Evidence for charge and spin order in single crystals of La₃Ni₂O₇ and La₃Ni₂O₆

Charge and spin order is intimately related to superconductivity in copper oxide superconductors. To elucidate the competing orders in various nickel oxide compounds are crucial given the fact that superconductivity has been discovered in Nd$_{0.8}$Sr$_{0.2}$NiO$_2$ films. Herein, we report structural, electronic transport, magnetic, and thermodynamic characterizations on single crystals of La$_3$Ni$_2$O$_7$ and La$_3$Ni$_2$O$_6$. La$_3$Ni$_2$O$_7$ is metallic with mixed Ni$^{2+}$ and Ni$^{3+}$ valent states. Resistivity measurements yield two transition-like kinks at $\sim$110 and 153 K, respectively. The kink at 153 K is further revealed from magnetization and specific heat measurements, indicative of the formation of charge and spin order. La$_3$Ni$_2$O$_6$ single crystals obtained from topochemical reduction of La$_3$Ni$_2$O$_7$ are insulating and show an anomaly at $\sim$176 K on magnetic susceptibility. The transition-like behaviors of La$_3$Ni$_2$O$_7$ and La$_3$Ni$_2$O$_6$ are analogous to the charge and spin order observed in La$_4$Ni$_3$O$_{10}$ and La$_4$Ni$_3$O$_8$, suggesting charge and spin order is a common feature in the ternary La-Ni-O system with mixed-valent states of nickel.