Wave-packet model for excitation by ultrashort pulses

In this paper we discuss the excitation of a localized molecular ground-state wave function by a short laser pulse. With a one-dimensional approach we show when it is possible to excite a considerable fraction of the ground state without too much distortion of the shape of the wave packet. This is of interest in time-resolved molecular experiments where an excited wave packet is often taken as the initial state. We solve the two coupled wave equations numerically and compare results to an analytical approximation based on the Rosen-Zener model. The validity of the approximation and its breakdown is considered in detail. Special attention is paid to the effect of lengthening the pulse duration and the consequences of the accompanying number of Rabi flops occurring in the area theorem. When the approximation breaks down, the wave packet becomes distorted and spread out, but there are still interesting coherence effects due to the interplay between the Rabi flopping and the molecular dynamics; these are displayed and discussed. Finally, the relationship to other works and possible generalizations are presented.