First-principles and cluster expansion study of the effect of magnetism on short-range order in Fe-Ni-Cr austenitic stainless steels

TL;DR

This study develops a spin cluster expansion model that explicitly incorporates magnetism to better understand and predict the short-range order in Fe-Ni-Cr austenitic stainless steels, revealing the significant influence of magnetic interactions.

Contribution

The paper introduces a generalized spin cluster expansion model that explicitly accounts for magnetic exchange interactions, improving predictions of SRO in Fe-Ni-Cr alloys over previous models.

Findings

Magnetic exchange interactions are comparable to chemical interactions in magnitude.

Increasing Cr content promotes SRO and raises order-disorder transition temperatures.

Explicit magnetic modeling improves agreement with experimental data across compositions.

Abstract

Short-range order (SRO) alters the mechanical properties of technologically relevant structural materials such as medium/high entropy alloys and austenitic stainless steels. In this study, we present a generalized spin cluster expansion (CE) model and show that magnetism is a primary factor influencing the level of SRO present in austenitic Fe-Ni-Cr alloys. The spin CE consists of a chemical cluster expansion combined with an Ising model for Fe-Ni-Cr alloys. It explicitly accounts for local magnetic exchange interactions, thereby capturing the effects of finite temperature magnetism on SRO. Model parameters are obtained by fitting to a first-principles data set comprising both chemically and magnetically diverse FCC configurations. The magnitude of the magnetic exchange interactions are found to be comparable to the chemical interactions. Compared to a conventional implicit magnetism CE built from only magnetic ground state configurations, the spin CE shows improved performance on several experimental benchmarks over a broad spectrum of compositions, particularly at higher temperatures due to the explicit treatment of magnetic disorder. We find that SRO is strongly influenced by alloy Cr content, since Cr atoms prefer to align antiferromagnetically with nearest neighbors but become magnetically frustrated with increasing Cr concentration. We predict that increasing the Cr concentration in typical austenitic stainless steels promotes the formation of SRO and increases order-disorder transition temperatures. This study underscores the significance of considering magnetic interactions explicitly when exploring the thermodynamic properties of complex transition metal alloys. It also highlights guidelines for customizing SRO through adjustments of alloy composition.