| In this dissertation the experimental control of molecular reactivity using tailored laser pulses has been presented. Control over the reaction dynamics of various molecular systems has been achieved by using strong tailored laser fields. These control fields are generated in a feedback optimized closed-loop experiment that makes use of a femtosecond pulse shaper and an iterative learning algorithm.;We implement the adaptive control strategy by combining a laser pulse shaping technique with mass spectrometry. Mass spectral distributions have been used to analyze and quantify the ionic fragment yields resulting from the interaction of strong laser fields with neutral gaseous molecular samples.;The successful applications of this control technique, as demonstrated for various molecular samples, emphasize its applicability to polyatomic molecules without the need to calculate the electronic structure of the molecules and the dynamics of field-molecule interactions. Advances in experimental techniques towards simplifying the understanding of the nature strong field control mechanisms, studies on the effects of external laser 171 parameters on the closed-loop control, and application of the optimal field design for discriminating components of a mixture are presented. |
