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Abstract Although continuum-scale segregation is a well-documented behavior in multi-species materials, detailed site-specific behavior remains largely unexplored. This is partially due to the complexity of analyzing materials at the requisite time and length scales for describing segregation with full atomic accuracy. Here, we better evaluate the segregation behavior of disordered grain boundary (GB) atomic environments through leveraging a set of Strain Functional Descriptors (SFDs) to generate an atomic descriptor (i.e., fingerprint). Using this atomic fingerprint, we resolve key relationships between atomic structure and segregation energy. Machine learning (ML) techniques are utilized in concert with this SFD fingerprint to elucidate complex relationships relating segregation potential to changes in specific features of the local Gaussian density captured by the SFDs. Finally, we identify relationships that indicate both individual and joint structure-property correlations. Linking atomic segregation energy to key structural features demonstrates the value of higher-order descriptors for uncovering complex structure-property relationships at an atomic scale.

The bandgap of ZnGeN2 changes with the degree of cation site disorder and is sought in light emitting diodes for emission at green to amber wavelengths. By combining the perspectives of carrier localization and defect states, we analyze the impact of different degrees of disorder on electronic properties in ZnGeN2, addressing a gap in current studies, which largely focus on dilute or fully disordered systems. The present study demonstrates changes in the density of states and localization of carriers in ZnGeN2 calculated using bandgap-corrected density functional theory and hybrid calculations on partially disordered supercells generated using the Monte Carlo method. We use localization and density of states to discuss the ill-defined nature of a bandgap in a disordered material and identify site disorder and its impact on the structure as a mechanism controlling electronic properties and potential device performance. Decreasing the order parameter results in a large reduction of the bandgap. The reduction in bandgap is due, in part, to isolated, localized states that form above the valence band continuum associated with nitrogen coordinated by more zinc than germanium. The prevalence of defect states in all but the perfectly ordered structure creates challenges for incorporating disordered ZnGeN2 into optical devices, but the localization associated with these defects provides insight into the mechanisms of electron/hole recombination in the material.

Atomistic simulations play an important role in unravelling the fundamental behavior of nanocrystalline (NC) metals/alloys. To ensure the validity of the simulated results, the initial NC structures must be representative of a real material to the extent possible. Using proper equilibration techniques, it must also be ensured that these NC structures reach a state of metastable equilibrium before probing their response. To this effect, the influence of simulated thermal equilibration of atomistic NC Ni structures on the resulting mechanical behavior is discussed in this work. It is shown that the well-equilibrated NC structures become stiffer in terms of both elastic response and yielding behavior and accumulate less residual strain upon unloading, thus, signifying the importance of proper equilibration. However, it is found that the regular equilibration method of thermal relaxations at 300 K, typically employed in atomistic modeling studies, takes significantly longer to drive the NC structures towards a metastable equilibrium state. Finally, an improved two-step equilibration method is presented that drastically expedites the equilibration process while resulting in the structural and mechanical properties comparable with the regular equilibration method performed for significantly larger simulation times. The major modification in the improved method involves: • Subjecting only the grain boundary and the surrounding atoms to thermal relaxations at relatively higher temperature.