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The use of advanced x-ray sources plays a key role in the study of dynamic processes in magnetically ordered materials. The progress in x-ray free-electron lasers enables the direct and simultaneous observation of the femtosecond evolution of electron and spin systems through transient x-ray absorption spectroscopy and x-ray magnetic circular dichroism, respectively. Such experiments allow us to resolve the response seen in the population of the spin-split valence states upon optical excitation. Here, we utilize circularly polarized ultrashort soft x-ray pulses from the new helical afterburner undulator at the free-electron laser FLASH in Hamburg to study the femtosecond dynamics of a laser-excited CoPt alloy at the Co L3-edge absorption. Despite employing a weaker electronic excitation level, we find a comparable demagnetization for the Co 3d-states in CoPt compared to previous measurements on CoPd. This is attributed to the distinctly different spin–orbit coupling between 3d and 4d vs 3d and 5d elements in the corresponding alloys and multilayers.

X-ray circular dichroism (XMCD), one of the main tools to study magnetism, benefits enormously from the capability of a fast alterable helicity of circularly polarized X-ray photons. Here we present a method for boosting the alternating frequency between right- and left-handed photons to the MHz regime, more than three orders of magnitude faster than state-of-the-art technologies. The method is based on a twin elliptical undulator installed in an electron storage ring being operated in a novel mode where the electron optics is tuned close to a resonance with electrons captured in transverse resonance island buckets. Propagating through the twin undulator, electrons from different islands emit photons of the same wavelength but of opposite helicity. These two helicity components can be alternated as fast as 2 ns. In a proof-of-principle experiment at BESSY II, we demonstrate XMCD at the L 2 , 3 absorption edges of Ni with an 800 ns helicity flip. Rapidly switching the helicity of polarised x-rays is desirable for studying magnetic dynamics via circular dichroism spectroscopy, but has not yet been realised from synchrotron radiation sources. Here, switching between ultrafast emission of monoenergetic, circularly polarized x-rays with opposite helicity is shown within a few nanoseconds.

We study the optical-pump induced ultrafast transient change of x-ray absorption at L3 absorption resonances of the transition metals Ni and Fe in the Fe0.5Ni0.5 alloy. We find the effect for both elements to occur simultaneously on a femtosecond timescale. This effect may hence be used as a handy cross correlation scheme, providing a time-zero reference for ultrafast optical-pump soft x-ray-probe measurement. The method benefits from a relatively simple experimental setup as the sample itself acts as time-reference tool. In particular, this technique works with low flux ultrafast soft x-ray sources. The measurements are compared to the cross correlation method introduced in an earlier publication.

X-ray absorption spectroscopy (XAS) and the directly linked X-ray reflectivity near absorption edges yield a wealth of specific information on the electronic structure around the resonantly addressed element. Observing the dynamic response of complex materials to optical excitations in pump–probe experiments requires high sensitivity to small changes in the spectra which in turn necessitates the brilliance of free electron laser (FEL) pulses. However, due to the fluctuating spectral content of pulses generated by self-amplified spontaneous emission (SASE), FEL experiments often struggle to reach the full sensitivity and time-resolution that FELs can in principle enable. Here, we implement a setup which solves two common challenges in this type of spectroscopy using FELs: First, we achieve a high spectral resolution by using a spectrometer downstream of the sample instead of a monochromator upstream of the sample. Thus, the full FEL bandwidth contributes to the measurement at the same time, and the FEL pulse duration is not elongated by a monochromator. Second, the FEL beam is divided into identical copies by a transmission grating beam splitter so that two spectra from separate spots on the sample (or from the sample and known reference) can be recorded in-parallel with the same spectrometer, enabling a spectrally resolved intensity normalization of pulse fluctuations in pump–probe scenarios. We analyze the capabilities of this setup around the oxygen K- and nickel L-edges recorded with third harmonic radiation of the free electron laser in Hamburg (FLASH), demonstrating the capability for pump–probe measurements with sensitivity to reflectivity changes on the per mill level.

Femtosecond laser pulses can be used to induce ultrafast changes of the magnetization in magnetic materials. Several microscopic mechanisms have been proposed to explain these observations, including the transport of ultrashort spin-polarized hot-electrons (SPHE). However, currently such ultrafast spin currents are only poorly characterized due to the measurement requirements for element and time resolution. Here, using time- and element-resolved X-ray magnetic circular dichroism alongside atomistic spin-dynamics simulations, we study the ultrafast transfer of the angular momentum from spin-polarized currents. We show that using a Co/Pt multilayer as a polarizer in a spin-valve structure, the SPHE drives the demagnetization of the two sub-lattices of the Fe 74 Gd 26 film. This behaviour can be explained with two physical mechanisms; spin transfer torque and thermal fluctuations induced by the SPHE. We provide a quantitative description of the heat transfer of the ultrashort SPHE pulse to the Fe 74 Gd 26 films, as well as the effect of spin-polarization of the SPHE current density responsible for the observed magnetization dynamics. Our work finally characterizes the spin-polarization of the SPHEs revealing unexpected opposite spin polarization to the Co magnetization. Prior studies have pointed to the role of spin-polarized hot electrons in ultrafast demagnetization. Here, by combining time and element resolved X-ray magnetic circular dichroism with theoretical calculations, Gupta et al quantitatively resolve both the effect of spin polarization and the current densities in ultrashort hot electron pulses.

The relationship between the magnetic interaction and photoinduced dynamics in antiferromagnetic perovskites is investigated in this study. In La1/3Sr2/3FeO3 thin films, commensurate spin ordering is accompanied by charge disproportionation, whereas SrFeO3−δ thin films show incommensurate helical antiferromagnetic spin ordering due to increased ferromagnetic coupling compared to La1/3Sr2/3FeO3. To understand the photoinduced spin dynamics in these materials, we investigate the spin ordering through time-resolved resonant soft x-ray scattering. In La1/3Sr2/3FeO3, ultrafast quenching of the magnetic ordering within 130 fs through a nonthermal process is observed, triggered by charge transfer between the Fe atoms. We compare this to the photoinduced dynamics of the helical magnetic ordering of SrFeO3−δ. We find that the change in the magnetic coupling through optically induced charge transfer can offer an even more efficient channel for spin-order manipulation.

Materials with insulator-metal transitions promise advanced functionalities for future information technology. Patterning on the microscale is key for miniaturized functional devices, but material properties may vary spatially across microstructures. Characterization of these miniaturized devices requires electronic structure probes with sufficient spatial resolution to understand the influence of structure size and shape on functional properties. The present study demonstrates the use of imaging soft X-ray absorption spectroscopy with a spatial resolution better than 2  μ m to study the insulator-metal transition in vanadium dioxide thin-film microstructures. This novel technique reveals that the transition temperature for the conversion from insulating to metallic vanadium dioxide is lowered by 1.2 K ± 0.4 K close to the structure edges compared to the center. Facilitated strain release during the phase transition is discussed as origin of the observed behavior. The experimental approach enables a detailed understanding of how the electronic properties of quantum materials depend on their patterning at the micrometer scale.

Investigation of ultrafast dynamic behaviors can provide novel insights about the coupling mechanisms among multiple degrees of freedom in condensed matters, such as lattice, magnetism and electronic structure. Here we investigate both the ferromagnetic (FM) and antiferromagnetic (AFM) dynamics of a strongly correlated oxide system, GdBaCo 2 O 5.5 thin film by time-resolved x-ray magnetic circular dichroism in reflectivity (XMCDR) and resonant magnetic x-ray diffraction (RMXD). A photo-induced AFM-FM transition characterized by an increase of the transient XMCDR (sensitive to FM order) beyond the unpumped value and a decay of RMXD (sensitive to AFM order) was observed. The photon-energy dependence of the transient XMCDR and reflectivity could be interpreted as a concomitant photo-induced spin-state transition (SST). The AFM-FM transition and SST couple with each other in the time domain, resulting in unusual dynamic behaviors of the magnetism. Ultrafast magnetisation dynamics can reveal transient magnetic states and enable the observation of exotic physics not accessible on shorter timescales. Here, the authors investigate a photo-induced antiferromagnetic-ferromagnetic transition in a strongly correlated thin film using time resolved X-ray based techniques.

In several strongly correlated electron systems, the short range ordering of defects, charge and local lattice distortions are found to show complex inhomogeneous spatial distributions. There is growing evidence that such inhomogeneity plays a fundamental role in unique functionality of quantum complex materials. La1.72Sr0.28NiO4 is a prototypical strongly correlated perovskite showing spin stripes order. In this work we present the spatial distribution of the spin order inhomogeneity by applying micro X-ray diffraction to La1.72Sr0.28NiO4, mapping the spin-density-wave order below the 120 K onset temperature. We find that the spin-density-wave order shows the formation of nanoscale puddles with large spatial fluctuations. The nano-puddle density changes on the microscopic scale forming a multiscale phase separation extending from nanoscale to micron scale with scale-free distribution. Indeed spin-density-wave striped puddles are disconnected by spatial regions with negligible spin-density-wave order. The present work highlights the complex spatial nanoscale phase separation of spin stripes in nickelate perovskites and opens new perspectives of local spin order control by strain.

We study the optical-pump induced ultrafast transient change of x-ray absorption at L3 absorption resonances of the transition metals Ni and Fe in the Fe0.5Ni0.5 alloy. We find the effect for both elements to occur simultaneously on a femtosecond timescale. This effect may hence be used as a handy cross correlation scheme, providing a time-zero reference for ultrafast optical-pump soft x-ray-probe measurement. The method benefits from a relatively simple experimental setup as the sample itself acts as time-reference tool. In particular, this technique works with low flux ultrafast soft x-ray sources. The measurements are compared to the cross correlation method introduced in an earlier publication.