Electron doping induces metal-to-insulator transition (MIT) in ${\mathrm{SmNiO}}_3$ as realized by experiments. While earlier density functional theory (DFT) studies with static correlations fell short of explaining the recent MIT observations at lower hydrogen concentrations, we present a comprehensive computational investigation employing an advanced approach. We combine DFT with dynamical mean field theory $(\mathrm{DFT}+\mathrm{DMFT})$ to efficiently analyze the insulating behavior of hydrogen-doped ${\mathrm{SmNiO}}_3$. In contrast to previous theoretical works, our calculations predict an insulator transition occurring at a reduced doping level of H:Ni = 0.5:1. Specifically, while the $\mathrm{DFT}+U$ method reveals a gap opening between $p\text{−}\mathrm{to}\text{−}d$ orbitals, the DMFT approach highlights a gap opening between $d\text{−}\mathrm{to}\text{−}d$ orbitals. Our findings uncover a selective Mott transition in site and orbital characteristics, with the Ni ions proximate to the doped hydrogen exhibiting Mott-like traits. Notably, DMFT calculations highlight a pronounced dependence on Hund's parameter $J$, implying the presence of Hundness in the Mott insulator. This study underscores the necessity of accounting for dynamical correlations to accurately describe the electronic structure of strongly correlated electron-doped rare-earth nickelates.

• Received 27 August 2023
• Accepted 25 April 2024

DOI:https://doi.org/10.1103/PhysRevB.109.205124