A constraint method for variational total energy calculations of electronic excitations within the Kohn-Sham scheme
POSTER
Abstract
We propose a general constraint on the occupations of single-particle orbitals within (hybrid) density-functional theory that allows a variational total energy formulation for extended systems containing arbitrary electronic excitations. This method is simple to implement and is ideal for studying structural relaxations and molecular-dynamics simulations in the presence of excitations since accurate forces can be calculated via the Hellman-Feynman theorem.
*This work performed under the auspices of the U.S. Department of Energy by LLNL under Contract DE-AC52-07NA27344 with support from the National Nuclear Security Administration (NNSA) office of Non-proliferation Research and Development (NA-22)