Configuration Interaction and Autoionization Dynamics

The Configuration Interaction, and a special case, autoionization, are both of fundamental interest as processes within the atom. As models of analogous processes in molecules, they take on greater import. We have studied several aspects of these interactions in two electron atoms towards the long term goal of controlling chemical reactions with light. In a molecule, energy can flow from one mode to another. Similarly, two electrons of an excited atom can arrange themselves in different ways, and energy can move from one configuration to another each time they interact. We have studied the time dependent oscillation between two very different configurations in Barium and examined a related redistribution process. By removing population from a second mode we have used the interaction between two autoionizing states in Calcium to alter the final configuration of the ions. The experiments reported in the appendices include additional studies and attempts to control processes through our understanding of the interactions. We have also developed a technique of rapid variation of delay combined with a lock in amplifier to study some of these subtle effects amidst significant noise.

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