Constructing phase diagrams for defects by correlated atomic-scale characterization

TL;DR

This paper introduces a combined experimental and modeling approach to construct phase diagrams for defects at the atomic scale, enabling new insights into defect chemistry and materials design.

Contribution

It presents a novel methodology to develop defect phase diagrams using atomic-resolution imaging and ab initio simulations, extending thermodynamic concepts to defects.

Findings

Atomic-scale phase transformations observed at grain boundaries.

Successful construction of a defect phase diagram for Mg grain boundary.

Method enables systematic defect chemistry analysis for materials design.

Abstract

Phase transformations and crystallographic defects are two essential tools to drive innovations in materials. Bulk materials design via tuning chemical compositions has been systematized using phase diagrams. We show here that the same thermodynamic concept can be applied to understand the chemistry at defects. We present a combined experimental and modelling approach to scope and build phase diagrams for defects. The discovery was enabled by triggering phase transformations of individual defects through local alloying, and sequentially imaging the structural and chemical changes using atomic-resolution scanning transmission electron microscopy. By observing atomic-scale phase transformations of a Mg grain boundary through Ga alloying, we exemplified the method to construct a grain boundary phase diagram using ab initio simulations and thermodynamic principles. The methodology enables a systematic development of defect phase diagrams to propel a new paradigm for materials design utilizing chemical complexity and phase transformations at defects.