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Wide-band-gap insulators such as NiO offer the exciting prospect of coherently manipulating electronic correlations with strong optical fields. Contrary to metals where rapid dephasing of optical excitation

Ever since its first observation, the microscopic origin of ultrafast magnetization dynamics has been actively debated. Even more questions arise when considering composite materials featuring a combination of intrinsic and proximity-induced magnetic moments. Currently, it is unknown whether the specific ultrafast dynamics of different sublattices in the popular ferromagnets consisting of 3d (Co, Fe) and 4d, 5d (Pd, Pt) transition metals are playing a crucial role in various effects, including all-optical magnetization switching. Here we investigate the element-specific dynamics of Co-Pt alloys on femtosecond and picosecond time scales using magneto-optical spectroscopy in the extended ultraviolet (EUV) region. Our results reveal that despite the proximity-induced nature of the magnetization of Pt atoms, the two sublattices in the alloy can have different responses to the optical excitation featuring distinct demagnetization rates. Additionally we show that it is important to consider the modification of magnetic anisotropy in opto-magnetic experiments as the vast majority of them are sensitive only to a single projection of the magnetic moment on the predefined axis, which may lead to experimental artifacts.

In this study, we applied electron energy-loss magnetic chiral dichmism (EMCD), an electron counterpart of X-ray magnetic circular dichmism (XMCD), to a network nanostructured FePt L1(0) ordered alloy film to examine the relative orientation of magnetic moments between neighboring Fe and Pt atoms using the Fe-M-2,M-3, Pt-O-2,O-3, and Pt-N-6,N-7 semi-core excitation spectra with transmission electron microscopy and electron energy-loss spectroscopy. EMCD signals were successfully extracted from a large number of spectra using a dedicated data analysis procedure to obtain sufficient noise statistics. Results showed that the relative sign relation of the EMCD signals between the Fe and Pt absorption edges was consistent with that of the theoretical dielectric tensor while assuming that parallel magnetic moments exist between neighboring Fe and Pt. We believe the results of this study can be applied to alloys with different nanostructures to determine whether the spin configuration depends on the size and geometry of the nanostructures.

Faraday discussions 237, 300 - 316 (2022). doi:10.1039/d2fd00005a, Wide-band-gap insulators such as NiO offer the exciting prospect of coherently manipulating electronic correlations with strong optical fields. Contrary to metals where rapid dephasing of optical excitation via electronic processes occurs, the sub-gap excitation in charge-transfer insulators has been shown to couple to low-energy bosonic excitations. However, it is currently unknown if the bosonic dressing field is composed of phonons or magnons. Here we use the prototypical charge-transfer insulator NiO to demonstrate that 1.5 eV sub-gap optical excitation leads to a renormalised NiO band-gap in combination with a significant reduction of the antiferromagnetic order. We employ element-specific X-ray reflectivity at the FLASH free-electron laser to demonstrate the reduction of the upper band-edge at the O 1s–2p core–valence resonance (K-edge) whereas the antiferromagnetic order is probed via X-ray magnetic linear dichroism (XMLD) at the Ni 2p–3d resonance (L$_2$-edge). Comparing the transient XMLD spectral line shape to ground-state measurements allows us to extract a spin temperature rise of 65 ± 5 K for time delays longer than 400 fs while at earlier times a non-equilibrium spin state is formed. We identify transient mid-gap states being formed during the first 200 fs accompanied by a band-gap reduction lasting at least up to the maximum measured time delay of 2.4 ps. Electronic structure calculations indicate that magnon excitations significantly contribute to the reduction of the NiO band gap., Published by Soc., Cambridge [u.a.]

Symmetry is a powerful concept in physics, but its applicability to far-from-equilibrium states is still being understood. Recent attention has focused on how far-from-equilibrium states lead to spontaneous symmetry breaking. Conversely, ultrafast optical pumping can be used to drastically change the energy landscape and quench the magnetic order parameter in magnetic systems. Here, we find a distinct symmetry-dependent ultrafast behaviour by use of ultrafast x-ray scattering from magnetic patterns with varying degrees of isotropic and anisotropic symmetry. After pumping with an optical laser, the scattered intensity reveals a radial shift exclusive to the isotropic component and exhibits a faster recovery time from quenching for the anisotropic component. These features arise even when both symmetry components are concurrently measured, suggesting a correspondence between the excitation and the magnetic order symmetry. Our results underline the importance of symmetry as a critical variable to manipulate the magnetic order in the ultrafast regime.

Abstract Despite their fundamental role in determining many important properties of materials, detailed momentum-dependent information on the strength of electron–phonon and phonon–phonon coupling across the entire Brillouin zone has remained elusive. Ultrafast electron diffuse scattering (UEDS) is a recently developed technique that is making a significant contribution to these questions. Here, we describe both the UEDS methodology and the information content of ultrafast, photoinduced changes in phonon-diffuse scattering from single-crystal materials. We present results obtained from Ni, WSe2, and TiSe2, materials that are characterized by a complex interplay between electronic (charge, spin) and lattice degrees of freedom. We demonstrate the power of this technique by unraveling carrier–phonon and phonon–phonon interactions in both momentum and time and following nonequilibrium phonon dynamics in detail on ultrafast time scales. By combining ab initio calculations with ultrafast diffuse electron scattering, insights into electronic and magnetic dynamics that impact UEDS indirectly can also be obtained. Graphic Abstract

Ultrafast optical pumping of spatially nonuniform magnetic textures is known to induce far-from-equilibrium spin transport effects. Here, we use ultrafast x-ray diffraction with unprecedented dynamic range to study the laser-induced dynamics of labyrinth domain networks in ferromagnetic CoFe/Ni multilayers. We detected azimuthally isotropic, odd order, magnetic diffraction rings up to 5th order. The amplitudes of all three diffraction rings quench to different degrees within 1.6 ps. In addition, all three of the detected diffraction rings both broaden by 15% and radially contract by 6% during the quench process. We are able to rigorously quantify a 31% ultrafast broadening of the domain walls via Fourier analysis of the order-dependent quenching of the three detected diffraction rings. The broadening of the diffraction rings is interpreted as a reduction in the domain coherence length, but the shift in the ring radius, while unambiguous in its occurrence, remains unexplained. In particular, we demonstrate that a radial shift explained by domain wall broadening can be ruled out. With the unprecedented dynamic range of our data, our results provide convincing evidence that labyrinth domain structures are spatially perturbed at ultrafast speeds under far-from-equilibrium conditions, albeit the mechanism inducing the perturbations remains yet to be clarified.

© 2017 American Chemical Society. Light-matter interaction at the nanoscale in magnetic materials is a topic of intense research in view of potential applications in next-generation high-density magnetic recording. Laser-assisted switching provides a pathway for overcoming the material constraints of high-anisotropy and high-packing density media, though much about the dynamics of the switching process remains unexplored. We use ultrafast small-angle X-ray scattering at an X-ray free-electron laser to probe the magnetic switching dynamics of FePt nanoparticles embedded in a carbon matrix following excitation by an optical femtosecond laser pulse. We observe that the combination of laser excitation and applied static magnetic field, 1 order of magnitude smaller than the coercive field, can overcome the magnetic anisotropy barrier between "up" and "down" magnetization, enabling magnetization switching. This magnetic switching is found to be inhomogeneous throughout the material with some individual FePt nanoparticles neither switching nor demagnetizing. The origin of this behavior is identified as the near-field modification of the incident laser radiation around FePt nanoparticles. The fraction of not-switching nanoparticles is influenced by the heat flow between FePt and a heat-sink layer.

Femtosecond laser excitation of solid-state systems creates out-of-equilibrium hot electrons that cool down by transferring their energy to other degrees of freedom and ultimately to lattice vibrations of the solid. By combining ab initio calculations with ultrafast diffuse electron scattering, we gain a detailed understanding of the complex nonequilibrium energy transfer between electrons and phonons in laser-excited Ni metal. Our experimental results show that the wave-vector-resolved population dynamics of phonon modes is distinctly different throughout the Brillouin zone and are in remarkable agreement with our theoretical results. We find that zone-boundary phonon modes become occupied first. As soon as the energy in these modes becomes larger than the average electron energy, a backflow of energy from lattice to electronic degrees of freedom occurs. Subsequent excitation of lower-energy phonon modes drives the thermalization of the whole system on the picosecond time scale. We determine the evolving nonequilibrium phonon occupations, which we find to deviate markedly from thermal occupations.

Vanadium dioxide (VO2) is a much-discussed material for oxide electronics and neuromorphic computing applications. Here, heteroepitaxy of VO2 is realized on top of oxide nanosheets that cover either the amorphous silicon dioxide surfaces of Si substrates or X-ray transparent silicon nitride membranes. The out-of-plane orientation of the VO2 thin films is controlled at will between (011)M1/(110)R and (−402)M1/(002)R by coating the bulk substrates with Ti0.87O2 and NbWO6 nanosheets, respectively, prior to VO2 growth. Temperature-dependent X-ray diffraction and automated crystal orientation mapping in microprobe transmission electron microscope mode (ACOM-TEM) characterize the high phase purity, the crystallographic and orientational properties of the VO2 films. Transport measurements and soft X-ray absorption in transmission are used to probe the VO2 metal–insulator transition, showing results of a quality equal to those from epitaxial films on bulk single-crystal substrates. Successful local manipulation of two different VO2 orientations on a single substrate is demonstrated using VO2 grown on lithographically patterned lines of Ti0.87O2 and NbWO6 nanosheets investigated by electron backscatter diffraction. Finally, the excellent suitability of these nanosheet-templated VO2 films for advanced lensless imaging of the metal–insulator transition using coherent soft X-rays is discussed.

Resonant X-ray absorption, where an X-ray photon excites a core electron into an unoccupied valence state, is an essential process in many standard X-ray spectroscopies. With increasing X-ray intensity, the X-ray absorption strength is expected to become nonlinear. Here, we report the onset of such a nonlinearity in the resonant X-ray absorption of magnetic Co/Pd multilayers near the Co L\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${}_{3}$$\end{document}3 edge. The nonlinearity is directly observed through the change of the absorption spectrum, which is modified in less than 40 fs within 2 eV of its threshold. This is interpreted as a redistribution of valence electrons near the Fermi level. For our magnetic sample this also involves mixing of majority and minority spins, due to sample demagnetization. Our findings reveal that nonlinear X-ray responses of materials may already occur at relatively low intensities, where the macroscopic sample is not destroyed, providing insight into ultrafast charge and spin dynamics., X-ray free electron lasers allow for studying the interaction of magnetic materials with intense X-rays beyond a linear response regime. Here, the authors demonstrate the onset of X-ray induced ultrafast demagnetization in Co/Pd multilayers via a redistribution of valence electrons on timescales shorter than 40 fs.

Magnetostriction, the strain induced by a change in magnetization, is a universal effect in magnetic materials. Owing to the difficulty in unraveling its microscopic origin, it has been largely treated phenomenologically. Here, we show how the source of magnetostriction—the underlying magnetoelastic stress—can be separated in the time domain, opening the door for an atomistic understanding. X-ray and electron diffraction are used to separate the sub-picosecond spin and lattice responses of FePt nanoparticles. Following excitation with a 50-fs laser pulse, time-resolved X-ray diffraction demonstrates that magnetic order is lost within the nanoparticles with a time constant of 146 fs. Ultrafast electron diffraction reveals that this demagnetization is followed by an anisotropic, three-dimensional lattice motion. Analysis of the size, speed, and symmetry of the lattice motion, together with ab initio calculations accounting for the stresses due to electrons and phonons, allow us to reveal the magnetoelastic stress generated by demagnetization., Although magnetostriction is universal in magnetic materials, understanding its microscopic origin remains challenging. Here the authors use X-ray and ultrafast electron diffraction to separate the material’s sub-picosecond spin and lattice responses and reveal the magnetoelastic stress generated by demagnetization.

X-ray free-electron lasers are unique sources of high-brightness coherent radiation. However, existing devices supply only linearly polarized light, precluding studies of chiral dynamics. A device called the Delta undulator has been installed at the Linac Coherent Light Source (LCLS) to provide tunable polarization. With a reverse tapered planar undulator line to pre-microbunch the beam and the novel technique of beam diverting, hundreds of microjoules of circularly polarized X-ray pulses are produced at 500–1,200 eV. These X-ray pulses are tens of femtoseconds long, have a degree of circular polarization of 0.98–0.04+0.02 at 707 eV and may be scanned in energy. We also present a new two-colour X-ray pump–X-ray probe operating mode for the LCLS. Energy differences of ΔE/E = 2.4% are supported, and the second pulse can be adjusted to any elliptical polarization. In this mode, the pointing, timing, intensity and wavelength of the two pulses can be modified. Tunable polarization control and a two-colour X-ray pump–X-ray probe operating mode are demonstrated at the Linac Coherent Light Source (LCLS).

Physical review letters 121(13), 137403 (2018). doi:10.1103/PhysRevLett.121.137403, Using ultrafast $≃2.5 fs$ and $≃25 fs$ self-amplified spontaneous emission pulses of increasing intensity and a novel experimental scheme, we report the concurrent increase of stimulated emission in the forward direction and loss of out-of-beam diffraction contrast for a $Co/Pd$ multilayer sample. The experimental results are quantitatively accounted for by a statistical description of the pulses in conjunction with the optical Bloch equations. The dependence of the stimulated sample response on the incident intensity, coherence time, and energy jitter of the employed pulses reveals the importance of increased control of x-ray free electron laser radiation., Published by APS, College Park, Md.

As a type of fermions without counterpart in high energy physics, triply degenerate fermions show exotic physical properties, which are represented by triply degenerate nodal points in topological semimetals. Here, based on the space group theory analysis, we propose a practical guidance for seeking a topological semimetal with triply degenerate nodal points located at a symmetric axis, which is applicable to both symmorphic and nonsymmorphic crystals. By using this guidance in combination with the first-principles electronic structure calculations, we predict a class of triply degenerate topological semimetals $R{\mathrm{Rh}}_{6}{\mathrm{Ge}}_{4}\phantom{\rule{4pt}{0ex}}(R=\text{Y},\text{La},\text{Lu})$. In these compounds, the triply degenerate nodal points are located at the $\mathrm{\ensuremath{\Gamma}}\text{\ensuremath{-}}A$ axis and not far from the Fermi level. Especially, ${\mathrm{LaRh}}_{6}{\mathrm{Ge}}_{4}$ has a pair of triply degenerate nodal points located at just $\ensuremath{\sim}3$ meV below the Fermi level. Considering the fact that the single crystals of $R{\mathrm{Rh}}_{6}{\mathrm{Ge}}_{4}$ have been synthesized experimentally, the $R{\mathrm{Rh}}_{6}{\mathrm{Ge}}_{4}$ class of compounds will be an appropriate platform for studying exotic physical properties of triply degenerate topological semimetals.

The interplay between the electronic and lattice degrees of freedom in nonequilibrium states of strongly correlated systems has been debated for decades. Although progress has been made in establishing a hierarchy of electronic interactions with the use of time-resolved techniques, the role of the phonons often remains in dispute, a situation highlighting the need for tools that directly probe the lattice. We present the first combined megaelectron volt ultrafast electron diffraction and time- and angle-resolved photoemission spectroscopy study of optimally doped Bi2Sr2CaCu2O8+δ. Quantitative analysis of the lattice and electron subsystems’ dynamics provides a unified picture of nonequilibrium electron-phonon interactions in the cuprates beyond the N-temperature model. The work provides new insights on the specific phonon branches involved in the nonequilibrium heat dissipation from the high-energy Cu–O bond stretching “hot” phonons to the lowest-energy acoustic phonons with correlated atomic motion along the crystal directions and their characteristic time scales. It reveals a highly nonthermal phonon population during the first several picoseconds after the photoexcitation. The approach, taking advantage of the distinct nature of electrons and photons as probes, is applicable for studying energy relaxation in other strongly correlated electron systems. OA gold - CA extern

“The technical support from SLAC Accelerator Directorate, Technology Innovation Directorate, LCLS laser division and Test Facility Division is gratefully acknowledged. We thank S.P. Weathersby, R.K. Jobe, D. McCormick, A. Mitra, S. Carron and J. Corbett for their invaluable help and technical assistance. Research at SLAC was supported through the SIMES Institute which like the LCLS and SSRL user facilities is funded by the Office of Basic Energy Sciences of the U.S. Department of Energy under Contract No. DE-AC02-76SF00515. The UED work was performed at SLAC MeV-UED, which is supported in part by the DOE BES SUF Division Accelerator & Detector R&D program, the LCLS Facility, and SLAC under contract Nos. DE-AC02-05-CH11231 and DE-AC02-76SF00515. Use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515.”and“Work at BNL was supported by DOE BES Materials Science and Engineering Division under Contract No: DE-AC02-98CH10886. J.C. would like to acknowledge the support from National Science Foundation Grant No. 1207252. E.E.F. would like to acknowledge support from the U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES) under Award No. DE-SC0003678.”This has been corrected in both the PDF and HTML versions of the Article.

Modern transmission electron microscopes can image individual atoms and molecules. But to unlock new science, the next generation of instruments must look beyond just higher spatial resolution.

Heterodyning by a phase stable reference electric field is a well known technique to amplify weak nonlinear signals. For short wavelength, the generation of a reference field in front of the sample is challenging because of a lack of suitable beamsplitters. Here, we use a permanent grating which matches the line spacing of the transient grating for the creation of a phase stable reference field. The relative phase among the two can be changed by a relative translation of the permanent and transient gratings in direction orthogonal to the grating lines. We demonstrate the technique for a transient grating on a VO2 thin film and observe constructive as well as destructive interference signals.

The magnetic field associated with a picosecond intense electron pulse is shown to switch locally the magnetization of extended films and nanostructures and to ignite locally spin waves excitations. Also, topologically protected magnetic textures such as skyrmions can be imprinted swiftly in a sample with a residual Dzyaloshinskii-Moriya spin-orbital coupling. Characteristics of the created excitations such as the topological charge or the width of the magnon spectrum can be steered via the duration and the strength of the electron pulses. The study points to a possible way for a spatiotemporally controlled generation of magnetic and skyrmionic excitations., Comment: 12 pages, 6 figures, SPIE proceedings

Both electron and lattice dynamics are directly observed in the nonequilibrium state of strongly correlated Bi-2212., The interplay between the electronic and lattice degrees of freedom in nonequilibrium states of strongly correlated systems has been debated for decades. Although progress has been made in establishing a hierarchy of electronic interactions with the use of time-resolved techniques, the role of the phonons often remains in dispute, a situation highlighting the need for tools that directly probe the lattice. We present the first combined megaelectron volt ultrafast electron diffraction and time- and angle-resolved photoemission spectroscopy study of optimally doped Bi2Sr2CaCu2O8+δ. Quantitative analysis of the lattice and electron subsystems’ dynamics provides a unified picture of nonequilibrium electron-phonon interactions in the cuprates beyond the N-temperature model. The work provides new insights on the specific phonon branches involved in the nonequilibrium heat dissipation from the high-energy Cu–O bond stretching “hot” phonons to the lowest-energy acoustic phonons with correlated atomic motion along the crystal directions and their characteristic time scales. It reveals a highly nonthermal phonon population during the first several picoseconds after the photoexcitation. The approach, taking advantage of the distinct nature of electrons and photons as probes, is applicable for studying energy relaxation in other strongly correlated electron systems.

We apply time-resolved MeV electron diffraction to study the electron-lattice energy relaxation in thin film Au-insulator heterostructures. Through precise measurements of the transient Debye-Waller-factor, the mean-square atomic displacement is directly determined, which allows to quantitatively follow the temporal evolution of the lattice temperature after short pulse laser excitation. Data obtained over an extended range of laser fluences reveal an increased relaxation rate when the film thickness is reduced or the Au-film is capped with an additional insulator top-layer. This behavior is attributed to a cross-interfacial coupling of excited electrons in the Au film to phonons in the adjacent insulator layer(s). Analysis of the data using the two-temperature-model taking explicitly into account the additional energy loss at the interface(s) allows to deduce the relative strength of the two relaxation channels. CA Sokolowski-Tinten

This article reviews static and dynamic interfacial effects in magnetism, focusing on interfacially-driven magnetic effects and phenomena associated with spin-orbit coupling and intrinsic symmetry breaking at interfaces. It provides a historical background and literature survey, but focuses on recent progress, identifying the most exciting new scientific results and pointing to promising future research directions. It starts with an introduction and overview of how basic magnetic properties are affected by interfaces, then turns to a discussion of charge and spin transport through and near interfaces and how these can be used to control the properties of the magnetic layer. Important concepts include spin accumulation, spin currents, spin transfer torque, and spin pumping. An overview is provided to the current state of knowledge and existing review literature on interfacial effects such as exchange bias, exchange spring magnets, spin Hall effect, oxide heterostructures, and topological insulators. The article highlights recent discoveries of interface-induced magnetism and non-collinear spin textures, non-linear dynamics including spin torque transfer and magnetization reversal induced by interfaces, and interfacial effects in ultrafast magnetization processes., 193 pages, including 28 figures inserted after text and references. Paper accepted in Reviews of Modern Physics

Bulk vanadium dioxide undergoes a metal–insulator transition near room temperature. It is now shown that by putting a thin layer of vanadium dioxide on a buffer, and varying the buffer’s thickness, the orbital occupancy in the metallic state and the transition temperature can be tuned.

The prospect of manipulating materials’ properties with femtosecond laser pulses, the shortest stimuli known to mankind, has fascinated researchers for decades. Discoveries of femtosecond demagnetization of ferromagnets and all-optical magnetic switching are fueled by the demand for faster information storage and processing. However, understanding when and how optical energy delivered into band electrons is transferred to spin and lattice degrees of freedom remains among the most challenging and important topics in condensed matter physics. Here we demonstrate for FePt nanoparticles how to disentangle these complex energy pathways. We show that femtosecond demagnetization launches a highly anisotropic ultrafast lattice motion characterized by a- and b-axis expansion and c-axis contraction. Picosecond lattice stress from non-equilibrium phonons increases the a,b-lattice spacing while invar-like near-zero c-axis expansion persists for tens of picoseconds. Our work establishes for a metallic system the existence of intimate spin, electron and lattice coupling, a hallmark usually reserved for strongly correlated electron systems.

Vanadium dioxide is of broad interest as a spin-1/2 electron system that realizes a metal-insulator transition near room temperature, due to a combination of strongly correlated and itinerant electron physics. Here, resonant inelastic X-ray scattering is used to measure the excitation spectrum of charge, spin, and lattice degrees of freedom at the vanadium L-edge under different polarization and temperature conditions. These spectra reveal the evolution of energetics across the metal-insulator transition, including the low temperature appearance of a strong candidate for the singlet-triplet excitation of a vanadium dimer., Comment: 5 pages, 4 figures

We use femtosecond time-resolved hard x-ray scattering to detect coherent acoustic phonons generated during ultrafast laser excitation of ferromagnetic bcc Fe films grown on MgO(001). We observe the coherent longitudinal-acoustic phonons as a function of wave vector through analysis of the temporal oscillations in the x-ray scattering signal. The width of the extracted strain wave front associated with this coherent motion is $\ensuremath{\sim}100$ fs. An effective electronic Gr\"uneisen parameter is extracted within a two-temperature model. However, ab initio calculations show that the phonons are nonthermal on the time scale of the experiment, which calls into question the validity of extracting physical constants by fitting such a two-temperature model.

We use single-cycle THz fields and the femtosecond magneto-optical Kerr effect to respectively excite and probe the magnetization dynamics in two thin-film ferromagnets with different lattice structure: crystalline Fe and amorphous CoFeB. We observe Landau-Lifshitz-torque magnetization dynamics of comparable magnitude in both systems, but only the amorphous sample shows ultrafast demagnetization caused by the spin-lattice depolarization of the THz-induced ultrafast spin current. Quantitative modelling shows that such spin-lattice scattering events occur on similar time scales than the conventional spin conserving electronic scattering ($\sim30$ fs). This is significantly faster that optical laser-induced demagnetization. THz conductivity measurements point towards the influence of lattice disorder in amorphous CoFeB as the driving force for enhanced spin-lattice scattering., Comment: 10 pages, 4 figures

© 2016 American Physical Society. We use polarization- and temperature-dependent x-ray absorption spectroscopy, in combination with photoelectron microscopy, x-ray diffraction, and electronic transport measurements, to study the driving force behind the insulator-metal transition in VO2. We show that both the collapse of the insulating gap and the concomitant change in crystal symmetry in homogeneously strained single-crystalline VO2 films are preceded by the purely electronic softening of Coulomb correlations within V-V singlet dimers. This process starts 7 K (±0.3 K) below the transition temperature, as conventionally defined by electronic transport and x-ray diffraction measurements, and sets the energy scale for driving the near-room-temperature insulator-metal transition in this technologically promising material.

Using time-resolved electron diffraction the electron-lattice equilibration in laser-excited thin Bi-films has been investigated. Our data reveal a pronounced thickness-dependence which is attributed to cross-interfacial coupling of hot electrons in the Bi-film to substrate phonons.

We present equilibrium and out-of-equilibrium studies of the Verwey transition in magnetite. In the equilibrium optical conductivity, we find a steplike change at the phase transition for photon energies below about 2 eV. The possibility of triggering a nonequilibrium transient metallic state in insulating magnetite by photo excitation was recently demonstrated by an x-ray study. Here we report a full characterization of the optical properties in the visible frequency range across the nonequilibrium phase transition. Our analysis of the spectral features is based on a detailed description of the equilibrium properties. The out-of-equilibrium optical data bear the initial electronic response associated to localized photoexcitation, the occurrence of phase separation, and the transition to a transient metallic phase for excitation density larger than a critical value. This allows us to identify the electronic nature of the transient state, to unveil the phase transition dynamics, and to study the consequences of phase separation on the reflectivity, suggesting a spectroscopic feature that may be generally linked to out-of-equilibrium phase separation.

The Advanced Photon Source (APS) operates with a timing structure advantageous for ultrafast dynamics experiments and, as a result, X-ray time-resolved studies on the 100-picosecond timescale have flourished. The standard operating mode, 24-bunch mode, runs 65% of the time and a hybrid singlet mode runs 15% of the time, yielding a total of 80% of beamtime easily accessible for studies of ultrafast dynamics using laser-pump/X-ray probe techniques. This article highlights recent enhanced capabilities for time-resolved studies at the APS.

We describe a novel experimental facility at the BESSY II synchrotron, aiming at probing element-specific magnetic properties at the nm-length scale. It consists of a novel photoemission electron microscope with photoelectron spin analysis combined with a microfocus beamline and full X-ray polarization control. The facility is capable of magnetic imaging in applied fields allowing the observation of magnetic switching phenomena on a 30-nm-length scale. Copyright © 2010 John Wiley & Sons, Ltd.

We demonstrate a tilted pulse-front transient grating (TG) technique that allows to optimally utilize time resolution as well as TG line density while probing under grazing incidence as typically done in extreme ultraviolet (EUV) or soft x-ray (SXR) experiments. Our optical setup adapts the pulse front tilt of the two pulses that create the TG to the grazing incident pulse. We demonstrate the technique using all 800 nm femtosecond laser pulses for TG generation on a vanadium dioxide film. We probe that grating via diffraction of a third 800 nm pulse. The time resolution of 90 fs is an improvement by a factor of 30 compared to our previous experiments on the same system. The scheme paves the way for EUV and SXR probing of optically induced TGs on any material.

For an isolated quantum particle, such as an electron, the orbital (L) and spin (S) magnetic moments can change provided that the total angular momentum of the particle is conserved. In condensed matter, an efficient transfer between L and S can occur owing to the spin-orbit interaction, which originates in the relativistic motion of electrons. Disentangling the absolute contributions of the orbital and spin angular momenta is challenging, however, as any transfer between the two occurs on femtosecond timescales. Here we investigate such phenomena by using ultrashort optical laser pulses to change the magnetization of a ferromagnetic film and then probe its dynamics with circularly polarized femtosecond X-ray pulses. Our measurements enable us to disentangle the spin and orbital components of the magnetic moment, revealing different dynamics for L and S. We highlight the important role played by the spin-orbit interaction in the ultrafast laser-induced demagnetization of ferromagnetic films, and show also that the magneto-crystalline anisotropy energy is an important quantity to consider in such processes. Our study provides insights into the dynamics in magnetic systems as well as perspectives for the ultrafast control of information in magnetic recording media.

Experiments are reviewed which extend ultraviolet photoemission and soft X-ray absorption spectroscopy to the femtosecond (fs) time domain. We show for the case of ferromagnetic Ni that the evolution of electronic temperature, exchange coupling, spin and orbital angular momentum following fs optical laser excitation can be individually probed. This provides new insights into ultrafast processes which involve energy and angular momentum transfer between charge, spin and lattice degrees of freedom.

We present the first X-ray absorption spectrum over an entire absorption edge using femtosecond pulses from a synchrotron-based slicing source. An ultrafast laser pulse excited a nickel film, and a succeeding X-ray pulse from the BESSY femtoslicing facility probed the Ni L3-edge. By choosing either linear or circular X-ray polarization, the spectra represent snapshots of the electronic or the magnetic state, respectively, with an exposure time of about 100 fs. We find an almost instantaneous response of the electronic system to the laser pulse, and provide a first direct measurement of the quenching of magnetic moments within 120 fs.

Two-dimensional materials are subject to intrinsic and dynamic rippling that modulates their optoelectronic and electromechanical properties. Here, we directly visualize the dynamics of these processes within monolayer transition metal dichalcogenide MoS2 using femtosecond electron scattering techniques as a real-time probe with atomic-scale resolution. We show that optical excitation induces large-amplitude in-plane displacements and ultrafast wrinkling of the monolayer on nanometer length-scales, developing on picosecond time-scales. These deformations are associated with several percent peak strains that are fully reversible over tens of millions of cycles. Direct measurements of electron-phonon coupling times and the subsequent interfacial thermal heat flow between the monolayer and substrate are also obtained. These measurements, coupled with first-principles modeling, provide a new understanding of the dynamic structural processes that underlie the functionality of two-dimensional materials and open up new opportunities for ultrafast strain engineering using all-optical methods.

We model room temperature soft x-ray resonant magnetic reflectivity to determine a 24% increase of the Fe magnetic moment of the 2–3 monolayers next to both MgO interfaces in a MgO(3 nm)/Fe(12 nm)/MgO(001) heterostructure. This direct measurement of such enhanced interface magnetic moments for buried interfaces confirms theoretical predictions and highlights the importance of considering inhomogeneous in-depth magnetic profile in Fe/MgO based magnetic tunnel junctions.

We have used a MHz lock-in x-ray spectro-microscopy technique to directly detect changes of magnetic moments in Cu due to spin injection from an adjacent Co layer. The elemental and chemical specificity of x-rays allows us to distinguish two spin current induced effects. We detect the creation of transient magnetic moments of $3\times 10^{-5}$ $\mu_\mathrm{B}$ on Cu atoms within the bulk of the 28 nm thick Cu film due to spin-accumulation. The moment value is compared to predictions by Mott's two current model. We also observe that the hybridization induced existing magnetic moments on Cu interface atoms are transiently increased by about 10% or $4\times 10^{-3}$ $\mu_\mathrm{B}$. This reveals the dominance of spin-torque alignment over Joule heat induced disorder of the interfacial Cu moments during current flow.

Terahertz driven magnetization dynamics are explored in the orthoferrite DyFeO3. A high-field, single cycle THz pulse is used to excite magnon modes in the crystal together with other resonances. Both quasi-ferromagnetic and quasi-antiferromagnetic magnon modes are excited and appear in time-resolved measurements of the Faraday rotation. Other modes are also observed in the measurements of the time-resolved linear birefringence. Analysis of the excitation process reveals that despite larger than expected electro-optical susceptibility it is mainly the THz magnetic field that couples to the quasi-ferromagnetic and quasi-antiferromagnetic magnon branches., Comment: 10 pages, 4 figures