Ab initio study of ultrafast spin dynamics in Gd_x(FeCo)_1−x alloys

Using an ultrashort laser pulse, we explore ab initio the spin dynamics of Gdx(FeCo)1-x at femtosecond time scales. Optical excitations are found to drive charges from Fe majority d-states to unoccupied Gd f-minority states with f-electron character excited occupation lagging behind that of the d-electron character, leading to substantial demagnetization of both species while leaving the global moment almost unchanged. For x > 0.33, this results in the creation of an ultrafast ferromagnetic (FM) transient by the end of the laser pulse with the Gd demagnetization rate slower than that of Fe. For all concentrations, the Gd moments begin to rotate from their ground state orientations developing in-plane moments of between 0.2 and 0.5 μB. Thus, the ultrafast spin dynamics of the material captures three important ingredients of all optical switching that occurs at much later (picosecond) times: (i) the development of a FM transient, (ii) the different rates of demagnetization of Fe and Gd, and (iii) the breaking of the collinear symmetry of the ground state. Furthermore, several predictions are made about the behavior of Fe-Gd alloys that can be experimentally tested and can lead to a spin-filtering device

Ab initio study of ultrafast spin dynamics in Gdx(FeCo)1−x alloys

Using an ultrashort laser pulse, we explore ab initio the spin dynamics of Gdx(FeCo)1− at femtosecond time scales. Optical excitations are found to drive charges from Fe majority d-states to unoccupied Gd f-minority states with f-electron character excited occupation lagging behind that of the d-electron character, leading to substantial demagnetization of both species while leaving the global moment almost unchanged. For x > 0.33, this results in the creation of an ultrafast ferromagnetic (FM) transient by the end of the laser pulse with the Gd demagnetization rate slower than that of Fe. For all concentrations, the Gd moments begin to rotate from their ground state orientations developing in-plane moments of between 0.2 and 0.5 μB. Thus, the ultrafast spin dynamics of the material captures three important ingredients of all optical switching that occurs at much later (picosecond) times: (i) the development of a FM transient, (ii) the different rates of demagnetization of Fe and Gd, and (iii) the breaking of the collinear symmetry of the ground state. Furthermore, several predictions are made about the behavior of Fe–Gd alloys that can be experimentally tested and can lead to a spin-filtering device

Mapping the energy-time landscape of spins with helical X-rays

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

Femtosecond nonlinear ultrasonics in gold probed with ultrashort surface plasmons

Fundamental interactions induced by lattice vibrations on ultrafast time scales become increasingly important for modern nanoscience and technology. Experimental access to the physical properties of acoustic phonons in the THz frequency range and over the entire Brillouin zone is crucial for understanding electric and thermal transport in solids and their compounds. Here, we report on the generation and nonlinear propagation of giant (1 percent) acoustic strain pulses in hybrid gold/cobalt bilayer structures probed with ultrafast surface plasmon interferometry. This new technique allows for unambiguous characterization of arbitrary ultrafast acoustic transients. The giant acoustic pulses experience substantial nonlinear reshaping already after a propagation distance of 100 nm in a crystalline gold layer. Excellent agreement with the Korteveg-de Vries model points to future quantitative nonlinear femtosecond THz-ultrasonics at the nano-scale in metals at room temperature

Toward ultrafast magnetic depth profiling using time resolved x ray resonant magnetic reflectivity

During the last two decades, a variety of models have been developed to explain the ultrafast quenching of magnetization following femtosecond optical excitation. These models can be classified into two broad categories, relying either on a local or a non local transfer of angular momentum. The acquisition of the magnetic depth profiles with femtosecond resolution, using time resolved x ray resonant magnetic reflectivity, can distinguish local and non local effects. Here, we demonstrate the feasibility of this technique in a pump probe geometry using a custom built reflectometer at the FLASH2 free electron laser FEL . Although FLASH2 is limited to the production of photons with a fundamental wavelength of 4 amp; 8201;nm amp; 8771;310 amp; 8201;eV , we were able to probe close to the Fe L3 edge 706.8 amp; 8201;eV of a magnetic thin film employing the third harmonic of the FEL. Our approach allows us to extract structural and magnetic asymmetry signals revealing two dynamics on different time scales which underpin a non homogeneous loss of magnetization and a significant dilation of 2 amp; 8201; of the layer thickness followed by oscillations. Future analysis of the data will pave the way to a full quantitative description of the transient magnetic depth profile combining femtosecond with nanometer resolution, which will provide further insight into the microscopic mechanisms underlying ultrafast demagnetizatio

Sub 15 fs X ray pump and X ray probe experiment for the study of ultrafast magnetization dynamics in ferromagnetic alloys

In this paper, we present a new setup for the measurement of element specific ultrafast magnetization dynamics in ferromagnetic thin films with a sub 15 fs time resolution. Our experiment relies on a split and delay approach which allows us to fully exploit the shortest X rays pulses delivered by X ray Free Electrons Lasers close to the attosecond range , in an X ray pump X ray probe geometry. The setup performance is demonstrated by measuring the ultrafast elemental response of Ni and Fe during demagnetization of ferromagnetic Ni and Ni80Fe20 Permalloy samples upon resonant excitation at the corresponding absorption edges. The transient demagnetization process is measured in both reflection and transmission geometry using, respectively, the transverse magneto optical Kerr effect T MOKE and the Faraday effect as probing mechanism

Dynamics and inertia of skyrmionic spin structures

Skyrmions are topologically protected winding vector fields characterized by a spherical topology. Magnetic skyrmions can arise as the result of the interplay of various interactions, including exchange, dipolar and anisotropy energy in the case of magnetic bubbles and an additional Dzyaloshinskii-Moriya interaction in the case of chiral skyrmions. Whereas the static and low-frequency dynamics of skyrmions are already well under control, their gigahertz dynamical behaviour has not been directly observed in real space. Here, we image the gigahertz gyrotropic eigenmode dynamics of a single magnetic bubble and use its trajectory to experimentally confirm its skyrmion topology. The particular trajectory points to the presence of strong inertia, with a mass much larger than predicted by existing theories. This mass is endowed by the topological confinement of the skyrmion and the energy associated with its size change. It is thereby expected to be found in all skyrmionic structures in magnetic systems and beyond. Our experiments demonstrate that the mass term plays a key role in describing skyrmion dynamics.