Theory and experiments are currently being developed in our laboratory to use tailored light fields to control the dynamics of molecular reactions. We have recently shown theoretically that a properly chirped light pulse can be used to overcome the natural tendency of wave packets to spread on anharmonic molecular potential energy surfaces. The optimal chirp rate can be readily obtained by solving a linear optimal control equation. In this paper we analyze a number of aspects crucial to the success of the experiments. We test the robustness of the optimal electric field with respect to variations in the field parameters (chirp rates, pulse duration, and carrier frequency). We also study the effects of finite temperature by using a thermal vibrational distribution as the initial state in the dynamics. Finally, we describe the experimental apparatus that we plan to use to perform the control experiments, and discuss several technical issues related to synthesizing the optimal field and detecting the focused wave packet. 1993 American Chemical Society.
