Molecular Double Ionization Using Strong Field Few-Cycle Laser Pulses.

We study strong field double ionization of a series of organic molecules by making use of coincidence detection of fragment ions. We measure the double ionization yield as a function of pulse duration, intensity, polarization, and molecular conjugation. For conjugated molecules we find strong enhancement in the double ionization rate over what one would expect on the basis of tunneling or multiphoton ionization rates. Calculations reveal a correlation between the electronic structure of the different molecules and the observed double ionization yields, highlighting the removal of electrons from inner orbitals.

Strong Field Molecular Ionization in the Impulsive Limit: Freezing Vibrations with Short Pulses.

We study strong-field molecular ionization as a function of pulse duration. Experimental measurements of the photoelectron yield for a number of molecules reveal competition between different ionization continua (cationic states) which depends strongly on pulse duration. Surprisingly, in the limit of short pulse duration, we find that a single ionic continuum dominates the yield, whereas multiple continua are produced for longer pulses. Using calculations which take vibrational dynamics into account, we interpret our results in terms of nuclear motion and nonadiabatic dynamics during the ionization process.