Pressure-dependent "Insulator-Metal-Insulator" Behavior in Sr-doped La$_3$Ni$_2$O$_7$

Abstract

Recently, superconductivity at high temperatures has been observed in bulk La$_3$Ni$_2$O$_{7-{\delta}}$ under high pressure. However, the attainment of high-purity La$_3$Ni$_2$O$_{7-{\delta}}$ single crystals, exhibiting controlled and homogeneous stoichiometry through the post-annealing process in an oxygen-rich floating zone furnace, remains a formidable challenge. Here, we report the crystal structure and physical properties of single crystals of Sr-doped La$_3$Ni$_2$O$_7$ synthesized at high pressure (20 GPa) and high temperature (1400 {\deg}C). Through single crystal X-ray diffraction, we showed that high-pressure-synthesized paramagnetic Sr-doped La$_3$Ni$_2$O$_7$ crystallizes in an orthorhombic structure with Ni-O-Ni bond angles of 173.4(2){\deg}out-of-plane and 175.0(2){\deg}and 176.7(2){\deg}in plane. The substitution of Sr alters in band filling and the ratio of Ni$^{2+}$/Ni$^{3+}$ in Sr-doped La$_3$Ni$_2$O$_7$, aligning them with those of "La$_3$Ni$_2$O$_{7.05}$", thereby leading to significant modifications in properties under high pressure relative to the unsubstituted parent phase. At ambient pressure, Sr-doped La$_3$Ni$_2$O$_7$ exhibits insulating properties, and the conductivity increases as pressure goes up to 10 GPa. However, upon further increasing pressure beyond 10.7 GPa, Sr-doped La$_3$Ni$_2$O$_7$ transits back from a metal-like behavior to an insulator. The insulator-metal-insulator trend under high pressure dramatically differs from the behavior of the parent compound La$_3$Ni$_2$O$_{7-{\delta}}$, despite their similar behavior in the low-pressure regime. These experimental results underscore the considerable challenge in achieving superconductivity in nickelates.