p semicore states are involved, a larger helicity dependence persisting even after the passage of light is exhibited. Finally, we were able to separate the part of the helicity-dependent dynamics due to the absorption from the part due to the inverse Faraday effect. Doing so, we show that the former has, overall, a greater impact on the magnetization than the latter, especially after the pulse and in the XUV regime. This work hints at the yet experimentally unexplored territory of the XUV light-induced helicity-dependent dynamics, which, according to our prediction, could magnify the helicity-dependent dynamics already exhibited in the optical regime.

Energy Efficient Control of Ultrafast Spin Current to Induce Single Femtosecond Pulse Switching of a Ferromagnet.

New methods to induce magnetization switching in a thin ferromagnetic material using femtosecond laser pulses without the assistance of an applied external magnetic field have recently attracted a lot of interest. It has been shown that by optically triggering the reversal of the magnetization in a GdFeCo layer, the magnetization of a nearby ferromagnetic thin film can also be reversed via spin currents originating in the GdFeCo layer. Here, using a similar structure, it is shown that the magnetization reversal of the GdFeCo is not required in order to reverse the magnetization of the ferromagnetic thin film. This switching is attributed to the ultrafast spin current and can be generated by the GdFeCo demagnetization. A larger energy efficiency of the ferromagnetic layer single pulse switching is obtained for a GdFeCo with a larger Gd concentration. Those ultrafast and energy efficient switchings observed in such spintronic devices open a new path toward ultrafast and energy efficient magnetic memories.

Engineering Single-Shot All-Optical Switching of Ferromagnetic Materials.

Since it was recently demonstrated in a spin-valve structure, magnetization reversal of a ferromagnetic layer using a single ultrashort optical pulse has attracted attention for future ultrafast and energy-efficient magnetic storage or memory devices. However, the mechanism and the role of the magnetic properties of the ferromagnet as well as the time scale of the magnetization switching are not understood. Here, we investigate single-shot all-optical magnetization switching in a GdFeCo/Cu/[CoxNi1-x/Pt] spin-valve structure. We demonstrate that the threshold fluence for switching both the GdFeCo and the ferromagnetic layer depends on the laser pulse duration and the thickness and the Curie temperature of the ferromagnetic layer. We are able to explain most of the experimental results using a phenomenological model. This work provides a way to engineer ferromagnetic materials for energy efficient single-shot all-optical magnetization switching.

Engineering Co2 MnAlx Si1- x Heusler Compounds as a Model System to Correlate Spin Polarization, Intrinsic Gilbert Damping, and Ultrafast Demagnetization.

Engineering of magnetic materials for developing better spintronic applications relies on the control of two key parameters: the spin polarization and the Gilbert damping, responsible for the spin angular momentum dissipation. Both of them are expected to affect the ultrafast magnetization dynamics occurring on the femtosecond timescale. Here, engineered Co2 MnAlx Si1- x Heusler compounds are used to adjust the degree of spin polarization at the Fermi energy, P, from 60% to 100% and to investigate how they correlate with the damping. It is experimentally demonstrated that the damping decreases when increasing the spin polarization from 1.1 × 10-3 for Co2 MnAl with 63% spin polarization to an ultralow value of 4.6 × 10-4 for the half-metallic ferromagnet Co2 MnSi. This allows the investigation of the relation between these two parameters and the ultrafast demagnetization time characterizing the loss of magnetization occurring after femtosecond laser pulse excitation. The demagnetization time is observed to be inversely proportional to 1 - P and, as a consequence, to the magnetic damping, which can be attributed to the similarity of the spin angular momentum dissipation processes responsible for these two effects. Altogether, the high-quality Heusler compounds allow control over the band structure and therefore the channel for spin angular momentum dissipation.

Controlling All-Optical Helicity-Dependent Switching in Engineered Rare-Earth Free Synthetic Ferrimagnets.

All-optical helicity-dependent switching in ferromagnetic layers has revealed an unprecedented route to manipulate magnetic configurations by circularly polarized femtosecond laser pulses. In this work, rare-earth free synthetic ferrimagnetic heterostructures made from two antiferromagnetically exchange coupled ferromagnetic layers are studied. Experimental results, supported by numerical simulations, show that the designed structures enable all-optical switching which is controlled, not only by light helicity, but also by the relative Curie temperature of each ferromagnetic layer. Indeed, through the antiferromagnetic exchange coupling, the layer with the larger Curie temperature determines the final orientation of the other layer and so the synthetic ferrimagnet. For similar Curie temperatures, helicity-independent back switching is observed and the final magnetic configuration is solely determined by the initial magnetic state. This demonstration of electrically-detected, optical control of engineered rare-earth free heterostructures opens a novel route toward practical opto-spintronics.

Femtosecond Laser-Excitation-Driven High Frequency Standing Spin Waves in Nanoscale Dielectric Thin Films of Iron Garnets.

We demonstrate that femtosecond laser pulses allow triggering high-frequency standing spin-wave modes in nanoscale thin films of a bismuth-substituted yttrium iron garnet. By varying the strength of the external magnetic field, we prove that two distinct branches of the dispersion relation are excited for all the modes. This is reflected in particular at a very weak magnetic field (∼33 mT) by a spin dynamics with a frequency up to 15 GHz, which is 15 times higher than the one associated with the ferromagnetic resonance mode. We argue that this phenomenon is triggered by ultrafast changes of the magnetic anisotropy via laser excitation of incoherent and coherent phonons. These findings open exciting prospects for ultrafast photo magnonics.

Creation of Magnetic Skyrmion Bubble Lattices by Ultrafast Laser in Ultrathin Films.

Magnetic skyrmions are topologically nontrivial spin textures which hold great promise as stable information carriers in spintronic devices at the nanoscale. One of the major challenges for developing novel skyrmion-based memory and logic devices is fast and controlled creation of magnetic skyrmions at ambient conditions. Here we demonstrate controlled generation of skyrmion bubbles and skyrmion bubble lattices from a ferromagnetic state in sputtered ultrathin magnetic films at room temperature by a single ultrafast (35 fs) laser pulse. The skyrmion bubble density increases with the laser fluence, and it finally becomes saturated, forming disordered hexagonal lattices. Moreover, we present that the skyrmion bubble lattice configuration leads to enhanced topological stability as compared to isolated skyrmions, suggesting its promising use in data storage. Our findings shed light on the optical approach to the skyrmion bubble lattice in commonly accessible materials, paving the road toward the emerging skyrmion-based memory and synaptic devices.

Single-Shot Multi-Level All-Optical Magnetization Switching Mediated by Spin Transport.

All-optical ultrafast magnetization switching in magnetic material thin film without the assistance of an applied external magnetic field is explored for future ultrafast and energy-efficient magnetic storage and memories. It is shown that femtosecond (fs) light pulses induce magnetization reversal in a large variety of magnetic materials. However, so far, only GdFeCo-based ferrimagnetic thin films exhibit magnetization switching via a single optical pulse. Here, the single-pulse switching of Co/Pt multilayers within a magnetic spin-valve structure ([Co/Pt]/Cu/GdFeCo) is demonstrated and four possible magnetic configurations of the spin valve can be accessed using a sequence of single fs light pulses. The experimental study reveals that the magnetization final state of the ferromagnetic [Co/Pt] layer is determined by spin-polarized currents generated by the light pulse interactions with the GdFeCo layer. This work provides an approach to deterministically switch ferromagnetic layers and a pathway to engineering materials for opto-magnetic multi-bit recording.

Ultrafast Magnetization Manipulation Using Single Femtosecond Light and Hot-Electron Pulses.

Current-induced magnetization manipulation is a key issue for spintronic applications. This manipulation must be fast, deterministic, and nondestructive in order to function in device applications. Therefore, single- electronic-pulse-driven deterministic switching of the magnetization on the picosecond timescale represents a major step toward future developments of ultrafast spintronic systems. Here, the ultrafast magnetization dynamics in engineered Gdx [FeCo]1-x -based structures are studied to compare the effect of femtosecond laser and hot-electron pulses. It is demonstrated that a single femtosecond hot-electron pulse causes deterministic magnetization reversal in either Gd-rich and FeCo-rich alloys similarly to a femtosecond laser pulse. In addition, it is shown that the limiting factor of such manipulation for perpendicular magnetized films arises from the formation of a multidomain state due to dipolar interactions. By performing time-resolved measurements under various magnetic fields, it is demonstrated that the same magnetization dynamics are observed for both light and hot-electron excitation, and that the full magnetization reversal takes place within 40 ps. The efficiency of the ultrafast current-induced magnetization manipulation is enhanced due to the ballistic transport of hot electrons before reaching the GdFeCo magnetic layer.

Pump-probe experiments at the TEMPO beamline using the low-α operation mode of Synchrotron SOLEIL.

The SOLEIL synchrotron radiation source is regularly operated in special filling modes dedicated to pump-probe experiments. Among others, the low-α mode operation is characterized by shorter pulse duration and represents the natural bridge between 50 ps synchrotron pulses and femtosecond experiments. Here, the capabilities in low-α mode of the experimental set-ups developed at the TEMPO beamline to perform pump-probe experiments with soft X-rays based on photoelectron or photon detection are presented. A 282 kHz repetition-rate femtosecond laser is synchronized with the synchrotron radiation time structure to induce fast electronic and/or magnetic excitations. Detection is performed using a two-dimensional space resolution plus time resolution detector based on microchannel plates equipped with a delay line. Results of time-resolved photoelectron spectroscopy, circular dichroism and magnetic scattering experiments are reported, and their respective advantages and limitations in the framework of high-time-resolution pump-probe experiments compared and discussed.

Indirect excitation of ultrafast demagnetization.

Does the excitation of ultrafast magnetization require direct interaction between the photons of the optical pump pulse and the magnetic layer? Here, we demonstrate unambiguously that this is not the case. For this we have studied the magnetization dynamics of a ferromagnetic cobalt/palladium multilayer capped by an IR-opaque aluminum layer. Upon excitation with an intense femtosecond-short IR laser pulse, the film exhibits the classical ultrafast demagnetization phenomenon although only a negligible number of IR photons penetrate the aluminum layer. In comparison with an uncapped cobalt/palladium reference film, the initial demagnetization of the capped film occurs with a delayed onset and at a slower rate. Both observations are qualitatively in line with energy transport from the aluminum layer into the underlying magnetic film by the excited, hot electrons of the aluminum film. Our data thus confirm recent theoretical predictions.