Orbital polarization, charge transfer, and fluorescence in reduced-valence nickelates

Norman, M. R.; Botana, A. S.; Karp, J.; Hampel, A.; LaBolita, H.; Millis, A. J.; Fabbris, G.; Shen, Y.; Dean, M. M.

doi:10.1103/physrevb.107.165124

Title: Orbital polarization, charge transfer, and fluorescence in reduced-valence nickelates

Journal Article · Wed Apr 12 00:00:00 EDT 2023 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.107.165124· OSTI ID:1969911

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Argonne National Laboratory (ANL), Lemont, IL (United States)
Arizona State University, Tempe, AZ (United States)
Columbia University, New York, NY (United States)
Flatiron Institute, New York, NY (United States)
Arizona State University, Tempe, AZ (United States); Flatiron Institute, New York, NY (United States)
Flatiron Institute, New York, NY (United States); Columbia University, New York, NY (United States)
Argonne National Laboratory (ANL), Lemont, IL (United States). Advanced Photon Source (APS)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Condensed Matter Physics

Herein this paper presents a simple formalism for calculating X-ray absorption (XAS) and resonant inelastic x-ray scattering (RIXS) that has as input orbital-resolved density of states from a single particle or many-body ab initio calculation and is designed to capture itinerant-like features. We use this formalism to calculate both the XAS and RIXS with input from DFT and DFT + DMFT for the recently studied reduced valence nickelates R₄Ni₃O₈ and RNiO₂ (R = rare earth), and these results are then contrasted with those for the cuprate CaCuO₂ and the unreduced nickelate R₄Ni₃O₁₀. In contrast to the unreduced R₄Ni₃O₁₀, the reduced valence nickelates as well as the cuprate show strong orbital polarization due to the dominance of x² – y² orbitals for the unoccupied 3d states. We also reproduce two key aspects of a recent RIXS experiment for R₄Ni₃O₈: (i) a charge transfer feature between 3d and oxygen 2p states whose energy we find to decrease as one goes from RNiO₂ to R₄Ni₃O₈ to the cuprate, and (ii) an energy-dependent polarization reversal of the fluorescence line that arises from hybridization of the unoccupied 3z² –r² states with R 5d states. We end with some implications of our results for the nature of the 3d electrons in reduced valence nickelates.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; AC02-06CH11357; SC0022311; DMR-2045826

OSTI ID:: 1969911

Alternate ID(s):: OSTI ID: 1970739

Report Number(s):: BNL-224242-2023-JAAM; TRN: US2313457

Journal Information:: Physical Review. B, Vol. 107, Issue 16; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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