We report recent results on the performance of FLASH (Free Electron Laser in Hamburg) operating at a wavelength of 13.7 nm where unprecedented peak and average powers for a coherent EUV radiation source have been measured. In the saturation regime the peak energy approached 170 µJ for individual pulses while the average energy per pulse reached 70 µJ. The pulse duration was in the region of 10 femtoseconds and peak

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

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Two-color, single-shot time-of-flight electron spectroscopy of atomic neon was employed at the Linac Coherent Light Source (LCLS) to measure laser-assisted Auger decay in the x-ray regime. This x-ray-optical cross-correlation technique provides a straightforward, non-invasive and online means of determining the duration of femtosecond (>40 fs) x-ray pulses.In combination with a theoretical model of the process based on the softphoton approximation, we were able to obtain the LCLS pulse duration and to extract a mean value of the temporal jitter between the optical pulses from a synchronized Ti-sapphire laser and x-ray pulses from the LCLS. We find that the experimentally determined values are systematically smaller than the length of the electron bunches. Nominal electron pulse durations of 175 and 75 fs, as provided by the LCLS control system, yield x-ray pulse shapes of 120 ± 20 fs full-width at half-maximum (FWHM) and an upper limit of 40 ± 20 fs FWHM, respectively. Simulations of the free-electron laser agree well with the experimental results. Contents

The advent of free electron laser (FEL) facilities capable of delivering high intensity pulses in the extreme-UV to X-ray spectral range has opened up a wide vista of opportunities to study and control light matter interactions in hitherto unexplored parameter regimes. In particular current short wavelength FELs can uniquely drive nonlinear processes mediated by inner shell electrons and in fields where the photon energy can be as high as 10 keV and so the corresponding optical period reaches below one attosecond. Combined with ultrafast optical lasers, or simply employing wavefront division, pump probe experiments can be performed with femtosecond time resolution. As single photon ionization of atoms and molecules is by now very well understood, they provide the ideal targets for early experiments by which not only can FELs be characterised and benchmarked but also the natural departure point in the hunt for nonlinear behaviour of atomistic systems bathed in laser fields of ultrahigh photon energy. In this topical review we illustrate with specific examples the gamut of apposite experiments in atomic, molecular physics currently underway at the SCSS test accelerator (Japan), FLASH (Hamburg) and LCLS (Stanford).

Two-color multiphoton ionization of atomic helium was investigated by combining extreme ultraviolet (XUV) radiation from the Free Electron Laser in Hamburg with an intense synchronized optical laser. In the photoelectron spectrum, lines associated with direct ionization and above-threshold ionization show strong variations of their amplitudes as a function of both the intensity of the optical dressing field and the relative orientation of the linear polarization vectors of the two fields. The polarization dependence provides direct insight into the symmetry of the outgoing electrons in above-threshold ionization. In the high field regime, the monochromaticity of the XUV radiation enables the unperturbed observation of nonlinear processes in the optical field. DOI: 10.1103/PhysRevLett.101.193002 PACS numbers: 32.80.Fb, 32.80.Rm Multiphoton single-color ionization in intense optical or infrared laser fields has been the subject of multiple experimental and theoretical studies for more than two decades and is by now a very well understood process (e.g., [1]). The extension of these studies to multiphoton absorption in the photoionization continuum was followed by the discovery that high order harmonics of the fundamental laser frequency are emitted in the extreme ultraviolet (XUV) when a strong femtosecond optical laser pulse interacts with a gas jet (e.g., [2,3]). The combination of different wavelengths, one in the XUV and the other in the visible or near infrared, opens new opportunities. It has recently permitted the investigation of above-threshold ionization (ATI) as the result of the combined interaction of both fields [4][5][6]. In this case the dominant contribution comes from processes in the course of which the emitted electron exchanges photons with the dressing laser field via stimulated emission (or absorption) resulting in a comb of sidebands disposed on both sides of the main photoelectron line.Theoretical studies have established that the sideband intensity depends on the electron kinetic energy as well as on the strength and polarization state of the optical laser field [7]. Fitting theoretical profiles to the measured sideband signals should yield the main parameters which govern the photon-atom interaction in this regime. For example, changing the polarization of either of the radiation beams gives rise to ''dichroic effects'' in the photoelectron spectrum. It therefore opens the possibility to control the relative contributions of photoionization channels with different angular momenta.This approach has been extensively used in studies of atomic ionization by weak monochromatic radiation from synchrotrons and continuous lasers, where at least one resonant intermediate state is involved, and the basic photon-electron interaction is completely dominated by this resonant excitation [8]. The use of high harmonic XUV sources to generate similar processes in the nonresonant continuum is complicated by very difficult analysis, since contributions from several harmonics and their mutual interferenc...

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

Two-color above threshold ionization of helium and xenon has been used to analyze the synchronization between individual pulses of the femtosecond extreme ultraviolet ͑XUV͒ free electron laser in Hamburg and an independent intense 120 fs mode-locked Ti:sapphire laser. Characteristic sidebands appear in the photoelectron spectra when the two pulses overlap spatially and temporally. The cross-correlation curve points to a 250 fs rms jitter between the two sources at the experiment. A more precise determination of the temporal fluctuation between the XUV and infrared pulses is obtained through the analysis of the single-shot sideband intensities.