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Ionic conductivity blocking at grain boundaries in polycrystalline electrolytes is one of the main obstacles that need to be overcome in order to improve the performance of solid state fuel cells and batteries. To this aim, harnessing the physical properties of grain boundaries in ionic conducting materials such as yttria‐stabilized zirconia (YSZ) down to the atomic scale arises as a greatly important task. Here a structural and compositional analysis of a single grain boundary in a 9 mol.% yttria content YSZ bicrystal by means of aberration‐corrected scanning transmission electron microscopy is presented. Studies here combine strain and compositional atomic resolution analysis with density‐functional‐theory calculations in order to find a preferential segregation of yttrium to the expansive atomic sites at the grain boundary dislocation cores. These results address a crucial step toward the understanding of the physical properties of grain boundaries down to atomic dimensions.

Localization of Yttrium Segregation within YSZ Grain Boundary Dislocation Cores