In this thesis, we present work on coherent control of multilevelquantum systems in the strong field limit using shaped ultrafastlaser pulses. In recent years there have been numerous multiphotonabsorption experiments in two,three, and four-level atomic/molecularsystems and many are performed in the limit of weak fields whereperturbation theory is valid. Here, we describe a series ofexperiments aimed at exploring and understanding multiphotontransitions when the exciting field is strong and perturbationtheory breaks down. Our approach to strong field control utilizesboth parameterized scans of various pulse shapes and closed-looplearning control to identify a pulse shape that is optimal forpopulating a target quantum state. With this we will highlight thedifference between sequential population transfer and adiabaticrapid passage in multilevel systems with multiphoton couplingbetween levels. Additionally, we examine strong field control of afour-level atomic interferometer and show how interference in atarget state changes from resonant pathways in the frequency domainto time-domain interference via a singe path.Further, we use shaped femtosecond pulses to demonstrate aphenomenon in which a three-level atom becomes a modulator of anultrafast pulse. The results are based on a pump-probe scheme thatis very similar to Electromagnetically Induced Transparency (EIT).Important dynamics associated with a time-dependent coupling fieldare examined. Lastly, we extend previous work on two-photon drivensuperfluorescence from a shaped ultrafast drive laser and show howstimulated emission near threshold can turn modest coherent controlyields into essentially perfect discrimination between systems wherea control factor of about 104 is achieved between atomic andmolecular species.
The aim to control the internal and external degrees of freedom of quantum systems is of great interest for many fields of physics and chemistry. One opportunity to realize such a coherent control is provided by strong, time depended, external fields. In this work the experimental realization of a model-system is presented. The coherent control of the tunneling dynamics of single atoms by means of a time-periodic, external field is demonstrated. Depending on the parameters of the driving force the tunneling rate can be varied up to a total suppression of the tunneling process in the extreme. This type of dynamical localization is known as "coherent destruction of tunneling". The experimental setup allows a direct access to the tunneling dynamics of single atoms in a double well structure and enables great freedom concerning the parameters. Not only the double well potential, the driving frequency and the driving amplitude can be varied, but also the temporal and spatial symmetry of the driving. A coherent beam of slow, metastable argon atoms serves as source of particles, which can be detected spatially resolved enabling the direct observation of the tunneling dynamics in momentum space.