Correlated Electronic Structure and Density-Wave Gap in Trilayer Nickelate La₄Ni₃O₁₀

Summary

The discovery of pressurized superconductivity at 80 K in La₃Ni₂O₇ officially brings nickelates into the family of high-temperature superconductors, which gives rise to not only new insights but also mysteries in the strongly correlated superconductivity. More recently, the sibling compound La₄Ni₃O₁₀ was also shown to be superconducting below about 25 K under pressure, further boosting the popularity of nickelates in the Ruddlesden-Popper phase. In this study, combining high-resolution angle-resolved photoemission spectroscopy and ab initio calculation, we systematically investigate the electronic structures of La₄Ni₃O₁₀ at ambient pressure. We reveal a high resemblance of La₄Ni₃O₁₀ with La₃Ni₂O₇ in the orbital-dependent fermiology and electronic structure, suggesting a similar electronic correlation between the two compounds. The temperature-dependent measurements imply an orbital-dependent energy gap related to the density-wave transition in La₄Ni₃O₁₀. B_y comparing the theoretical pressure-dependent electronic structure, clues about the superconducting high-pressure phase can be deduced from the ambient measurements, providing crucial information for deciphering the unconventional superconductivity in nickelates.

Materials

• La₄Ni₃O₁₀

Methods

• ARPES
• ab initio calculation

Keywords

• electronic correlation
• density wave gap
• orbital dependent fermiology
• unconventional superconductivity

Highlights

• B_y comparing theoretical pressure-dependent electronic structure, clues about the superconducting high-pressure phase can be deduced from ambient measurements.

Conclusions

• High resemblance of La₄Ni₃O₁₀ with La₃Ni₂O₇ in orbital-dependent fermiology and electronic structure, suggesting similar electronic correlation.
• Temperature-dependent measurements imply an orbital-dependent energy gap related to the density-wave transition in La₄Ni₃O₁₀.

Main claims

• La₄Ni₃O₁₀ and La₃Ni₂O₇ show high similarity in their orbital-dependent fermiology and electronic structure at ambient pressure.
  • Evidence: ARPES data reveal similar FS topology and energy dispersions; calculated band structures are analogous.
• An anisotropic energy gap related to the density-wave transition is observed in La₄Ni₃O₁₀, with stronger gap along Γ-S direction where dz2 and dx2-y2 hybridization is maximum.
  • Evidence: Temperature-dependent ARPES shows leading-edge shift of ≈12 meV along ΓS, negligible along ΓX for α band; β band shows smaller shift.

Workflow

• Crystal Growth and Characterization — La₄Ni₃O₁₀ shows a density-wave transition near 132 K.
  • Materials: La₄Ni₃O₁₀ single crystals
  • Methods: floating zone growth; Laue diffraction; magnetic susceptibility and specific heat
  • Observations: High-quality crystals; anomalies at ≈132 K in susceptibility and specific heat
• Angle-Resolved Photoemission Spectroscopy (ARPES) — Orbital-dependent energy gap related to density-wave transition with anisotropic character.
  • Materials: La₄Ni₃O₁₀ crystals
  • Methods: high-resolution ARPES (laser and synchrotron); temperature-dependent EDCs
  • Observations: Fermi surface with α, β, γ bands; γ band flat top near EF; gap opening below 130K
• Ab Initio Band Structure Calculations — Calculated bands agree with ARPES after orbital-dependent renormalization (5 for dz2, 3 for dx2-y2).
  • Materials: La₄Ni₃O₁₀
  • Methods: DFT with Wannier orbital construction
  • Observations: Band structure dominated by Ni eg orbitals; dz2 and dx2-y2 hybridized; bandwidth increases ≈20% at high pressure