Abstract
A generalized Floquet formalism combined with Bloch’s wave operatormethodology is applied to the study of adiabatic versus sudden transportmechanisms in molecular responses to ultrashort and intense laser pulses. Themodel considers the laser pulse as a whole to be periodic, instead of theoptical cycle as in standard Floquet treatments. This leads to a betterunderstanding of the dynamics and a considerable simplification in termsof the number of generalized Floquet eigenstates needed to accuratelydescribe the dynamics. The method is illustrated for the phenomenon ofabove threshold dissociation and inelastic transitions in H2+ inthe presence of ultrashort (a few femtoseconds) and intense (of the order of TW cm−2)laser fields. It is found that, while the dissociation probabilities and fragmentkinetic energy spectra can be accurately described by a single generalized Floqueteigenstate within the adiabatic limit, an accurate description of inelastictransitions requires more than one generalized Floquet state, due to the role ofnon-adiabatic dynamics.
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