Many recent applications of time-dependent density functional theory begin in an initially excited state and propagate it using an adiabatic approximation for the exchange-correlation potential. This, however, inserts the excited-state density into a ground-state approximation. By studying a series of model calculations, we highlight the relevance of initial-state dependence of the exact functional when starting in an excited state, discuss different valid choices of the initial Kohn-Sham state, and explore the errors inherent in the adiabatic approximation that neglects this dependence.
|Original language||English (US)|
|Journal||Physical Review A - Atomic, Molecular, and Optical Physics|
|State||Published - May 22 2012|
All Science Journal Classification (ASJC) codes
- Atomic and Molecular Physics, and Optics