Using time-differential perturbed angular correlation of γ rays, we investigated the electric-field gradient of polycrystalline EuTiO3 and Eu2Ti2O7, with 181Hf(181Ta) as a probe, following different thermal treatments. The measurements were performed at ISOLDE-CERN following 80 keV implantation at the Bonn Radioisotope Separator. The experimental results indicated successful induction of different phases in the implantation recovery process at 1273 and 1373 K. These observations were combined with ab initio calculations and X-ray diffraction measurements. A comparison of ab initio calculated electric-field gradients with the measured values discriminates between different structures and defects and rules out many possible cases. The Ta probe at the Ti site in the Eu2Ti2O7 phase is found to be the most probable case of site occupation after annealing at 1373 K, while annealing at 1273 K keeps EuTiO3 in the vicinity of the Ta probe. A discussion of the hyperfine interactions that promote variation in the interaction strength at the 181Ta site is presented.
