High-repetition-rate and high-photon-flux 70 eV high-harmonic source for coincidence ion imaging of gas-phase molecules.

Unraveling and controlling chemical dynamics requires techniques to image structural changes of molecules with femtosecond temporal and picometer spatial resolution. Ultrashort-pulse x-ray free-electron lasers have significantly advanced the field by enabling advanced pump-probe schemes. There is an increasing interest in using table-top photon sources enabled by high-harmonic generation of ultrashort-pulse lasers for such studies. We present a novel high-harmonic source driven by a 100 kHz fiber laser system, which delivers 1011 photons/s in a single 1.3 eV bandwidth harmonic at 68.6 eV. The combination of record-high photon flux and high repetition rate paves the way for time-resolved studies of the dissociation dynamics of inner-shell ionized molecules in a coincidence detection scheme. First coincidence measurements on CH3I are shown and it is outlined how the anticipated advancement of fiber laser technology and improved sample delivery will, in the next step, allow pump-probe studies of ultrafast molecular dynamics with table-top XUV-photon sources. These table-top sources can provide significantly higher repetition rates than the currently operating free-electron lasers and they offer very high temporal resolution due to the intrinsically small timing jitter between pump and probe pulses.

Femtosecond crystallographic experiment in wide-bandgap LiF crystal.

We report a femtosecond crystallographic study of the dependence of the free-carries generation to the alignment of a crystalline sample to the laser polarization. The probe pulse transmission exhibits a π/2 modulation that is shown to be correlated with the direction dependence of the effective electron mass. This observation suggests that nonlinear ionization is the first channel for free electron generation during the laser pulse. Moreover, the temporal evolution of the probe pulse transmission indicates the dominance of the avalanche ionization and that nonlinear ionization provides the initial seed electrons for avalanche."

Thresholds of plasma formation in silicon identified by optimizing the ablation laser pulse form.

Using an evolutionary algorithm combined with pulse shaping, we have identified that rapid plasma formation in Silicon can occur already at a fluence of about 150 mJ/cm2 if a substantial part of the laser energy is deposited efficiently around 200 fs after an exciting laser pulse. Nonthermal solid-to-liquid phase transition leads to the increase of the deposited energy in the material. Highly charged ions have been observed in the mass spectrum. While the pulse optimization procedure allowed us to identify the plasma formation, further experiments where the influence of the laser pulse width on the ablation yield was studied and Two-Pulse-Correlation experiments provided additional proof for the appearance of rapid plasma formation.