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An open-loop control scheme of molecular fragmentation based on transient molecular alignment combined with single-photon ionization induced by a short-wavelength free electron laser (FEL) is demonstrated for the acetylene cation. Photoelectron spectra are recorded, complementing the ion yield measurements, to demonstrate that such control is the consequence of changes in the electronic response with molecular orientation relative to the ionizing field. We show that stable C2H2+ cations are mainly produced when the molecules are parallel or nearly parallel to the FEL polarization, while the hydrogen fragmentation channel (C2H2+ → C2H+ + H) predominates when the molecule is perpendicular to that direction, thus allowing one to distinguish between the two photochemical processes. The experimental findings are supported by state-of-the art theoretical calculations.

Physica scripta 97(8), 084002 - (2022). doi:10.1088/1402-4896/ac7a69, We have conceived and built the HILITE (High-Intensity Laser-Ion Trap Experiment) Penning-trap setup for the production, confinement and preparation of pure ensembles of highly charged ions in a defined quantum state as a target for various high-intensity lasers. This enables a broad suite of laser-ion interaction studies at high photon energies and/or intensities, such as non-linear photo-ionisation studies. The setup has now been used to perform experiments at one such laser facility, namely the FLASH Free-Electron Laser at DESY in Hamburg, Germany. We describe the experimental possibilities of the apparatus, the results of the first measurements and future experiments at other laser facilities., Published by The Royal Swedish Academy of Sciences, Stockholm

Physical review / A 104(5), 053102 (2021). doi:10.1103/PhysRevA.104.053102, The effects of postcollision interaction (PCI) in the time evolution of photoinduced Auger decay, assisted by a terahertz (THz) field, is theoretically investigated. We propose a time-dependent model which is based on the quantum-mechanical description of the photoinduced Auger process and quasiclassical description of the PCI. The suggested model is used for calculating the PCI distortion of the Auger spectrum at different temporal overlaps of the exciting extreme ultraviolet pulse and the streaking THz pulse., Published by Inst., Woodbury, NY

Journal of physics / B 54(8), 085601 (2021). doi:10.1088/1361-6455/abf154, Auger electron spectra were simulated in the presence of a terahertz streaking field to study post-collision interaction (PCI) effects in the time-evolution of photoinduced Auger decays. The PCI is characterized by the ratio of the spectral line width for Auger electron emission in opposite directions with respect to the THz-field. These calculations have been performed using the analytical semiclassical model developed by Bauch and Bonitz (2012 Physical Review A 85 053416). The results are shown for Ne(KLL), Ar(LMM), Kr(MNN) and Xe(NOO) Auger transitions whereby different possible experimental conditions were evaluated., Published by IOP Publ., Bristol

The Free-electron LASer in Hamburg (FLASH) has been extended with a new undulator line FLASH2 in 2014. A compact grazing-incident wide-spectral-range spectrometer based on spherical-variable-line-spacing (SVLS) gratings in the extreme ultraviolet (XUV) region was constructed to optimize and characterize the free-electron laser (FEL) performance at FLASH2. The spectrometer is equipped with three different concave SVLS gratings covering a spectral range from 1 to 62 nm to analyze the spectral characteristics of the XUV radiation. Wavelength calibration and evaluation of the spectral resolution were performed at the plane grating monochromator beamline PG2 at FLASH1 before the installation at FLASH2, and compared with analytical simulations. The first light using self-amplified spontaneous emission from FLASH2 was observed by the spectrometer during a simultaneous operation of both undulator lines—FLASH1 and FLASH2. In addition, the spectral resolution of the spectrometer was evaluated by comparing the measured spectrum from FLASH2 with FEL simulations.

We present time-resolved ultraviolet-pump x-ray probe Auger spectra of 2-thiouracil. An ultraviolet induced shift towards higher kinetic energies is observed in the sulfur 2p Auger decay. The difference Auger spectra of pumped and unpumped molecules exhibit ultrafast dynamics in the shift amplitude, in which three phases can be recognized. In the first 100 fs, a shift towards higher kinetic energies is observed, followed by a 400 fs shift back to lower kinetic energies and a 1 ps shift again to higher kinetic energies. We use a simple Coulomb-model, aided by quantum chemical calculations of potential energy states, to deduce a C–S bond expansion within the first 100 fs. The bond elongation triggers internal conversion from the photoexcited S2 to the S1 state. Based on timescales, the subsequent dynamics can be interpreted in terms of S1 nuclear relaxation and S1-triplet internal conversion.

The prototypical photoinduced dissociation of Fe(CO)

We prove the hitherto hypothesized sequential dissociation of Fe(CO)5 in the gas phase upon photoexcitation at 266 nm via a singlet pathway with time-resolved valence and core-level photoelectron spectroscopy with an x-ray free-electron laser. Valence photoelectron spectra are used to identify free CO molecules and to determine the time constants of stepwise dissociation to Fe(CO)4 within the temporal resolution of the experiment and further to Fe(CO)3 within 3 ps. Fe 3p core-level photoelectron spectra directly reflect the singlet spin state of the Fe center in Fe(CO)5, Fe(CO)4, and Fe(CO)3 showing that the dissociation exclusively occurs along a singlet pathway without triplet-state contribution. Our results are important for assessing intra- and intermolecular relaxation processes in the photodissociation dynamics of the prototypical Fe(CO)5 complex in the gas phase and in solution, and they establish time-resolved core-level photoelectron spectroscopy as a powerful tool for determining the multiplicity of transition metals in photochemical reactions of coordination complexes.

Physical review letters 118(1), 013002 (2017). doi:10.1103/PhysRevLett.118.013002, Intense, circularly polarized extreme-ultraviolet and near-infrared (NIR) laser pulses are combined to double ionize atomic helium via the oriented intermediate He+(3p) resonance state. Applying angle-resolved electron spectroscopy, we find a large photon helicity dependence of the spectrum and the angular distribution of the electrons ejected from the resonance by NIR multiphoton absorption. The measured circular dichroism is unexpectedly found to vary strongly as a function of the NIR intensity. The experimental data are well described by theoretical modeling and possible mechanisms are discussed., Published by APS, College Park, Md.

We prove the hitherto hypothesized sequential dissociation of Fe(CO)(5) in the gas phase upon photoexcitation at 266 nm via a singlet pathway with time-resolved valence and core-level photoelectron spectroscopy with an x-ray free-electron laser. Valence photoelectron spectra are used to identify free CO molecules and to determine the time constants of stepwise dissociation to Fe(CO)(4) within the temporal resolution of the experiment and further to Fe(CO)(3) within 3 ps. Fe 3p core-level photoelectron spectra directly reflect the singlet spin state of the Fe center in Fe(CO)(5), Fe(CO)(4), and Fe(CO)(3) showing that the dissociation exclusively occurs along a singlet pathway without triplet-state contribution. Our results are important for assessing intra- and intermolecular relaxation processes in the photodissociation dynamics of the prototypical Fe(CO)(5) complex in the gas phase and in solution, and they establish time-resolved core-level photoelectron spectroscopy as a powerful tool for determining the multiplicity of transition metals in photochemical reactions of coordination complexes. Published by AIP Publishing.

We report on soft X-ray scattering experiments on cryogenic hydrogen and simple metal samples. As a source of intense, ultrashort soft X-ray pulses we have used free-electron laser radiation at 92 eV photon energy from FLASH at DESY, Hamburg. X-ray pulses with energies up to 150 μJ and durations 15-50 fs provide interaction with the sample leading simultaneously to plasma formation and scattering. Experiments exploiting both of these interactions have been carried out, using the same experimental setup. Firstly, recording of soft X-ray inelastic scattering from near-solid density hydrogen plasmas at few electron volt temperatures confirms the feasibility of this diagnostics technique. Secondly, the soft X-ray excitation of few electron volt solid-density plasmas in bulk metal samples could be studied by recording soft X-ray line and continuum emission integrated over emission times from fs to ns. © 2009 Elsevier B.V.

We report on the x-ray absorption of Warm Dense Matter experiment at the FLASH Free Electron Laser (FEL) facility at DESY. The FEL beam is used to produce Warm Dense Matter with soft x-ray absorption as the probe of electronic structure. A multilayer-coated parabolic mirror focuses the FEL radiation, to spot sizes as small as 0.3μm in a ∼15fs pulse of containing >10 12 photons at 13.5 nm wavelength, onto a thin sample. Silicon photodiodes measure the transmitted and reflected beams, while spectroscopy provides detailed measurement of the temperature of the sample. The goal is to measure over a range of intensities approaching 10 18 W/cm 2. Experimental results will be presented along with theoretical calculations. A brief report on future FEL efforts will be given. © 2009 SPIE.

We used a terahertz (THz) field driven streak camera with capabilities to deliver the pulse duration and the arrival time information with around 10 fs resolution for each single XUV FEL pulse at FLASH. The setup was operated simultaneously with an alternative method to determine the FEL pulse duration based on spectral measurements. A comparison will be shown.

New journal of physics 18(4), 043017 (2016). doi:10.1088/1367-2630/18/4/043017, 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., Published by Dt. Physikalische Ges., [Bad Honnef]

The ability to fully characterize ultrashort, ultra-intense X-ray pulses at free-electron lasers (FELs) will be crucial in experiments ranging from single-molecule imaging to extreme-timescale X-ray science. This issue is especially important at current-generation FELs, which are primarily based on self-amplified spontaneous emission and radiate with parameters that fluctuate strongly from pulse to pulse. Using single-cycle terahertz pulses from an optical laser, we have extended the streaking techniques of attosecond metrology to measure the temporal profile of individual FEL pulses with 5 fs full-width at half-maximum accuracy, as well as their arrival on a time base synchronized to the external laser to within 6 fs r.m.s. Optical laser-driven terahertz streaking can be utilized at any X-ray photon energy and is non-invasive, allowing it to be incorporated into any pump–probe experiment, eventually characterizing pulses before and after interaction with most sample environments.

One of the most challenging tasks for extreme ultraviolet, soft and hard x ray free electron laser photon diagnostics is the precise determination of the photon pulse duration, which is typically in the sub 100 fs range. Nine different methods, able to determine such ultrashort photon pulse durations, were compared experimentally at FLASH, the self amplified spontaneous emission free electron laser at DESY in Hamburg, in order to identify advantages and disadvantages of different methods. Radiation pulses at a wavelength of 13.5 and 24.0 nm together with the corresponding electron bunch duration were measured by indirect methods like analyzing spectral correlations, statistical fluctuations, and energy modulations of the electron bunch and also by direct methods like autocorrelation techniques, terahertz streaking, or reflectivity changes of solid state samples. In this paper, we present a comprehensive overview of the various techniques and a comparison of the individual experimental results. The information gained is of utmost importance for the future development of reliable pulse duration monitors indispensable for successful experiments with ultrashort extreme ultraviolet pulses

Tabletop Ti : sapphire lasers, such as the Jena multi-Terawatt laser, can nowadays reach focused intensities of up to 1020 W cm−2. The interaction of this intense light field with a solid target—in our case tantalum—leads to the production of energetic bremsstrahlung x-rays. These are used to induce (γ,n)- and (γ,f)-reactions in 181Ta, 129I, 232Th, 238U and 9Be. The results are discussed in the context of laser plasma diagnostics and photo transmutation studies on radioactive material.We also report on fusion experiments in low-Z targets where the fusion neutrons are utilized to characterize ion acceleration processes.

The influence of prepulses on the conversion efficiency (CE) of laser radiation into 13 nm extreme ultraviolet (EUV) radiation, resulting from lithium-like oxygen ions from O20 μm water droplets, was investigated. The laser pulse durations in the experiment ranged from 200 fs to 120 ps. Applying prepulses preceding the main pulse at various delays of up to 11 ns, it was shown that the CE increases differently for each measured pulse duration. The strongest dependence on the introduction of a prepulse was observed for 2 ps laser pulses with a 20 mJ laser pulse energy. The EUV CE was improved by a factor of 15 by the introduction of a prepulse. Calculations on the atomic physics of oxygen ions and simulations of the laser–plasma interaction revealed the influence of the prepulse on the EUV yield.

Synopsis Intense, circularly polarized extreme-ultraviolet (XUV) and near-infrared (NIR) laser pulses are combined to double-ionize atomic helium via the oriented intermediate He+ (3p) resonance state. A strong and NIR-intensity dependent circular dichroism is accounted to a helicity dependent AC-Stark shift.

The ionization and fragmentation dynamics of iodine molecules (I2) are traced using very intense (∼1014 W cm−2) ultra-short (∼60 fs) light pulses with 87 eV photons of the Free-electron LASer at Hamburg (FLASH) in combination with a synchronized femtosecond optical laser. Within a pump–probe scheme the IR pulse initiates a molecular fragmentation and then, after an adjustable time delay, the system is exposed to an intense FEL pulse. This way we follow the creation of highly-charged molecular fragments as a function of time, and probe the dynamics of multi-photon absorption during the transition from a molecule to individual atoms.

The charge rearrangement in dissociating ${\mathrm{I}}_{2}^{n+}$ molecules is measured as a function of the internuclear distance $R$ using extreme ultraviolet pulses delivered by the free-electron laser in Hamburg. Within an extreme ultraviolet pump-probe scheme, the first pulse initiates dissociation by multiply ionizing ${\mathrm{I}}_{2}$, and the delayed probe pulse further ionizes one of the two fragments at a given time, thus triggering charge rearrangement at a well-defined $R$. The electron transfer between the fragments is monitored by analyzing the delay-dependent ion kinetic energies and charge states. The experimental results are in very good agreement with predictions of the classical over-the-barrier model demonstrating its validity in a thus far unexplored quasimolecular regime relevant for free-electron laser, plasma, and chemistry applications.

Ultrafast extreme ultraviolet and X-ray free-electron lasers are set to revolutionize many domains such as bio-photonics and materials science, in a manner similar to optical lasers over the past two decades. Although their number will grow steadily over the coming decade, their complete characterization remains an elusive goal. This represents a significant barrier to their wider adoption and hence to the full realization of their potential in modern photon sciences. Although a great deal of progress has been made on temporal characterization and wavefront measurements at ultrahigh extreme ultraviolet and X-ray intensities, only few, if any progress on accurately measuring other key parameters such as the state of polarization has emerged. Here we show that by combining ultra-short extreme ultraviolet free electron laser pulses from FERMI with near-infrared laser pulses, we can accurately measure the polarization state of a free electron laser beam in an elegant, non-invasive and straightforward manner using circular dichroism. © 2014 Macmillan Publishers Limited.

We optimize the conversion of laser energy into extreme ultraviolet (EUV) radiation by tailoring the laser parameters for a laser-produced plasma generated from 20 μm diameter water droplets. It is shown that mass-limited targets require careful adaption of laser-pulse energy and laser-pulse duration separately, rather than laser intensity, which seems to be adequate for bulk targets. The optimal pulse duration scales with the droplet radius, and the optimal pulse energy with the droplet volume. With optimized parameters, we obtain a conversion efficiency of 0.23% in 4π and 2.5% bandwidth for 13 nm radiation, the future EUV lithography light.

While huge progress has been achieved for EUVL system design and multilayer optics during the last years the decision on the best suited source is still open. In a German basic research cooperation on short-wavelength plasma based sources some key issues also relevant for EUVL are addressed: the comparison of existing sources, investigations on the scalability of source concepts and the demonstration of key features. Preliminary results of investigations on parameters for best conversion efficiency of laser produced plasmas, concepts for high-power lasers and scalability of gas discharge based sources are presented. Comparability of results is assured by calibrated metrology tools which are cross checked with ASML’s flying circus.

We report on a fully angular resolved spectrum of hard x-rays emitted from a laser produced plasma, which is generated by a laser intensity of 5 x 10 18 W/cm 2 on a tantalum surface. MeV x-rays were utilized to generate photoneutrons via photofission of beryllium.

Short-wavelength free-electron lasers are now well established as essential and unrivalled sources of ultrabright coherent X-ray radiation. One of the key characteristics of these intense X-ray pulses is their expected few-femtosecond duration. No measurement has succeeded so far in directly determining the temporal structure or even the duration of these ultrashort pulses in the few-femtosecond range. Here, by deploying the so-called streaking spectroscopy technique at the Linac Coherent Light Source, we demonstrate a non-invasive scheme for temporal characterization of X-ray pulses with sub-femtosecond resolution. This method is independent of photon energy, decoupled from machine parameters, and provides an upper bound on the X-ray pulse duration. We measured the duration of the shortest X-ray pulses currently available to be on average no longer than 4.4 fs. Analysing the pulse substructure indicates a small percentage of the free-electron laser pulses consisting of individual high-intensity spikes to be on the order of hundreds of attoseconds. Using a spectroscopy streaking technique at LCLS (Linac Coherent Light Source), researchers demonstrate temporal characterization of X-ray pulses with sub-femtosecond resolution.

The dissociation dynamics induced by a 100 fs, 400 nm laser pulse in a rotationally cold Br-2 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 Br-2 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 Br-2 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.

Initiating the gain process in a free-electron laser (FEL) from an external highly coherent source of radiation is a promising way to improve the pulse properties such as temporal coherence and synchronization performance in time-resolved pump-probe experiments at FEL facilities, but this so-called "seeding" suffers from the lack of adequate sources at short wavelengths. We report on the first successful seeding at a wavelength as short as 38.2 nm, resulting in GW-level, coherent FEL radiation pulses at this wavelength as well as significant second harmonic emission at 19.1 nm. The external seed pulses are about 1 order of magnitude shorter compared to previous experiments allowing an ultimate time resolution for the investigation of dynamic processes enabling breakthroughs in ultrafast science with FELs. The seeding pulse is the 21st harmonic of an 800-nm, 15-fs (rms) laser pulse generated in an argon medium. Methods for finding the overlap of seed pulses with electron bunches in spatial, longitudinal, and spectral dimensions are discussed and results are presented. The experiment was conducted at FLASH, the FEL user facility at DESY in Hamburg, Germany. (Less)

We present results of single-shot resonant magnetic scattering experiments of $\mathrm{Co}/\mathrm{Pt}$ 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 $5\text{ }\text{ }\mathrm{J}/{\mathrm{cm}}^{2}$. Simultaneously, the speckle contrast of the high-fluence scattering pattern is significantly reduced. We performed simulations of the nonequilibrium evolution of the $\mathrm{Co}/\mathrm{Pt}$ 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.

Single-shot time-of-flight spectra for Coulomb explosion of N-2 and I-2 molecules have been recorded at the Free Electron LASer in Hamburg (FLASH) and have been analysed using a partial covariance mapping technique. The partial covariance analysis unravels a detailed picture of all significant Coulomb explosion pathways, extending up to the N4+-N5+ channel for nitrogen and up to the I8+-I9+ channel for iodine. The observation of the latter channel is unexpected if only sequential ionization processes from the ground state ions are considered. The maximum kinetic energy release extracted from the covariance maps for each dissociation channel shows that Coulomb explosion of nitrogen molecules proceeds much faster than that of the iodine. The N-2 ionization dynamics is modelled using classical trajectory simulations in good agreement with the outcome of the experiments. The results suggest that covariance mapping of the Coulomb explosion can be used to measure the intensity and pulse duration of free-electron lasers.

We traced the femtosecond nuclear-wave-packet dynamics in ionic states of oxygen and nitrogen diatomic molecules employing 38-eV XUV-pump--XUV-probe experiments at the free-electron laser in Hamburg (FLASH). The nuclear dynamics is monitored via the detection of coincident ionic fragments using a reaction microscope and a split-mirror setup to generate the pump and probe pulses. By comparing measured kinetic-energy-release spectra with classical and quantum-mechanical simulations, we identified electronic states of the molecular ions that are populated by ionization of the neutral molecule. For specific fragment charge states, this comparison allows us to assess the relevance of specific dissociation paths.

We present a time-resolved infrared (IR) pump and extreme-ultraviolet (XUV) probe diffraction experiment to investigate ultrafast structural dynamics in colloidal crystals with picosecond resolution. The experiment was performed at the FLASH facility at DESY with a fundamental wavelength of 8 nm. In our experiment, the temporal changes of Bragg peaks were analyzed and their frequency components were calculated using Fourier analysis. Periodic modulations in the colloidal crystal were localized at a frequency of about 4-5 GHz. Based on the Lamb theory, theoretical calculations of vibrations of the isotropic elastic polystyrene spheres of 400 nm in size reveal a 5.07 GHz eigenfrequency of the ground (breathing) mode., 12 pages, 3 figures

Using a split focusing mirror, XUV pump–probe measurements have been performed at the free-electron laser at Hamburg (FLASH). The obtained non-linear autocorrelation signals can be used to characterize the ultra-short photon pulses generated by the machine at different control parameters.

Two-color ($\mathrm{x}\mathrm{\text{\ensuremath{-}}}\mathrm{ray}+\mathrm{\text{infrared}}$) electron spectroscopy is used for investigating laser-assisted $KLL$ Auger decay following $1s$ photoionization of atomic Ne with few-femtosecond x-ray pulses from the Linac Coherent Light Source. In an angle-resolved experiment, the overall width of the laser-modified Auger-electron spectrum and its structure change significantly as a function of the emission angle. The spectra are characterized by a strong intensity variation of the sidebands revealing a gross structure. This variation is caused, as predicted by theory, by the interference of electrons emitted at different times within the duration of one optical cycle of the infrared dressing laser, which almost coincides with the lifetime of the Ne $1s$ vacancy.

It has been proposed that radiation from free electron laser (FEL) at Hamburg (FLASH) can be used for ultrafast time-resolved x-ray diffraction experiments based on the near-infrared (NIR) pump/FEL probe scheme. Here, investigation probing the ultrafast structural dynamics of periodic nano-crystalline organic matter (silver behenate) with such a scheme is reported. Excitation with a femtosecond NIR laser leads to an ultrafast lattice modification which time evolution has been studied through the scattering of vacuum ultraviolet FEL pulses. The found effect last for 6 ps and underpins the possibility for studying nanoperiodic dynamics down to the FEL source time resolution. Furthermore, the possibility of extending the use of silver behenate (AgBh) as a wavelength and temporal calibration tool for experiments with soft x-ray/FEL sources is suggested.

We introduce a time-domain approach to explore rotational dynamics caused by intramolecular coupling or the interaction with dissipative media. It pushes the time resolution toward the ultimate limit determined by the rotational period. Femtosecond pulses create a coherent superposition of two rotational states of carbon monoxide. The wave-packet motion is observed by subsequent Coulomb explosion, which results in a time-dependent asymmetry of spatial fragmentation patterns. The asymmetry oscillation prevails for at least 1 ns, covering more than 300 periods with no decoherence. Long time scans will allow weak perturbations of the order of $\ensuremath{\Delta}E/E={10}^{\ensuremath{-}4}$ to be discerned. Our conclusions are confirmed by a fully quantum-mechanical model.

Resonant soft x-ray diffraction (RSXD) with femtosecond (fs) time resolution is a powerful tool for disentangling the interplay between different degrees of freedom in strongly correlated electron materials. It allows addressing the coupling of particular degrees of freedom upon an external selective perturbation, e. g., by an optical or infrared laser pulse. Here, we report a time-resolved RSXD experiment from the prototypical correlated electron material magnetite using soft x-ray pulses from the free-electron laser FLASH in Hamburg. We observe ultrafast melting of the charge-orbital order leading to the formation of a transient phase, which has not been observed in equilibrium.

Using a split-mirror stage combined with a reaction microscope, nonlinear autocorrelation traces of XUV pulses from the Free-electron LASer at Hamburg were recorded for ${\mathrm{N}}_{2}$ multiphoton-induced fragmentation into noncoincident ${\mathrm{N}}^{2+}$ and coincident ${\mathrm{N}}^{2+}+{\mathrm{N}}^{2+}$ channels. We find a pulse duration of $40\ifmmode\pm\else\textpm\fi{}10 \mathrm{fs}$ along with a sharp spike pointing to a coherence time of $4\ifmmode\pm\else\textpm\fi{}1 \mathrm{fs}$, almost twice as short as in previous observations. Both are well reproduced by a simulation based on the partial-coherence model that includes the molecular dynamics leading to an $~12\ensuremath{-}\mathrm{fs}$ substructure in the trace.

Two-photon excitation of a single-photon forbidden Auger resonance has been observed and investigated using the intense extreme ultraviolet radiation from the free electron laser in Hamburg. At the wavelength 26.9 nm (46 eV) two photons promoted a 3d core electron to the outer 4d shell. The subsequent Auger decay, as well as several nonlinear above threshold ionization processes, were studied by electron spectroscopy. The experimental data are in excellent agreement with theoretical predictions and analysis of the underlying multiphoton processes.

We investigate ultrafast (fs) electron dynamics in a liquid hydrogen sample, isochorically and volumetrically heated to a moderately coupled plasma state. Thomson scattering measurements using 91.8 eV photons from the free-electron laser in Hamburg (FLASH at DESY) show that the hydrogen plasma has been driven to a nonthermal state with an electron temperature of 13 eV and an ion temperature below 0.1 eV, while the free-electron density is 2.8x10{20} cm{-3}. For dense plasmas, our experimental data strongly support a nonequilibrium kinetics model that uses impact ionization cross sections based on classical free-electron collisions.

Physical review letters 104, 213001 (2010). doi:10.1103/PhysRevLett.104.213001, Published by APS, College Park, Md.

Physical review letters 105, 263002 (2010). doi:10.1103/PhysRevLett.105.263002, Published by APS, College Park, Md.