Valence, charge transfer, and orbital-dependent correlation in bilayer nickelates Nd 3 Ni 2 O 7

Takegami, Daisuke; Okauchi, Takaki; Morales, Edgar Abarca; Fujinuma, Koto; Furo, Mizuki; Yoshimura, Masato; Tsuei, Ku-Ding; Pan, Grace A.; Segedin, Dan Ferenc; Song, Qi; Paik, Hanjong; Brooks, Charles M.; Mundy, Julia A.; Mizokawa, Takashi; Tjeng, Liu Hao; Goodge, Berit H.; Hariki, Atsushi

doi:10.1103/PhysRevB.111.165101

Valence, charge transfer, and orbital-dependent correlation in bilayer nickelates ${Nd}_{3} {Ni}_{2} O_{7}$

Journal Article · Tue Apr 01 00:00:00 EDT 2025 · Physical Review. B

DOI:https://doi.org/10.1103/PhysRevB.111.165101· OSTI ID:2545119

; ; ; ; ; Yoshimura, Masato; Tsuei, Ku-Ding; ; Segedin, Dan Ferenc; Song, Qi; ; ; ; ; ; ;

We examine the bulk electronic structure of ${Nd}_{3} {Ni}_{2} O_{7}$ using Ni $2 p$ core-level hard x-ray photoemission spectroscopy combined with density functional theory $+$ dynamical mean-field theory. Our results reveal a large deviation of the Ni $3 d$ occupation from the formal ${Ni}^{2.5 +}$ valency, highlighting the importance of the charge transfer from oxygen ligands. We find that the dominant $d^{8}$ configuration is accompanied by nearly equal contributions from $d^{7}$ and $d^{9}$ states, exhibiting an unusual valence state among Ni-based oxides. Finally, we discuss the Ni $d_{x^{2} - y^{2}}$ and $d_{z^{2}}$ orbital-dependent hybridization, correlation and local spin dynamics.

Published by the American Physical Society 2025

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Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0021925

OSTI ID:: 2545119

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 16 Vol. 111; ISSN 2469-9950; ISSN PRBMDO

Publisher:: American Physical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Valence, charge transfer, and orbital-dependent correlation in bilayer nickelates ${Nd}_{3} {Ni}_{2} O_{7}$