Atomistic analysis and large-scale atomistic simulations using the Bozzolo-Ferrante-Smith (BFS) method for alloys were performed to investigate surface segregation in Ni-Pd alloys as a function of temperature, crystal face, and composition. Pd-enrichment of the first layer was observed in (I 1 1) and (10 0) surfaces, and enrichment of the top two layers occurred for (I 10) surfaces. In all cases, the segregation profile shows alternating planes enriched and depleted in Pd in a decreasing oscillatory profile. Based on atom-by-atom static energy calculations, an explanation for the observed surface features is presented in terms of competing chemical and strain energy effects. (C) 2003 Elsevier Science B.V. All rights reserved.