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.
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.
Institute of Theoretical and Computational Chemistry, Heinrich Heine University Düsseldorf, Universitätsstrasse 1, D-40591 Düsseldorf, Germany. timo@theochem.uni-duesseldorf.de
Timo
T
Fleig
Hans Jørgen Aa
HJ
Jensen
Jeppe
J
Olsen
Lucas
L
Visscher