LOCAL DENSITY-FUNCTIONAL POLARIZABILITIES AND HYPERPOLARIZABILITIES AT THE BASIS-SET LIMIT

We have performed finite-field calculations of the dipole polarizabili ties and hyperpolarizabilities of some first-row compounds in the loca l spin-density approximation (LDA) at the basis-set limit using the nu merical density-functional code NUMOL. We show that the calculations o f Guan et al. [J. Chem. Phys. 1993, 98, 4753] on dipole moments and po larizabilities are well converged with their high-quality double-zeta basis set which includes field-induced polarization functions. However , hyperpolarizabilities are not similarly well converged. We provide r eference values for first hyperpolarizabilities and estimated LDA valu es of some second hyperpolarizabilities.