Time-, k-, and energy-resolved photoemission data for C 1s in H-intercalated graphene on SiC (QFMLG). Here we use a free electron laser to investigate the effect of a transiently excited hot electron gas on the core level spectrum of graphene, showing that it leads to a substantial broadening of the C 1s line shape.

The performance of time-resolved photoemission experiments at fs-pulsed photon sources is ultimately limited by the e-e Coulomb interaction, downgrading energy and momentum resolution. Here, we present an approach to effectively suppress space-charge artifacts in momentum microscopes and photoemission microscopes. A retarding electrostatic field generated by a special objective lens repels slow electrons, retaining the k-image of the fast photoelectrons. The suppression of space-charge effects scales with the ratio of the photoelectron velocities of fast and slow electrons. Fields in the range from -20 to -1100 V/mm for Ekin = 100 eV to 4 keV direct secondaries and pump-induced slow electrons back to the sample surface. Ray tracing simulations reveal that this happens within the first 40 to 3 μm above the sample surface for Ekin = 100 eV to 4 keV. An optimized front-lens design allows switching between the conventional accelerating and the new retarding mode. Time-resolved experiments at Ekin = 107 eV using fs extreme ultraviolet probe pulses from the free-electron laser FLASH reveal that the width of the Fermi edge increases by just 30 meV at an incident pump fluence of 22 mJ/cm2 (retarding field -21 V/mm). For an accelerating field of +2 kV/mm and a pump fluence of only 5 mJ/cm2, it increases by 0.5 eV (pump wavelength 1030 nm). At the given conditions, the suppression mode permits increasing the slow-electron yield by three to four orders of magnitude. The feasibility of the method at high energies is demonstrated without a pump beam at Ekin = 3830 eV using hard x rays from the storage ring PETRA III. The approach opens up a previously inaccessible regime of pump fluences for photoemission experiments.

We present the experimental end-station TRIXS dedicated to time-resolved soft x-ray resonant inelastic x-ray scattering (RIXS) experiments on solid samples at the free-electron laser FLASH. Using monochromatized ultrashort femtosecond XUV/soft x-ray photon pulses in combination with a synchronized optical laser in a pump-probe scheme, the TRIXS setup allows measuring sub-picosecond time-resolved high-resolution RIXS spectra in the energy range from 35 eV to 210 eV, thus spanning the M-edge (M1 and M2,3) absorption resonances of 3d transition metals and N4,5-edges of rare earth elements. A Kirkpatrick–Baez refocusing mirror system at the first branch of the plane grating monochromator beamline (PG1) provides a focus of (6 × 6) μm2 (FWHM) at the sample. The RIXS spectrometer reaches an energy resolution of 35–160 meV over the entire spectral range. The optical laser system based on a chirped pulse optical parametric amplifier provides approximately 100 fs (FWHM) long photon pulses at the fundamental wavelength of 800 nm and a fluence of 120 mJ/cm2 at a sample for optical pump-XUV probe measurements. Furthermore, optical frequency conversion enables experiments at 400 nm or 267 nm with a fluence of 80 and 30 mJ/cm2, respectively. Some of the first (pump-probe) RIXS spectra measured with this setup are shown. The measured time resolution for time-resolved RIXS measurements has been characterized as 287 fs (FWHM) for the used energy resolution.

Severin Meister ,1,* Aaron Bondy,2,3 Kirsten Schnorr,4 Sven Augustin,4 Hannes Lindenblatt ,1 Florian Trost ,1 Xinhua Xie,4 Markus Braune ,5 Rolf Treusch ,5 Bastian Manschwetus,5 Nora Schirmel,5 Harald Redlin,5 Nicolas Douguet,6 Thomas Pfeifer,1 Klaus Bartschat ,2 and Robert Moshammer1 1Max-Planck-Institute for Nuclear Physics, 69117 Heidelberg, Germany 2Department of Physics and Astronomy, Drake University, Des Moines, Iowa 50311, USA 3Department of Physics, University of Windsor, Windsor, Ontario N9B 3P4, Canada 4Paul Scherrer Institute, 5232 Villigen, Switzerland 5Deutsches Elektronen-Synchrotron, 22607 Hamburg, Germany 6Department of Physics, Kennesaw State University, Marietta, Georgia 30060, USA

Time-resolved photoemission with ultrafast pump and probe pulses is an emerging technique with wide application potential. Real-time recording of nonequilibrium electronic processes, transient states in chemical reactions, or the interplay of electronic and structural dynamics offers fascinating opportunities for future research. Combining valence-band and core-level spectroscopy with photoelectron diffraction for electronic, chemical, and structural analyses requires few 10 fs soft X-ray pulses with some 10 meV spectral resolution, which are currently available at high repetition rate free-electron lasers. We have constructed and optimized a versatile setup commissioned at FLASH/PG2 that combines free-electron laser capabilities together with a multidimensional recording scheme for photoemission studies. We use a full-field imaging momentum microscope with time-of-flight energy recording as the detector for mapping of 3D band structures in (kx, ky, E) parameter space with unprecedented efficiency. Our instrument can image full surface Brillouin zones with up to 7 Å-1 diameter in a binding-energy range of several eV, resolving about 2.5 × 105 data voxels simultaneously. Using the ultrafast excited state dynamics in the van der Waals semiconductor WSe2 measured at photon energies of 36.5 eV and 109.5 eV, we demonstrate an experimental energy resolution of 130 meV, a momentum resolution of 0.06 Å-1, and a system response function of 150 fs.

The evolution of individual, large gas-phase xenon clusters, turned into a nanoplasma by a high power infrared laser pulse, is tracked from femtoseconds up to nanoseconds after laser excitation via coherent diffractive imaging, using ultra-short soft x-ray free electron laser pulses. A decline of scattering signal at high detection angles with increasing time delay indicates a softening of the cluster surface. Here we demonstrate, for the first time a representative speckle pattern of a new stage of cluster expansion for xenon clusters after a nanosecond irradiation. The analysis of the measured average speckle size and the envelope of the intensity distribution reveals a mean cluster size and length scale of internal density fluctuations. The measured diffraction patterns were reproduced by scattering simulations which assumed that the cluster expands with pronounced internal density fluctuations hundreds of picoseconds after excitation.

In this paper, we report results on two-colour above-threshold ionisation, where extreme ultraviolet pulses of femtosecond duration were synchronised to intense infrared laser pulses of picosecond duration, in order to study the laser-assisted photoelectric effect of atomic helium, neon, krypton and xenon which leads to the appearance of characteristic sidebands in the photoelectron spectra. The observed trends are found to be well described by a simple model based on the soft-photon approximation, at least for the relatively low optical intensities of up to 5 x 10(11)Wcm(-2) employed in these early experiments.

Time resolved core level photoemission (trXPS) allows real-time atom-specific investigation of ultrafast surface dynamics. Core levels contain information on the chemical state and the structure of the surface as well as the local charge distribution around specific atoms. Monitoring their evolution after optically exciting the surface, can give valuable information on the electronic (few picosecond time scale) and lattice dynamics (several picosecond timescale). We have performed a trXPS experiment at the free-electron laser FLASH at DESY in Hamburg on a clean Ir(111) surface measuring the temporal evolution of the 4f core levels of Ir(111) after optically exciting the sample. The spectral changes due to X-ray and optical laser induced space charge effects which occur in trXPS experiments with high fluence pump and probe pulses have been fully characterized and controlled during the measurements. At early time scales after the optical excitation we observe time-dependent energy shifts and intensity changes which can be partially attributed to the formation of sidebands. Furthermore, we can clearly identify contributions which result from a change in the surface electron density which then relaxes on a time scale on the order of 2ps.

A key feature of extreme ultraviolet (XUV) radiation from free-electron lasers (FELs) is its spatial and temporal coherence. We measured the spatio-temporal coherence properties of monochromatized FEL pulses at 13.5 nm using a Michelson interferometer. A temporal coherence time of (59±8) fs has been determined, which is in good agreement with the spectral bandwidth given by the monochromator. Moreover, the spatial coherence in vertical direction amounts to about 15% of the beam diameter and about 12% in horizontal direction. The feasibility of measuring spatio-temporal coherence properties of XUV FEL radiation using interferometric techniques advances machine operation and experimental studies significantly.

Spin-resolved photoemission is one of the most direct ways of measuring the magnetization of a ferromagnet. If all valence band electrons contribute, the measured average spin polarization is proportional to the magnetization. This is even the case if electronic excitations are present, and thus is of particular interest for studying the response of the magnetization to a pump laser pulse. Here, we demonstrate the feasibility of ultrafast spin-resolved photoemission using free electron laser (FEL) radiation and investigate the effect of space charge on the detected spin polarization. The sample is exposed to the radiation of the FEL FLASH in Hamburg. Surprisingly, the measured spin polarization depends on the fluence of the FEL radiation: a higher FEL fluence reduces the measured spin polarization. Space-charge simulations can explain this effect. These findings have consequences for future spin-polarized photoemission experiments using pulsed photon sources.

Surprisingly, if a ferromagnet is exposed to an ultrafast laser pulse, its apparent magnetization is reduced within less than a picosecond. Up to now, the total magnetization, i.e., the average spin polarization of the whole valence band, was not detectable on a sub-picosecond time scale. Here, we present experimental data, confirming the ultrafast reduction of the total magnetization. Soft x-ray pulses from the free electron laser in Hamburg (FLASH) extract polarized cascade photoelectrons from an iron layer excited by a femtosecond laser pulse. The spin polarization of the emitted electrons is detected by a Mott spin polarimeter.

We present results of single-shot resonant magnetic scattering experiments of Co/Pt multilayer systems using 100 fs long ultraintense pulses from an extreme ultraviolet (XUV) free-electron laser. An x-ray-induced breakdown of the resonant magnetic scattering channel during the pulse duration is observed at fluences of 5 J/cm(2). Simultaneously, the speckle contrast of the high-fluence scattering pattern is significantly reduced. We performed simulations of the nonequilibrium evolution of the Co/Pt multilayer system during the XUV pulse duration. We find that the electronic state of the sample is strongly perturbed during the first few femtoseconds of exposure leading to an ultrafast quenching of the resonant magnetic scattering mechanism.

The free-electron laser (FEL) sources FLASH in Hamburg, LCLS at Stanford, and FERMI in Trieste provide XUV to soft X-ray radiation (FLASH and FERMI) or soft to hard X-ray radiation (LCLS) with unprecedented parameters in terms of ultrashort pulse length, high photon flux, and coherence. These properties make FELs ideal tools for studying ultrafast dynamics in matter on a previously unaccessible level. This paper first reviews results obtained at FEL sources during the last few years in the field of magnetism research. We start with pioneering experiments at FLASH demonstrating the feasibility of magnetic scattering at FELs [1, 2], then present pump–probe scattering experiments [3, 4] as well as the first FEL magnetic imaging experiments [5], and finally discuss a limitation of the scattering methods due to a quenching of the magnetic scattering signal by high-fluence FEL pulses [6]. All of the presented experiments exploit the X-ray magnetic circular dichroism effect [7, 8] to obtain element-specific magnetic scattering contrast, as known from synchrotron experiments [9–12].

The dissociation dynamics induced by a 100 fs, 400 nm laser pulse in a rotationally cold Br2 sample was characterized by Coulomb explosion imaging (CEI) using a time-delayed extreme ultra-violet (XUV) FEL pulse, obtained from the Free electron LASer in Hamburg (FLASH). The momentum distribution of atomic fragments resulting from the 400 nm-induced dissociation was measured with a velocity map imaging spectrometer and used to monitor the internuclear distance as the molecule dissociated. By employing the simultaneously recorded in-house timing electro-optical sampling data, the time resolution of the final results could be improved to 300 fs, compared to the inherent 500 fs time-jitter of the FEL pulse. Before dissociation, the Br2 molecules were transiently 'fixed in space' using laser-induced alignment. In addition, similar alignment techniques were used on CO2 molecules to allow the measurement of the photoelectron angular distribution (PAD) directly in the molecular frame (MF). Our results on MFPADs in aligned CO2 molecules, together with our investigation of the dissociation dynamics of the Br2 molecules with CEI, show that information about the evolving molecular structure and electronic geometry can be retrieved from such experiments, therefore paving the way towards the study of complex non-adiabatic dynamics in molecules through XUV time-resolved photoion and photoelectron spectroscopy.

1 DESY, Notkestr. 85, 22607 Hamburg, Germany 2 Department of Chemistry, University of Leicester, University Road, Leicester, LE1 7RH, UK 3 Department of Physics and Astronomy, University of Leicester, University Road, Leicester, LE1 7RH, UK 4 Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, USA 5 Helmholtz-Institute Jena, Max-Wien-Platz 1, 07743 Jena, Germany

During ultrafast demagnetization of a magnetically ordered solid, angular momentum has to be transferred between the spins, electrons, and phonons in the system on femto-and picosecond timescales. Although the intrinsic spin-transfer mechanisms are intensely debated, additional extrinsic mechanisms arising due to nanoscale heterogeneity have only recently entered the discussion. Here we use femtosecond X-ray pulses from a free-electron laser to study thin film samples with magnetic domain patterns. We observe an infrared-pump-induced change of the spin structure within the domain walls on the sub-picosecond timescale. This domain-topography-dependent contribution connects the intrinsic demagnetization process in each domain with spin-transport processes across the domain walls, demonstrating the importance of spin-dependent electron transport between differently magnetized regions as an ultrafast demagnetization channel. This pathway exists independent from structural inhomogeneities such as chemical interfaces, and gives rise to an ultrafast spatially varying response to optical pump pulses.

Static and time-resolved photoelectron diffraction of laser-aligned polyatomic molecules photoionized by Free-Electron Laser pulses is presented. The results are a proof-of-principle for imaging dynamic structural changes in molecules with femtosecond temporal and Angstrom spatial resolution.

We present a systematic study of the photoionization of noble gas atoms exposed simultaneously to ultrashort (20 fs) monochromatic (1–2% spectral width) extreme ultraviolet (XUV) radiation from the Free-electron Laser in Hamburg (FLASH) and to intense synchronized near-infrared (NIR) laser pulses with intensities up to about 1013 W cm−2. Already at modest intensities of the NIR dressing field, the XUV-induced photoionization lines are split into a sequence of peaks due to the emission or absorption of several additional infrared photons. We observed a plateau-shaped envelope of the resulting sequence of sidebands that broadens with increasing intensity of the NIR dressing field. All individual lines of the nonlinear two-color ionization process are Stark-shifted, reflecting the effective intensity of the NIR field. The intensity-dependent cut-off energies of the sideband plateau are in good agreement with a classical model. The detailed structure of the two-color spectra, including the formation of individual sidebands, the Stark shifts and the contributions beyond the classical cut-off, however, requires a fully quantum mechanical description, as is demonstrated with time-dependent quantum calculations in single-active electron approximation.