We put forward a co-axial pump(optical)-probe(X-rays) experimental concept and show performance of the optical component. A Bessel beam generator with a central 100 micrometers-diameter hole (on the optical axis) was fabricated using femtosecond (fs) laser structuring inside a silica plate. This flat-axicon optical element produces a needle-like axial intensity distribution which can be used for the optical pump pulse. The fs-X-ray free electron laser (X-FEL) beam of sub-1 micrometer diameter can be introduced through the central hole along the optical axis onto a target as a probe. Different realisations of optical pump are discussed. Such optical elements facilitate alignment of ultra-short fs-pulses in space and time and can be used in light-matter interaction experiments at extreme energy densities on the surface and in the volume of targets. Full advantage of ultra-short 10 fs X-FEL probe pulses with fs-pump(optical) opens an unexplored temporal dimension of phase transitions and the fastest laser-induced rates of material heating and quenching. A wider field of applications of fs-laser-enabled structuring of materials and design of specific optical elements for astrophotonics is presented.
Coherent diffraction imaging (CDI) using synchrotron radiation, X-ray free electron lasers (X-FELs), high harmonic generation, soft X-ray lasers, and optical lasers has found broad applications across several disciplines. An active research direction in CDI is to determine the structure of single particles with intense, femtosecond X-FEL pulses based on diffraction-before-destruction scheme. However, single-shot 3D structure determination has not been experimentally realized yet. Here we report the first experimental demonstration of single-shot 3D structure determination of individual nanocrystals using ~10 femtosecond X-FEL pulses. Coherent diffraction patterns are collected from high-index-faceted nanocrystals, each struck by a single X-FEL pulse. Taking advantage of the symmetry of the nanocrystal, we reconstruct the 3D structure of each nanocrystal from a single-shot diffraction pattern at ~5.5 nm resolution. As symmetry exists in many nanocrystals and virus particles, this method can be applied to 3D structure studies of such particles at nanometer resolution on femtosecond time scales.
A scheme for an X-ray free electron laser is proposed, based on a Raman process occurring during the interaction between a moderately relativistic bunch of free electrons, and twin intense short pulse lasers interfering to form a transverse standing wave along the electron trajectories. In the high intensity regime of the Kapitza-Dirac effect, the laser ponderomotive potential forces the electrons into a lateral oscillatory motion, resulting in a Raman scattering process. I show how a parametric process is triggered, resulting in the amplification of the Stokes component of the Raman-scattered photons. Experimental operating parameters and implementations, based both on LINAC and Laser Wakefield Acceleration techniques, are discussed.
Pump-probe experiments combining pulses from a X-ray FEL and an optical femtosecond laser are very attractive for sub-picosecond time-resolved studies. Since the synchronization between the two independent light sources to an accuracy of 100 fs is not yet solved, it is proposed to derive both femtosecond radiation pulses from the same electron bunch but from two insertion devices. This eliminates the need for synchronization and developing a tunable high power femtosecond quantum laser. In the proposed scheme a GW-level soft X-ray pulse is naturally synchronized with a GW-level optical pulse, independent of any jitter in the arrival time of the electron bunches. The concept is based on the generation of optical radiation in a master oscillator-power FEL amplifier (MOPA) configuration. X-ray radiation is generated in an X-ray undulator inserted between the modulator and radiator sections of the optical MOPA scheme. An attractive feature of the FEL amplifier scheme is the absence of any apparent limitations which could prevent operation in the femtosecond regime in a wide (200-900 nm) wavelength range. A commercially available long (nanosecond) pulse dye laser can be used as seed laser.
The capability of generating two intense, femtosecond x-ray pulses with controlled time delay opens the possibility of performing time-resolved experiments for x-ray induced phenomena. We have applied this capability to study the photoinduced dynamics in diatomic molecules. In molecules composed of low-Z elements, textit{K}-shell ionization creates a core-hole state in which the main decay mode is an Auger process involving two electrons in the valence shell. After Auger decay, the nuclear wavepackets of the transient two-valence-hole states continue evolving on the femtosecond timescale, leading either to separated atomic ions or long-lived quasi-bound states. By using an x-ray pump and an x-ray probe pulse tuned above the textit{K}-shell ionization threshold of the nitrogen molecule, we are able to observe ion dissociation in progress by measuring the time-dependent kinetic energy releases of different breakup channels. We simulated the measurements on N$_2$ with a molecular dynamics model that accounts for textit{K}-shell ionization, Auger decay, and the time evolution of the nuclear wavepackets. In addition to explaining the time-dependent feature in the measured kinetic energy release distributions from the dissociative states, the simulation also reveals the contributions of quasi-bound states.
We demonstrate the possibility to run a single-pass free-electron laser in a new dynamical regime, which can be exploited to perform two-colour pump-probe experiments in the VUV/X-ray domain, using the free-electron laser emission both as a pump and as a probe. The studied regime is induced by triggering the free-electron laser process with a powerful laser pulse, carrying a significant and adjustable frequency chirp. As a result, the emitted light is eventually split in two sub-pulses, whose spectral and temporal separations can be independently controlled. We provide a theoretical description of this phenomenon, which is found in good agreement with experiments performed on the FERMI@Elettra free-electron laser.