Paper

Using density functional theory, we calculate the electronic structure of the bilayer infinite-layer nickelate La₃Ni₂O₅F, revealing its ideal two-dimensional character and the coexistence of two distinct quasiparticle behaviors. After treating the oxygen/fluorine disorder with the virtual crystal approximation, band structure calculations show that the conventional Ni dpσ band forms a hole-like Fermi surface, whereas an E* band originating from interstitial density gives rise to a cylindrical electron Fermi surface, resulting in a self-doping of 0.18 electrons. This interstitial density is distributed between the La layers that lack apical oxygen, and as the Ni dₓz/dyz bands approach the M point with parallel linear dispersion, they couple with it to form a nearly non-analytic Dirac point, exhibiting an exotic interstitial-orbital band coupling effect. Concurrently, the d_z² band undergoes a symmetry-driven splitting of approximately 1 eV through interaction with the interstitial density. This dual electron–hole character is expected to govern normal-state transport and far-infrared properties, may influence the superconducting state of nickelates, and offers a fresh perspective for understanding the physics of infinite-layer nickelates.

This study investigates the dimensionality of the superconducting state in infinite-layer nickel oxides by mapping the vortex phase diagram of superconducting Pr0.8Sr0.2NiO2 thin films from multiple perspectives. Experimental results reveal that low-disorder films exhibit a quasi-two-dimensional vortex liquid-to-glass transition, while increasing disorder drives the system into a pure two-dimensional state. This finding indicates that pure two-dimensionality is not an intrinsic property but an extrinsic phenomenon caused by the decoupling of NiO2 layers due to enhanced disorder. The work establishes disorder as a key tuning parameter for superconductivity in infinite-layer nickel oxides and identifies that disorder primarily resides within the NiO2 layers, offering two fundamental insights for understanding this class of materials.

This study used Ni M1-edge s-core-level nonresonant inelastic X-ray scattering (s-NIXS), a bulk-sensitive method, to determine the angular distribution of Ni 3d holes in the ambient-pressure single-crystal bilayer nickelate La2SmNi2O7. Fitting yielded an e_g hole occupancy ratio h_z/h_x = 0.94 ± 0.06, significantly higher than the 2/3 expected from the model of a fully occupied d_{z^2} bonding band and close to the picture of approximately one hole per e_g orbital under Hund coupling, and consistent with DMFT charge-transfer calculations for the high-pressure phase. On this basis, it is argued that the superconducting pairing scenario for this material should allow both e_g orbitals to participate in electron pairing rather than being dominated solely by a single d_{z^2} orbital; however, this constitutes experimental support for the relevant pairing theory and does not directly establish the pairing mechanism.

Disorder-Induced Suppression of Superconductivity in Infinite-Layer Nickelates

This study employs resonant inelastic X-ray scattering (RIXS) to directly compare the electronic and magnetic excitation properties of trilayer nickelate La₄Ni₃O₁₀ and bilayer La₃Ni₂O₇. The results show that La₄Ni₃O₁₀ exhibits more itinerant behavior, evidenced by broader Ni d-d orbital excitations and a stronger fluorescence background, indicating weaker electronic correlations than in the bilayer system. Despite the weaker correlations, clear collective spin excitations are observed, including dispersive acoustic and optical magnon branches as well as incommensurate spin density waves (SDW). Using linear spin-wave theory analysis, the interlayer superexchange interaction Jz is extracted to be approximately 22 meV, significantly smaller than that in La₃Ni₂O₇. The weaker electron correlations and reduced interlayer magnetic exchange together account for the substantially lower superconducting transition temperature of the trilayer compound (about 30 K) compared to the bilayer (about 80 K). This study establishes interlayer magnetic coupling and electronic correlations as key parameters for superconductivity in layered nickelates, providing important constraints for understanding the superconducting pairing mechanism in this emerging family.

Using muon spin rotation/relaxation (μSR), this study systematically measured a series of infinite-layer nickelate (La,Sr)NiO₂ samples spanning from the parent compound through the superconducting dome to the overdoped regime (Sr doping 0% ≤ x ≤ 25%) to probe the magnetic ground state and temperature-dependent static and dynamic magnetism. The results show that, regardless of doping level, local magnetic moments undergo spin freezing at temperatures on the order of tens of kelvin and enter a glassy state, and no anomaly is observed near the superconducting onset, indicating that the magnetism is intrinsic and essentially independent of hole concentration. With increasing hole doping, the glassy state shows only a weak tendency toward destabilization. These observations suggest that magnetism and superconductivity in nickelates are largely decoupled, and that their indirect interactions need to be understood within a multiorbital framework.

Using Ni (L_3)-edge resonant inelastic X-ray scattering (RIXS), this work systematically investigates the evolution of electronic and spin excitations with carrier doping in coherently compressively strained La(_{3-x})Sr(_x)Ni(_2)O(_7)/SrLaAlO(_4) thin films, covering the superconducting ((x = 0, 0.09, 0.21)) and overdoped non-superconducting ((x = 0.38)) regimes. In the superconducting films, dispersive spin excitations persist along the ([H,H]) and ([H,0]) directions, with the dispersion remaining almost doping-independent and exhibiting minimal damping, while the spectral weight only moderately decreases, indicating robust bistripe spin correlations. However, in the non-superconducting film at (x = 0.38), the magnetic response becomes strongly broadened and weakened, accompanied by significantly enhanced damping and a spectral weight reduction of approximately 50%, signaling the collapse of coherent bistripe spin excitations. The simultaneous disappearance of magnetic coherence with superconductivity directly establishes the link between doping-controlled magnetism and superconductivity in layered nickelate thin films.

Using a minimal bilayer two-orbital model and the random phase approximation, we investigate the superconducting pairing symmetry and its doping evolution in pressurized La₃Ni₂O₇. In the undoped system, the most favorable pairing state is an s± wave whose gap function changes sign between different Fermi pockets; the analysis indicates that this unconventional pairing arises from repulsive interactions mediated by the magnetic odd mode of the bilayer nickelate. Hole doping enlarges the γ Fermi pocket, and the intrapocket repulsion driven by the magnetic even mode gradually strengthens and dominates the pairing interaction, eventually driving the pairing symmetry from s± wave to dxy wave in the heavily hole-doped regime. In contrast, under electron doping the s±-wave pairing persists and remains stable even in the deeply electron-doped region where a Lifshitz transition occurs, indicating that the γ Fermi pocket is not a necessary condition for superconductivity in bilayer nickelates; owing to favorable nesting between the α and β pockets that enhances spin fluctuations, the s± wave becomes even more robust in the absence of the γ pocket. This study reveals the doping control of pairing symmetry and provides a new route for testing the superconducting pairing mechanism in pressurized La₃Ni₂O₇.

Through muon spin rotation/relaxation and resistivity measurements combined with oxygen isotope substitution, the pressure and isotope effects on density wave transitions in the trilayer Ruddlesden-Popper nickelate La₄Ni₃O₁₀ were systematically investigated. Under ambient pressure, two incommensurate spin density wave (SDW) transitions were observed at 132 K and 80–90 K; the magnetic structure reveals that the outer two Ni layers exhibit an antiferromagnetically coupled SDW order, while the inner layer has a smaller magnetic moment, and a c-axis component of the magnetic moment emerges below T*. The abrupt onset of the internal field at T_SDW indicates that the SDW transition resembles a first-order phase change and is closely intertwined with the charge density wave (CDW) occurring at the same temperature. Under applied pressure, T_SDW, T*, and T_CDW are uniformly suppressed at a rate of approximately -13 K/GPa, differing from the behavior in bilayer La₃Ni₂O₇ where pressure increases the separation between SDW and CDW. Substitution of ¹⁶O with ¹⁸O raises T_CDW; in the region where CDW and SDW are intertwined, T_SDW also exhibits a significant isotope effect similar in magnitude to the shift in T_CDW, whereas no isotope effect is observed for the SDW at T* where it evolves independently. These results reveal the strongly intertwined nature of SDW and CDW in La₄Ni₃O₁₀ and suggest that pressure-induced suppression of the CDW order may be a key mechanism for high-pressure superconductivity in Ruddlesden-Popper nickelates.

Using first-principles density functional theory calculations, we systematically investigate the electron-doping effects of tetravalent element substitution in double-layer Ruddlesden-Popper nickelate La₃Ni₂O₇ thin films. Unlike cuprates, cerium (Ce) doping is found to be inefficient in introducing electron carriers into low-energy bands, whereas zirconium (Zr), hafnium (Hf), and thorium (Th) serve as effective electron dopants. These elemental substitutions significantly enhance the interlayer hopping integral t⊥ between Ni-dz² orbitals, potentially strengthening the interlayer superexchange coupling J⊥ and thereby potentially increasing the superconducting transition temperature Tc. Using the constrained random phase approximation to evaluate interaction parameters, we find that electron doping increases the occupancy of low-energy orbitals (including Ni-dx²-y² and dz² along with their hybridized oxygen orbitals) and alters the electron filling ratio between in-plane and interlayer orbitals. Structural analysis reveals that differences in dopant ionic radii cause variations in Ni–O bond lengths, with Zr and Hf inducing lattice contraction and Th exhibiting the strongest doping effect. These results indicate that Zr, Hf, and Th are promising candidates for achieving electron doping in La₃Ni₂O₇, offering a new avenue to clarify the ongoing debate over the electron pairing mechanism in this system.