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Relaxor ferroelectrics have been intensely studied for decades based on their unique electromechanical responses which arise from local structural heterogeneity involving polar nanoregions or domains. Here, we report first studies of the ultrafast dynamics and reconfigurability of the polarization in freestanding films of the prototypical relaxor 0.68PbMg

Magnetism in topological materials creates phases exhibiting quantized transport phenomena with potential technological applications. The emergence of such phases relies on strong interaction between localized spins and the topological bands, and the consequent formation of an exchange gap. However, this remains experimentally unquantified in intrinsic magnetic topological materials. Here, this interaction is quantified in MnBi

The inspection of Friedel's law in ultrafast electron diffraction (UED) is important to gain a comprehensive understanding of material atomic structure and its dynamic response. Here, monoclinic gallium telluride (GaTe), as a low-symmetry, layered crystal in contrast to many other 2D materials, is investigated by mega-electronvolt UED. Strong out-of-phase oscillations of Bragg peak intensities are observed for Friedel pairs, which does not obey Friedel's law. As evidenced by the preserved mirror symmetry and supported by both kinematic and dynamic scattering simulations, the intensity oscillations are provoked by the lowest-order longitudinal acoustic breathing phonon. Our results provide a generalized understanding of Friedel's law in UED and demonstrate that by designed misalignment of surface normal and primitive lattice vectors, coherent lattice wobbling and effective shear strain can be generated in crystal films by laser pulse excitation, which is otherwise hard to achieve and can be further utilized to dynamically tune and switch material properties.

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.

Engineering novel states of matter with light is at the forefront of materials research. An intensely studied direction is to realize broken-symmetry phases that are "hidden" under equilibrium conditions but can be unleashed by an ultrashort laser pulse. Despite a plethora of experimental discoveries, the nature of these orders and how they transiently appear remain unclear. To this end, we investigate a nonequilibrium charge density wave (CDW) in rare-earth tritellurides, which is suppressed in equilibrium but emerges after photoexcitation. Using a pump-pump-probe protocol implemented in ultrafast electron diffraction, we demonstrate that the light-induced CDW consists solely of order parameter fluctuations, which bear striking similarities to critical fluctuations in equilibrium despite differences in the length scale. By calculating the dynamics of CDW fluctuations in a nonperturbative model, we further show that the strength of the light-induced order is governed by the amplitude of equilibrium fluctuations. These findings highlight photoinduced fluctuations as an important ingredient for the emergence of transient orders out of equilibrium. Our results further suggest that materials with strong fluctuations in equilibrium are promising platforms to host "hidden" orders after laser excitation.

The emergence of magnetism in quantum materials creates a platform to realize spin-based applications in spintronics, magnetic memory, and quantum information science. A key to unlocking new functionalities in these materials is the discovery of tunable coupling between spins and other microscopic degrees of freedom. We present evidence for interlayer magnetophononic coupling in the layered magnetic topological insulator MnBi2Te4. Employing magneto-Raman spectroscopy, we observe anomalies in phonon scattering intensities across magnetic field-driven phase transitions, despite the absence of discernible static structural changes. This behavior is a consequence of a magnetophononic wave-mixing process that allows for the excitation of zone-boundary phonons that are otherwise ‘forbidden’ by momentum conservation. Our microscopic model based on density functional theory calculations reveals that this phenomenon can be attributed to phonons modulating the interlayer exchange coupling. Moreover, signatures of magnetophononic coupling are also observed in the time domain through the ultrafast excitation and detection of coherent phonons across magnetic transitions. In light of the intimate connection between magnetism and topology in MnBi2Te4, the magnetophononic coupling represents an important step towards coherent on-demand manipulation of magnetic topological phases.

The emergence of magnetism in quantum materials creates a platform to realize spin-based applications in spintronics, magnetic memory, and quantum information science. A key to unlocking new functionalities in these materials is the discovery of tunable coupling between spins and other microscopic degrees of freedom. We present evidence for interlayer magnetophononic coupling in the layered magnetic topological insulator MnBi

Nonradiative processes limit optoelectronic functionality of nanocrystals and curb their device performance. Nevertheless, the dynamic structural origins of nonradiative relaxations in such materials are not understood. Here, femtosecond electron diffraction measurements corroborated by atomistic simulations uncover transient lattice deformations accompanying radiationless electronic processes in colloidal semiconductor nanocrystals. Investigation of the excitation energy dependence in a core/shell system shows that hot carriers created by a photon energy considerably larger than the bandgap induce structural distortions at nanocrystal surfaces on few picosecond timescales associated with the localization of trapped holes. On the other hand, carriers created by a photon energy close to the bandgap of the core in the same system result in transient lattice heating that occurs on a much longer 200 picosecond timescale, dominated by an Auger heating mechanism. Elucidation of the structural deformations associated with the surface trapping of hot holes provides atomic-scale insights into the mechanisms deteriorating optoelectronic performance and a pathway towards minimizing these losses in nanocrystal devices., Nature Communications, 12 (1), ISSN:2041-1723

Due to the absence of matching carbon atoms at honeycomb centers with carbon atoms in adjacent graphene sheets, theorists predicted that a sliding process is needed to form AA, $A{B}^{\ensuremath{'}}$, or ABC stacking when directly converting graphite into $s{p}^{3}$ bonded diamond. Here, using twisted bilayer graphene, which naturally provides AA and $A{B}^{\ensuremath{'}}$ stacking configurations, we report the ultrafast formation of a transient two-dimensional diamondlike structure (which is not observed in aligned graphene) under femtosecond laser irradiation. This photoinduced phase transition is evidenced by the appearance of bond lengths of 1.94 and 3.14 \AA{} in the time-dependent differential pair distribution function using MeV ultrafast electron diffraction. Molecular dynamics and first-principles calculation indicate that $s{p}^{3}$ bonds nucleate at AA and $A{B}^{\ensuremath{'}}$ stacked areas in a moir\'e pattern. This work sheds light on the direct graphite-to-diamond transformation mechanism, which has not been fully understood for more than 60 years.

We explore the ultrafast generation of spin currents in magnetic multilayer samples by applying fs laser pulses to one layer and measuring the magnetic response in the other layer by element-resolved x-ray spectroscopy. In Ni(5~nm)/Ru(2~nm)/Fe(4~nm), the Ni and Fe magnetization directions couple antiferromagnetically due to the RKKY interaction, but may be oriented parallel through an applied magnetic field. After exciting the top Ni layer with a fs laser pulse, we find that also the Fe layer underneath demagnetizes, with a $4.1 \pm 1.9$\% amplitude difference between parallel and antiparallel orientation of the Ni and Fe magnetizations. We attribute this difference to the influence of a spin current generated by the fs laser pulse that transfers angular momentum from the Ni into the Fe layer. Our results confirm that superdiffusive spin transport plays a role in determining the sub-ps demagnetization dynamics of synthetic antiferromagnetic layers, but also evidence large depolarization effects due to hot electron dynamics, which are independent of the relative alignment of the magnetization in Ni and Fe., Comment: This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing

Metal nanocrystals exhibit important optoelectronic and photocatalytic functionalities in response to light. These dynamic energy conversion processes have been commonly studied by transient optical probes to date, but an understanding of the atomistic response following photoexcitation has remained elusive. Here, we use femtosecond resolution electron diffraction to investigate transient lattice responses in optically excited colloidal gold nanocrystals, revealing the effects of nanocrystal size and surface ligands on the electron-phonon coupling and thermal relaxation dynamics. First, we uncover a strong size effect on the electron-phonon coupling, which arises from reduced dielectric screening at the nanocrystal surfaces and prevails independent of the optical excitation mechanism (i.e., inter- and intraband). Second, we find that surface ligands act as a tuning parameter for hot carrier cooling. Particularly, gold nanocrystals with thiol-based ligands show significantly slower carrier cooling as compared to amine-based ligands under intraband optical excitation due to electronic coupling at the nanocrystal/ligand interfaces. Finally, we spatiotemporally resolve thermal transport and heat dissipation in photoexcited nanocrystal films by combining electron diffraction with stroboscopic elastic scattering microscopy. Taken together, we resolve the distinct thermal relaxation time scales ranging from 1 ps to 100 ns associated with the multiple interfaces through which heat flows at the nanoscale. Our findings provide insights into optimization of gold nanocrystals and their thin films for photocatalysis and thermoelectric applications.

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.

Electrons and holes in quantum materials often self-organize into ordered electronic phases, such as charge or spin density waves. These states are widely regarded as competing with superconductivity, and achieving their control could lead to higher superconducting transition temperatures. By using ultrafast optical and soft x-ray pulses, here, the authors observe a novel sliding state of the charge density wave in the cuprate superconductor La${}_{1.875}$Ba${}_{0.125}$CuO${}_{4}$, in which the condensate translates with respect to the lattice due to the ultrafast pump field.

© 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.

Phase transitions driven by ultrashort laser pulses have attracted interest both for understanding the fundamental physics of phase transitions and for potential new data storage or device applications. In many cases these transitions involve transient states that are different from those seen in equilibrium. To understand the microscopic properties of these states, it is useful to develop elementally selective probing techniques that operate in the time domain. Here we show fs-time-resolved measurements of V Ledge Resonant Inelastic X-Ray Scattering (RIXS) from the insulating phase of the Mott- Hubbard material V2O3 after ultrafast laser excitation. The probed orbital excitations within the d-shell of the V ion show a sub-ps time response, which evolve at later times to a state that appears electronically indistinguishable from the high-temperature metallic state. Our results demonstrate the potential for RIXS spectroscopy to study the ultrafast orbital dynamics in strongly correlated materials., 12 pages, 4 figures

Charge order is universal among high-Tc cuprates, but its relation to superconductivity is unclear. While static order competes with superconductivity, dynamic order may be favorable and even contribute to Cooper pairing. Using time-resolved resonant soft x-ray scattering at a free-electron laser, we show that the charge order in prototypical La2−xBaxCuO4 exhibits transverse fluctuations at picosecond time scales. These sub–millielectron volt excitations propagate by Brownian-like diffusion and have an energy scale remarkably close to the superconducting Tc. At sub–millielectron volt energy scales, the dynamics are governed by universal scaling laws defined by the propagation of topological defects. Our results show that charge order in La2−xBaxCuO4 exhibits dynamics favorable to the in-plane superconducting tunneling and establish time-resolved x-rays as a means to study excitations at energy scales inaccessible to conventional scattering techniques.

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.

For the LCLS-II X-ray instruments, we have developed laser power meters as compact X-ray power monitors. A calibration of the responsivity of the power meters was carried out against a silicon photodiode with synchrotron radiation and a gas monitor detector with FEL X-rays. A manipulator with two power meters was installed in various locations at the LCLS. In the LCLS front end, the power meters were compared with the gas detectors, which are calibrated by the electron energy loss method. The agreement between the power meters and the gas detectors was better than 20% at 1500 eV with the pulse energy measured by the gas detectors higher than that from the power meters. In the AMO instrument, the power meters evaluated the improvement in beamline transmission caused by the oxygen plasma cleaning of the Kirkpatrick-Baez mirrors. Measurements were also conducted one and two years later to observe the effect of further contamination of the optical surfaces. Finally at the SXR instrument, the power meters determined the pulse energy at the sample for a beamtime, where the X-ray intensity was an important parameter.

Photons, electrons, and their interplay are at the heart of photonic devices and modern instruments for ultrafast science [1-10]. Nowadays, electron beams of the highest intensity and brightness are created by photoemission with short laser pulses, and then accelerated and manipulated using GHz radiofrequency electromagnetic fields. The electron beams are utilized to directly map photoinduced dynamics with ultrafast electron scattering techniques, or further engaged for coherent radiation production at up to hard X-ray wavelengths [11-13]. The push towards improved timing precision between the electron beams and pump optical pulses though, has been stalled at the few tens of femtosecond level, due to technical challenges with synchronizing the high power rf fields with optical sources. Here, we demonstrate attosecond electron metrology using laser-generated single-cycle THz radiation, which is intrinsically phase locked to the optical drive pulses, to manipulate multi-MeV relativistic electron beams. Control and single-shot characterization of bright electron beams at this unprecedented level open up many new opportunities for atomic visualization.

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.

The journal of chemical physics 149(23), 234707 (2018). doi:10.1063/1.5044579, We report on atom-specific activation of CO oxidation on Ru(0001) via resonant X-ray excitation. We show that resonant 1s core-level excitation of atomically adsorbed oxygen in the co-adsorbed phase of CO and oxygen directly drives CO oxidation. We separate this direct resonant channel from indirectly driven oxidation via X-ray induced substrate heating. Based on density functional theory calculations, we identify the valence-excited state created by the Auger decay as the driving electronic state for direct CO oxidation. We utilized the fresh-slice multi-pulse mode at the Linac Coherent Light Source that provided time-overlapped and 30 fs delayed pairs of soft X-ray pulses and discuss the prospects of femtosecond X-ray pump X-ray spectroscopy probe, as well as X-ray two-pulse correlation measurements for fundamental investigations of chemical reactions via selective X-ray excitation., Published by American Institute of Physics, Melville, NY

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.

We design and realize an arrival time diagnostic for ultrashort X-ray pulses achieving unprecedented high sensitivity in the soft X-ray regime via cross-correlation with a ≈1550 nm optical laser. An interferometric detection scheme is combined with a multi-layer sample design to greatly improve the sensitivity of the measurement. We achieve up to 275% of relative signal change when exposed to 1.6 mJ/cm2 of soft X-rays at 530 eV, more than a hundred-fold improvement in sensitivity as compared to previously reported techniques. The resolution of the arrival time measurement is estimated to around 2.8 fs (rms). The demonstrated X-ray arrival time monitor paves the way for sub-10 fs-level timing jitter at high repetition rate X-ray facilities.

Magnetic skyrmions are topologically protected spin textures with promising prospects for applications in data storage. They can form a lattice state due to competing magnetic interactions and are commonly found in a small region of the temperature—magnetic field phase diagram. Recent work has demonstrated that these magnetic quasi-particles fluctuate at the μeV energy scale. Here, we use a coherent x-ray correlation method at an x-ray free-electron laser to investigate these fluctuations in a magnetic phase coexistence region near a first-order transition boundary where fluctuations are not expected to play a major role. Surprisingly, we find that the relaxation of the intermediate scattering function at this transition differs significantly compared to that deep in the skyrmion lattice phase. The observation of a compressed exponential behavior suggests solid-like dynamics, often associated with jamming. We assign this behavior to disorder and the phase coexistence observed in a narrow field-window near the transition, which can cause fluctuations that lead to glassy behavior.

A fluorescence intensity monitor has been developed for the non-invasive, pulse-by-pulse normalization of LCLS-II experiments. The linearity, noise and position sensitivity of the detectors have been characterized., For LCLS-II, a fluorescence intensity monitor for the non-invasive, pulse-by-pulse normalization of experiments has been developed. A prototype diagnostic was constructed with a microchannel plate assembly and two photodiodes. The diagnostic was then installed in the LCLS SXR instrument Kirkpatrick–Baez mirror chamber with the detectors located above the vertically reflecting mirror. The linearity, noise and position sensitivity of the detectors have been characterized. The photodiode responsivity is suitable for high pulse energies. The microchannel plate detector shows sufficient responsivity over a wide range of pulse energies. The relative signal from the two photodiodes provides a sensitive measure of the X-ray beam position. The fluorescence intensity monitor provides intensity normalization while being compatible with high incident power, a 0.93 MHz repetition rate and ultra-high vacuum.

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.

Topological quantum materials exhibit fascinating properties1–3, with important applications for dissipationless electronics and fault-tolerant quantum computers4,5. Manipulating the topological invariants in these materials would allow the development of topological switching applications analogous to switching of transistors6. Lattice strain provides the most natural means of tuning these topological invariants because it directly modifies the electron–ion interactions and potentially alters the underlying crystalline symmetry on which the topological properties depend7–9. However, conventional means of applying strain through heteroepitaxial lattice mismatch10 and dislocations11 are not extendable to controllable time-varying protocols, which are required in transistors. Integration into a functional device requires the ability to go beyond the robust, topologically protected properties of materials and to manipulate the topology at high speeds. Here we use crystallographic measurements by relativistic electron diffraction to demonstrate that terahertz light pulses can be used to induce terahertz-frequency interlayer shear strain with large strain amplitude in the Weyl semimetal WTe2, leading to a topologically distinct metastable phase. Separate nonlinear optical measurements indicate that this transition is associated with a symmetry change to a centrosymmetric, topologically trivial phase. We further show that such shear strain provides an ultrafast, energy-efficient way of inducing robust, well separated Weyl points or of annihilating all Weyl points of opposite chirality. This work demonstrates possibilities for ultrafast manipulation of the topological properties of solids and for the development of a topological switch operating at terahertz frequencies. Terahertz light pulses induce transitions between a topological and a trivial phase in the Weyl semimetal WTe2 through an interlayer shear strain.

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

We demonstrate a terahertz pump-ultrafast electron diffraction probe apparatus. Using the instrument, we show that intense focused THz pulses can characterize ultrashort electron bunches.

“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.

Golden ultrafast melting Understanding fast melting of metals is important for applications such as welding and micromachining. However, fast melting leaves simulation as the only option for probing the process. Mo et al. performed ultrafast electron diffraction experiments on laser-pulsed gold films. This allowed detailed mapping of the melting process, which proceeds through two distinct regimes while the bonding behavior changes in unexpected ways. The results require adding new physical processes to high-energy melting models. Science , this issue p. 1451

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 report an x-ray photon correlation spectroscopy method that exploits the recent development of the two-pulse mode at the Linac Coherent Light Source. By using coherent resonant x-ray magnetic scattering, we studied spontaneous fluctuations on nanosecond time scales in thin films of multilayered Fe/Gd that exhibit ordered stripe and Skyrmion lattice phases. The correlation time of the fluctuations was found to differ between the Skyrmion phase and near the stripe-Skyrmion boundary. This technique will enable a significant new area of research on the study of equilibrium fluctuations in condensed matter.

To understand and control the basic functions of physical, chemical and biological processes from micron to nano-meter scale, an instrument capable of visualizing transient structural changes of inhomogeneous materials with atomic spatial and temporal resolutions, is required. One such technique is femtosecond electron microdiffraction, in which a short electron pulse with femtosecond-scale duration is focused into a micron-scale spot and used to obtain diffraction images to resolve ultrafast structural dynamics over a localized crystalline domain. In this letter, we report the experimental demonstration of time-resolved mega-electron-volt electron microdiffraction which achieves a 5 μm root-mean-square (rms) beam size on the sample and a 110 fs rms temporal resolution. Using pulses of 10k electrons at 4.2 MeV energy with a normalized emittance 3 nm-rad, we obtained high quality diffraction from a single 10 μm paraffin ( C 44 H 90 ) crystal. The phonon softening mode in optical-pumped polycrystalline Bi was also time-resolved, demonstrating the temporal resolution limits of the instrument. This new characterization capability will open many research opportunities in material and biological sciences.

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

Magnetic nanoparticles are increasingly used in nanotechnologies and biomedical applications, such as drug targeting, MRI, bio-separation. Magnetite (Fe3O4) nanoparticles stand to be effective in these roles due to the non-toxic nature of magnetite and its ease of manufacture. To be more effective in these applications, a greater understanding of the magnetic behavior of a collection of magnetite nanoparticles is needed. This research seeks to discover the local magnetic ordering of ensembles of magnetite nanoparticles occurring under various external fields. To complete this study, we use x-ray resonant magnetic scattering (XRMS). Here we discuss the modeling of the magnetic scattering data using a one-dimensional chain of nanoparticles with a mix of ferromagnetic, anti-ferromagnetic, and random orders. By fitting the model to the experimental data, we extracted information about the magnetic correlations in the nanoparticle assembly.

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.

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.