title: Calculation of the static electronic second hyperpolarizability or chi(3) tensor of three-dimensional periodic compounds with a local basis set.
abstract: The coupled perturbed Hartree-Fock (CPHF) method for evaluating static first (beta) and second (gamma) hyperpolarizability tensors of periodic systems has recently been implemented in the CRYSTAL code [Bishop et al., J. Chem. Phys. 114, 7633 (2001)]. We develop here an efficient and accurate computational protocol, along with the local basis sets needed for first and second row atoms. Application is made to several high symmetry three-dimensional systems including one (pyrope) with an 80 atom unit cell. CPHF second-order hyperpolarizabilities substantially undershoot experimental values, due to an overestimate of the band gap, but trends are satisfactorily reproduced for beta as well as gamma.
authors.affiliation: Dipartimento di Scienze e Tecnologie Avanzate, Universita del Piemonte Orientale, Viale T. Michel 11, 15121 Alessandria, Italy. roberto.orlando@unito.it
authors.forename: Roberto
authors.initials: R
authors.lastname: Orlando
authors.forename: Mauro
authors.initials: M
authors.lastname: Ferrero
authors.forename: Michel
authors.initials: M
authors.lastname: Rérat
authors.forename: Bernard
authors.initials: B
authors.lastname: Kirtman
authors.forename: Roberto
authors.initials: R
authors.lastname: Dovesi