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We demonstrate for the case of photoexcited [Ru 2,2 amp; 8242; bipyridine 3]2 how femtosecond resonant inelastic X ray scattering RIXS at the ligand K edge allows one to uniquely probe changes in the valence electronic structure following a metal to ligand charge transfer MLCT excitation. Metal ligand hybridization is probed by nitrogen 1s resonances providing information on both the electron accepting ligand in the MLCT state and the hole density of the metal center. By comparing to spectrum calculations based on density functional theory, we are able to distinguish the electronic structure of the electron accepting ligand and the other ligands and determine a temporal upper limit of 250 40 fs for electron localization following the charge transfer excitation. The spin of the localized electron is deduced from the selection rules of the RIXS process establishing new experimental capabilities for probing transient charge and spin densities

In the mixed-valence manganites, a near-infrared laser typically melts the orbital and spin order simultaneously, corresponding to the photoinduced d1d0→d0d1 excitations in the Mott-Hubbard bands of manganese. Here, we use ultrafast methods-both femtosecond resonant X-ray diffraction and optical reflectivity-to demonstrate that the orbital response in the layered manganite Nd1-xSr1+xMnO4(x=2/3) does not follow this scheme. At the photoexcitation saturation fluence, the orbital order is only diminished by a few percent in the transient state. Instead of the typical d1d0→d0d1 transition, a near-infrared pump in this compound promotes a fundamentally distinct mechanism of charge transfer, the d0→d1L, where L denotes a hole in the oxygen band. This finding may pave a different avenue for selectively manipulating specific types of order in complex materials of this class.

Author(s): Hemsing, E; Marcus, G; Fawley, WM; Schoenlein, RW; Coffee, R; Dakovski, G; Hastings, J; Huang, Z; Ratner, D; Raubenheimer, T; Penn, G | Abstract: We present the results from studies of soft X-ray seeding options for the LCLS-II X-ray free electron laser (FEL) at SLAC. The LCLS-II will use superconducting accelerator technology to produce X-ray pulses at up to 1 MHz repetition rate using 4 GeV electron beams. If properly seeded, these pulses will be nearly fully coherent, and highly stable in photon energy, bandwidth, and intensity, thus enabling unique experiments with intense high-resolution soft X-rays. Given the expected electron beam parameters from start to end simulations and predicted FEL performance, our studies reveal echo enabled harmonic generation (EEHG) and soft X-ray self-seeding (SXRSS) as promising and complementary seeding methods. We find that SXRSS has the advantage of simplicity and will deliver 5-35 times higher spectral brightness than EEHG in the 1-2 nm range, but lacks some of the potential for phase-stable multipulse and multicolor FEL operations enabled by external laser seeding with EEHG.

Laser power meters are being developed as a compact X-ray power diagnostic for LCLS-II and are characterized for their responsivity, linearity and vacuum compatibility. The power meters are calibrated against X-ray photodiodes and a gas monitor detector., For the LCLS-II X-ray instruments, laser power meters are being developed as compact X-ray power diagnostics to operate at soft and tender X-ray photon energies. These diagnostics can be installed at various locations along an X-ray free-electron laser (FEL) beamline in order to monitor the transmission of X-ray optics along the beam path. In addition, the power meters will be used to determine the absolute X-ray power at the endstations. Here, thermopile power meters, which measure average power, and have been chosen primarily for their compatibility with the high repetition rates at LCLS-II, are evaluated. A number of characteristics in the soft X-ray range are presented including linearity, calibrations conducted with a photodiode and a gas monitor detector as well as ultra-high-vacuum compatibility tests using residual gas analysis. The application of these power meters for LCLS-II and other X-ray FEL sources is discussed.

Silicon drift detectors (SDDs) revolutionized spectroscopy in fields as diverse as geology and dentistry. For a subset of experiments at ultra-fast, x-ray free-electron lasers (FELs), SDDs can make substantial contributions. Often the unknown spectrum is interesting, carrying science data, or the background measurement is useful to identify unexpected signals. Many measurements involve only several discrete photon energies known a priori, allowing single event decomposition of pile-up and spectroscopic photon counting. We designed a pulse function and demonstrated that the signal amplitude and rise time are obtained for each pulse by fitting, thus removing the need for pulse shaping. By avoiding pulse shaping, rise times of tens of nanoseconds resulted in reduced pulse pile-up and allowed decomposition of remaining pulse pile-up at photon separation times down to hundreds of nanoseconds while yielding time-of-arrival information with precision of 10 nanoseconds. Waveform fitting yields simultaneously high energy resolution and high counting rates (2 orders of magnitude higher than current digital pulse processors). We showed that pile-up spectrum fitting is relatively simple and preferable to pile-up spectrum deconvolution. We developed a photon pile-up statistical model for constant intensity sources, extended it to variable intensity sources (typical for FELs) and used it to fit a complex pile-up spectrum. We subsequently developed a Bayesian pile-up decomposition method that allows decomposing pile-up of single events with up to 6 photons from 6 monochromatic lines with 99% accuracy. The usefulness of SDDs will continue into the x-ray FEL era of science. Their successors, the ePixS hybrid pixel detectors, already offer hundreds of pixels, each with similar performance to an SDD, in a compact, robust and affordable package, 16 pages, 11 figures, 4 tables

© 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

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).

The Linac Coherent Light Source (LCLS) of SLAC is upgrading the facility to a more flexible design, permitting both, high energy per pulse mode and High Repetition Rate mode. Two independent “sources” Soft and Hard X-ray will serve five of the existing beamlines and three completely new ones. We will present here, one of the new beamlines, mainly dedicated to Resonant Inelastic Scattering (RIXS) and Liquid Jet based experiments. The beamline is designed to deliver the beam to the floor upstairs of the existing experimental area by using a large deflection, grating based monochromator. The monochromator is designed to provide both, very high resolving power (E/ΔE

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.

The journal of physical chemistry letters 9(12), 3538 - 3543 (2018). doi:10.1021/acs.jpclett.8b01429, Soft X-ray spectroscopies are ideal probes of the local valence electronic structure of photocatalytically active metal sites. Here, we apply the selectivity of time-resolved resonant inelastic X-ray scattering at the iron L-edge to the transient charge distribution of an optically excited charge-transfer state in aqueous ferricyanide. Through comparison to steady-state spectra and quantum chemical calculations, the coupled effects of valence-shell closing and ligand-hole creation are experimentally and theoretically disentangled and described in terms of orbital occupancy, metal–ligand covalency, and ligand field splitting, thereby extending established steady-state concepts to the excited-state domain. π-Back-donation is found to be mainly determined by the metal site occupation, whereas the ligand hole instead influences σ-donation. Our results demonstrate how ultrafast resonant inelastic X-ray scattering can help characterize local charge distributions around catalytic metal centers in short-lived charge-transfer excited states, as a step toward future rationalization and tailoring of photocatalytic capabilities of transition-metal complexes., Published by ACS, Washington, DC

A gas monitor detector was implemented and characterized at the Soft X-ray Research instrument (SXR) to measure the average, absolute and pulse-resolved photon flux of the LCLS beam in the energy range between 280 and 2000 eV., A gas monitor detector was implemented and characterized at the Soft X-ray Research (SXR) instrument to measure the average, absolute and pulse-resolved photon flux of the LCLS beam in the energy range between 280 and 2000 eV. The detector is placed after the monochromator and addresses the need to provide reliable absolute pulse energy as well as pulse-resolved measurements for the various experiments at this instrument. This detector provides a reliable non-invasive measurement for determining flux levels on the samples in the downstream experimental chamber and for optimizing signal levels of secondary detectors and for the essential need of data normalization. The design, integration into the instrument and operation are described, and examples of its performance are given.

A description of the Soft X-ray Research instrument (SXR) at the Linac Coherent Light Source is given. Recent scientific highlights illustrate the wide variety of experiments and detectors that can be accommodated at SXR., The Soft X-ray Research instrument provides intense ultrashort X-ray pulses in the energy range 280–2000 eV. A diverse set of experimental stations may be installed to investigate a broad range of scientific topics such as ultrafast chemistry, highly correlated materials, magnetism, surface science, and matter under extreme conditions. A brief description of the main instrument components will be given, followed by some selected scientific highlights.

Catching CO oxidation Details of the transition state that forms as carbon monoxide (CO) adsorbed on a ruthenium surface is oxidized to CO 2 have been revealed by ultrafast excitation and probe methods. Öström et al. initiated the reaction between CO and adsorbed oxygen atoms with laser pulses that rapidly heated the surface and then probed the changes in electronic structure with oxygen x-ray absorption spectroscopy. They observed transition-state configurations that are consistent with density functional theory and a quantum oscillator model. Science , this issue p. 978

Ultrafast x-ray scattering studies of the topological Skyrmion phase in Cu_{2}OSeO_{3} show the dynamics to be strongly dependent on the excitation energy and fluence. At high photon energies, where the electron-spin scattering cross section is relatively high, the excitation of the topological Skyrmion phase shows a nonlinear dependence on the excitation fluence, in contrast to the excitation of the conical phase which is linearly dependent on the excitation fluence. The excitation of the Skyrmion order parameter is nonlinear in the magnetic excitation resulting from scattering during electron-hole recombination, indicating different dominant scattering processes in the conical and Skyrmion phases.

The recent advent of X-ray free-electron lasers (XFELs) marks the beginning of a new era in X-ray science, providing coherent ultrafast X-ray pulses with unprecedented peak brightness. The first generation of these facilities (FLASH, LCLS, and SACLA) have already had tremendous scientific impact, and numerous similar facilities are now being developed around the world. These first-generation XFELs are based on pulsed-radio frequency (RF) accelerator technology with limited repetition rates. Thus, they provide only modest average brightness, comparable to or lower than that available from existing storage rings, and this limits their impact in key areas of science. A new generation of XFELs is now under development, exploiting continuous-wave RF superconducting accelerator technology (CW-SCRF) to provide ultrafast X-ray pulses up to MHz repetition rates in a uniform or programmable time structure. This chapter highlights some compelling new science opportunities that will be enabled by such high-repetition-rate XFELs. These opportunities have been identified and developed through numerous workshops over the past decade. In February 2015, a series of workshops were held at SLAC focusing on the new science opportunities that will be enabled by LCLS-II, which will provide ultrafast X-rays in the 0.25–5 keV range at repetition rates up to 1 MHz.

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.

A method for measuring resonant inelastic X-ray scattering based on the conversion of X-ray photons into photoelectrons is presented. The setup is compact, relies on commercially available detectors, and offers significant flexibility. This method is demonstrated at the Linac Coherent Light Source with ∼0.5 eV resolution at the cobaltL3-edge, with signal rates comparable with traditional grating spectrometers.

We investigate the lattice coupling to the spin and charge orders in the striped nickelate, ${\mathrm{La}}_{1.75}{\mathrm{Sr}}_{0.25}{\mathrm{NiO}}_{4}$, using time-resolved resonant x-ray scattering. Lattice-driven dynamics of both spin and charge orders are observed when the pump photon energy is tuned to that of an ${E}_{u}$ bond- stretching phonon. We present a likely scenario for the behavior of the spin and charge order parameters and its implications using a Ginzburg-Landau theory.

Resonant optical excitation of apical oxygen vibrational modes in the normal state of underdoped YBa2Cu3O6+x induces a transient state with optical properties similar to those of the equilibrium superconducting state. Amongst these, a divergent imaginary conductivity and a plasma edge are transiently observed in the photo-stimulated state. Femtosecond hard x-ray diffraction experiments have been used in the past to identify the transient crystal structure in this non-equilibrium state. Here, we start from these crystallographic features and theoretically predict the corresponding electronic rearrangements that accompany these structural deformations. Using density functional theory, we predict enhanced hole-doping of the CuO2 planes. The empty chain Cu dy2-z2 orbital is calculated to strongly reduce in energy, which would increase c-axis transport and potentially enhance the interlayer Josephson coupling as observed in the THz-frequency response. From these calculations, we predict changes in the soft x-ray absorption spectra at the Cu L-edge. Femtosecond x-ray pulses from a free electron laser are used to probe these changes in absorption at two photon energies along this spectrum, and provide data consistent with these predictions., Comment: 20 pages with 6 figures

We measured the fluorescence photon yield of neon upon soft x-ray ionization (~1200 eV) from the x-ray free electron laser at Linac Coherent Light Source, and demonstrated the usage of a grazing incidence spectrometer with a variable linespacing grating to perform x-ray fluorescence spectroscopy on a gas phase system. Our measurements also allowed us to estimate the focal size of the beam from the theoretical description developed, in terms of the rate equation approximation accounting for photoionization shake-off of neutral neon and double Auger decay of single core holes., Comment: 9 pages, 6 figures, 1 table

X-ray absorption spectroscopy at the L-edge of 3d transition metals provides unique information on the local metal charge and spin states by directly probing 3d-derived molecular orbitals through 2p-3d transitions. However, this soft x-ray technique has been rarely used at synchrotron facilities for mechanistic studies of metalloenzymes due to the difficulties of x-ray-induced sample damage and strong background signals from light elements that can dominate the low metal signal. Here, we combine femtosecond soft x-ray pulses from a free-electron laser with a novel x-ray fluorescence-yield spectrometer to overcome these difficulties. We present L-edge absorption spectra of inorganic high-valent Mn complexes (Mn ∼ 6–15 mmol/l) with no visible effects of radiation damage. We also present the first L-edge absorption spectra of the oxygen evolving complex (Mn4CaO5) in Photosystem II (Mn

Silicon drift detectors (SDDs) are a well-established technology that has revolutionized spectroscopy in fields as diverse as geology and dentistry. At a first glance it would seem that detectors with such a slow response would not be suitable for the new ultra-fast x-ray free-electron lasers (FEL) coming online. However, for a subset of experiments at FELs, SDDs can make substantial contributions. Many measurements involve only several distinct photon energies known a priori, allowing pile-up deconvolution and accurate spectroscopic photon counting. Often the unknown spectrum is interesting, carrying science data, or the background measurement is useful to identify unexpected signals. We investigated the performance of SDDs at x-ray FELs, in particular the ability to deconvolve the spectrum that results from various combinations of a few wavelengths and the possibility of separately recording photons that are absorbed at different radii (thus having varying drift times). The analytic approach presented here permits isolating individual photon energies and interaction radii from pile-up events of 0 to 5 photons sampled from 6 monochromatic lines in a single SDD with accurate pile-up deconvolution, timing extraction and clipping correction. The usefulness of SDDs will continue into the x-ray FEL era of science. Their successors, the ePixS hybrid pixel detectors, already offer hundreds of pixels with similar performance in a compact, robust and affordable package.

A deeper look into iron selenide In the past 10 years, iron-based superconductors have created more puzzles than they have helped resolve. Some of the most fundamental outstanding questions are how strong the interactions are and what the electron pairing mechanism is. Now two groups have made contributions toward resolving these questions in the intriguing compound iron selenide (FeSe) (see the Perspective by Lee). Gerber et al. used photoemission spectroscopy coupled with x-ray diffraction to find that FeSe has a very sizable electron-phonon interaction. Quasiparticle interference imaging helped Sprau et al. determine the shape of the superconducting gap and find that the electron pairing in FeSe is orbital-selective. Science , this issue p. 71 , p. 75 ; see also p. 32

The journal of physical chemistry letters 7(18), 3647 - 3651(2016). doi:10.1021/acs.jpclett.6b01543, The concept of bonding and antibonding orbitals is fundamental in chemistry. The population of those orbitals and the energetic difference between the two reflect the strength of the bonding interaction. Weakening the bond is expected to reduce this energetic splitting, but the transient character of bond-activation has so far prohibited direct experimental access. Here we apply time-resolved soft X-ray spectroscopy at a free-electron laser to directly observe the decreased bonding–antibonding splitting following bond-activation using an ultrashort optical laser pulse., Published by ACS, Washington, DC

We report a time-resolved study of the ultrafast dynamics of the magnetic moments formed by the [Formula: see text] states in Sr2IrO4 by directly probing the localized iridium 5d magnetic state through resonant x-ray diffraction. Using optical pump-hard x-ray probe measurements, two relaxation time scales were determined: a fast fluence-independent relaxation is found to take place on a time scale of 1.5 ps, followed by a slower relaxation on a time scale of 500 ps-1.5 ns.

We use intense broadband THz pulses to excite the cuprate superconductors YBCO and NBCO in their underdoped phase, where superconducting and charge density wave ground states compete. We observe pronounced coherent oscillations at attributed to renormalized low-energy phonon modes. These oscillation features are much more prominent than those observed in all-optical pump-probe measurements, suggesting a different excitation mechanism.

Scientific Reports 6: Article number: 18970; published online: 06 January 2016; updated: 04 March 2016 The original version of this Article contained a typographical error in the spelling of the author Bharati Tudu, which was incorrectly given as Bahrati Tudu. This has now been corrected in the PDF and HTML versions of the Article.

International audience; Does the excitation of ultrafast magnetization require direct interaction between the photons of the optical pump pulse and the magnetic layer? Here, we demonstrate unambiguously that this is not the case. For this we have studied the magnetization dynamics of a ferromagnetic cobalt/palladium multilayer capped by an IR-opaque aluminum layer. Upon excitation with an intense femtosecond-short IR laser pulse, the film exhibits the classical ultrafast demagnetization phenomenon although only a negligible number of IR photons penetrate the aluminum layer. In comparison with an uncapped cobalt/ palladium reference film, the initial demagnetization of the capped film occurs with a delayed onset and at a slower rate. Both observations are qualitatively in line with energy transport from the aluminum layer into the underlying magnetic film by the excited, hot electrons of the aluminum film. Our data thus confirm recent theoretical predictions. Ultrafast demagnetization is a very intriguing phenomenon. The existence and origin of this rapid loss of a thin film's magnetization on the femtosecond timescale has been controversially debated ever since its discovery in 1996 1. Recently, it has been proposed that the origin of this magnetization loss could be due to spin-dependent motion of the optically excited hot valence electrons causing a spatial redistribution of the magnetization, either to an adjacent metallic layer 2,3 or within the magnetic layer itself 4. Strong experimental evidence for this so-called superdiffusive spin transport has been found lately 5-8. However, the experiment of Eschenlohr and co-workers 8 , similar to our study reported here, has been challenged recently. Khorsand and co-workers 9 showed that the Au cap layer employed in that experiment does not yield the postulated, and for the interpretation of the data crucial, attenuation of the incident IR pump pulse. Implementing a truly IR-opaque capping layer, we evade the limitation affecting the interpretation of the results of Eschenlohr and co-workers 8. Proper characterization of the number of photons reaching the magnetic layer demonstrates that the transmitted intensity is by orders of magnitude too small to excite the ultrafast demagnet-ization process.

X-ray free electron lasers (XFELs) enable unprecedented new ways to study the electronic structure and dynamics of transition metal systems. L-edge absorption spectroscopy is a powerful technique for such studies and the feasibility of this method at XFELs for solutions and solids has been demonstrated. However, the required x-ray bandwidth is an order of magnitude narrower than that of self-amplified spontaneous emission (SASE), and additional monochromatization is needed. Here we compare L-edge x-ray absorption spectroscopy (XAS) of a prototypical transition metal system based on monochromatizing the SASE radiation of the linac coherent light source (LCLS) with a new technique based on self-seeding of LCLS. We demonstrate how L-edge XAS can be performed using the self-seeding scheme without the need of an additional beam line monochromator. We show how the spectral shape and pulse energy depend on the undulator setup and how this affects the x-ray spectroscopy measurements. (C) 2016 Optical Society of America

Graphene, a recently discovered two-dimensional form of carbon, is a strong candidate for many future electronic devices. There is, however, still much debate over how the electronic properties of graphene behave on ultrashort time scales. Here by employing the technique of time-resolved photoemission, we obtain the evolving quantum distributions of the electrons and holes: on an ultrashort 500 fs time scale, the electron and hole populations can be described by two separate Fermi–Dirac distributions, whereas on longer time scales the populations coalesce to form a single Fermi–Dirac distribution at an elevated temperature. These studies represent the first direct measure of carrier distribution dynamics in monolayer graphene after ultrafast photoexcitation.

Terahertz time-domain spectroscopy was employed to investigate photogenerated excitons in PbSe and CdSe quantum dots (QD) of radii less than their exciton Bohr radius. The exciton response was found to be “atom”-like and rise with increasing the carrier effective mass. Excitons in CdSe were found to be about two times more polarizable than those in PbSe QDs of equal size. These experimental findings including both the magnitude of the exciton polarizability and its variation with the QD radius were well described by an effective mass model with multiband structures of the QD materials.

A hallmark in the cuprate family of high-temperature superconductors is the nodal-antinodal dichotomy. In this regard, angle-resolved photoemission spectroscopy (ARPES) has proven especially powerful, providing band structure information directly in energy-momentum space. Time-resolved ARPES (trARPES) holds great promise of adding ultrafast temporal information, in an attempt to identify different interaction channels in the time domain. Previous studies of the cuprates using trARPES were handicapped by the low probing energy, which significantly limits the accessible momentum space. Using 20.15 eV, 12 fs pulses, we show for the first time the evolution of quasiparticles in the antinodal region of Bi2Sr2CaCu2O8+δ and demonstrate that non-monotonic relaxation dynamics dominates above a certain fluence threshold. The dynamics is heavily influenced by transient modification of the electron-phonon interaction and phase space restrictions, in stark contrast to the monotonic relaxation in the nodal and off-nodal regions.

Static strain in complex oxide heterostructures has been extensively used to engineer electronic and magnetic properties at equilibrium. In the same spirit, deformations of the crystal lattice with light may be used to achieve functional control across hetero-interfaces dynamically. Here, by exciting large amplitude infrared-active vibrations in a LaAlO3 substrate we induce magnetic order melting in a NdNiO3 film across a hetero-interface. Femtosecond Resonant Soft X-ray Diffraction is used to determine the spatial and temporal evolution of the magnetic disordering. We observe a magnetic melt front that grows from the substrate interface into the film, at a speed that suggests electronically driven propagation. Light control and ultrafast phase front propagation at hetero-interfaces may lead to new opportunities in optomagnetism, for example by driving domain wall motion to transport information across suitably designed devices., Comment: 35 pages, 8 Figures (both incl. Supplement)

The structure of bulk liquid water was recently probed by x-ray scattering below the temperature limit of homogeneous nucleation (T-H) of similar to 232 K [J. A. Sellberg et al., Nature 510, 381-384 (2014)]. Here, we utilize a similar approach to study the structure of bulk liquid water below T-H using oxygen K-edge x-ray emission spectroscopy (XES). Based on previous XES experiments [T. Tokushima et al., Chem. Phys. Lett. 460, 387-400 (2008)] at higher temperatures, we expected the ratio of the 1b(1)' and 1b(1)" peaks associated with the lone-pair orbital in water to change strongly upon deep supercooling as the coordination of the hydrogen (H-) bonds becomes tetrahedral. In contrast, we observed only minor changes in the lone-pair spectral region, challenging an interpretation in terms of two interconverting species. A number of alternative hypotheses to explain the results are put forward and discussed. Although the spectra can be explained by various contributions from these hypotheses, we here emphasize the interpretation that the line shape of each component changes dramatically when approaching lower temperatures, where, in particular, the peak assigned to the proposed disordered component would become more symmetrical as vibrational interference becomes more important. (C) 2015 AIP Publishing LLC.

We use femtosecond resonant soft x-ray diffraction to measure the optically stimulated ultrafast changes of charge-density wave correlations in underdoped $\mathrm{YB}{\mathrm{a}}_{2}\mathrm{C}{\mathrm{u}}_{3}{\mathrm{O}}_{6.6}$. We find that when coherent interlayer transport is enhanced by optical excitation of the apical oxygen distortions, at least 50% of the in-plane charge-density wave order is melted. These results indicate that charge ordering and superconductivity may be competing up to the charge ordering transition temperature, with the latter becoming a hidden phase that is accessible only by nonlinear phonon excitation.

We show that coadsorbed oxygen atoms have a dramatic influence on the CO desorption dynamics from Ru(0001). In contrast to the precursor-mediated desorption mechanism on Ru(0001), the presence of surface oxygen modifies the electronic structure of Ru atoms such that CO desorption occurs predominantly via the direct pathway. This phenomenon is directly observed in an ultrafast pump-probe experiment using a soft x-ray free-electron laser to monitor the dynamic evolution of the valence electronic structure of the surface species. This is supported with the potential of mean force along the CO desorption path obtained from density-functional theory calculations. Charge density distribution and frozen-orbital analysis suggest that the oxygen-induced reduction of the Pauli repulsion, and consequent increase of the dative interaction between the CO 5 sigma and the charged Ru atom, is the electronic origin of the distinct desorption dynamics. Ab initio molecular dynamics simulations of CO desorption from Ru(0001) and oxygen-coadsorbed Ru(0001) provide further insights into the surface bond-breaking process., US Department of Energy, Basic Energy Science; Swedish Research Council (VR); Department of Energy, Laboratory Directed Research and Development; VolkswagenStiftung; LCLS, Stanford University; Lawrence Berkeley National Laboratory (LBNL); University of Hamburg; Center for Free Electron Laser Science (CFEL)

High-intensity x-ray pulses from an x-ray free-electron laser are used to heat and probe a solid-density aluminum sample. The photon-energy-dependent transmission of the heating beam is studied through the use of a photodiode. Saturable absorption is observed, with the resulting transmission differing significantly from the cold case, in good agreement with atomic-kinetics simulations.

We report on oxygen K-edge soft x-ray emission spectroscopy from a liquid water jet at the Linac Coherent Light Source. We observe significant changes in the spectral content when tuning over a wide range of incident x-ray fluences. In addition the total emission yield decreases at high fluences. These modifications result from reabsorption of x-ray emission by valence-excited molecules generated by the Auger cascade. Our observations have major implications for future x-ray emission studies at intense x-ray sources. We highlight the importance of the x-ray pulse length with respect to the core-hole lifetime.

Ultrafast Manipulation Multiferroic materials commonly show both magnetism and ferroelectricity, such that the electric field can be used to manipulate the magnetic order, and vice versa. Kubacka et al. (p. 1333 , published online 6 March) used a strong terahertz electromagnetic pulse in resonance with an electromagnon—an excitation based on both electric and magnetic ordering—to control the spin dynamics of the multiferroic TbMnO 3 on a sub-picosecond time scale and induce the rotation of the spin-cycloid plane of the material.