Grain boundary diffusion and its relation to segregation of multiple elements in yttrium aluminum garnet

Polednia, Joana; Dohmen, Ralf; Marquardt, Katharina

We studied grain boundary diffusion and segregation of La, Fe, Mg, and Ti in a crystallographically defined grain boundary in yttrium aluminum garnet (YAG). Bi-crystals were synthesized by wafer bonding. Perpendicular to the grain boundary, a thin-film diffusion source of a Lainline-formula3.60Alinline-formula4.40Oinline-formula12 was deposited by pulsed laser deposition. Diffusion anneals were performed at 1000 and 1450 inline-formulaC. Via a gas phase small amounts of elements were added during the experiment. The element concentration distributions in our bi-crystals were mapped using analytical transmission electron microscopy (ATEM). Our results show strong segregation of La and Ti at the grain boundary. However, in the presence of Ti, the La concentrations dropped below the detection limit. Quantitative element distribution profiles along and across the grain boundary were fitted by a numerical diffusion model for our bi-crystal geometry that considers the segregation of elements into the grain boundary. The shape of the diffusion profiles of Fe requires the presence of two diffusion modes, e.g., the co-diffusion of Feinline-formula2+ as well as Feinline-formula3+. The absence of a detectable concentration gradient along the grain boundary in many experiments allows a minimum value to be determined for the product of sDinline-formulagb. The resulting sDinline-formulagb are a minimum of 7 orders of magnitude larger than their respective volume diffusion coefficient, specifically for La inline-formula= 10inline-formula−14inline-formulam2 s−1, Fe inline-formula= 10inline-formula−11inline-formulam2 s−1, Mg inline-formula= Si inline-formula= 10inline-formula−12inline-formulam2 s−1, and Ti inline-formula= 10inline-formula−14inline-formulam2 s−1 at 1450 inline-formulaC. Additionally, we model the effect of convolution arising from the given spatial resolution of our analysis with the resolution of our modeled system. Such convolution effects result in a non-unique solution for the segregation coefficient, e.g., for example for Mg between 2–3. Based on our data we predict that bulk diffusion of impurities in a mono-phase polycrystalline aggregate of YAG is effectively always dominated by grain boundary diffusion.

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Polednia, Joana / Dohmen, Ralf / Marquardt, Katharina: Grain boundary diffusion and its relation to segregation of multiple elements in yttrium aluminum garnet. 2020. Copernicus Publications.

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