Unconventional crystal structure of the high-pressure superconductor La${}_3$Ni${}_2$O${}_7$

Abstract

The discovery of high-temperature superconductivity in La${}_3$Ni${}_2$O${}_7$ at pressures above 14 GPa has spurred extensive research efforts. Yet, fundamental aspects of the superconducting phase, including the possibility of a filamentary character, are currently subjects of controversial debates. Conversely, a crystal structure with NiO${}_6$ octahedral bilayers stacked along the $c$-axis direction was consistently posited in initial studies on La${}_3$Ni${}_2$O${}_7$. Here we reassess this structure in optical floating zone-grown La${}_3$Ni${}_2$O${}_7$ single crystals that show signs of filamentary superconductivity. Employing scanning transmission electron microscopy and single-crystal x-ray diffraction under high pressures, we observe multiple crystallographic phases in these crystals, with the majority phase exhibiting alternating monolayers and trilayers of NiO${}_6$ octahedra, signifying a profound deviation from the previously suggested bilayer structure. Using density functional theory, we disentangle the individual contributions of the monolayer and trilayer structural units to the electronic band structure of La${}_3$Ni${}_2$O${}_7$, providing a firm basis for advanced theoretical modeling and future evaluations of the potential of the monolayer-trilayer structure for hosting superconductivity.

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Cited by in corpus (47)

• Ambient-pressure superconductivity onset above 40 K in bilayer nickelate ultrathin films
• Pressure-enhanced spin-density-wave transition in double-layer nickelate $L{a}_{3}N{i}_2{O}_{7-\delta }$
• Long-Range Structural Order in a Hidden Phase of Ruddlesden-Popper Bilayer Nickelate La${}_3$Ni${}_2$O${}_7$
• Identification of the superconductivity in bilayer nickelate La${}_3$Ni${}_2$O${}_7$ upon 100 GPa
• Pressure-enhanced splitting of density wave transitions in La${}_3$Ni${}_2$O${}_{7-\delta }$
• Angle-resolved photoemission spectroscopy of superconducting (La,Pr)3Ni2O7/SrLaAlO4 heterostructures
• Superconductivity and normal-state transport in compressively strained La${}_2$PrNi${}_2$O${}_7$ thin films
• Theory of Pressure Dependence of Superconductivity in Bilayer Nickelate La${}_3$Ni${}_2$O${}_7$
• Density-wave-like gap evolution in La${}_3$Ni${}_2$O${}_7$ under high pressure revealed by ultrafast optical spectroscopy
• Bulk superconductivity up to 96 K in pressurized nickelate single crystals
• Correlated electronic structures and unconventional superconductivity in bilayer nickelate heterostructures
• Resolving the Electronic Ground State of La3Ni2O7-δ Films
• Strain-tuning for superconductivity in La${}_3$Ni${}_2$O${}_7$ thin films
• The $s^{\pm }$-Wave Superconductivity in the Pressurized La${}_4$Ni${}_3$O${}_{10}$
• Recent progress in nickelate superconductors
• Phase diagram of pressure-induced high temperature superconductor La${}_3$Ni${}_2$O${}_{7+\delta }$
• Band Structure and Pairing Nature of La${}_3$Ni${}_2$O${}_7$ Thin Film at Ambient Pressure
• Anisotropic Spin Stripe Domains in Bilayer La${}_3$Ni${}_2$O${}_7$
• Imaging the Meissner effect in pressurized bilayer nickelate with integrated multi-parameter quantum sensor
• Superconductivity and Electronic Structures of Nickelate Thin Film Superstructures
• Electronic correlations, layer distinction, and electron doping in the alternating single-layer trilayer La${}_3$Ni${}_2$O${}_7$ polymorph
• Signature of superconductivity in pressurized La4Ni3O10-x single crystals grown at ambient pressure
• Out-of-plane bond-order phase, superconductivity, and their competition in the $t$-$J_{\parallel }$-$J_{\perp }$ model: Possible implications for bilayer nickelates
• Phase diagrams and two key factors to superconductivity of Ruddlesden-Popper nickelates
• DFT+DMFT study of correlated electronic structure in the monolayer-trilayer phase of La${}_3$Ni${}_2$O${}_7$
• The electronic structure and disorder effect of La${}_3$Ni${}_2$O${}_7$ superconductor
• $t$-$J$ model for strongly correlated two-orbital systems: Application to bilayer nickelate superconductors
• Theoretical study of the crystal structure of the bilayer nickel oxychloride Sr${}_3$Ni${}_2$O${}_5$Cl${}_2$ and analysis of possible unconventional superconductivity
• Magnetic Correlations and Pairing Tendencies of the Hybrid Stacking Nickelate Superlattice La${}_7$Ni${}_5$O${}_{17}$ (La${}_3$Ni${}_2$O${}_7$/La${}_4$Ni${}_3$O${}_{10}$) under Pressure
• Origin of the Diagonal Double-Stripe Spin-Density-Wave and Potential Superconductivity in Bulk La${}_3$Ni${}_2$O${}_7$ at Ambient Pressure
• Possible Liquid-Nitrogen-Temperature Superconductivity Driven by Perpendicular Electric Field in the Single-Bilayer Film of La${}_3$Ni${}_2$O${}_7$ at Ambient Pressure
• Superconductivity governed by Janus-faced fermiology in strained bilayer nickelates
• Strain-Engineered Electronic Structure and Superconductivity in La${}_3$Ni${}_2$O${}_7$ Thin Films
• Electronic Structure, Magnetic and Pairing Tendencies of Alternating Single-layer Bilayer Stacking Nickelate La${}_5$Ni${}_3$O${}_{11}$ Under Pressure
• Pressure Effect on the Spin Density Wave Transition in La${}_2$PrNi${}_2$O${}_{6.96}$
• Damage of bilayer structure in La3Ni2O7-d induced by high pO2 annealing
• Stabilizing and Tuning Superconductivity in La${}_3$Ni${}_2$O${}_{7-\delta }$ Films: Oxygen Recycling Protocol Reveals Hole-Doping Analogue
• Charge distribution and magnetism in bilayer La${}_3$Ni${}_2$O${}_7$: a hybrid functional study
• Universal electronic structure of multi-layered nickelates via oxygen-centered planar orbitals
• A rutile-based homologous series Na(PtO${}_2$)${}_{2n+1}$ discovered by computationally assisted high-pressure synthesis
• Pairing mechanism and superconductivity in pressurized La${}_5$Ni${}_3$O${}_{11}$
• Multiorbital character of the density wave in trilayer nickelate superconductors
• Floating zone growth at high oxygen pressures in Ruddlesden-Popper bilayer nickelate Y${}_y$Sr${}_{3-y}$Ni${}_{2-x}$Al${}_x$O${}_{7-\delta }$
• Pairing mechanism and superconductivity in 1313 phase La${}_3$Ni${}_2$O${}_7$
• Expanding the trilayer Ruddlesden-Popper nickelate family: Synthesis and characterization of Sm${}_4$Ni${}_3$O${}_{10-\delta }$ single crystals
• Structural stability, electronic structure, and magnetic properties of the single-layer trilayer La3Ni2O7 polymorph
• $L{a}_{3}P{d}_{2}Na{O}_9$: A High-Valent Insulating Palladate