The Cotton-Mouton effect of Neon and Argon gases revisited: a benchmark study using highly correlated coupled cluster wave functions

Antonio Rizzo1, Miháli Kállay2, Jürgen Gauss2, Filip Pawlowski3, Poul Jørgensen3, and Christof Hättig4
1Istituto per i Processi Chimico-Fisici del Consiglio Nazionale delle Ricerche, Area della Ricerca, via G. Moruzzi 1, loc. S. Cataldo, I-56124 Pisa, Italy
2Institut für Physikalische Chemie, Universität Mainz, D-55099 Mainz, Germany
3Department of Chemistry, Århus University, Langelandsgade 140, DK-8000 Århus C, Denmark
4Forschungszentrum Karlsruhe, Institute of Nanotechnology, P.O. Box 3640, D-76021 Karlsruhe, Germany

J. Chem. Phys. 121, 9461-9473 (2004).
(Received 19 July 2004; accepted 19 August 2004)

The Cotton-Mouton effect (magnetic field induced linear birefringence) has been studied for neon and argon using state-of-the-art coupled cluster techniques. The coupled cluster singles, doubles and triples (CCSDT) approach has been used to obtain static benchmark results and the CC3 model with an approximate treatment of triple excitations to obtain frequency-dependent results. In the case of neon the effect of excitations beyond triples has also been estimated via coupled cluster calculations including quadruple excitations (CCSDTQ), pentuple excitations (CCSDTQP), etc. up to the full configuration-interaction level. The results obtained for the anisotropy of the hypermagnetizability Deltaeta(omega), the molecular property that determines the magnetic field induced birefringence of spherically symmetric systems, are Deltaeta=2.89 a.u. for neon and Deltaeta=24.7 a.u. for argon, with a negligible effect of frequency dispersion. For neon we could estimate an absolute error on Deltaeta of 0.1 a.u. The accuracy of these results surpasses that of recently reported experimental data. (C) 2004 American Institute of Physics.

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