Charge-Transfer Electronic Structure of NiX2 (X = S, Se)
Abstract
We investigate the electronic structures of NiS2 and NiSe2 using density functional theory combined with dynamical mean-field theory (DFT+DMFT). A realistic electronic structure within DFT+DMFT was determined by optimizing the double-counting correction to reproduce experimental valence-band photoemission spectra. The validity of the present model is further confirmed by its successful description of the Ni 2p core-level photoemission and Ni L-edge x-ray absorption spectra of NiS2. Our results reveal a smaller charge-transfer energy than previously assumed, resulting in substantial ligand-to-Ni charge transfer and a reduced Ni local moment. We clarify how the relative position and interaction between the Ni upper Hubbard band and the antibonding chalcogen-dimer states shape the evolution of the low-energy electronic structure across the NiS2−xSex series.
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BibTeX
@misc{hariki2026chargetransfer,
title = {{Charge-Transfer Electronic Structure of NiX$_2$ (X = S, Se)}},
author = {Atsushi Hariki and Takaki Okauchi and Daisuke Takegami and Naoki Ito and Mizuki Furo and Ayako Yamamoto and Tomoya Higo and Satoru Nakatsuji and Masato Yoshimura and Takashi Mizokawa and Jan Kunes},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.02148},
eprint = {2609.02148},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.02148},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Charge-Transfer Electronic Structure of NiX_2 (X = S, Se)
AU - Atsushi Hariki
AU - Takaki Okauchi
AU - Daisuke Takegami
AU - Naoki Ito
AU - Mizuki Furo
AU - Ayako Yamamoto
AU - Tomoya Higo
AU - Satoru Nakatsuji
AU - Masato Yoshimura
AU - Takashi Mizokawa
AU - Jan Kunes
PY - 2026
DA - 2026/09/02
PB - arXiv
DO - 10.48550/arxiv.2609.02148
UR - https://arxiv.org/abs/2609.02148
AB - We investigate the electronic structures of NiS_2 and NiSe_2 using density functional theory combined with dynamical mean-field theory (DFT+DMFT). A realistic electronic structure within DFT+DMFT was determined by optimizing the double-counting correction to reproduce experimental valence-band photoemission spectra. The validity of the present model is further confirmed by its successful description of the Ni 2p core-level photoemission and Ni L-edge x-ray absorption spectra of NiS_2. Our results reveal a smaller charge-transfer energy than previously assumed, resulting in substantial ligand-to-Ni charge transfer and a reduced Ni local moment. We clarify how the relative position and interaction between the Ni upper Hubbard band and the antibonding chalcogen-dimer states shape the evolution of the low-energy electronic structure across the NiS_2−xSe_x series.
ER -