Long-range charge-transfer excitations pose a major challenge for time-dependent density-functional approximations. We show that spin-symmetry breaking offers a simple solution for molecules composed of open-shell fragments, yielding accurate excitations at large separations when the acceptor effectively contains one active electron. Unrestricted exact-exchange and self-interaction-corrected functionals are performed on one-dimensional models and on the real LiH molecule within the pseudopotential approximation to demonstrate our results.
|Original language||English (US)|
|Journal||Physical Review A - Atomic, Molecular, and Optical Physics|
|State||Published - Apr 5 2011|
All Science Journal Classification (ASJC) codes
- Atomic and Molecular Physics, and Optics