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Absence of mixed valency for Pr in pristine and hole-doped PrNiO2

Journal Article · · Physical Review. B
 [1];  [2];  [3]
  1. Univ. of Chicago, IL (United States)
  2. Argonne National Laboratory (ANL), Argonne, IL (United States)
  3. Univ. of Chicago, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
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Infinite-layer nickelates (𝑅⁒NiO2) exhibit some distinct differences as compared to cuprate superconductors, leading to a debate concerning the role of rare-earth ions (𝑅=La,Pr,Nd) in the low-energy many-body physics. Although rare-earth 4⁒𝑓 orbitals are typically treated as inert β€œcore” electrons in studies, this approximation has been questioned. An active participation of 4⁒𝑓 states is most likely for PrNiO2 based on an analogy to cuprates where Pr cuprates differ significantly from other cuprates. Here, we adopt density functional plus dynamical mean-field theory to investigate the role of Pr 4⁒𝑓 orbitals and more generally the correlated electronic structure of PrNiO2 and its hole-doped variant. We find that the Pr 4⁒𝑓 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 5⁒𝑑 and 4⁒𝑓 states further away from the Fermi energy whereas enhancing the Ni 3β’π‘‘βˆ’O 2⁒𝑝 hybridization, thus, reducing correlation effects as the O 2⁒𝑝 states get closer to the Fermi energy. We again find no evidence for either Kondo or Zhang-Rice physics for the 4⁒𝑓 states upon hole doping. Finally, we conclude by commenting on implications for other reduced valence nickelates.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
American Chemical Society Petroleum Research Fund (ACS-PRF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
2377395
Journal Information:
Physical Review. B, Journal Name: Physical Review. B Journal Issue: 16 Vol. 107; ISSN 2469-9950
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
Density functional theory
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Nickelates
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