The goal to control short-wavelength radiation for the investigation and manipulation of ultrafast dynamics in quantum systems coevolves with the growing availability of extreme-ultraviolet (XUV) and x-ray sources from high-harmonic generation and free-electron lasers. Here, we present an XUV spatio-spectral phase modulator based on an intense XUV laser beam propagating through an optically thick resonant target, introducing dispersion profile variations around the resonance both perpendicular to and along the laser propagation direction. The resulting dipole radiation gets spectrally reshaped and becomes more divergent as compared to the original beam in the far field. As an experimental demonstration, the intense-XUV-induced double-peak off-axis structure in the far-field spectrum obtained at the Free-Electron Laser in Hamburg (FLASH) shows indications of the underlying XUV-driven Rabi dynamics and resonant pulse propagation effects. The presented work highlights a ubiquitous phenomenon occurring when an intense laser beam passes through a resonant medium.

The photophysics of nucleobases has been the subject of both theoretical and experimental studies over the past decades due to the challenges posed by resolving the steps of their radiationless relaxation dynamics, which cannot be described in the framework of the Born-Oppenheimer approximation (BOA). In this context, the ultrafast dynamics of 2-thiouracil has been investigated with a time-resolved NEXAFS study at the Free Electron Laser FLASH. Near Edge X-ray Absorption Fine Structure spectroscopy (NEXAFS) can be used to observe electronic transitions in ultrafast molecular relaxation. We performed time-resolved UV-pump/X-ray probe absorption measurements at the sulfur 2s (L1) and 2p (L2/3) edges. We are able to identify absorption features corresponding to the S2 (ππ*) and S1 (nπ*) electronic states. We observe a delay of 102 ± 11 fs in the population of the nπ* state with respect to the initial optical excitation and interpret the delay as the time scale for the S2 → S1 internal conversion. We furthermore identify oscillations in the absorption signal that match a similar observation in our previous X-ray photoelectron spectroscopy study on the same molecule.

The relaxation processes in atomic xenon following core ionization of the 4d and 4p subshells by extreme ultraviolet (XUV) pulses from a free-electron laser (FLASH) are investigated using ion time-of-flight spectroscopy. We compare the dynamics following ionization and Auger-Meitner decays at 90-eV photon energy, i.e., near the giant resonance, with those at 160 eV, near the Cooper minimum, where cross sections for photoionization of the 4d and 4p subshells are similar. Final states with charges higher than 4 show signatures of sequential absorption of two XUV photons, followed by subsequent Auger-Meitner decay. The averaged lifetimes of some important excited states are measured in a two-color XUV-pump-near-infrared-probe experiment. A transient enhancement in the ion yield of Xe5+ with an average lifetime of (49 +/- 3) fs is obtained, attributed to transient intermediate states following the decay of 4d double-core-hole states.

The temporal stability of laser pulses after a high-energy compression stage using a multi-pass cell with transport beamline was investigated, resulting in correctable ~1 ps long-term drift, and 11 fs residual jitter (10 s integration).

The electronic and nuclear dynamics inside molecules are essential for chemical reactions, where different pathways typically unfold on ultrafast timescales. Extreme ultraviolet (XUV) light pulses generated by free-electron lasers (FELs) allow atomic-site and electronic-state selectivity, triggering specific molecular dynamics while providing femtosecond resolution. Yet, time-resolved experiments are either blind to neutral fragments or limited by the spectral bandwidth of FEL pulses. Here, we combine a broadband XUV probe pulse from high-order harmonic generation with an FEL pump pulse to observe dissociation pathways leading to fragments in different quantum states. We temporally resolve the dissociation of a specific O2+ state into two competing channels by measuring the resonances of ionic and neutral fragments. This scheme can be applied to investigate convoluted dynamics in larger molecules relevant to diverse science fields.

Within the FLASH2020+ upgrade, the pump-probe laser capabilities of the extreme ultraviolet and soft x-ray free-electron laser (XFEL) FLASH in Hamburg will be extended. In particular, providing wavelength tunability, shorter pulse durations, and reduced arrival time jitter will increase the scientific opportunities and the time resolution for the XFEL-optical laser pump-probe experiments. We present here a novel concept for the pump-probe laser at FLASH that is based on the post-compression of picosecond pulses emitted from high-power Ytterbium:YAG slab amplifiers. Flexible reduction of the pulse duration is facilitated by spectral broadening in pressure-tunable multi-pass cells. As an application, we show the pumping of a commercial optical parametric amplifier with 150 fs post-compressed pulses. By means of an additional difference frequency generation stage, tunable spectral coverage from 1.3 to 16 μm is reached with multi-μJ, sub-150 fs pulses. Finally, a modular reconfiguration approach to the optical setups close to the free-electron laser instruments is implemented. This enables fast installation of the nonlinear frequency converters at the end stations for user operation and flexibility between different instruments in the two experimental halls.

The majority of user experiments at the high repetition-rate free electron laser (FEL) facility FLASH are of pump-probe type, combining the extreme ultraviolet (XUV) or soft x-ray radiation from the FEL with ultrashort pulses generated by optical lasers. In this contribution, we demonstrate the advantages of using high-power Yb:YAG lasers with subsequent nonlinear pulse compression stages based on multi-pass cells (MPC). The approach enables the combination of hundreds of kHz to MHz repetition-rates, hundreds of watts of average powers and excellent intensity stabilities. We present the characteristics of the MPC-based pump-probe laser at the FLASH plane-grating beamlines. Furthermore, we report pulse compression to 8.2 fs pulse duration and the seeding of an optical parametric amplifier generating mid-IR radiation tunable from 1.4 µm to 16 µm.

We describe the ultrafast laser systems which are currently planned, under construction or installed to operate the high repetition rate free electron laser facilities FLASH and European XFEL.

We report on the experimental demonstration of the laser induced aerosol formation driven by fs high-energy mid-IR pulses and facilitated by resonance excitation and subsequent oxidation of the ambient volatile organic compounds.

The conversion of photon energy into other energetic forms in molecules is accompanied by charge moving on ultrafast timescales. We directly observe the charge motion at a specific site in an electronically excited molecule using time-resolved x-ray photoelectron spectroscopy (TR-XPS). We extend the concept of static chemical shift from conventional XPS by the excited-state chemical shift (ESCS), which is connected to the charge in the framework of a potential model. This allows us to invert TR-XPS spectra to the dynamic charge at a specific atom. We demonstrate the power of TR-XPS by using sulphur 2p-core-electron-emission probing to study the UV-excited dynamics of 2-thiouracil. The new method allows us to discover that a major part of the population relaxes to the molecular ground state within 220-250 fs. In addition, a 250-fs oscillation, visible in the kinetic energy of the TR-XPS, reveals a coherent exchange of population among electronic states.

Post-compression of ultra-short laser pulses via self-phase modulation is routinely employed for the generation of laser pulses with optical bandwidths reaching far beyond the laser gain limitations. While high compression factors can be routinely achieved, the compressed pulses typically suffer from temporal quality degradation. We numerically and experimentally analyze the deterioration of different measures of temporal quality with increasing compression factor and show how appropriate dispersion management and cascading of the post-compression process can be employed to limit the impact of this effect. The demonstrated saturation of pulse quality degradation at large compression factors puts novel femtosecond laser architectures based on post-compressed pico- or even nanosecond laser systems in sight.

The serrodyne principle enables an electromagnetic signal to be frequency shifted by applying a linear phase ramp in the time domain. This phenomenon has been exploited to frequency shift signals in the radiofrequency, microwave and optical regions of the electromagnetic spectrum over ranges of up to a few gigahertz, for example, to analyse the Doppler shift of radiofrequency signals for noise suppression and frequency stabilization. Here we employ this principle to shift the centre frequency of high-power femtosecond laser pulses over a range of several terahertz with the help of a nonlinear multi-pass cell. We demonstrate our method experimentally by shifting the central wavelength of a state-of-the-art 75 W frequency comb laser from 1,030 nm to 1,060 nm and to 1,000 nm. Furthermore, we experimentally show that this wavelength-shifting technique supports coherence characteristics at the few hertz-level while improving the temporal pulse quality. The technique is generally applicable to wide parameter ranges and different laser systems, enabling efficient wavelength conversion of high-power lasers to spectral regions beyond the gain bandwidth of available laser platforms.

Nonlinear pulse post-compression, mainly enabled by self-phase modulation (SPM), opens new avenues towards high peak power laser pulses at high average power while bypassing the need for a gain medium with large bandwidth. However, SPM-induced spectral broadening typically introduces spectral amplitude modulations as well as a chirp of third and higher orders, limiting the temporal contrast of the compressed pulse. While some recent works address this issue and discuss mitigation strategies [1] , [2] , not much attention has been devoted to the physical processes and limitations that determine the temporal contrast of post-compressed pulses. As novel compression techniques expand the achievable compression ratio [3] , it is increasingly important to fully understand the underlying pulse quality limitations. Here, we outline the role of two important characteristics — dispersion and compression ratio — on the temporal quality of post-compressed pulses. Using both numerical simulations as well as experimental tests employing a gas-filled multi-pass cell (MPC), we study the temporal contrast of post-compressed pulses over large compression-ratio and dispersion range. Using a 730 fs input pulse we were able to generate a 55 fs post-compressed pulse with up to 78% energy contained in the main compressed pulse (defined via the first local minima near the highest peak) against its picosecond background.

This paper reports on nonlinear spectral broadening of 1.1 ps pulses in a gas-filled multi-pass cell to generate sub-100 fs optical pulses at 1030 nm and 515 nm at pulse energies of 0.8 mJ and 225 µJ, respectively, for pump-probe experiments at the free-electron laser FLASH. Combining a 100 kHz Yb:YAG laser with 180 W in-burst average power and a post-compression platform enables reaching simultaneously high average powers and short pulse durations for high-repetition-rate FEL pump-probe experiments.

We present high-power Yb:YAG lasers combined with nonlinear pulse compression in multi-pass cells. We show that these are suitable for integration in FEL facilities in terms of pulse stability, jitter, temporal contrast and intra-burst behaviour.

We show that a combination of OPCPA and cascaded SFM can efficiently generate 100 µJ, MHz repetition rate, 50 fs, tunable pulses from 279 nm to 317 nm for seeding superconducting X-ray free electron lasers.

Since its first demonstration, laser induced aerosol formation (LIAF) has been studied in various environmental conditions and laser parameters. LIAF driven by UV and near-IR lasers mainly relies on the nitrogen photo-oxidative chemistry, leading to the production of hygroscopic H N O 3 , which stabilizes the growth of aerosol nanoparticles. Mid-IR lasers were expected to be drastically less effective for LIAF, due to their much lower multiphoton photodissociation and ionization rates. Here, we report on the observation of surprisingly high yields of nanometric and sub-µm aerosol formation driven by mid-IR laser pulses, which cannot be explained by the H N O 3 -pathway. We hereby evidence a new mechanism of aerosol stabilization and growth, based on the resonant excitation of volatile organic compounds (VOCs) by mid-IR pulses whose spectrum is broadened during filamentation.

We present the design, integration, and operation of the novel vacuum ultraviolet (VUV) beamline installed at the free-electron laser (FEL) FLASH. The VUV source is based on high-order harmonic generation (HHG) in gas and is driven by an optical laser system synchronized with the timing structure of the FEL. Ultrashort pulses in the spectral range from 10 to 40 eV are coupled with the FEL in the beamline FL26, which features a reaction microscope (REMI) permanent endstation for time-resolved studies of ultrafast dynamics in atomic and molecular targets. The connection of the high-pressure gas HHG source to the ultra-high vacuum FEL beamline requires a compact and reliable system, able to encounter the challenging vacuum requirements and coupling conditions. First commissioning results show the successful operation of the beamline, reaching a VUV focused beam size of about 20 µm at the REMI endstation. Proof-of-principle photo-electron momentum measurements in argon indicate the source capabilities for future two-color pump-probe experiments.

High energy tunable ultrafast UV pulses are of great interest for a variety of applications. These pulses are also required for high repetition rate, fully coherent UV seeded free electron lasers [1] . In the absence of proper laser gain materials, optical parametric chirped pulse amplification (OPCPA) is considered as a foremost technique to generate high power tunable ultra-short laser pulses in various spectral ranges [2] . A typical example is the broadband green pumped OPCPA system driven by frequency doubled Ytterbium based chirped pulse laser amplifiers (CPA). The excellent power scalability of the OPCPAs allows generation of multi-millijoule, few femtosecond pulses with hundreds of watts of average power harnessing high energy and repetition rate commercially available CPA pump systems [3] . The absence of proper nonlinear crystals hinders operating OPCPAs directly in the UV spectral range. Therefore, frequency doubling, tippling or quadrupling of conventional OPCPAs are the usual techniques of generating tunable UV pulses. However, these schemes suffer from the strong two-photon absorption, narrow phase matching bandwidth, and non-linear phase transfer to UV range. As a consequence, for ultra-short pulses the maximum conversion efficiency of such schemes is typically limited to below 10%, and usually accompanied by pulse compression complications.