Estimating excitonic effects in the absorption spectra of solids: problems and insight from a guided iteration scheme.

@article{Rigamonti2015EstimatingEE,
  title={Estimating excitonic effects in the absorption spectra of solids: problems and insight from a guided iteration scheme.},
  author={Santiago Rigamonti and Silvana Botti and Val{\'e}rie V{\'e}niard and Claudia Draxl and Lucia Reining and Francesco Sottile},
  journal={Physical review letters},
  year={2015},
  volume={114 14},
  pages={
          146402
        }
}
A major obstacle for computing optical spectra of solids is the lack of reliable approximations for capturing excitonic effects within time-dependent density functional theory. We show that the accurate prediction of strongly bound electron-hole pairs within this framework using simple approximations is still a challenge and that available promising results have to be revisited. Deriving a set of analytical formulas we analyze and explain the difficulties. We deduce an alternative approximation… Expand
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References

SHOWING 1-10 OF 68 REFERENCES
DENSITY FUNCTIONAL THEORY OF TIME-DEPENDENT PHENOMENA
A density-functional formalism comparable to the theory of Hohenberg, Kohn and Sham is developed for electronic systems subject to time-dependent external fields. The formalism leads to a set ofExpand
Nuclear instruments and methods in physics research section B : beam interactions with materials and atoms
The impact-induced deposition of Al13 clusters with icosahedral structure on Ni(0 0 1) surface was studied by molecular dynamics (MD) simulation using Finnis–Sinclair potentials. The incident kineticExpand
Phys
  • Rev. Lett. 107, 186401
  • 2011
L
  • Reining, H.- C. Weissker, A. Rubio, G. Onida, R. Del Sole, and R. W. Godby, Phys. Rev. B 69, 155112
  • 2004
Phys
  • Rev. B 69, 155112
  • 2004
Rep
  • Prog. Phys. 70, 357
  • 2007
Rev
  • Mod. Phys. 74, 601
  • 2002
Phys
  • Rev. Lett. 52, 997
  • 1984
Condens
  • Matter 26, 363202
  • 2014
Journal of Physics: Condensed Matter 26
  • 363202
  • 2014
...
1
2
3
4
5
...