Defect and solute properties in dilute Fe-Cr-Ni austenitic alloys from first principles

We present results of an extensive set of first-principles density functional theory calculations of point defect formation, binding, and clustering energies in austenitic Fe with dilute concentrations of Cr and Ni solutes. A large number of possible collinear magnetic structures were investigated as appropriate reference states for austenite. We found that the antiferromagnetic single- and double-layer structures with tetragonal relaxation of the unit cell were the most suitable reference states and highlighted the inherent instabilities in the ferromagnetic states. Test calculations for the presence and influence of noncollinear magnetism were performed but proved mostly negative. We calculate the vacancy formation energy to be between 1.8 and 1.95 eV. Vacancy cluster binding was initially weak at 0.1 eV for divacancies but rapidly increased with additional vacancies. Clusters of up to six vacancies were studied and a highly stable octahedral cluster and stacking fault tetrahedron were found with total binding energies of 2.5 and 2.3 eV, respectively. The < 100 > dumbbell was found to be the most stable self-interstitial with a formation energy of between 3.2 and 3.6 eV and was found to form strongly bound clusters, consistent with other fcc metals. Pair interaction models were found to be capable of capturing the trends in the defect cluster binding energy data. Solute-solute interactions were found to be weak in general, with a maximal positive binding of 0.1 eV found for Ni-Ni pairs and maximum repulsion found for Cr-Cr pairs of -0.1 eV. Solute cluster binding was found to be consistent with a pair interaction model, with Ni-rich clusters being the most stable. Solute-defect interactions were consistent with Ni and Cr being modestly oversized and undersized solutes, respectively, which is exactly opposite to the experimentally derived size factors for Ni and Cr solutes in type 316 stainless steel and in the pure materials. Ni was found to bind to the vacancy and to the < 100 > dumbbell in the tensile site by 0.1 eV and was repelled from mixed and compressive sites. In contrast, Cr showed a preferential binding to interstitials. Calculation of tracer diffusion coefficients found that Ni diffuses significantly more slowly than both Cr and Fe, which is consistent with the standard mechanism used to explain radiation-induced segregation effects in Fe-Cr-Ni austenitic alloys by vacancy-mediated diffusion. Comparison of our results with those for bcc Fe showed strong similarity for pure Fe and no correlation with dilute Ni and Cr.