Correlated electronic structures and unconventional superconductivity in bilayer nickelate heterostructures

TL;DR

This paper models the electronic structure of bilayer nickelate heterostructures, revealing correlation effects and unconventional superconductivity mechanisms, with implications for high-temperature superconductor design.

Contribution

It develops a comprehensive multi-orbital Hubbard model integrating ab initio and experimental data, accurately reproducing experimental Fermi surfaces and identifying spin-fluctuation-driven pairing.

Findings

Correlation effects are essential for Fermi surface topology.

Strong spin fluctuations lead to $s^{}$-wave pairing instability.

The approach accurately predicts superconducting tendencies without fine-tuning.

Abstract

The recent discovery of ambient-pressure superconductivity in thin-film bilayer nickelates opens new possibilities for investigating electronic structures in this new class of high-transition temperature $T_C$ superconductors. Here, we construct a realistic multi-orbital Hubbard model for the thin-film system, by integrating ab initio calculations with scanning transmission electron microscopy (STEM) measurements, which reveal a higher-symmetry lattice. The interaction parameters are calculated with the constrained random phase approximation (cRPA). Density functional theory (DFT) plus cluster dynamical mean-field theory (CDMFT) calculations, with cRPA calculated on-site Coulomb repulsive $U$ and experimentally measured electron filling $n$, quantitatively reproduces Fermi surfaces from angle-resolved photoemission spectroscopy (ARPES) experiments. The distinct Fermi surface topology from simple DFT+$U$ results features the indispensable role of correlation effects. Based upon the correlated electronic structures, A modified random-phase-approximation (RPA) approach yields a pronounced $s^{\pm}$-wave pairing instability, due to the strong spin fluctuations originated from Fermi surface nesting between bands with predominantly $d_{z^{2}}$ characters. Our findings highlight the quantitative effectiveness of the DFT+cRPA+CDMFT approach that precisely determines correlated electronic structure parameters without fine-tuning. The revealed intermediate correlation effect may explain the same order-of-magnitude onset $T_C$ observed both in pressured bulk and strained thin film bilayer nickelates.