Efficient ab initio stacking fault energy mapping for dilute interstitial alloys

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Density Functional Theory (DFT) is the prevalent first principles computational method for determining the stacking fault energy (SFE) of face centered cubic (fcc) metals and alloys. Due to several theoretical and computational challenges, SFE determination for interstitial alloys with alloying elements such as carbon, nitrogen, and hydrogen, has so far been limited to few studies at relatively high interstitial content. We propose a new method, rooted in the axial interaction model, that allows rapid and robust mapping of SFE for virtually arbitrary interstitial contents. Instead of computing the total energy of a very large supercell to represent dilute interstitial solutions, representative interstitial-affected and bulk regions are treated separately at the equivalent volume. The SFE is obtained by balancing the SFE values of the regions with a lever rule approach. The method matches SFE values from the axial interaction model within ≤4 mJ.m−2 error, as validated for non-magnetic fcc Fe-N and paramagnetic fcc Fe-N and AISI 304 alloys. The significantly reduced computational workload and equidistant SFE mapping vs. interstitial content down to extremely low values allows accurate fitting of the SFE vs. interstitial content with only few datapoints. This further improves the computational efficiency. So far DFT-based SFE mapping was limited to purely substitutional alloys; we demonstrate the first-time DFT-based SFE mapping in fcc AISI 304 vs. N and Ni, revealing a non-additive contribution of N and Ni to the SFE. Finally, the remaining challenges and future application for high-throughput DFT SFE computation in interstitial alloys is discussed.