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We present a detailed nuclear magnetic resonance (NMR) study of ${}^{239}$Puin bulk and powdered single-crystal plutonium tetraboride (PuB$_4$), which hasrecently been investigated as a potential correlated topological insulator.This study constitutes the second-ever observation of the ${}^{239}$Pu NMRsignal, and provides unique on-site sensitivity to the rich $f$-electronphysics and insight into the bulk gap-like behavior in PuB$_4$. The${}^{239}$Pu NMR spectra are consistent with axial symmetry of the shift tensorshowing for the first time that ${}^{239}$Pu NMR can be observed in ananisotropic environment and up to room temperature. The temperature dependenceof the ${}^{239}$Pu shift, combined with a relatively long spin-latticerelaxation time ($T_1$), indicate that PuB$_4$ adopts a non-magnetic state withgap-like behavior consistent with our density functional theory (DFT)calculations. The temperature dependencies of the NMR Knight shift and$T_1^{-1}$--microscopic quantities sensitive only to bulk states--imply bulkgap-like behavior confirming that PuB$_4$ is a good candidate topologicalinsulator. The large contrast between the ${}^{239}$Pu orbital shifts in theionic insulator PuO$_2$ ($\sim$~+24.7~\%) and PuB$_4$ ($\sim$~-0.5~\%) providesa new tool to investigate the nature of chemical bonding in plutoniummaterials.

${}^{239}$Pu nuclear magnetic resonance in the candidate topological insulator PuB$_4$