Investigating the cause of crossover from charge/spin stripe insulator to correlated metallic phase in layered T' nickelates -- R$_4$Ni$_3$O$_8$

Abstract

The $T^{\prime}$ infinite layered nickelates have recently garnered significant attention owing to the discovery of superconductivity in hole-doped RNiO$_2$ (R $=$ La, Pr, or Nd), which is the $n = \infty$ member of the series R$_{n+1}$Ni$_n$O$_{2n+2}$. Here, we investigate the $n = 3$ member, namely R$_4$Ni$_3$O$_8$ (R $=$ La, Pr, or Nd) of this family. The compound La$_4$Ni$_3$O$_8$ exhibits simultaneous charge/spin-stripe ordering at T$_N^\ast$ $=$ 105 K, which is also concomitant with the onset of metal-to-insulator (MIT) transition upon lowering the temperature below T$_N^\ast$. We investigate the conspicuous absence of this transition in the Pr and Nd analogues of La$_4$Ni$_3$O$_8$. To achieve this purpose, we synthesized solid-solutions of the form (La, Pr)$_4$Ni$_3$O$_8$ and (La, Nd)$_4$Ni$_3$O$_8$ and examined the behavior of T$_N^\ast$ as a function of the average R-site ionic radius ($r_{\overline{R}}$). We show that after an initial quasilinear decrease with decreasing $r_{\overline{R}}$, T$_N^\ast$ suddenly vanishes in the narrow range 1.134 $\AA$ $\leq$ $r_{\overline{R}}$ $\leq$ 1.143 $\AA$. In the same range, we observed the emergence of a new transition below T$^\ast$, whose onset temperature increases as $r_{\overline{R}}$ further decreases. We, therefore, argue that the sudden vanishing of charge/spin-stripe/MIT ordering upon decreasing $r_{\overline{R}}$ is due to the appearance of a new competing phase. The point $r_{\overline{R}}$ $\approx$ $r_c$, where T$_N^\ast$ vanishes and T$^\ast$ appears -- a quantum critical point -- should be investigated further. In this regard, Pr$_4$Ni$_3$O$_8$ and Pr-rich samples should be useful due to the weak magnetization response associated with the Pr-sublattice, as shown here.