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Numerous technological applications of Ni-based Zr and Hf intermetallicalloys promoted comprehensive studies in Zr$_8$Ni$_{21}$ and Hf$_8$Ni$_{21}$ byperturbed angular correlation (PAC) spectroscopy, which were not studiedearlier until this report. The different phases produced in the samples havebeen identified by PAC and X-ray diffraction (XRD) measurements. Using$^{181}$Hf probe, two non-equivalent Zr/Hf sites have been observed in bothZr$_8$Ni$_{21}$ and Hf$_8$Ni$_{21}$ compounds. From present PAC measurements inZr$_8$Ni$_{21}$, a component due to the production of Zr$_7$Ni$_{10}$ byeutectic reaction from the liquid metals is also observed. The phaseZr$_7$Ni$_{10}$, however, is not found from the XRD measurement. InZr$_8$Ni$_{21}$, while the results do not change appreciably up to 973 Kexhibit drastic changes at 1073 K. In Hf$_8$Ni$_{21}$, similar results for thetwo non-equivalent sites have been found but site fractions are in reverseorder. In this alloy, a different contaminating phase, possibly due toHfNi$_3$, has been found from PAC measurements but is not found from XRDmeasurement. Density functional theory (DFT) based calculations of electricfield gradient (EFG) and asymmetry parameter ($\eta$) at the sites of$^{181}$Ta probe nucleus allowed us to assign the observed EFG fractions to thevarious lattice sites in (Zr/Hf)$_8$Ni$_{21}$ compounds.

Electric field gradients in Zr$_8$Ni$_{21}$ and Hf$_8$Ni$_{21}$  intermetallic compounds; Results from perturbed angular correlation  measurements and first-principles density functional theory