Pressure-Driven Evolution of Electronic and Magnetic Correlations in Bilayer Nickelate La3Ni2O7

Abstract

The recent discovery of high-temperature superconductivity in pressurized bilayer La3Ni2O7 has sparked intense research interest, yet the microscopic mechanism governing its pressure-dependent superconducting transition temperature (Tc) remains elusive. In this work, we investigate the electronic and magnetic correlations of La3Ni2O7 under high pressure using a combination of density-functional theory (DFT), constrained random phase approximation (cRPA), and dynamical mean-field theory (DMFT). We find that while hydrostatic pressure enhances the interlayer hopping and the bare superexchange energy scale (4t2/U), it simultaneously drives the system toward a more itinerant regime by reducing the relative correlation strength (U/W). Crucially, our results reveal a distinct orbital-selective evolution: the Ni dx2-y2 states become increasingly itinerant, whereas the Ni dz2 orbitals retain a more localized character. This pressure-induced itinerancy significantly enhances the hybridization between the two, leading to a dramatic amplification of the Kondo-like screening of the local dz2 moments by the itinerant dx2-y2 electrons. Consequently, the effective magnetic exchange coupling (Jeff), which serves as the pairing glue, is suppressed in the high-pressure regime. Our findings suggest that the monotonic decrease of Tc at high pressures is driven by the dominance of Kondo screening over superexchange interactions, providing a coherent microscopic explanation for the dome-shaped superconducting phase diagram in La3Ni2O7.