Femtosecond laser-induced Coulomb explosion imaging

We review recent progress in the field of Coulomb imaging using femtosecond laser pulses of variable length, referred to as Femtosecond Multiple Pulse Length Spectroscopy (FEMPULS). This method introduces a multi-dimensional approach to the study of the molecular dynamics of the multiply ionized triatomic molecules: CO₂, OCS, and N₂O. We describe the experimental setup used and the approaches needed to optimize the multi-particle detection, coincidence technique. The results show the degree of high resolution imaging which can be achieved with few cycle pulses, and how the onset of charge resonance enhanced ionization (CREI) can be observed as pulse length is increased. By coupling pulse length variation with Dalitz and Newton plotting techniques, stepwise processes can be identified for all three molecules, giving insight into the dynamics, particularly on the 3+ state, which has been revealed as the doorway state to CREI. Finally, in the case of OCS, pulse length variation is shown to have the potential as a control mechanism, as it modulates the ratio of stepwise to concerted processes.