The Cotton-Mouton effect of gaseous CO2, N2O, OCS, and CS2. A cubic response multiconfigurational self-consistent field study

The hypermagnetizability and the hypermagnetizability anisotropy of CO2, N2 O, OCS, and CS2 are computed at a wavelength of 632.8 nm using cubic respon se theory with multiconfigurational self-consistent field wave functions. T he anisotropies of the electric dipole polarizability and of the magnetizab ility are also obtained. This allows us to study the temperature dependence of the Cotton-Mouton constant for all four molecules and thus to compare t o the results of the experimental study by Kling and Huttner [Chem. Phys. L ett. 90, 207 (1984)]. We also assess the importance of pure and zero-point vibrational effects on the relevant molecular properties. In particular, we show that for CO2, OCS, and CS2, the pure vibrational effects to the hyper magnetizability anisotropy can be even more important than the electronic c ontribution. (C) 2001 American Institute of Physics.