The generalized active space concept for the relativistic treatment of electron correlation. III. Large-scale configuration interaction and multiconfiguration self-consistent-field four-component methods with application to UO2

摘要

We present an implementation for large-scale relativistic electronic structure calculations including spin-dependent contributions and electron correlation in a fully variational procedure. The modular implementation of the double group configuration interaction (CI) program into a multiconfiguration self-consistent-field (MCSCF) code allows for the treatment of large CI expansions in both the spinor optimization step and the post-MCSCF dynamic electron correlation step. As an illustration of the potential of the new code, we calculate the spectroscopic properties of the UO2 molecule where we study the ground state and a few excited states in vertical and adiabatic calculations. (c) 2006 American Institute of Physics.