The frequency-dependent first dipole hyperpolarizabilities and their geometric derivatives have been calculated for HF, HC1, CO and LiF, using the quadratic response coupled cluster singles and doubles (CCSD) method and quadratic response density functional theory. Results obtained by means of different functionals have been compared with CCSD numbers, and, whenever possible, with experiment. Additionally, convergence of hyperpolarizabilities and their geometric derivatives in a hierarchy of correlationconsistent basis sets has been studied. (C) 2005 Elsevier B.V. All rights reserved.