BODY-FRAME COHERENCES AND ROTATIONAL-ELECTRONIC WAVE-PACKET DYNAMICS OF CAF IN NON-PENETRATING RYDBERG STATES

Author Institution: Department of Chemistry, Massachusetts Institute of TechnologyThe time dependent wave-packet dynamics of a non-penetrating Rydberg electron in a body-frame coherent superposition state of CaF is investigated using an effective Hamiltonian model. Our results indicate that the information about the ioncore quadrupole moment can be directly inferred by monitoring the time required for the Rydberg wave-packet to return to its initial state. The effective Hamiltonian model is then embedded in a time-dependent multichannel quantum defect theory model which has the advantage of capturing all molecular resonances(i.e. the short range electron-nuclear scattering processes which lead to rotational transitions of the core) in a single, unified calculation. Both theories can be applied to quantitatively describe the data that will be provided from the ongoing time-domain experiments. Extensions to include vibrational interactions, predicted by the R-dependence of the quantum defect matrix elements, are possible and constitute the natural future directions in this work