Paper

Identification of superconductivity in the Ruddlesden-Popper phases of nickelates under high pressure remains challenging. Here, we report a comprehensive study of the crystal structure, electrical resistance, and Meissner effect in single crystals of bilayer nickelate La3Ni2O7 under hydrostatic pressures up to 104 GPa. Using high-pressure X-ray diffraction, we observe a structural transition from an orthorhombic to a tetragonal phase above 40 GPa. Superconductivity emerges with a maximum onset transition temperature Tconset of 83 K at 18.0 GPa, accompanied by zero resistance. The superconducting phase is gradually suppressed and vanishes above 80 GPa, forming a right-triangle-like superconducting region. Direct-current magnetic susceptibility measurements demonstrate the Meissner effect and reveal a superconducting volume fraction of ∼41% at 22.0 GPa and 20 K, confirming the bulk nature of superconductivity in La3Ni2O7. Our results highlight the intricate relationship between superconductivity, oxygen content, and structural transitions in this material.

Using high-pressure variable-temperature Raman spectroscopy and polarization analysis, this work systematically tracks the structural evolution of a La₃Ni₂O₇ single crystal down to 3 K and up to 32.7 GPa. Based on rigorous symmetry selection rules, the disappearance and renormalization of multiple phonon modes in the spectra indicate a first-order structural phase transition from the orthorhombic Amam phase to the orthorhombic Fmmm phase at approximately 14.5 GPa, precisely coinciding with the emergence of bulk superconductivity. Polarized Raman measurements further reveal that above 1.92 GPa the sample recovers its intrinsic D₂h symmetry through detwinning, and in the superconducting state (3 K, 19.45 GPa) phonon modes are still observed in polarization channels, directly ruling out the tetragonal I4/mmm phase. These results confirm that the intrinsic crystal structure of the pressurized superconducting state below 19.45 GPa is orthorhombic Fmmm, rather than the previously disputed tetragonal phase, and disclose that the 180° Ni–O–Ni bond angle along the c-axis is a key structural prerequisite for achieving a high superconducting transition temperature, thereby establishing a vital structural foundation for understanding the superconducting mechanism of bilayer nickelates.

This study employed spin-polarized scanning tunneling microscopy to perform real-space imaging of the stripe order in the trilayer nickelate La₄Ni₃O₁₀, revealing its local magnetic and charge distributions. The experiments showed that the stripe order exhibits a four-unit-cell periodicity, highly reminiscent of the stripe order in cuprate high-temperature superconductors, and opens a nearly complete energy gap of approximately 66 meV near the Fermi level. More importantly, when the tunneling electron energy exceeds a threshold of about 20 meV, discrete phase slips can be triggered, enabling atomic-scale imaging of stripe dynamics. These results underscore the crucial role of correlated physics in driving stripe-like order in lanthanum nickelates and reveal striking similarities to cuprate superconductors, providing important clues for understanding the pairing mechanism in nickel-based superconductors.

This study employs a multi-orbital tight-binding model to analyze non-Fermi liquid transport phenomena in the bilayer nickelate La₃Ni₂O₇, focusing on the influence of multiband effects on the Hall coefficient. Using the Green’s function method, a rigorous formula for the Hall coefficient incorporating the quasi-quantum metric (qQM) term is derived, revealing that the temperature dependence of this qQM term is crucial in strongly correlated multiband systems. Calculations show that spin fluctuations in the Ni d₂² orbital lead to stronger quasiparticle damping, while the Ni dₓ²₋ᵧ² orbital forms cold spots. The pronounced temperature dependence of the Hall coefficient in La₃Ni₂O₇ originates from the competition between the positive contribution of the hole band and the negative contribution of the electron band, with the qQM term enhancing the positive Hall coefficient at low temperatures and explaining the experimentally observed T-linear resistivity and the increase of the Hall coefficient upon cooling. Furthermore, the qQM term also plays a key role in describing the Nernst coefficient and other transport phenomena involving second derivatives of velocity. This study reveals the core mechanism of spin-fluctuation-induced orbital-selective renormalization in non-Fermi liquid transport, providing a theoretical framework for understanding the anomalous transport properties of this system.

The bilayer nickelate La3Ni2O7 under pressure has recently emerged as a promising system for high-Tc superconductivity. In this work, we investigate the fate of the superconducting properties in La3Ni2O7 under pressure, focusing on the effects of structural deformation and apical oxygen vacancies. Employing a low-energy effective t-J∥-J⊥ model for the $$3{d}_{{x}^{2}-{y}^{2}}$$orbitals within the slave-boson mean-field approach, we demonstrate that the pairing strength is significantly enhanced in the high-pressure tetragonal I4/mmm phase compared to the ambient pressure orthorhombic Amam phase. Furthermore, by simulating random configurations of apical oxygen vacancies, we show that oxygen vacancies suppress both pairing strength and superfluid density. These results underscore the critical role of pressure and oxygen stoichiometry in tuning the SC of La3Ni2O7, providing key insights into optimizing its high-Tc behavior.

The recent discovery of superconductivity in the bilayer Ruddlesden-Popper nickelate La 3 Ni 2 O 7 under high pressure has generated much interest in the superconducting pairing mechanism of nickelates. Despite extensive work, the superconducting pairing symmetry in La 3 Ni 2 O 7 remains unresolved, with conflicting results even for identical methods. We argue that different superconducting states in La 3 Ni 2 O 7 are in close competition and highly sensitive to the choice of interaction parameters as well as pressure-induced changes in the electronic structure. Our study uses a multiorbital Hubbard model, incorporating all Ni 3 d and O 2 p states. We analyze the superconducting pairing mechanism of La 3 Ni 2 O 7 within the random phase approximation and find a transition between d -wave and sign-changing s -wave pairing states as a function of pressure and interaction parameters, which is driven by spin fluctuations with different wave vectors. These spin fluctuations with incommensurate wave vectors cooperatively stabilize a superconducting order parameter with d x 2 − y 2 symmetry for realistic model parameters. Simultaneously, their competition may be responsible for the absence of magnetic order in La 3 Ni 2 O 7 , demonstrating that magnetic frustration and superconducting pairing can arise from the same set of incommensurate spin fluctuations.

The effects of Co doping in a series of La3Ni2−xCoxO7−δ samples before and after high oxygen pressure annealing have been investigated. The structural refinemen

This study employed the six-terminal method to perform high-precision transport measurements on Ruddlesden–Popper nickelate bilayer and trilayer single crystals, self-consistently extracting the in-plane and out-of-plane resistivities. The results reveal strong intrinsic electronic anisotropy, with out-of-plane resistivity exhibiting a non-monotonic temperature dependence that signals a universal interlayer coherent-to-incoherent crossover. Under pressure, the maximum superconducting transition temperature is inversely proportional to the resistivity anisotropy at ambient pressure, indicating that stronger interlayer electronic coherence favors superconductivity. Moreover, out-of-plane resistivity serves as a sensitive probe of magnetic and density-wave orders, whereas the in-plane resistivity shows a weaker response. These findings highlight interlayer coherence as a key tuning parameter that both tracks magnetic correlations and is closely linked to superconductivity, providing stringent constraints for microscopic theories of nickelate high-temperature superconductivity.

Using resonant X-ray scattering and spectroscopy, we investigate the relationship between spin-density wave (SDW) order and superconductivity in bilayer nickelate La₂PrNi₂O₇ thin films. Superconductivity is found to emerge only in regions without SDW and with complete oxygen stoichiometry, whereas oxygen deficiency promotes SDW order, indicating phase separation between the two. Further Ni-L₃ and O-K edge spectroscopy reveal that the superconducting phase exhibits a metallic ground state dominated by Ni d⁸ and oxygen ligand-hole character; oxygen deficiency induces electron localization and the appearance of low-energy excitations. Combined with theoretical analysis, we propose that ligand holes primarily reside on the interlayer apical oxygen sites, forming stable interlayer five-spin polaron states as the ground state of superconducting bilayer nickelates. This study demonstrates that oxygen stoichiometry is a key parameter controlling interlayer coupling and electronic structure, and that SDW order is not the intrinsic parent state of superconductivity.

By stabilizing bilayer nickelate (La,Pr)₃Ni₂O₇ superconducting thin films with a protective capping layer and employing X-ray absorption and resonant inelastic X-ray scattering spectroscopy, this study directly probes the evolution of electronic structures across insulating, superconducting, and metallic states. Experimental and theoretical analyses reveal that the in-plane d_{x²-y²} states constitute an itinerant electron backbone, whereas superconductivity emerges only when the out-of-plane d_{z²}-p_z-d_{z²} interlayer hybridization becomes coherent, accompanied by suppression of static spin order and the appearance of strongly damped spin excitations. Oxygen stoichiometry and epitaxial strain jointly regulate this interlayer channel, confining the superconducting phase to a narrow window of interlayer coherence and correlation strength. These findings elucidate the microscopic prerequisites for superconductivity in bilayer nickelates and provide a multi-orbital framework to describe its emergent mechanism.