We report Pd nuclear magnetic resonance (NMR) and nuclear quadrupolar resonance (NQR) measurements on a single crystal of CePdSi, where antiferroquadrupolar and antiferromagnetic orders develop at low temperature. From the analysis of NQR and NMR spectra, we have determined the electric field gradient (EFG) tensors and the anisotropic Knight shift (K) components for both inequivalent Pd sites-Pd(32f) and Pd(48h). The observed EFG values are in excellent agreement with our state-of-the-art density functional theory calculations. The principal values of the quadrupolar coupling are [Formula: see text] MHz and [Formula: see text] MHz, for the Pd(32f) and Pd(48h) sites, respectively, which is large compared to the Larmor frequency defined by the gyromagnetic constant [Formula: see text] MHz/T for Pd. Therefore, the complete knowledge of K and the EFG tensors is crucial to establish the correspondence between NMR spectra and crystallographic sites, which is needed for a complete analysis of the magnetic structure, static spin susceptibility, and the spin-lattice relaxation rate data and a better understanding of the groundstate of CePdSi.
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