Low-temperature mean valence of nickel ions in pressurized La$_3$Ni$_2$O$_7$

Abstract

The discovery of high critical temperature (Tc) superconductivity in pressurized La$_3$Ni$_2$O$_7$ has ignited renewed excitement in the search of novel high-Tc superconducting compounds with 3d transition metals. Compared to other ambient-pressure superconductors, such as copper-oxide and iron-oxypnictides, unraveling the mechanisms of the pressure-induced superconductivity poses significant and unique challenges. A critical factor in this phenomenon seems to be related to the electronic configuration of 3d orbitals, which may play a fundamental role in driving high-Tc superconductivity. However, the pressure effects on the mixed-valence states of 3d-orbital cations and their influence on the emergence of high-Tc superconductivity remain poorly understood. Here, we use high-pressure (P) and low-temperature synchrotron X-ray absorption spectroscopy to investigate the influence of pressure on the mean valence change of Ni ions in La$_3$Ni$_2$O$_7$. Our results demonstrate that at a low-temperature of 20 K, the mean valence remains relatively stable across the pressures range from 1 atm to 40 GPa. Based on analyzing the absorption data, we find that, at a critical pressure, the ambient-pressure ordered phases disappear and both the structural and the superconducting phase transition occur. The pressure-induced structural phase transition revealed by our absorption results is consistent with that determined by X-ray diffraction, offering new information for a comprehensive understanding on the pressure-induced superconductivity in La$_3$Ni$_2$O$_7$.