Application of the coupled-cluster theory to atomic frequency-dependent polarizabilities

Abstract

A time-dependent coupled-cluster approach may be employed to describe dynamic processes of many-electron systems. Atomic properties, such as the frequency-dependent polarizability, can be treated as a response of the system described by the coupled-cluster expansion to an external radiation field. The major difficulty in the realization of such a formalism is to deal with dynamic pair functions. The procedure reported here is to simplify the full set of single- and pair-excitation expansion equations to a subset of equations which includes polarization and relaxation effects to all orders and is solved by using a complete set of discrete basis functions. Calculations of excitation energies and frequency-dependent electric dipole polarizabilities for helium are presented. Application of the procedure to calculate photoionization cross sections is discussed.