Single‐Crystal Structure Determination of Superconducting La ₄ Ni ₃ O _10‐δ under High Pressure

Abstract

Abstract Ruddlesden‐Popper nickelates have attracted enormous attention since the discovery of high‐temperature superconductivity in bilayer La 3 Ni 2 O 7 under high pressure. However, the crystal structure under high pressure remains elusive due to the lack of single crystal diffraction data. Here, high‐pressure superconductivity with a superconducting onset temperature approaching 30K and a zero‐resistance state at 7K at 53.8 GPa is reported in high‐quality single crystals of trilayer La 4 Ni 3 O 10‐δ grown at ambient pressure. A cascade of structural transitions from P 2 1 / a at 5.7 GPa to Bmab at 11.0 GPa and to I 4/ mmm at 16.6 GPa is unambiguously determined via synchrotron X‐ray single crystal diffraction, revealing a correlation between the tetragonal I 4/ mmm and the emergence of superconductivity. These results not only demonstrate that ambient‐pressure grown nickelate single crystals can superconduct under high pressure but also reveal an intermediate structure that was not reported under high pressure, providing new insights into the physics of nickelate superconductivity.