An efficient method to study highly excited states at the ab initio level and application to ultralong Rydberg CsNe...

An efficient method to study highly excited states at the ab initio level has been introduced and applied to ultralong Rydberg CsNe molecules. Vibrational properties of Rydberg CsNe molecules are investigated on corresponding potential energy curves obtained by perturbation theory. The Rydberg CsNe molecules are associated with a Rydberg Cs(ns∕np) atom (n = 20-60) and a ground state Ne((1)S0) atom. The starting point for the perturbation treatment of corresponding Rydberg molecular potential energy curves is to generate accurate atomic Rydberg states from realistic ab initio effective core potential. According to the authors' knowledge this is a good reference for ultralong range molecules (order of 1000 Bohr radii) to be studied at the ab initio level.