Chemisorption of sulfur at the (100), (110), and (111) surface of nickel has been studied, using the linear combination of Gaussian-type orbitals local density functional (LCGTO-LDF) method. Employing various cluster models consisting of 11 to 29 substrate atoms, adsorption at the experimentally known sites has been considered. Besides the equilibrium distance and the force constant of the vertical adsorbate motion, the dynamical dipole moment was evaluated and it turned out to provide a sensitive probe of cluster convergence. The influence of atoms from the third substrate layer on the various observables is found to be considerable in some cases. With increasing cluster size, bond lengths are stabilized to 0.02 Angstrom, frequencies to 20 cm(-1), and dipole moments to 0.1 D. The converged results agree very well with experiment. Adsorption induced population changes are restricted to only four to six neighboring substrate atoms of the modifier atom. However, energy resolved charge density differences reveal a possible mechanism for the transmission of the long-range electronic effects caused by the adatom.