Parameter-free calculation of response functions in time-dependent density-functional theory.
We have established and implemented a fully ab initio method which allows one to calculate optical absorption spectra, including excitonic effects, without solving the cumbersome Bethe-Salpeter equation, but obtaining results of the same precision. This breakthrough has been achieved in the framework of time-dependent density-functional theory, using new exchange-correlation kernels f(xc) that are free of any empirical parameter. We show that the same excitonic effects in the optical spectra can be reproduced through different f(xc)'s, ranging from frequency-dependent ones to a static one, by varying the kernel's spatial degrees of freedom. This indicates that the key quantity is not f(xc), but f(xc) combined with a response function. We present results for the optical absorption of bulk Si and SiC in good agreement with experiment, almost indistinguishable from those of the Bethe-Salpeter approach.
Sottile
Francesco
F
Laboratoire des Solides Irradiés UMR 7642, CNRS-CEA/DSM, Ecole Polytechnique, F-91128 Palaiseau, France.
Olevano
Valerio
V
Reining
Lucia
L