Chemical and Magnetic Order in Vapor-Deposited Metal Films

A stochastic Monte Carlo model of vapor deposition and growth of a crystalline, binary, A_3 B metallic alloy with a negative energy of mixing has been developed which incorporates deposition and surface diffusion in a physically correct manner and allows the simulation of deposition rates that are experimentally realizable. The effects of deposition rate and growth temperature on the development of short range order (SRO) in vapor-deposited films have been examined using this model. SRO in the simulated films increases with growth temperature up to the point at which the temperature corresponds to the energy of mixing, but we see no corresponding development of anisotropic SRO (preferential ordering of A-B pairs along the growth direction). Epitaxial (100) and (111) CoPt_3 films have been deposited over a range of growth temperatures from -50^circ C to 800^circC. Curie temperature (T_{rm c}) and saturation magnetization are dramatically enhanced in those films grown near 400^circ C over the values expected for the chemically homogeneous alloy. Magnetization data indicates that the high T _{rm c} films are inhomogeneous. These phenomena are interpreted as evidence of a previously unobserved magnetically driven miscibility gap in the Co-Pt phase diagram. Films grown near 400^circ C exhibit large uniaxial perpendicular magnetic anisotropy that cannot be accounted for by strain. The observed anisotropy coincides with the chemical phase separation and it seems likely that these two phenomena are related. Long range order (LRO) in the as-deposited films peaks at a growth temperature of 630^circC and then decreases with decreasing growth temperature. The decrease in LRO is either due to kinetic frustration or to competition from magnetically induced Co clustering. Theoretical phase diagrams based on the appropriate Blume-Emery-Griffiths Hamiltonian suggest the latter.