The Generating-Coordinate Method in Static and Time-Dependent Density Functional Theory*

The generating-coordinate method represents a many-body wave function as a superposition of non-orthogonal Kohn-Sham Slater determinants arising from different Hamiltonians. This method provides additional variational degrees of freedom in the calculation of static and dynamical properties of electronic systems. We present results for atomic ground- and excited- state energies for various choices of generating coordinates. We then apply our variational approach to discuss a particularly challenging problem in TDDFT, the calculation of correlated double-ionization processes. We present results for single- and double-ionization probabilities of a strongly driven two-electron Hooke’s atom.