Sonia Coriani^a, Christof Hättig^a, Poul Jørgensen^a, Antonio Rizzo^b, Kenneth Ruud^c
a Department of Chemistry, Århus University, DK-8000 Århus C, Denmark
^b Istituto di Chimica Quantistica ed Energetica Moleculare del Consiglio Nazionale delle Ricerche, I-56126 Pisa, Italy
^c Department of Chemistry, University of Oslo, P.O. Box 1033 Blindern, N-0316, Oslo, Norway

J. Chem. Phys. 109, 7176-7184 (1998).
(Received 3 June 1998; accepted 28 July 1998)

An ab initio investigation of the electric field gradient induced birefringence of H₂, N₂, C₂H₂ and CH₄ is presented. All linear and non-linear optical properties contributing to the induced anisotropy of the refractive index are computed by means of Coupled Cluster Singles and Doubles response theory. For systems of cubic or icosahedral symmetry, the only non-vanishing contribution to the induced birefringence within the semi-classical approach is due to the frequency-dependent dipole-dipole-quadrupole and dipole-dipole-magnetic dipole hyperpolarizabilities. These hyperpolarizabilities are important for accurate experimental determinations of the molecular quadrupole moment from electric field gradient induced birefringence measurements.

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