Self-propagating reactions in Al/Zr multilayers: Anomalous dependence of reaction velocity on bilayer thickness

High temperature, self-propagating reactions are observed in vapor-deposited Al/Zr multilayered foils of overall atomic ratios 3 Al:1 Zr and 2 Al:1 Zr and nanoscale layer thicknesses; however, the reaction velocities do not exhibit the inverse dependence on bilayer thickness that is expected based on changes in the average diffusion distance. Instead, for bilayer thicknesses of 20-30 nm, the velocity is essentially constant at ∼7.7 m/s. We explore several possible explanations for this anomalous behavior, including microstructural factors, changes in the phase evolution, and phase transformations in the reactant layers, but find no conclusive explanations. We determine that the phase evolution during self-propagating reactions in foils with a 3 Al:1 Zr stoichiometry is a rapid transformation from Al/Zr multilayers to the equilibrium intermetallic Al3Zr compound with no intermediate crystalline phases. This phase evolution is the same for foils of 90 nm bilayer thicknesses and foils of bilayer thicknesses in the range of 27 nm to 35 nm. Further, for foils with a bilayer thickness of 90 nm and a 3 Al:1 Zr overall chemistry, the propagation front is planar and steady, in contrast to unsteady reaction fronts in foils with 1 Al:1 Zr overall chemistry and similar bilayer thicknesses.