Journal of Chemical Physics, Vol.117, No.4, 1575-1588, 2002
Polyatomic molecules in strong laser fields: Nonadiabatic multielectron dynamics
We report the observation and characterization of a new nonresonant strong field ionization mechanism in polyatomic molecules: Nonadiabatic multi-electron (NME) dynamics. The strong field response of a given molecule depends on important properties such as molecular geometry and bonding, the path length of delocalized electrons and/or ionization potential as well as on basic laser pulse parameters such as wavelength and intensity. Popular quasi-static tunnelling models of strong field molecular ionization, based upon the adiabatic response of a single active electron, are demonstrated to be inadequate when electron delocalization is important. The NME ionization mechanism greatly affects molecular ionization, its fragmentation and its energetics. In addition, multi-electron effects are shown to be present even in the adiabatic long wavelength limit.