$^{105}$Pd NMR and NQR study of the cubic heavy fermion system Ce$_3$Pd$_{20}$Si$_6$

TL;DR

This study uses $^{105}$Pd NMR and NQR to analyze the electric field gradients and magnetic properties of Ce$_3$Pd$_{20}$Si$_6$, revealing detailed insights into its magnetic and quadrupolar orderings.

Contribution

The paper provides the first detailed NMR and NQR analysis of Ce$_3$Pd$_{20}$Si$_6$, including EFG tensors and Knight shifts, supported by DFT calculations, enhancing understanding of its magnetic ground state.

Findings

EFG tensors determined for two Pd sites.

Excellent agreement between experimental EFGs and DFT calculations.

Large quadrupolar coupling compared to Larmor frequency.

Abstract

We report $^{105}$Pd NMR and NQR measurements on a single crystal of Ce$_3$Pd$_{20}$Si$_6$, 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 DFT calculations. The principal values of the quadrupolar coupling are $(20.37 \pm 0.02)$ MHz and $(5.45 \pm 0.02)$ MHz, for the Pd($32f$) and Pd($48h$) site, respectively, which is large compared to the Larmor frequency defined by the gyromagnetic constant $\gamma = 1.94838$ MHz/T for $^{105}$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 Ce$_3$Pd$_{20}$Si$_6$.