The second hyperpolarizability of the N2 molecule calculated using the approximate coupled cluster triples model CC3

Filip Pawlowskia,*, Poul Jørgensena, Christof Hättigb
aDepartment of Chemistry, Århus University, DK-8000 Århus C, Denmark
bForschungszentrum Karlsruhe, Institute of Nanotechnology, P.O. Box 3640, D-76021 Karlsruhe, Germany

Chem. Phys. Lett. 413, 272-279 (2005).
Received 31 March 2005; revised 24 June 2005. Available online 18 August 2005.

The static and frequency-dependent hyperpolarizabilities of the N-2 molecule have been calculated using the coupled cluster approximate triples model CC3. The CC3 basis-set limit of the hyperpolarizability has been estimated. Considering the zero-point vibrational correction and neglecting the relativistic contributions (which are found to be small) the best estimate of the static hyperpolarizability is 912.9 +/- 4.3 a.u. (the uncertainty of 4.3 a.u. does not account for correlation effects beyond CC3). The effect of triples is important and increases with frequency. The hyperpolarizabilities calculated at the M level agree well with experiment, the discrepancies being of 0.1-2.2%. The largest CC3 calculations employed 326 basis functions. (c) 2005 Elsevier B.V. All rights reserved.

*Corresponding autho. Present Address: Department of Chemisty, University of Oslo, P.O. Box 1033, Blindern N-0315 Oslo, Norway. Fax: +47 22855441. E-mail address (F. Pawlowski).

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