Measurements of a single shot femtosecond laser pump-probe technique on sub
stituted benzalacetones are reported. The technique is based on counter pro
pagating femtosecond laser pulses in a supersonic beam of low density of sa
mple molecules and simultaneous probe detection by ion or fragment ion form
ation through a reflectron time-of-flight mass spectrometer, It will be sho
wn that the range of the pump-probe delays covers the time span between 100
fs and 10 ps depending on the pulse width of the laser used and the stabil
ity of the voltages of the mass spectrometer, The application of this techn
ique to medium-sized organic molecules reveals some insight into the electr
on transfer process during ionisation through a 1 + 1 multi-photon absorpti
on procedure. Furthermore it is demonstrated that this technique is also ap
plicable to the investigation of ultra-fast isomerisation and fragmentation
processes.