English

Absence of mixed valency for Pr in pristine and hole-doped PrNiO$_2$

Strongly Correlated Electrons 2023-07-31 v2

Abstract

Infinite-layer nickelates (RRNiO2_2) exhibit some distinct differences as compared to cuprate superconductors, leading to a debate concerning the role of rare-earth ions (RR=La, Pr, Nd) in the low-energy many-body physics. Although rare-earth 4f4f orbitals are typically treated as inert `core' electrons in studies, this approximation has been questioned. An active participation of 4f4f states is most likely for PrNiO2_2 based on an analogy to cuprates where Pr cuprates differ significantly from other cuprates. Here, we adopt density functional plus dynamical mean field theory (DFT+DMFT) to investigate the role of Pr 4f4f orbitals and more generally the correlated electronic structure of PrNiO2_2 and its hole-doped variant. We find that the Pr 4f4f states are insulating and show no evidence for either a Kondo resonance or Zhang-Rice singlet formation as they do not have any hybridization channels near the Fermi energy. The biggest effects of hole doping are to shift the Pr 5d5d and 4f4f states further away from the Fermi energy while enhancing the Ni 3d3d - O 2p2p hybridization, thus reducing correlation effects as the O 2p2p states get closer to the Fermi energy. We again find no evidence for either Kondo or Zhang-Rice physics for the 4f4f states upon hole doping. We conclude by commenting on implications for other reduced valence nickelates.

Keywords

Cite

@article{arxiv.2302.08460,
  title  = {Absence of mixed valency for Pr in pristine and hole-doped PrNiO$_2$},
  author = {Xingyu Liao and Michael R. Norman and Hyowon Park},
  journal= {arXiv preprint arXiv:2302.08460},
  year   = {2023}
}

Comments

12 pages, 13 figures