UDKM1DSIM A simulation toolkit for 1D ultrafast dynamics in condensed matter

The UDKM1DSIM toolbox is a collection of MATLAB MathWorks Inc. classes and routines to simulate the structural dynamics and the according X ray diffraction response in one dimensional crystalline sample structures upon an arbitrary time dependent external stimulus, e.g. an ultrashort laser pulse. The toolbox provides the capabilities to define arbitrary layered structures on the atomic level including a rich database of corresponding element specific physical properties. The excitation of ultrafast dynamics is represented by an N temperature model which is commonly applied for ultrafast optical excitations. Structural dynamics due to thermal stress are calculated by a linear chain model of masses and springs. The resulting X ray diffraction response is computed by dynamical X ray theory. The UDKM1DSIM toolbox is highly modular and allows for introducing user defined results at any step in the simulation procedur

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

Electronic origin of x-ray absorption peak shifts

Encoded in the transient x-ray absorption (XAS) and magnetic circular (MCD) response functions resides a wealth of information of the microscopic processes of ultrafast demagnetization. Employing state-of-the-art first-principles dynamical simulations we show that the experimentally observed energy shift of the L3 XAS peak in Ni, and the absence of a corresponding shift in the dichroic MCD response, can be explained in terms of laser-induced changes in band occupation. Strikingly, we predict that for the same ultrashort pump pulse applied to Co the opposite effect will occur: a substantial shift upward in energy of the MCD peaks will be accompanied by very small change in the position of XAS peaks, a fact we relate to the reduced d-band filling of Co that allows a greater energetic range above the Fermi energy into which charge can be excited. We also carefully elucidate the dependence of this effect on pump pulse parameters. These findings (i) establish an electronic origin for early-time peak shifts in transient XAS and MCD spectroscopy and (ii) illustrate the rich information that may be extracted from transient response functions of the underlying dynamical system

Optical inter-site spin transfer probed by energy and spin-resolved transient absorption spectroscopy

Optically driven spin transport is the fastest and most efficient process to manipulate macroscopic magnetization as it does not rely on secondary mechanisms to dissipate angular momentum. In the present work, we show that such an optical inter-site spin transfer (OISTR) from Pt to Co emerges as a dominant mechanism governing the ultrafast magnetization dynamics of a CoPt alloy. To demonstrate this, we perform a joint theoretical and experimental investigation to determine the transient changes of the helicity dependent absorption in the extreme ultraviolet spectral range. We show that the helicity dependent absorption is directly related to changes of the transient spin-split density of states, allowing us to link the origin of OISTR to the available minority states above the Fermi level. This makes OISTR a general phenomenon in optical manipulation of multi-component magnetic systems

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

Transient magnetic gratings on the nanometer scale

Laser-driven non-local electron dynamics in ultrathin magnetic samples on a sub-10 nm length scale is a key process in ultrafast magnetism. However, the experimental access has been challenging due to the nanoscopic and femtosecond nature of such transport processes. Here, we present a scattering-based experiment relying on a laser-induced electro- and magneto-optical grating in a Co/Pd ferromagnetic multilayer as a new technique to investigate non-local magnetization dynamics on nanometer length and femtosecond timescales. We induce a spatially modulated excitation pattern using tailored Al near-field masks with varying periodicities on a nanometer length scale and measure the first four diffraction orders in an x-ray scattering experiment with magnetic circular dichroism contrast at the free-electron laser facility FERMI, Trieste. The design of the periodic excitation mask leads to a strongly enhanced and characteristic transient scattering response allowing for sub-wavelength in-plane sensitivity for magnetic structures. In conjunction with scattering simulations, the experiment allows us to infer that a potential ultrafast lateral expansion of the initially excited regions of the magnetic film mediated by hot-electron transport and spin transport remains confined to below three nanometers