Transient degenerate four-wave mixing in molecular systems

Abstract

The dependence of the degenerate four-wave mixing (DFWM) signal on laser intensity, molecular transition moment and molecular concentration were examined experimentally by taking the iodine molecule (l2) as a testing example. The experimental results will be interpreted by a non-steady-state DFWM theory, an extension of the non-degenerate two-level system previously proposed. The distinctive physical feature of this mechanism is that the present observation is the result of non-stationary evolution of the excited-state population, in contrast to the conventional theory based on the steady-state treatment. In this study, we have also taken into account the magnetic sub-levels of molecular rovibronic quantum states. The non-steady-state model we developed in this paper is applicable to fast pump and slow relaxation conditions, thus being more suitable for gas-phase systems than the condensed-phase where fast relaxations usually take place.