Basis set and electron correlation effects on the first and second static hyperpolarizability of SO2

Accurate values are reported for the static hyperpolarizability of SO2. We have obtained near-Hartree-Fock SCF values of mu(z) = -0.7916 e a(0) for th e dipole moment, <(alpha)over bar> = 23.59 and Delta alpha = 11.73 e(2) a(0 )(2) E-h(-1) for the mean and the anisotropy of the dipole polarizability, <(beta)over bar> = 35.0 e(3) a(0)(3) E-h(-2) for the mean first and <(gamma )over bar> = 2061 e(4) a(0)(4) E-h(-3) for the mean second dipole hyperpola rizability. Our CCSD(T) values for the election correlation correction to t hese properties are -0.1676 e a(0), 2.25 and 1.38 e(2) a(0)(2) E-h(-1), -4. 8 e(3) a(0)(3) E-h(-2) and 1325 e(4) a(0)(4) E-h(-3). The mean <(beta)over bar> = 30.1 e(3) a(0)(3) E-h(-2) and <(gamma)over bar> = 3390 e(4) a(0)(4) E-h(-3) are larger than the experimental Kerr effect values at 632.8 nm. (C ) 2000 Published by Elsevier Science B.V. All rights reserved.