Superexchanges and Charge Transfer in the La$_3$Ni$_2$O$_7$ Thin Films

TL;DR

This study investigates the electronic and magnetic properties of La$_3$Ni$_2$O$_7$ thin films using advanced computational methods, revealing weaker superexchange couplings and altered charge transfer characteristics compared to bulk, with implications for understanding superconductivity.

Contribution

It provides a detailed theoretical analysis of the magnetic interactions and charge transfer in La$_3$Ni$_2$O$_7$ thin films, highlighting differences from bulk material and informing future models.

Findings

Superexchange couplings are significantly weaker in films than in bulk.

Biaxial compression reduces the charge transfer gap.

Pronounced particle-hole asymmetry in orbital charge distribution.

Abstract

The recent discovery of ambient-pressure superconductivity with $T_c$ above 40 K in La$_3$Ni$_2$O$_7$ thin films represents a significant advance in the field of nickelate superconductor. Motivated by the experimental reports, here we study an 11-band $d-p$ Hubbard model with tight-binding parameters derived from \textit{ab initio} calculations, using large scale determinant quantum Monte Carlo and cellular dynamical mean-field theory. Our results reveal that the major superexchange couplings in La$_3$Ni$_2$O$_7$ thin films can be substantially weaker than in the bulk material at 29.5 Gpa. Specifically, the out-of-plane antiferromagnetic correlation between Ni$-d_{3z^2-r^2}$ orbitals is reduced by about 27\% in film, while the in-plane magnetic correlations remain largely unaffected. We evaluate the corresponding antiferromagnetic coupling constants, $J_{\perp}$ and $J_{\parallel}$ using perturbation theory. With regard to charge transfer properties, we find that the biaxial compression in films reduces charge transfer gap. We also resolve the orbital distribution of doped holes and electrons among the in-plane (Ni$-d_{x^2-y^2}$ and O$-p_x/p_y$) and the out-of-plane (Ni$-d_{3z^2-r^2}$ and O$-p_z$) orbitals, uncovering a pronounced particle-hole asymmetry. Theses findings lay a groundwork for the study of low-energy $t-J$ model of La$_3$Ni$_2$O$_7$ films and provide key insights into the understanding of physical distinctions between the film and bulk bilayer nickelates.