Predicting grain boundary segregation in magnesium alloys: An atomistically informed machine learning approach

• Vibrational free energy distribution in Mg GBs differs significantly from bulk, indicating unique thermal properties at GBs. • Segregation energies and free energies show skew-normal distributions at finite temperatures in Mg alloys. • Machine learning models effectively predict segregation energy; hydrostatic stress is the most influential feature. • Flexibility volume enhances understanding of local atomic environments, influencing solute segregation. • Nd displays higher GB segregation up to 800 K, aligning with observed strong segregation tendencies. Grain boundary (GB) segregation substantially influences the mechanical properties and performance of magnesium (Mg). Atomic-scale modeling, typically using ab-initio or semi-empirical approaches, has mainly focused on GB segregation at highly symmetric GBs in Mg alloys, often failing to capture the diversity of local atomic environments and segregation energies, resulting in inaccurate structure-property predictions. This study employs atomistic simulations and machine learning models to systematically investigate the segregation behavior of common solute elements in polycrystalline Mg at both 0 K and finite temperatures. The machine learning models accurately predict segregation thermodynamics by incorporating energetic and structural descriptors. We found that segregation energy and vibrational free energy follow skew-normal distributions, with hydrostatic stress, an indicator of excess free volume, emerging as an important factor influencing segregation tendency. The local atomic environment’s flexibility, quantified by flexibility volume, is also crucial in predicting GB segregation. Comparing the grain boundary solute concentrations calculated via the Langmuir-McLean isotherm with experimental data, we identified a pronounced segregation tendency for Nd, highlighting its potential for GB engineering in Mg alloys. This work demonstrates the powerful synergy of atomistic simulations and machine learning, paving the way for designing advanced lightweight Mg alloys with tailored properties.