Efficient ab initio stacking fault energy mapping for dilute interstitial alloys

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 nonmagnetic 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.

Automated summary

Density Functional Theory (DFT) is a commonly used method for determining stacking fault energy (SFE) in fcc metals and alloys. However, the determination of SFE in interstitial alloys with elements like carbon, nitrogen, and hydrogen has been limited. This study proposes a new method based on the axial interaction model that allows for rapid and accurate mapping of SFE for various interstitial contents. The method has been validated and shown to be computationally efficient, and it also reveals the non-additive contribution of certain elements to the SFE.