Generalized local frame-transformation theory for ultralong-range Rydberg molecules
P. Giannakeas, Matthew T. Eiles, F. Robicheaux, Jan M. Rost
Abstract
A detailed theoretical framework for highly excited Rydberg molecules is developed based on the generalized local frame transformation. Our approach avoids the use of pseudopotentials and yields analytical expressions for the body-frame reaction matrix. The latter is used to obtain the molecular potential energy curves, but equally it can be employed for photodissociation, photoionization, and other processes. To illustrate the reliability and accuracy of our treatment we consider the ${\mathrm{Rb}}^{*}$-Rb Rydberg molecule and compare our treatment with state-of-the-art alternative approaches. As a second application, the present formalism is used to reanalyze the vibrational spectra of ${\mathrm{Sr}}^{*}$-Sr molecules, providing additional physical insight into their properties and a comparison of our results with corresponding measurements.