Distinguishing Intrinsic Descriptors of Grain Boundary Segregation Between Metallic and Non‐Metallic Solutes in BCC Fe via Machine Learning

ABSTRACT Elemental segregation at grain boundaries (GBs) is widely recognized to influence the mechanical properties of structural materials. However, the intrinsic descriptors governing GB segregation have not been systematically clarified. Herein, first‐principles calculations combined with interpretable machine learning analysis are used to identify the key factors governing elemental segregation at GBs in BCC Fe. A GB segregation database is constructed for 39 solutes commonly present in steels, including 33 metallic and 6 nonmetallic solutes. An interpretable machine learning framework is then developed to rank the intrinsic descriptors that govern segregation behavior. The results indicate that GB segregation of metallic solutes is primarily controlled by geometric features (Voronoi volume), whereas nonmetallic is more strongly governed by electronic features (Chemical bonding). Moreover, an overall contrasting trend is observed in the correlation between Voronoi volume and segregation energy for metallic and nonmetallic solutes. This study provides a new insight into GB engineering and the design of high‐performance steels.