Light-phase-sensitive techniques, such as coherent multidimensional spectroscopy, are well-established in a broad spectral range, already spanning from radio-frequencies in nuclear magnetic resonance spectroscopy to visible and ultraviolet wavelengths in nonlinear optics with table-top lasers. In these cases, the ability to tailor the phases of electromagnetic waves with high precision is essential. Here we achieve phase control of extreme-ultraviolet pulses from a free-electron laser (FEL) on the attosecond timescale in a Michelson-type all-reflective interferometric autocorrelator. By varying the relative phase of the generated pulse replicas with sub-cycle precision we observe the field interference, that is, the light-wave oscillation with a period of 129 as. The successful transfer of a powerful optical method towards short-wavelength FEL science and technology paves the way towards utilization of advanced nonlinear methodologies even at partially coherent soft X-ray FEL sources that rely on self-amplified spontaneous emission.

We report on a direct time-domain measurement of the temporal properties of a seeded free-electron laser pulse in the extreme ultraviolet spectral range. Utilizing the oscillating electromagnetic field of terahertz radiation, a single-shot THz streak-camera was applied for measuring the duration as well as spectral phase of the generated intense XUV pulses. The experiment was conducted at FLASH, the free electron laser user facility at DESY in Hamburg, Germany. In contrast to indirect methods, this approach directly resolves and visualizes the frequency chirp of a seeded free-electron laser (FEL) pulse. The reported diagnostic capability is a prerequisite to tailor amplitude, phase and frequency distributions of FEL beams on demand. In particular, it opens up a new window of opportunities for advanced coherent spectroscopic studies making use of the high degree of temporal coherence expected from a seeded FEL pulse.

In this work we present a reflective split-and-delay unit (SDU) developed for interferometric time-resolved experiments utilizing an (extreme ultraviolet) XUV pump-XUV probe scheme with focused free-electron laser beams. The developed SDU overcomes limitations for phase-resolved measurements inherent to conventional two-element split mirrors by a special design using two reflective lamellar gratings. The gratings produce a high-contrast interference signal controlled by the grating displacement in every diffraction order. The orders are separated in the focal plane of the focusing optics, which enables one to avoid phase averaging by spatially selective detection of a single interference state of the two light fields. Interferometry requires a precise relative phase control of the light fields, which presents a challenge at short wavelengths. In our setup the phase delay is determined by an in-vacuum white light interferometer (WLI) that monitors the surface profile of the SDU in real time and thus measures the delay for each laser shot. The precision of the WLI is 1 nm as determined by optical laser interferometry. In the presented experimental geometry it corresponds to a time delay accuracy of 3 as, which enables phase-resolved XUV pump-XUV probe experiments at free-electron laser (FEL) repetition rates up to 60 Hz.

Fullerene complexes may play a key role in the design of future molecular electronics and nanostructured devices with potential applications in light harvesting using organic solar cells. Charge and energy flow in these systems is mediated by many-body effects. We studied the structure and dynamics of laser-induced multi-electron excitations in isolated C 60 by two-photon photoionization as a function of excitation wavelength using a tunable fs UV laser and developed a corresponding theoretical framework on the basis of ab initio calculations. The measured resonance line width gives direct information on the excited state lifetime. From the spectral deconvolution we derive a lower limit for purely electronic relaxation on the order of t = -+ 10 el 3 5 fs. Energy dissipation towards nuclear degrees of freedom is studied with time-resolved techniques. The evaluation of the nonlinear autocorrelation trace gives a characteristic time constant of t =  400 100 vib fs for the exponential decay. In line with the experiment, the observed transient dynamics is explained theoretically by nonadiabatic (vibronic) couplings involving the correlated electronic, the nuclear degrees of freedom (accounting for the Herzberg-Teller coupling), and their interplay.

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Measurements of the longitudinal phase-space distributions of electron bunches seeded with an external laser were done in order to study the impact of collective effects on seeded microbunches in free-electron lasers. When the collective effects of Coulomb forces in a drift space and coherent synchrotron radiation in a chicane are considered, velocity bunching of a seeded microbunch appears to be a viable alternative to compression with a magnetic chicane under high-gain harmonic generation seeding conditions. Measurements of these effects on seeded electron microbunches were performed with a rf deflecting structure and a dipole magnet which streak out the electron bunch for single-shot images of the longitudinal phase-space distribution. Particle tracking simulations in 3D predicted the compression dynamics of the seeded microbunches with collective effects.

Free-electron lasers are unique sources of intense and ultra-short x-ray pulses that led to major scientific breakthroughs across disciplines from matter to materials and life sciences. The essential element of these devices are micrometer-sized electron bunches with high peak currents, low energy spread, and low emittance. Advanced FEL concepts such as seeded amplifiers rely on the capability of analyzing and controlling the electron beam properties with few-femtosecond time resolution. One major challenge is to extract tomographic slice parameters instead of projected electron beam properties. Here, we demonstrate that a radio-frequency deflector in combination with a dipole spectrometer not only allows for single-shot extraction of a seeded FEL pulse profile, but also provides information on the electron slice emittance and energy spread. The seeded FEL power profile can be directly related to the derived slice emittance as a function of intra-bunch coordinate with a resolution down to a few femtoseconds.

Free-electron lasers (FELs) generate femtosecond XUV and X-ray pulses at peak powers in the gigawatt range. The FEL user facility FLASH at DESY (Hamburg, Germany) is driven by a superconducting linear accelerator with up to 8000 pulses per second. Since 2014, two parallel undulator beamlines, FLASH1 and FLASH2, have been in operation. In addition to the main undulator, the FLASH1 beamline is equipped with an undulator section, sFLASH, dedicated to research and development of fully coherent extreme ultraviolet photon pulses using external seed lasers. In this contribution, the first simultaneous lasing of the three FELs at 13.4 nm, 20 nm and 38.8 nm is presented.