Electric field gradients at 181Ta probe in ZrNi: Results from perturbed angular correlation and first-principles calculations

• Temperature dependent PAC studies have been carried out in ZrNi.
• ZrNi is characterized also by XRD and XPS measurements.
• No magnetic interaction is observed down to 77 K.
• Electric field gradient varies as T3/2 below 350 K and as T above 350 K.
• Calculations for EFG and magnetic field have been carried out by DFT.

Results of temperature dependent perturbed angular correlation (PAC) measurements in the equiatomic ZrNi alloy have been reported for the first time using 181Hf probe. At room temperature, values of quadrupole frequency and asymmetry parameter for the major component (~80%) are found to be ωQ=26.8(4) Mrad/s, and η=0.413(7). The resulting electric field gradient comes out to be Vzz=2.99 ×1017 V/cm2 and this corresponds to the probe nuclei occupying the regular substitutional Zr sites. In ZrNi system, no magnetic interaction is observed down to 77 K indicating absence of any magnetism in this material. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) studies on an inactive but similarly prepared sample confirm the dominant presence of the orthorhombic ZrNi phase in the sample. A complementary density functional theory (DFT) calculation results in Vzz=−2.35×1017 V/cm2, η=0.46 at the 181Ta probe impurity site and zero magnetic moment on each atomic site, in close agreement with the experimental results. Furthermore, it is found that electric field gradient for the regular component follows a T3/2 temperature dependence between 77 and 353 K, beyond which it varies linearly with temperature.