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 μz=−0.7916 e a0 for the dipole moment, ᾱ=23.59 and Δα=11.73 e2 a02 Eh−1 for the mean and the anisotropy of the dipole polarizability, β̄=35.0 e3 a03 Eh−2 for the mean first and γ̄=2061 e4 a04 Eh−3 for the mean second dipole hyperpolarizability. Our CCSD(T) values for the electron correlation correction to these properties are −0.1676 e a0, 2.25 and 1.38 e2 a02 Eh−1, −4.8 e3 a03 Eh−2 and 1325 e4 a04 Eh−3. The mean β̄=30.1 e3 a03 Eh−2 and γ̄=3390 e4 a04 Eh−3 are larger than the experimental Kerr effect values at 632.8 nm.