From anisotropy of dielectric tensors to birefringence: a quantum mechanics approach

Abstract

The way quantum mechanical ab initio computer codes allow to compute, through perturbation theory (the so-called SC-CP, self-consistent coupled-perturbed scheme), many properties resulting from the interaction of the electric field with a crystalline system is illustrated. The polarizability, which leads to the dielectric tensors as well as to the refractive indices and to the birefringence of materials, is the simplest on this list. Higher order tensors, like the first and second hyperpolarizabilities, can be obtained as well with the CRYSTAL code here used. These properties, resulting from the Taylor expansion of the total energy of the solid as a function of the electric field, belong to a large family of phenomena generated by combining in different ways the frequencies of the fields. Second-harmonic generation (SHG), Pockels effect, intensity-dependent refractive index (IDRI), and other quantities now accessible to experiment can be computed at a relatively low cost and with high accuracy.