Band theory of linear and nonlinear susceptibilities of some binary ionic insulators
Abstract
The linear and nonlinear optical responses in a large number of cubic insulators are studied by means of first-principles local-density calculations. Complete results on band structures, frequency-dependent dielectric functions, and frequency-dependent third-order nonlinear susceptibilities χ(3)(ω) (in the simplest form as the third-harmonic generations) are presented for 27 alkali halides, alkali-earth fluorides, oxides, and sulfides. They are LiF, LiCl, LiBr, LiI, NaF, NaCl, NaBr, NaI, KF, KCl, KBr, KI, RbF, RbCl, RbBr, RbI, CaF2, SrF2, CdF2, BaF2, MgO, CaO, SrO, BaO, MgS, CaS, and SrS. The results are compared with the existing experimental data and other calculations. The effectiveness of using a ``scissor operator'' to correct the gap underestimation in the local-density-approximation theory is assessed. It is shown that the full band-structure approach for the χ(3)(0) calculation in these crystals gives results in very good agreement with experimental data, especially in the anisotropic coefficient of the nonvanishing tensor elements.
- Publication:
-
Physical Review B
- Pub Date:
- July 1995
- DOI:
- 10.1103/PhysRevB.52.1596
- Bibcode:
- 1995PhRvB..52.1596C
- Keywords:
-
- 78.20.Wc;
- 42.65.Ky;
- 42.65.An;
- 78.20.Ci;
- Frequency conversion;
- harmonic generation including higher-order harmonic generation;
- Optical susceptibility hyperpolarizability;
- Optical constants