Large angular variations in film composition have been found for ablation of a metallic AuCu alloy (Au/Cu ratio $\sim 1)$ in vacuum and background gases of Ne and Xe. The AuCu films grown in vacuum at a laser fluence of $5\mathrm{Jc}{\mathrm{m}}^{-2}$ exhibit a large loss in the Cu content, with the Au/Cu ratio $\sim 2.4$ at angles close to normal incidence. At this fluence, a distortion of the plume front is observed followed by the appearance of a secondary emission at the substrate, suggesting that resputtering of the film by energetic ions and reflection of ions/atoms at the substrate can lead to a nonstoichiometric transfer in pulsed laser deposition. Further, we have found that depending on the mass of the background gas employed during growth (Ne or Xe), the ratio of elements in the film can vary significantly over a wide range of angles of deposition. In the presence of the light gas Ne, the degree of nonstoichiometric transfer is gradually reduced with increasing background pressure, resulting in a nearly stoichiometric AuCu films at a Ne pressure of 2 mbar. The behavior in the heavy gas Xe is more complex, and both theoretical and experimental data indicate that the loss of Cu in the deposits is caused by the preferential scattering, as well as by backscattering of the light Cu atoms in the plume upon collisions with the background gas.

• Received 14 June 2017

DOI:https://doi.org/10.1103/PhysRevMaterials.1.073402