Ab initio calculation of the nonlinear susceptibility χ⁽²⁾ of a crystal surface

Issue title: Computational aspects of electric polarizability calculations: Atoms, Molecules and clusters, Part I

Article type: Research Article

Authors: Baraille, Isabelle | Darrigan, Clovis | Rérat, Michel^{; *}

Affiliations: Laboratoire de Chimie Théorique et Physico-Chimie Moléculaire, UMR 5624 – FR2606, Université de Pau, 64000 Pau, France

Correspondence: [*] Corresponding author. E-mail: [email protected].

Abstract: The polarizability and first hyperpolarizability of a crystal surface are calculated from a sum over states method using crystalline orbitals of the CRYSTAL program. The linear and nonlinear optical properties of the (001) LiF surfaces are evaluated layer by layer, showing that the response of inner layers to an electric field tends effectively to the bulk response value while the χ(2) susceptibility components responsible of second harmonic generation (SHG) are no longer equal to zero at the surface of the crystal.

Keywords: quantum chemistry, surface, nonlinear optics, lithium fluoride

DOI: 10.3233/JCM-2004-4312

Journal: Journal of Computational Methods in Sciences and Engineering, vol. 4, no. 3, pp. 357-364, 2004