Superexchanges and Charge Transfer in the La₃Ni₂O₇ Thin Films

The recent discovery of ambient-pressure superconductivity with T_c above 40 K in La₃Ni₂O₇ 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 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 La₃Ni₂O₇ 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_3z²-r² 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_⊥ and J_|| 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_x²-y² and O-p_x/p_y) and the out-of-plane (Ni-d_3z²-r² 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 La₃Ni₂O₇ films and provide key insights into the understanding of physical distinctions between the film and bulk bilayer nickelates.