Ab Initio Modeling of fcc Fe-Co-Cr-Ni High Entropy Alloys with Full Composition Range

Abstract

The Fe-Co-Cr-Ni quaternary system has been studied extensively in the past decade, not only because of the superior properties achieved like high tensile ductility and fracture toughness, but also it is the foundation for the development of FeCrCoNi-based HEAs. However, most of the investigations are mainly focusing on the equiatomic and semi-equiatomic compositions. The physical properties of non-equiatomic compositions are barely explored. In the current work, the ab initio approach is adopted to predict the lattice parameter, structure stabilities, elastic properties, and enthalpy of formations of fcc Fe-Cr-Co-Ni HEA single crystals with the special quasirandom structure (SQS) method. To expand the design of Fe-Co-Cr-Ni HEAs into a full composition range, the current simulations cover all the binaries, ternaries, and the whole quaternary system. The 2-D composition-property contour diagrams are created to show the physical properties in the ternary and quaternary systems. Our investigation shows that the fcc alloys' lattice parameter increases with the addition of Fe and Cr and decreases with Ni and Co. In addition to the enthalpy of formation at 0 K, the shape distortion rate is proposed to be another essential parameter to evaluate the crystal stability. The results show the addition of Cr would destabilize the fcc lattice and cause symmetry breaking. Finally, the result of Pugh’s ratio shows that most of the fcc alloys show ductile behavior (\(P\,\)> 1.75), especially for the alloys around Fe3Ni, FeCo, and Fe2NiCo (\(P\,\)> 2.5). The brittle behavior (\(P\,\)< 1.75) is located around Fe3Cr and Fe2CoCr. Meanwhile, Cr2NiCo and Cr2FeNiCo are considered promising compositions to be tried and verified experimentally because of the higher bulk modulus and moderate shear modulus.