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Spatially encoded measurements of transient optical transmissivity became a standard tool for temporal diagnostics of free-electron-laser (FEL) pulses, as well as for the arrival time measurements in X-ray pump and optical probe experiments. The modern experimental techniques can measure changes in optical coefficients with a temporal resolution better than 10 fs. This, in an ideal case, would imply a similar resolution for the temporal pulse properties and the arrival time jitter between the FEL and optical laser pulses. However, carrier transport within the material and out of its surface, as well as carrier recombination may, in addition, significantly decrease the number of carriers. This would strongly affect the transient optical properties, making the diagnostic measurement inaccurate. Below we analyze in detail the effects of those processes on the optical properties of XUV and soft X-ray irradiated Si$${_3}$$ 3 N$$_4$$ 4 , on sub-picosecond timescales. Si$${_3}$$ 3 N$$_4$$ 4 is a wide-gap insulating material widely used for FEL pulse diagnostics. Theoretical predictions are compared with the published results of two experiments at FERMI and LCLS facilities, and with our own recent measurement. The comparison indicates that three body Auger recombination strongly affects the optical response of Si$${_3}$$ 3 N$$_4$$ 4 after its collisional ionization stops. By deconvolving the contribution of Auger recombination, in future applications one could regain a high temporal resolution for the reconstruction of the FEL pulse properties measured with a Si$${_3}$$ 3 N$$_4$$ 4 -based diagnostics tool.

Laser and particle beams 37(2), 235 - 241 (2019). doi:10.1017/S0263034619000326, Modern free-electron lasers (FEL) operating in XUV (extreme ultraviolet) or X-ray range allow an access to novel research areas. An example is the ultrafast ionization of a solid by an intense femtosecond FEL pulse in XUV which consequently leads to a change of the complex index of refraction on an ultrashort timescale. The photoionization and subsequent impact ionization resulting in electronic and atomic dynamics are modeled with our hybrid code XTANT(X-ray thermal and non-thermal transitions) and a Monte Carlo code XCASCADE(X-ray-induced electron cascades). The simulations predict the temporal kinetics of FEL-induced electron cascades and thus yield temporally and spatially resolved information on the induced changes of the optical properties. In a series of experiments at FERMI and LCLS, single shot measurements with spatio-temporal encoding of the ionization process have been performed by a correlation of the FEL pump pulse with an optical femtosecond probe pulse. An excellent agreement between the experiment and the simulation has been found. We also show that such kind of experiments forms the basis for pulse duration and arrival time jitter monitoring as currently under development for XUV-FELs, Published by Cambridge Univ. Press, Cambridge

Using the Linac Coherent Light Source facility at the Stanford Linac Coherent Light Source National Accelerator Laboratory, we have observed X-ray scattering from iron compressed with laser-driven shocks to earth-core-like pressures above 400 GPa. The data show cases where melting is incomplete and we observe hexagonal-close-packed crystal structure at shock compressed densities up to 14.0 g cm-3 but no evidence of a double-hexagonal-close-packed crystal. The observation of a crystalline structure at these densities, where shock heating is expected to be in excess of the equilibrium melt temperature, may indicate superheating of the solid. These results are important for equation of state modeling at high strain rates relevant for impact scenarios and laser-driven shock-wave experiments.

Manipulating the atomic and electronic structure of matter with strong terahertz (THz) fields while probing the response with ultrafast pulses at x-ray free electron lasers (FELs) has offered unique insights into a multitude of physical phenomena in solid state and atomic physics. Recent upgrades of x-ray FEL facilities are pushing to much higher repetition rates, enabling unprecedented signal to noise for pump probe experiments. This requires the development of suitable THz pump sources that are able to deliver intense pulses at compatible repetition rates. Here we present a high power laser-driven THz source based on optical rectification in LiNbO3 using tilted pulse front pumping. Our source is driven by a kilowatt-level Yb:YAG amplifier system operating at 100 kHz repetition rate and employing nonlinear spectral broadening and recompression to achieve sub-100 fs pulses at 1030 nm wavelength. We demonstrate a maximum of 144 mW average THz power (1.44 uJ pulse energy), consisting of single-cycle pulses centered at 0.6 THz with a peak electric field strength exceeding 150 kV/cm. These high field pulses open up a range of possibilities for nonlinear time-resolved experiments with x-ray probing at unprecedented rates., 17 pages, 10 figures

In situ x-ray diffraction and wave-profile measurements were carried out on polycrystalline boron carbide under laser- induced shock compression at 51 GPa at the Matter in Extreme Conditions end-station of the Linac Coherent Light Source. The diffraction data indicate that boron carbide remains crystalline to this pressure and there is no evidence for a major structural phase transition. The peak elastic stress for boron carbide was found to be 15.9 GPa, in agreement with previous gas-gun measurements, despite differences in sample thickness and loading rate between laser and gas-gun compression. The starting sample contained excess carbon in the form of graphite. The graphite peaks disappeared upon compression of the sample, indicating that carbon was incorporated into the structure of boron carbide behind the shock front and retained upon decompression.

Soft x-rays were applied to induce graphitization of diamond through a non-thermal solid-to-solid phase transition. This process was observed within poly-crystalline diamond with a time-resolved experiment using ultrashort soft x-ray pulses of duration 52.5 fs and cross correlated by an optical pulse of duration 32.8 fs. This scheme enabled for the first time the measurement of a phase transition on a timescale of ~150 fs. Excellent agreement between experiment and theoretical predictions was found, using a dedicated code that followed the non-equilibrium evolution of the irradiated diamond including all transient electronic and structural changes. These observations confirm that soft x-rays can induce a non-thermal ultrafast solid-to-solid phase transition on a hundred femtosecond timescale., Comment: 27 pages, 17 figures (includes supplementary materials)

We present molecular dynamics simulations of shock and release in micron-scale tantalum crystals that exhibit postbreakout temperatures far exceeding those expected under the standard assumption of isentropic release. We show via an energy-budget analysis that this is due to plastic-work heating from material strength that largely counters thermoelastic cooling. The simulations are corroborated by experiments where the release temperatures of laser-shocked tantalum foils are deduced from their thermal strains via in situ x-ray diffraction and are found to be close to those behind the shock.

New high-repetition-rate x-ray free electron lasers (XFELs) require for their operation highly reliable ultrafast laser systems with high pulse energy, high repetition rate, and high average power. In this Letter, we present high-average-power scaling of near-infrared optical parametric chirped pulse amplification (OPCPA) in potassium titanyl arsenate (KTA) with tunable center wavelengths from 1.5 to 2.0 μm. Using a three-stage amplification scheme and a kW-level InnoSlab Yb:YAG pump amplifier for the final non-collinear KTA stage, we demonstrate an amplified output power of 106.2 W at a center wavelength of 1.75 μm and 100 kHz. Idler absorption introduces a potential upper limit on the average power scaling of center wavelengths

The behavior of silicon carbide (SiC) under shock compression is of interest due to its applications as a high-strength ceramic and for general understanding of shock-induced polymorphism. Here we use the Matter in Extreme Conditions beamline of the Linac Coherent Light Source to carry out a series of time-resolved pump-probe x-ray diffraction measurements on SiC laser-shocked to as high as 206 GPa. Experiments on single crystals and polycrystals of different polytypes show a transformation from a low-pressure tetrahedral phase to the high-pressure rocksalt-type (B1) structure. We directly observe coexistence of the low- and high-pressure phases in a mixed-phase region and complete transformation to the B1 phase above 200 GPa. The densities measured by x-ray diffraction are in agreement with both continuum gas-gun studies and a theoretical B1 Hugoniot derived from static-compression data. Time-resolved measurements during shock loading and release reveal a large hysteresis upon unloading, with the B1 phase retained to as low as 5 GPa. The sample eventually reverts to a mixture of polytypes of the low-pressure phase at late times. Our study demonstrates that x-ray diffraction is an effective means to characterize the time-dependent structural response of materials undergoing shock-induced phase transformations at megabar pressures.

Laser amplifiers at high repetition rate are critical for many applications in the chemical, physical and biological sciences. A variety of laser sources from XUV to THz can be derived from Ti:Sapphire laser amplifiers at moderate to low conversion efficiencies. High repetition rate applications require NIR and IR sources based on optical parametric chirped pulse amplifier (OPCPA) to drive these sources, offsetting the conversion efficiency losses with an even higher average power beam to drive the frequency conversion processes. We use these technologies at next generation free-electron laser (FEL) facilities. The Linac Coherent Light Source (LCLS), LCLS-II upgrade, will provide sub-femtosecond and femtosecond X-ray pulses at 100 kHz, and later up to 1 MHz repetition rate. The higher repetition rate benefits pump-probe experiments for weakly scattering samples and serves a variety of experiments which require attenuation to avoid perturbation and damage of the sample by the X-ray probe. A millijoule R&D laser amplifier was developed to test experimental conditions for optical laser beam delivery at LCLS-II. The laser can be operated at two distinct wavelength ranges. At 800 nm center wavelength we use the second harmonic of an Yb:YAG amplifier system to pump an OPCPA in a BBO crystal. A second tunable version operates between 1.45-2 m center wavelength using the fundamental Yb:YAG beam to pump a KTA OPCPA with average output powers in excess of 100 W. Currently the amplifier is operated 24 hours, 7 days a week. It is based on a simple and robust design, which ensures long term stability with good output beam quality.

We present the experimental thermal study of a 88.6 W average power optical parametric chirped pulse amplifier (OPCPA) system operating at 100 kHz, delivering sub-20 fs pulses at a center wavelength of 800 nm. A 15 W pump laser at 1030 nm is used to derive the seed pulses via white-light continuum generation and to pre-amplify the seed pulses to a 1 W level. Further amplification takes place in two high power stages, that are pumped with a frequency doubled Yb:YAG InnoSlab amplifier. The system is a prototype for the future LCLS-II pump-probe laser system.

Science advances 5(3), eaau8044 - (2019). doi:10.1126/sciadv.aau8044, Under rapid high-temperature, high-pressure loading, lattices exhibit complex elastic-inelastic responses. The dynamics of these responses are challenging to measure experimentally because of high sample density and extremely small relevant spatial and temporal scales. Here, we use an x-ray free-electron laser providing simultaneous in situ direct imaging and x-ray diffraction to spatially resolve lattice dynamics of silicon under high–strain rate conditions. We present the first imaging of a new intermediate elastic feature modulating compression along the axis of applied stress, and we identify the structure, compression, and density behind each observed wave. The ultrafast probe x-rays enabled time-resolved characterization of the intermediate elastic feature, which is leveraged to constrain kinetic inhibition of the phase transformation between 2 and 4 ns. These results not only address long-standing questions about the response of silicon under extreme environments but also demonstrate the potential for ultrafast direct measurements to illuminate new lattice dynamics., Published by AAAS, Washington, DC [u.a.]

Silicon, being one of the most abundant elements in nature, attracts wide-ranging scientific and technological interest. Specifically, in its elemental form, crystals of remarkable purity can be produced. One may assume that this would lead to silicon being well understood, and indeed, this is the case for many ambient properties, as well as for higher-pressure behaviour under quasi-static loading. However, despite many decades of study, a detailed understanding of the response of silicon to rapid compression—such as that experienced under shock impact—remains elusive. Here, we combine a novel free-electron laser-based X-ray diffraction geometry with laser-driven compression to elucidate the importance of shear generated during shock compression on the occurrence of phase transitions. We observe lowering of the hydrostatic phase boundary in elemental silicon, an ideal model system for investigating high-strength materials, analogous to planetary constituents. Moreover, we unambiguously determine the onset of melting above 14 GPa, previously ascribed to a solid–solid phase transition, undetectable in the now conventional shocked diffraction geometry; transitions to the liquid state are expected to be ubiquitous in all systems at sufficiently high pressures and temperatures.

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 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.

We have used femtosecond x-ray diffraction (XRD) to study laser-shocked fiber-textured polycrystalline tantalum targets as the 37-253 GPa shock waves break out from the free surface. We extract the time and depth-dependent strain profiles within the Ta target as the rarefaction wave travels back into the bulk of the sample. In agreement with molecular dynamics (MD) simulations the lattice rotation and the twins that are formed under shock-compression are observed to be almost fully eliminated by the rarefaction process.

We explore the scaling behavior of THz generation through optical rectification in DSTMS as function of repetition rate from 100 Hz to 200 kHz. We observe a strong drop-off in conversion efficiency above 10 kHz.

Applied physics letters 113(11), 114102 (2018). doi:10.1063/1.5046070, Recent studies confirmed that the materials used in the extreme UV and soft X-ray regime for precise characterization of intense free-electron laser pulses (e.g., Si$_3$N$_4$) do not work efficiently in the hard X-ray regime, which is due to the fact that the impact of a hard X-ray photon is followed by a series of electron cascading processes. Following theoretical indication, we show that this limitation can be circumvented and the cascading time can be significantly reduced if the X-ray photon energy is double the ionization energy. We investigate an alternative material for pulse diagnostics, SnO$_2$, using the Linac Coherent Light Source at photon energies of 5 keV and 9 keV. We prove the validity of the concept and show that it has a large potential for practical applications. By applying the proposed criteria, the temporal accuracy of the non-invasive pulse diagnostic tools can be improved in current and emerging hard X-ray facilities., Published by American Inst. of Physics, Melville, NY

Pressure-driven shock waves in solid materials can cause extreme damage and deformation. Understanding this deformation and the associated defects that are created in the material is crucial in the study of a wide range of phenomena, including planetary formation and asteroid impact sites, the formation of interstellar dust clouds, ballistic penetrators, spacecraft shielding and ductility in high-performance ceramics. At the lattice level, the basic mechanisms of plastic deformation are twinning (whereby crystallites with a mirror-image lattice form) and slip (whereby lattice dislocations are generated and move), but determining which of these mechanisms is active during deformation is challenging. Experiments that characterized lattice defects have typically examined the microstructure of samples after deformation, and so are complicated by post-shock annealing and reverberations. In addition, measurements have been limited to relatively modest pressures (less than 100 gigapascals). In situ X-ray diffraction experiments can provide insights into the dynamic behaviour of materials, but have only recently been applied to plasticity during shock compression and have yet to provide detailed insight into competing deformation mechanisms. Here we present X-ray diffraction experiments with femtosecond resolution that capture in situ, lattice-level information on the microstructural processes that drive shock-wave-driven deformation. To demonstrate this method we shock-compress the body-centred-cubic material tantalum-an important material for high-energy-density physics owing to its high shock impedance and high X-ray opacity. Tantalum is also a material for which previous shock compression simulations and experiments have provided conflicting information about the dominant deformation mechanism. Our experiments reveal twinning and related lattice rotation occurring on the timescale of tens of picoseconds. In addition, despite the common association between twinning and strong shocks, we find a transition from twinning to dislocation-slip-dominated plasticity at high pressure (more than 150 gigapascals), a regime that recovery experiments cannot accurately access. The techniques demonstrated here will be useful for studying shock waves and other high-strain-rate phenomena, as well as a broad range of processes induced by plasticity.

We study the feasibility of using small angle X-ray scattering (SAXS) as a new experimental diagnostic for intense laser-solid interactions. By using X-ray pulses from a hard X-ray free electron laser, we can simultaneously achieve nanometer and femtosecond resolution of laser-driven samples. This is an important new capability for the Helmholtz international beamline for extreme fields at the high energy density endstation currently built at the European X-ray free electron laser. We review the relevant SAXS theory and its application to transient processes in solid density plasmas and report on first experimental results that confirm the feasibility of the method. We present results of two test experiments where the first experiment employs ultra-short laser pulses for studying relativistic laser plasma interactions, and the second one focuses on shock compression studies with a nanosecond laser system.

High power OPCPAs above 10 W at short-wave IR wavelengths (SWIR: 1.4 - 3 μm) may be limited because of thermal heat dissipation in the nonlinear crystals. In this work we provide up-to-date measurements of the absorption coefficients of the nonlinear crystals used at these wavelengths and simulations of the thermal effects on critical parameters. In particular, power scaling limits will be discussed.

We present a 100 kHz, sub-20 fs optical parametric chirped-pulse amplifier (OPCPA) system delivering 88.6 W average power at a center wavelength of 800 nm. The seed pulses are derived from the pump laser via white-light continuum generation and are amplified in three non-collinear OPCPA stages. The final two high-power stages are pumped with a 661 W Yb:YAG InnoSlab amplifier. A simple and robust design is used for the OPCPA system to avoid thermal effects and enhance long-term stability, resulting in excellent beam quality and high conversion efficiency. To the best of our knowledge, this is the highest average power OPCPA system reported to date.

Review of scientific instruments 87(10), 103701 (2016). doi:10.1063/1.4963906, We describe the phase-contrast imaging instrument at the Matter in Extreme Conditions (MEC) endstation of the Linac Coherent Light Source. The instrument can image phenomena with a spatial resolution of a few hundreds of nanometers and at the same time reveal the atomic structure through X-ray diffraction, with a temporal resolution better than 100 fs. It was specifically designed for studies relevant to high-energy-density science and can monitor, e.g., shock fronts, phase transitions, or void collapses. This versatile instrument was commissioned last year and is now available to the MEC user community., Published by American Institute of Physics, [S.l.]

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.

Next-generation X-ray sources have allowed new opportunities for ultrafast imaging, but such schemes require femtosecond synchronization between the pump and probe laser pulses. Here, researchers present few-femtosecond timing between a free-electron laser and an external laser exploiting terahertz radiation.

We report on investigations of high-order harmonic generation from solid surfaces in the coherent wake emission regime with relativistically intense few-cycle (8 fs) laser pulses. Significant spectral broadening compared to previous experiments with many-cycle pulses and the appearance of substructures on the harmonics are observed that strongly fluctuate from shot-to-shot. Measurements in which the linear polarization was rotated or ellipticity of the laser pulse was varied exhibit a strong dependence of the harmonic emission on the polarization state of the incident pulse. We show that the observed spectral features are ultimately connected to the sub-cycle electron dynamics in the laser-solid interaction and thus proof of the few-cycle nature of the observed harmonic emission. Using a simple model we have investigated the factors that play an important role in the shape of the emitted spectrum.

We report on laser-driven electron acceleration with 8 fs, i.e. three optical cycles, pulse duration and 40 mJ energy. Theory and numerical simulations predict that this experimentally unexplored parameter range is relevant for laser wake-field acceleration. The electron spectra produced are monoenergetic with a peak up to 50 MeV and free of low-energy electrons with thermal spectrum. The electron beam has a typical divergence of 5–10 mrad. The accelerator is routinely operated at 10 Hz and correspondingly it is a promising source for several applications. To cite this article: L. Veisz et al., C. R. Physique 10 (2009).

Quasi-phase matching (QPM) can be used to increase the conversion efficiency of the high harmonic generation (HHG) process. We observed QPM with an improved dual-gas foil target with a 1 kHz, 10 mJ, 30 fs laser system. Phase tuning and enhancement were possible within a spectral range from 17 nm to 30 nm. Furthermore analytical calculations and numerical simulations were carried out to distinguish QPM from other effects, such as the influence of adjacent jets on each other or the laser gas interaction. The simulations were performed with a 3 dimensional code to investigate the phase matching of the short and long trajectories individually over a large spectral range.

Optical parametric chirped-pulse amplification (OPCPA) is the most promising method for providing compact, wavelength tunable, high power, femtosecond lasers. We have recently achieved a 112 W OPCPA with wavelength tunability around 800 nm and 30 fs pulse duration in burst mode (100 kHz in a 800 µs burst at 10 Hz). In this work, we discuss the various laser architectures and the critical parameters in achieving similar laser parameters but in continuous operation.

The use of temporally shaped pump pulses for optical parametric chirped-pulse amplification can increase the efficiency and suppress possible spectral distortions in this process. With this goal in mind a novel method for shaping narrowband picosecond pulses has been developed. The method is based on the pulse stacking principle, where replicas of the incoming pulse are created in a specially designed four-beam interferometer. The replicas are recombined with appropriate relative delays. The interferometer design allows for a unique flexibility in varying the pulse shape, since all relevant degrees of freedom, such as relative intensities and delays between the pulse replicas are independently adjustable. Here we describe the design of our device in detail and report on the experimental demonstration of its pulse-shaping capabilities.

We report on the pulse contrast-ratio characterization of a few-cycle 0.2 TW optical parametric chirped pulse amplifier system operating at 20 Hz. A specially designed third-order correlator was used to characterize and optimize the contrast of the system. We demonstrate that the pulse contrast depends much more on the temporal overlap between the pump and the seed pulse than the shape of the amplified spectrum. The best amplified pulse contrast-ratio was 10-4 at Δt=±25 ps and >10-9 at Δt=±150 ps delays.

This manuscript serves as a reference to describe the optical laser sources and capabilities at the Linac Coherent Light Source., Ultrafast optical lasers play an essential role in exploiting the unique capabilities of recently commissioned X-ray free-electron laser facilities such as the Linac Coherent Light Source (LCLS). Pump–probe experimental techniques reveal ultrafast dynamics in atomic and molecular processes and reveal new insights in chemistry, biology, material science and high-energy-density physics. This manuscript describes the laser systems and experimental methods that enable cutting-edge optical laser/X-ray pump–probe experiments to be performed at LCLS.

Optical parametric chirped-pulse amplifiers with high average power are possible with novel high-power Yb:YAG amplifiers with kW-level output powers. We demonstrate a compact wavelength-tunable sub-30-fs amplifier with 11.4 W average power with 20.7% pump-to-signal conversion efficiency. For parametric amplification, a beta-barium borate crystal is pumped by a 140 W, 1 ps Yb: YAG InnoSlab amplifier at 3.25 MHz repetition rate. The broadband seed is generated via supercontinuum generation in a YAG crystal.

The potential of borate crystals, BBO, LBO and BiBO, for high average power scaling of optical parametric chirped-pulse amplifiers is investigated. Up-to-date measurements of the absorption coefficients at 515 nm and the thermal conductivities are presented. The measured absorption coefficients are a factor of 10-100 lower than reported by the literature for BBO and LBO. For BBO, a large variation of the absorption coefficients was found between crystals from different manufacturers. The linear and nonlinear absorption coefficients at 515 nm as well as thermal conductivities were determined for the first time for BiBO. Further, different crystal cooling methods are presented. In addition, the limits to power scaling of OPCPAs are discussed.

A conceptual design of a high power, ultrabroadband optical parametric chirped-pulse amplifier (OPCPA) was carried out comparing nonlinear crystals (LBO and BBO) for 810 nm centered, sub-7.0 fs pulses with energies above 1 mJ. These amplifiers are only possible with a parallel development of kilowatt-level OPCPA-pump amplifiers. It is therefore important to know good strategies to use the available OPCPA-pump energy efficiently. Numerical simulations, including self- and cross-phase modulation, were used to investigate the critical parameters to achieve sufficient spectral and spatial quality. At high output powers, thermal absorption in the nonlinear crystals starts to degrade the output beam quality. Strategies to minimize thermal effects and limits to the maximum average power are discussed.

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.

The high repetition rate laser systems providing the ELI-ALPS facility with TW-to-PW peak intensity pulses are designed to generate secondary light sources with a duration of tens of attosecond for basic and applied researches.

Nature Communications 4, 1731 (2013). doi:10.1038/ncomms2754, The resolution of ultrafast studies performed at extreme ultraviolet and X-ray free-electron lasers is still limited by shot-to-shot variations of the temporal pulse characteristics. Here we show a versatile single-shot temporal diagnostic tool that allows the determination of the extreme ultraviolet pulse duration and the relative arrival time with respect to an external pump-probe laser pulse. This method is based on time-resolved optical probing of the transient reflectivity change due to linear absorption of the extreme ultraviolet pulse within a solid material. In this work, we present measurements performed at the FLASH free-electron laser. We determine the pulse duration at two distinct wavelengths, yielding (184±14) fs at 41.5 nm and (21±19) fs at 5.5 nm. Furthermore, we demonstrate the feasibility to operate the tool as an online diagnostic by using a 20-nm-thin Si3N4 membrane as target. Our results are supported by detailed numerical and analytical investigations., Published by Nature Publishing Group, London

Attosecond science is enabled by the ability to convert femtosecond near-infrared laser light into coherent harmonics in the extreme ultraviolet spectral range. While attosecond sources have been utilized in experiments that have not demanded high intensities, substantially higher photon flux would provide a natural link to the next significant experimental breakthrough. Numerical simulations of dual-gas high harmonic generation indicate that the output in the cutoff spectral region can be selectively enhanced without disturbing the single-atom gating mechanism. Here, we summarize the results of these simulations and present first experimental findings to support these predictions.

An Yb:YAG thin-disk multipass laser amplifier system was developed operating in a 10 Hz burst operation mode with 800 µs burst duration and 100 kHz intra-burst repetition rate. Methods for the suppression of parasitic amplified spontaneous emission are presented. The average output pulse energy is up to 44.5 mJ and 820 fs compressed pulse duration. The average power of 4.45 kW during the burst is the highest reported for this type of amplifier.

An Yb:YAG thin-disk laser amplifier is presented capable of amplifying pulses to a maximum average power of 4.45 kW at burst repetition rates of 100 kHz as pump amplifier for an optical parametric amplifier system.

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.

Physical review letters 107, 175002 (2011). doi:10.1103/PhysRevLett.107.175002, Published by APS, College Park, Md.