Paper

Using polarization-resolved electronic Raman scattering measurements on high-quality La₃Ni₂O₇ single crystals, we observe a pronounced, symmetry-dependent spectral weight redistribution across the density-wave transition below 150 K: the B₁g channel exhibits an asymmetric peak, while the B₂g channel shows a symmetric broad peak, corresponding to electronic excitations near the X/Y points of the Brillouin zone and along the diagonal directions, respectively. Quantitative analysis extracts two sets of SDW gap values, with the B₁g channel gap approximately 37.5–40.4 meV (2Δ/kBTc ≈ 5.5–5.9) and the B₂g channel gap about 23.0 meV (2Δ/kBTc ≈ 3.4), indicating intermediate-to-strong coupling for the former and weak coupling for the latter. This momentum-selective anisotropic coupling strength cannot be explained by simple weak-coupling nesting theory, revealing that the unconventional SDW originates from anisotropic electronic correlations. The temperature dependence of the gap is significantly weaker than mean-field expectations, and the isotropy of the B₂g channel along with the weak anisotropy of the B₁g channel further support the coexistence of two distinct coupling mechanisms. This work establishes the electronic characteristics of the SDW in La₃Ni₂O₇, providing a microscopic foundation for understanding the emergence of high-temperature superconductivity in nickelates under pressure.

This study employs first-principles density functional theory (GGA and GGA+U) to investigate the electronic and magnetic properties of La3Ni2O5F, which features a bilayer NiO2 infinite-layer structure where La(O/F)La blocking layers achieve strict isolation of the NiO2 bilayers, forming a purely two-dimensional electronic and magnetic system. Calculations reveal an E* single band composed of electron density in the interstitial region, which is not associated with any atomic orbital, dips below the Fermi level along the M-A direction, and provides a self-doping of 0.09 holes per Ni, resulting in an actual Ni valence of +1.09; the Fermi surface of this E* band is cylindrical, occupying 9% of the Brillouin zone area. The dpσ band is nearly half-filled but is shifted near a Van Hove singularity due to the self-doping, and the magnetic response exhibits anomalous characteristics distinct from previous nickelates, with the magnetic susceptibility tending to vanish under a large magnetic field. The absence of a magnetic phase transition can be attributed to strong two-dimensional spin fluctuations and the self-doping effect away from half-filling, revealing the unique behavior of Ni¹⁺ ions in this system and the critical influence of the interfacial blocking layer on the interstitial band morphology.

This study employs atomic-resolution scanning tunneling microscopy and spectroscopy to characterize 1.5 unit-cell-thick (La,Pr)₃Ni₂O₇ ultrathin films grown on SrLaAlO₄. Through low-temperature ultrahigh vacuum sample transfer, an ordered √2×√2 surface reconstruction is preserved, and a U-shaped spectrum with two gap scales (approximately 14 and 20 meV) and a flat zero-bias conductance is observed in the tunneling spectra, indicating a nodeless superconducting gap. In contrast, if the sample is exposed to ultrahigh vacuum for a longer time during transfer without cooling, although the surface reconstruction and a transport superconducting onset temperature above 40 K are maintained, the tunneling spectrum becomes V-shaped, and the wide-energy spectrum shows that oxygen deficiency mixes spectral weight related to density waves. By comparing samples with different transfer times, it is determined that controlling the oxygen content is necessary to obtain an intrinsic superconducting gap, providing atomic-scale observational evidence for the intrinsic nodeless superconducting gap in bilayer nickelate ultrathin films.

This study realized a superconductor-insulator transition by fabricating infinite-layer samarium nickel oxide superconducting thin films into a spatially periodic network structure, thereby modulating the phase coherence of Cooper pairs. The observation of magnetoresistance oscillations with a period of h/2e in the experiments directly confirmed the existence of 2e Cooper pairs in nickel oxides. The transition was primarily driven by enhanced superconducting fluctuations, with Cooper pairs participating in charge transport throughout the entire transition process. Two anomalous metallic states were also identified: one emerging under finite magnetic fields and the other appearing even at zero magnetic field; both states could be characterized by bosonic excitations, suggesting the dynamic role of vortices in the ground state. This work establishes nickel oxides as a key platform for studying the rich bosonic phases arising from the modulation of Cooper pair phase coherence.

Bosonic Phases across the Superconductor-Insulator Transitions in Infinite-Layer Samarium Nickelate

This study systematically investigates the superconductivity of compressively strained La₂LnNi₂O₇ thin films (Ln = lanthanide) under ambient and high pressure to clarify the relationship between ambient-pressure and high-pressure superconducting mechanisms. By suppressing the superconducting state with a 59 T magnetic field, the normal-state resistivity at ambient pressure tends toward T² behavior; after applying high pressure in a cubic anvil chamber, Tc increases from 41–42 K at ambient pressure to 67–73 K at 16 GPa. However, lattice compression induced by Ln substitution, although it may mimic pressure effects, lowers Tc. In both cases, Tc correlates with the evolution of normal-state transport between T² and T-linear behavior, indicating that lattice structural changes in bilayer nickelates have an important influence on superconductivity and providing clues for understanding the intrinsic connection between ambient-pressure strained films and high-pressure bulk superconducting states.

The Ruddlesden–Popper (R–P) bilayer nickelate, La3Ni2O7, was recently found to show signatures of high-temperature superconductivity (HTSC) at pressures above 14 GPa (ref. 1). Subsequent investigations achieved zero resistance in single-crystalline and polycrystalline samples under hydrostatic pressure conditions2–4. Yet, obvious diamagnetic signals, the other hallmark of superconductors, are still lacking owing to the filamentary nature with low superconducting volume fraction2,4,5. The presence of a new 1313 polymorph and competing R–P phases obscured proper identification of the phase for HTSC6–9. Thus, achieving bulk HTSC and identifying the phase at play are the most prominent tasks. Here we address these issues in the praseodymium (Pr)-doped La2PrNi2O7 polycrystalline samples. We find that substitutions of Pr for La effectively inhibit the intergrowth of different R–P phases, resulting in a nearly pure bilayer structure. For La2PrNi2O7, pressure-induced orthorhombic to tetragonal structural transition takes place at Pc ≈ 11 GPa, above which HTSC emerges gradually on further compression. The superconducting transition temperatures at 18–20 GPa reach $${T}_{{\rm{c}}}^{{\rm{onset}}}=82.5\,{\rm{K}}$$and $${T}_{{\rm{c}}}^{{\rm{zero}}}=60\,{\rm{K}}$$, which are the highest values, to our knowledge, among known nickelate superconductors. Importantly, bulk HTSC was testified by detecting clear diamagnetic signals below about 75 K with appreciable superconducting shielding volume fractions at a pressure of above 15 GPa. Our results not only resolve the existing controversies but also provide directions for exploring bulk HTSC in the bilayer nickelates.

Recently, the Ruddlesden–Popper bilayer nickelate La3Ni2O7 has emerged as a superconductor with a transition temperature (Tc) of approximately 80 K above 14 GPa (refs. 1–3). Achieving a higher Tc in nickelate superconductors, along with the synthesis of reproducible high-quality single crystals without relying on high-oxygen-pressure growth conditions, remains a significant challenge4–7. Here we report superconductivity up to 96 K under high pressure in bilayer nickelate single crystals synthesized at ambient pressure. Energy-dispersive spectroscopy, single-crystal X-ray diffraction, nuclear quadrupole resonance and scanning transmission electron microscopy evidenced high crystal quality of the flux-grown La2SmNi2O7−δ single crystals. La2SmNi2O7 exhibits clear bulk superconductivity, including zero resistivity ( $${T}_{{\rm{c}},\max }^{{\rm{onset}}}$$ = 92 K and $${T}_{{\rm{c}},\max }^{{\rm{zero}}}$$ = 73 K at 21.6 GPa) and the Meissner effect (Tc = 60 K at 20.6 GPa). A low-temperature high-pressure structural study indicates that both monoclinic and tetragonal structures can support superconductivity in this bilayer nickelate. Furthermore, we established a correlation between higher Tc under high pressures and larger in-plane lattice distortion under ambient conditions, corroborated by observing even higher $${T}_{{\rm{c}}}^{{\rm{onset}}}$$of 96 K in La1.57Sm1.43Ni2O7−δ. This study overcomes key limitations in growing nickelate superconductor crystals, resolves the crystal structure in the superconducting state and demonstrates an effective pathway towards achieving higher Tc.

Based on the effective three-orbital model, this study systematically analyzes the interplay between multiorbital and nonlocal self-energy effects in the normal state of the high-pressure superconducting bilayer nickelate La₃Ni₂O₇ using the D-TRILEX many-body framework beyond dynamical mean-field theory. The results reveal that the low-energy physics is highly dependent on the interorbital interaction strength: when the interaction is weak, the renowned γ quasiparticle flat band lies below the Fermi level; as the interaction strengthens, this flat band crosses the Fermi level, causing electrons to scatter with ferromagnetic paramagnon excitations, thereby forming spin-polaron bound states. These bound states manifest as incoherent spectral weight shadow bands below the Fermi level. The findings unveil the existence of additional competing electronic states in bilayer nickelates, providing a theoretical basis for resolving recent controversies in angle-resolved photoemission spectroscopy experiments regarding spectral structures near the Fermi surface.

Resonant inelastic X-ray scattering (RIXS) at the Ni L edge on single crystals of the trilayer nickelate La4Ni3O10 reveals collective spin excitations with a bandwidth of approximately 60 meV, comparable to that of the bilayer nickelate La3Ni2O7, but with significantly reduced spectral weight, indicating weaker electronic correlations in the trilayer system. Localized spin excitations at around 100 and 200 meV are also observed, originating from local dipole and quadrupole excitations. The dispersive magnetic excitations exhibit three-dimensional characteristics, and fitting with linear spin-wave theory yields comparable in-plane and out-of-plane exchange coupling parameters, with the interlayer coupling being the strongest. The results indicate that La4Ni3O10 possesses stronger three-dimensional magnetism, with its spin dynamics consistent with spin-density-wave order, while the reduced electronic correlations and three-dimensional multi-orbital character are key factors leading to differences in its magnetic excitation spectrum compared to the bilayer nickelate, providing important insights into the evolution of magnetism and its connection to superconductivity in the Ruddlesden-Popper nickelate family.