Grain Boundary Segregation Predicted by Quantum-Accurate Segregation Spectra but not by Classical Models

TL;DR

This paper demonstrates that classical models fail to predict certain grain boundary segregations, which can be accurately forecasted using quantum-accurate segregation spectra, as shown by experimental validation in gold-aluminum alloys.

Contribution

The study introduces quantum-accurate segregation spectra to predict grain boundary segregation, revealing phenomena missed by classical models.

Findings

Quantum-accurate spectra predict strong gold segregation in aluminum.

Experimental results confirm two orders of magnitude gold enrichment.

Classical models cannot explain observed segregation patterns.

Abstract

In alloys, solute segregation at grain boundaries is classically attributed to three driving forces: a high solution enthalpy, a high size mismatch, and a high difference in interfacial energy. These effects are generally cast into a single scalar segregation energy and used to predict grain boundary solute enrichment or depletion. This approach neglects the physics of segregation at many competing grain boundary sites, and can also miss electronic effects that are energetically significant to the problem. In this paper, we demonstrate that such driving forces cannot explain, nor thus predict, segregation in some alloys. Using quantum-accurate segregation spectra that have recently become available for some polycrystalline alloys, we predict strong segregation for gold in aluminum, a solvent-solute combination that does not conform to classical driving forces. Our experiments confirm these predictions and reveal gold enrichment at grain boundaries that is two orders of magnitude over the bulk lattice solute concentration.