Dynamics of laser-induced desorption from dielectric surfaces on a sub-picosecond timescale

Abstract

Abstract The impact of ultra-short laser pulses induces intensity-dependent non-equilibrium processes in the surface region of dielectric targets, resulting in desorption of surface constituents. We report time-resolved studies on particle ejection from CaF 2 and BaF 2 targets. Pump–probe time-of-flight mass spectrometry (ToF MS) was used to measure the particle yields as a function of the delay time between pairs of sub-damage threshold laser pulses, thus obtaining the temporal dynamics of the laser-excited charged particle emission. In a correlative manner, the positive ion, electron and negative ion desorption yields dependence on the pump–probe delay time reveal a coherence peak around zero delay (similar to a two-pulse autocorrelation), accounting for the increase of the ion yield with laser intensity. Additionally, the measurements reveal a delayed peaks at ∼900 fs (BaF 2 ) and ∼300 fs (CaF 2 ). For comparison, we present time-resolved studies on electron emission from aluminum targets with pump and probe pulses below the damage threshold. The measurements show, again, the autocorrelation peak in the coherence region and an additional increase in the electron yield when the pulses are several picoseconds apart. The autocorrelation could also stand for the dephasing time of the electronic coherence, while the delayed peaks may reveal for the time needed for the collisional energy to be transferred to the lattice. The pump pulse induces a new unstable phase, which is further destabilized by the probe pulse. A corresponding qualitative picture for temporal dynamics of femtosecond (fs) laser-induced particle emission is proposed.