| Abstract Scope |
As in other classes of materials, the chemistry and structure of grain boundaries in complex oxides dictate their impact on functionality. Using computational modeling, we describe how, even at their thermodynamic ground state, grain boundaries in spinels exhibit higher degrees of cation disorder than the bulk. The extent to which a given boundary accommodates more disorder depends both on the structure of the boundary and the chemistry of the spinel. We further provide evidence that the functional properties of these boundaries, in this particular case mass transport through and along the boundary, is very sensitive to the amount of disorder at the boundary, emphasizing the need for a reasonable description of the chemical order at the boundary to adequately describe their properties. We discuss the general implications of this behavior and connect with experimental observations that corroborate these observations. |