2023--Liang-A-Goodelman-D-C-Hodge-A-M-et-al--Fe-Ni-Cr-Co-Ti

Abstract: High entropy alloys (HEA) composition-structure relationships are crucial for guiding their design and applications. Here, we use a combined experimental and molecular dynamics (MD) approach to investigate phase formation during physical vapor deposition (PVD) of CoFeNiTi_x and CrFeNiTi_x HEA thin films. We vary titanium molar ratio from 0 to 1 to understand the role of a larger element in the alloy mixture. The experiments show that a high titanium content favors amorphous phase formation in the samples produced by magnetron co-sputtering. In contrast, a low titanium content results in the formation of a face-centered cubic (FCC) structure in both HEA families. This effect of titanium content on the stability of the amorphous and FCC phases is reproduced in PVD MD simulations. The threshold titanium molar ratio is identified to be ~0.53 and ~0.16 for the CoFeNiTi_x and CrFeNiTi_x films in the experiments, and ~0.53 and ~0.53 in the MD simulations. In addition, the atomistic modeling allows for energy versus volume calculations with increasing titanium content, which demonstrate the stabilization of the amorphous phase with respect to crystalline structures. To isolate the effect of atomic sizes, additional simulations are performed using an average-atom model, which disregards differences in atomic radii while preserving the average properties of the alloy. In these simulations, the energetic stability of the amorphous phase disappears. The combined experimental and simulation results demonstrate that the formation of the amorphous phase in HEA thin films generated by PVD is directly caused by the atomic size difference.