Exploring multiple degrees of freedom in Rydberg wave packets

Recent advances in the study of Rydberg atoms have focused on the control, manipulation and detection of Rydberg wave packets using novel external fields such as half-cycle pulses. The radial degree of freedom has been controlled and used to process information encoded in Rydberg states. However, these previous experiments make use of only a single degree of freedom, restricting the potential of other degrees of freedom for quantum computing in Rydberg atoms. In this dissertation, we explore the control and detection of other degrees of freedom in an electron wave packet, such as the angular momentum quantum number ℓ, the magnetic quantum number m and the electron spin; so that the full range of quantum numbers can participate in information processing.; We first propose an interferometric control of the population of angular momentum states using two time-delayed phase-locked ultrafast laser pulses. The population of arbitrary angular momentum states can be greatly enhanced by optimizing the time delay and the relative phases between two laser pulses. We then qualitatively measure the evolution of angular momentum components in Stark wave packets by a weak half-cycle pulse (HCP). This measurement utilizes a time-delayed HCP and is proved to be effective for detecting various aspects of wave packet dynamics, particularly, the evolution of non-stationary states. The technique relies on the fact that the HCP redistributes the eigenstate populations and induced the population variation which reflects the evolution of eigenstate phases. Finally, we find that the dynamics of m-states could be highly correlated with the internal degree of freedom of the electron, the spin. We study the effect of spin-orbit coupling on the wave packet dynamics and observe the angular precession of a Rydberg wave packet. The population redistribution from p to s states is highly sensitive to the polarization of the HCP and changes with the precession of the electron orbit. We obtain the selection rules and give an intuitive classical interpretation of angular momentum redistribution by an HCP. In short, new dynamics involving multiple degrees of freedom of an electron wave packet are discovered, observed and understood.