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Time-resolved ultrafast EUV magnetic scattering was used to test a recent prediction of >10 km/s domain wall speeds by optically exciting a magnetic sample with a nanoscale labyrinthine domain pattern. Ultrafast distortion of the diffraction pattern was observed at markedly different timescales compared to the magnetization quenching. The diffraction pattern distortion shows a threshold-dependence with laser fluence, not seen for magnetization quenching, consistent with a picture of domain wall motion with pinning sites. Supported by simulations, we show that a speed of $\approx$ 66 km/s for highly curved domain walls can explain the experimental data. While our data agree with the prediction of extreme, non-equilibrium wall speeds locally, it differs from the details of the theory, suggesting that additional mechanisms are required to fully understand these effects., 5 pages, 4 figures; Supplemental Material: 9 pages, 9 figures

Time-resolved X-ray Emission/Absorption Spectroscopy (Tr-XES/XAS) is an informative experimental tool sensitive to electronic dynamics in materials, widely exploited in diverse research fields. Typically, Tr-XES/XAS requires X-ray pulses with both a narrow bandwidth and sub-picosecond pulse duration, a combination that in principle finds its optimum with Fourier transform-limited pulses. In this work, we explore an alternative xperimental approach, capable of simultaneously retrieving information about unoccupied (XAS) and occupied (XES) states from the stochastic fluctuations of broadband extreme ultraviolet pulses of a free-electron laser. We used this method, in combination with singular value decomposition and Tikhonov regularization procedures, to determine the XAS/XES response from a crystalline silicon sample at the L2,3-edge, with an energy resolution of a few tens of meV. Finally, we combined this spectroscopic method with a pump-probe approach to measure structural and electronic dynamics of a silicon membrane. Tr-XAS/XES data obtained after photoexcitation with an optical laser pulse at 390 nm allowed us to observe perturbations of the band structure, which are compatible with the formation of the predicted precursor state of a non-thermal solid-liquid phase transition associated with a bond softening phenomenon.

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.

We demonstrate the measurement of ultrafast dynamics using ghost spectroscopy and a pump-probe approach with an optical pump and a short-wavelength radiation probe. The ghost spectroscopy approach is used to overcome the challenge of the strong intensity and spectrum fluctuations at free-electron lasers and to provide high -spectral resolution, which enables the measurement of small energy shifts in the absorption spectrum. We exploit the high resolution to explore the dynamics of the charge carrier excitations and relaxations and their impact on the photoinduced structural changes in silicon by measuring the variation of the absorption spectrum of a Si(100) membrane near the silicon L2,3 edge and the accompanying edge shifts in response to the optical illumination.

We use a pump-probe scheme to measure the time evolution of the C K-edge X-ray absorption spectrum (XAS) from CO/Ru(0001) after excitation by an ultrashort high-intensity optical laser pulse. Due to the short duration of the X-ray probe pulse and precise control of the pulse delay, the excitation-induced dynamics during the first ps after the pump can be resolved with unprecedented time resolution. By comparing with theoretical (DFT) spectrum calculations we find high excitation of the internal stretch and frustrated rotation modes occurring within 200 fs of laser excitation, as well as thermalization of the system in the ps regime. The ~100 fs initial excitation of these CO vibrational modes is not readily rationalized by traditional theories of nonadiabatic coupling of adsorbates to metal surfaces, e. g. electronic frictions based on first order electron-phonon coupling or transient population of adsorbate resonances. We suggest that coupling of the adsorbate to non-thermalized electron-hole pairs is responsible for the ultrafast initial excitation of the modes., Comment: 16 pages, 16 figures. To be published in Physical Review Letters: https://journals.aps.org/prl/accepted/c1070Y74M8b18063d9cd0221b000631d50ef7a249

In chemistry, biology and materials science, the ability to access interatomic interactions and their dynamical evolution has become possible with the advent of femtosecond lasers. In particular, the observation of vibrational wave packets via optical (UV-visible-IR) spectroscopies has been a major achievement as it can track the motion of nuclei within the system. However, optical spectroscopies only detect the effect of the interatomic vibrations on the global electronic surfaces. New tuneable, pulsed and polarized sources of short-wavelength radiation, such as X-Ray Free electron lasers, can overcome this limitation, allowing for chemical and, of primary importance in biochemistry, enantiomeric selectivity. This selectivity may be complemented by taking into account the chemical shifts of atoms belonging to different molecular moieties

While chiral spin structures stabilized by Dzyaloshinskii-Moriya interaction (DMI) are candidates as novel information carriers, their dynamics on the fs-ps timescale is little known. Since with the bulk Heisenberg exchange and the interfacial DMI two distinct exchange mechanisms are at play, the ultra-fast dynamics of the chiral order needs to be ascertained and compared to the dynamics of the conventional collinear order. Using an XUV free-electron laser we determine the fs-ps temporal evolution of the chiral order in domain walls in a magnetic thin film sample by an IR pump - X-ray magnetic scattering probe experiment. Upon demagnetisation we observe that the dichroic (CL-CR) signal connected with the chiral order correlator $m_z m_x$ in the domain walls recovers significantly faster than the (CL+CR) sum signal representing the average collinear domain magnetisation $m_z^2 + m_x^2$. We explore possible explanations based on spin structure dynamics and reduced transversal magnetisation fluctuations inside the domain walls and find that the latter can explain the experimental data leading to different dynamics for collinear magnetic order and chiral magnetic order., 28 pages, 14 figures

Non-collinear spin textures in ferromagnetic ultrathin films are attracting a renewed interest fueled by possible fine engineering of several magnetic interactions, notably the interfacial Dzyaloshinskii-Moriya interaction. This allows the stabilization of complex chiral spin textures such as chiral magnetic domain walls (DWs), spin spirals, and magnetic skyrmions. We report here on the ultrafast behavior of chiral DWs after optical pumping in perpendicularly magnetized asymmetric multilayers, probed using time-resolved circular dichroism in x-ray resonant magnetic scattering (CD-XRMS). We observe a picosecond transient reduction of the CD-XRMS, which is attributed to the spin current-induced coherent and incoherent torques within the continuously dependent spin texture of the DWs. We argue that a specific demagnetization of the inner structure of the DW induces a flow of hot spins from the interior of the neighboring magnetic domains. We identify this time-varying change of the DW textures shortly after the laser pulse as a distortion of the homochiral N'eel shape toward a transient mixed Bloch-N��el-Bloch textures along a direction transverse to the DW. Our study highlights how time-resolved CD-XRMS can be a unique tool for studying the time evolution in other systems showing a non-collinear electric/magnetic ordering such as skyrmion lattices, conical/helical phases, as well as the recently observed antiskyrmion lattices, in metallic or insulating materials.

Ultrafast phenomena on a femtosecond timescale are commonly examined by pump-probe experiments. This implies multiple measurements, where the sample under investigation is pumped with a short light pulse and then probed with a second pulse at various time delays to follow its dynamics. Recently, the principle of streaking extreme ultraviolet (XUV) pulses in the temporal domain has enabled recording the dynamics of a system within a single pulse. However, separate pump-probe experiments at different absorption edges still lack a unified timing, when comparing the dynamics in complex systems. Here, we report on an experiment using a dedicated optical element and the two-color emission of the FERMI XUV free-electron laser to follow the charge and spin dynamics in composite materials at two distinct absorption edges, simultaneously. The sample, consisting of ferromagnetic Fe and Ni layers, separated by a Cu layer, is pumped by an infrared laser and probed by a two-color XUV pulse with photon energies tuned to the M-shell resonances of these two transition metals. The experimental geometry intrinsically avoids any timing uncertainty between the two elements and unambiguously reveals an approximately 100 fs delay of the magnetic response with respect to the electronic excitation for both Fe and Ni. This delay shows that the electronic and spin degrees of freedom are decoupled during the demagnetization process. We furthermore observe that the electronic dynamics of Ni and Fe show pronounced differences when probed at their resonance, while the demagnetization dynamics are similar. These observations underline the importance of simultaneous investigation of the temporal response of both charge and spin in multi-component materials. In a more general scenario, the experimental approach can be extended to continuous energy ranges, promising the development of jitter-free transient absorption spectroscopy in the XUV and soft X-ray regimes.