Interaction between Al and atomic layer deposited (ALD) ZrN under high-energy heavy ion irradiation

Uranium-molybdenum (U-Mo) particles dispersed in an aluminum matrix is the most promising candidate fuel to convert high-power research and test reactors in Europe from using high-enriched to using low-enriched fuel. However, chemical interaction between the U-Mo and the Al matrix leads to undesirable fuel behavior. Zirconium nitride (ZrN) is used as a diffusion barrier between the U-Mo fuel particles and the Al matrix. To understand the potential microstructural evolution of ZrN during irradiation, a high-energy heavy ion (84 MeV Xe) irradiation experiment was performed on atomic layer deposited (ALD) nanocrystalline ZrN deposited on an Al plate. A fluence of 1.86×10¹⁷ ions/cm², or 90.3 dpa was reached during this experiment. Both analytic transmission electron microscopy (TEM) and synchrotron microbeam X-ray diffraction (μXRD) techniques were utilized to investigate the kinetics of radiation-induced grain growth of ZrN at various radiation doses based on the Williamson-Hall analyses. The grain growth kinetics can be described by a power law expression, Dⁿ−D₀ ⁿ=Kϕ with n = 5.1. The Al-ZrN interaction products (Al₃Zr and AlN) created by radiation-induced ballistic mixing/radiation-enhanced diffusion and their corresponding formation mechanism were determined from electron diffraction and elemental composition analysis. These experimental results were confirmed by first principle thermodynamic density functional theory (DFT) calculations. The results from this ion irradiation study were also compared to in-pile irradiation data from physical vapor deposited (PVD) ZrN samples for a comprehensive evaluation of the interaction between Al and ZrN and its influence on diffusion barrier performance.