Experimental nuclear quadrupole resonance and computational study of the structurally refined topological semimetal ${\mathrm{TaSb}}_2$

The local electric field gradients and magnetic dynamics of ${\mathrm{TaSb}}_2$ have been studied using ${}_{121}\mathrm{Sb}$, ${}_{123}\mathrm{Sb}$, and ${}_{181}\mathrm{Ta}$ nuclear quadrupole resonance (NQR) with density functional theory (DFT) calculations using XRD-determined crystal structures. By measuring all structurally expected 13 NQR lines, the nuclear quadrupole coupling constant $\left({\nu }_Q\right)$ and asymmetric parameter $\left(\eta \right)$ for Ta, Sb(1), and Sb(2) sites were obtained. These values are all in good agreement with the presented DFT calculations. Principal axes of the electric field gradients was determined for a single-crystal sample by measuring the angular dependencies of NMR frequency under a weak magnetic field. The unusual temperature dependence of $\eta \left(T\right)$ of Sb(2) hints at the suppressed thermal expansion along the $a$ axis. Spin-lattice relaxation rate $(1/T_{1}T)$ measurements reveal an activated-type behavior and an upturn below 30 K. Neither the low-temperature upturn nor the high-temperature activation-type behaviors are reproduced by the calculated $1/T_{1}T$ based on the calculated density of states (DOS). On the other hand, the agreement between the calculated DOS and specific heat measurements indicates that the band renormalization is small. This fact indicates that ${\mathrm{TaSb}}_2$ deviates from the simple semimetal scenario, and magnetic excitations are not captured by Fermi liquid theory.