Ground-state oxygen holes and the metal–insulator transition in the negative charge-transfer rare-earth nickelates
Abstract
The metal-insulator transitions and the intriguing physical properties of rare-earth perovskite nickelates have attracted considerable attention in recent years. However, a complete understanding of these materials remains elusive. Here, taking a NdNiO3 thin film as a representative example, we utilize a combination of x-ray absorption (XAS) and resonant inelastic x-ray scattering (RIXS) spectroscopies to resolve important aspects of the complex electronic structure of the rare-earth nickelates. The unusual coexistence of bound and continuum excitations observed in the RIXS spectra provides strong evidence for the abundance of oxygen 2p holes in the ground state of these materials. Using cluster calculations and Anderson impurity model interpretation, we show that these distinct spectral signatures arise from a Ni 3d8 configuration along with holes in the oxygen 2p valence band, confirming suggestions that these materials do not obey a “conventional” positive charge-transfer picture, but instead exhibit a negative charge-transfer energy, in line with recent models interpreting the metal to insulator transition in terms of bond disproportionation.
- Authors:
-
- Paul Scherrer Inst. (PSI), Villigen (Switzerland). Research Dept. Synchrotron Radiation and Nanotechnology; Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- Univ. of Geneva (Switzerland). Dept. of Quantum Matter Physics
- Univ. of British Columbia, Vancouver, BC (Canada). Dept. of Physics and Astronomy; Univ. of British Columbia, Vancouver, BC (Canada). Quantum Matter Inst.
- Univ. of Geneva (Switzerland). Dept. of Quantum Matter Physics
- Paul Scherrer Inst. (PSI), Villigen (Switzerland). Research Dept. Synchrotron Radiation and Nanotechnology; Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Lab. for Condensed Matter Physics, and Inst. of Physics
- Paul Scherrer Inst. (PSI), Villigen (Switzerland). Research Dept. Synchrotron Radiation and Nanotechnology
- Univ. of Geneva (Switzerland). Dept. of Quantum Matter Physics; University College London, London (United Kingdom). London Centre for Nanotechnology and Dept. of Physics and Astronomy
- Univ. of British Columbia, Vancouver, BC (Canada). Dept. of Physics and Astronomy
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1341699
- Report Number(s):
- BNL-113446-2017-JA
Journal ID: ISSN 2041-1723
- Grant/Contract Number:
- SC00112704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 7; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE
Citation Formats
Bisogni, Valentina, Catalano, Sara, Green, Robert J., Gibert, Marta, Scherwitzl, Raoul, Huang, Yaobo, Strocov, Vladimir N., Zubko, Pavlo, Balandeh, Shadi, Triscone, Jean-Marc, Sawatzky, George, and Schmitt, Thorsten. Ground-state oxygen holes and the metal–insulator transition in the negative charge-transfer rare-earth nickelates. United States: N. p., 2016.
Web. doi:10.1038/ncomms13017.
Bisogni, Valentina, Catalano, Sara, Green, Robert J., Gibert, Marta, Scherwitzl, Raoul, Huang, Yaobo, Strocov, Vladimir N., Zubko, Pavlo, Balandeh, Shadi, Triscone, Jean-Marc, Sawatzky, George, & Schmitt, Thorsten. Ground-state oxygen holes and the metal–insulator transition in the negative charge-transfer rare-earth nickelates. United States. https://doi.org/10.1038/ncomms13017
Bisogni, Valentina, Catalano, Sara, Green, Robert J., Gibert, Marta, Scherwitzl, Raoul, Huang, Yaobo, Strocov, Vladimir N., Zubko, Pavlo, Balandeh, Shadi, Triscone, Jean-Marc, Sawatzky, George, and Schmitt, Thorsten. Tue .
"Ground-state oxygen holes and the metal–insulator transition in the negative charge-transfer rare-earth nickelates". United States. https://doi.org/10.1038/ncomms13017. https://www.osti.gov/servlets/purl/1341699.
@article{osti_1341699,
title = {Ground-state oxygen holes and the metal–insulator transition in the negative charge-transfer rare-earth nickelates},
author = {Bisogni, Valentina and Catalano, Sara and Green, Robert J. and Gibert, Marta and Scherwitzl, Raoul and Huang, Yaobo and Strocov, Vladimir N. and Zubko, Pavlo and Balandeh, Shadi and Triscone, Jean-Marc and Sawatzky, George and Schmitt, Thorsten},
abstractNote = {The metal-insulator transitions and the intriguing physical properties of rare-earth perovskite nickelates have attracted considerable attention in recent years. However, a complete understanding of these materials remains elusive. Here, taking a NdNiO3 thin film as a representative example, we utilize a combination of x-ray absorption (XAS) and resonant inelastic x-ray scattering (RIXS) spectroscopies to resolve important aspects of the complex electronic structure of the rare-earth nickelates. The unusual coexistence of bound and continuum excitations observed in the RIXS spectra provides strong evidence for the abundance of oxygen 2p holes in the ground state of these materials. Using cluster calculations and Anderson impurity model interpretation, we show that these distinct spectral signatures arise from a Ni 3d8 configuration along with holes in the oxygen 2p valence band, confirming suggestions that these materials do not obey a “conventional” positive charge-transfer picture, but instead exhibit a negative charge-transfer energy, in line with recent models interpreting the metal to insulator transition in terms of bond disproportionation.},
doi = {10.1038/ncomms13017},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {Tue Oct 11 00:00:00 EDT 2016},
month = {Tue Oct 11 00:00:00 EDT 2016}
}
Web of Science
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Bond disproportionation and dynamical charge fluctuations in the perovskite rare earth nickelates
text, January 2016
- Green, Robert J.; Haverkort, Maurits W.; Sawatzky, George A.
- arXiv
Mott Transition and Magnetism in Rare Earth Nickelates and its Fingerprint on the X-ray Scattering
text, January 2017
- Haule, Kristjan; Pascut, Gheorghe L.
- arXiv
Electronic structure of Pr2MnNiO6 from x-ray photoemission, absorption and density functional theory
text, January 2017
- Balasubramanian, Padmanabhan; Joshi, Shalik Ram; Yadav, Ruchika
- arXiv
Continuum Charge Excitations in High-Valence Transition-Metal Oxides Revealed by Resonant Inelastic X-ray Scattering
text, January 2018
- Hariki, Atsushi; Winder, Mathias; Kuneš, Jan
- arXiv
Phenomenological Three-Orbital Spin-Fermion Model for Cuprates
text, January 2018
- Hussein, Mostafa Sherif Derbala Aly; Daghofer, Maria; Dagotto, Elbio
- arXiv
Emergent c-axis magnetic helix in manganite-nickelate superlattices
text, January 2018
- Fabbris, G.; Jaouen, N.; Meyers, D.
- arXiv
Epitaxial strain modulated electronic properties of interface controlled nickelate superlattice
text, January 2018
- Middey, S.; Meyers, D.; Ojha, Shashank Kumar
- arXiv
Fingerprints of an Exotic Orbital-Selective Mott Phase in the Block Magnetic State of BaFe$_2$Se$_3$ Ladders
text, January 2018
- Patel, Niravkumar D.; Nocera, Alberto; Alvarez, Gonzalo
- arXiv
Complex magnetic order in nickelate slabs
text, January 2019
- Hepting, Matthias; Green, Robert J.; Zhong, Zhicheng
- arXiv
High pO2 Floating Zone Crystal Growth of the Perovskite Nickelate PrNiO3
text, January 2019
- Zheng, Hong; Zhang, Junjie; Wang, Bixia
- arXiv
Conductivity noise across temperature driven transitions of rare-earth nickelate heterostructures
text, January 2019
- Daptary, Gopi Nath; Kumar, Siddharth; Kareev, M.
- arXiv
Electronic Localization in CaVO3 Films via Bandwidth Control
text, January 2019
- McNally, Daniel E.; Lu, Xingye; Pelliciari, Jonathan
- arXiv
Electronic structure of the parent compound of superconducting infinite-layer nickelates
text, January 2019
- Hepting, M.; Li, D.; Jia, C. J.
- arXiv
Structurally triggered metal-insulator transition in rare-earth nickelates
journal, November 2017
- Mercy, Alain; Bieder, Jordan; Íñiguez, Jorge
- Nature Communications, Vol. 8, Issue 1
Experimental evidence for bipolaron condensation as a mechanism for the metal-insulator transition in rare-earth nickelates
journal, January 2018
- Shamblin, Jacob; Heres, Maximilian; Zhou, Haidong
- Nature Communications, Vol. 9, Issue 1
Transmission zone plates as analyzers for efficient parallel 2D RIXS-mapping
journal, August 2017
- Marschall, Felix; Yin, Zhong; Rehanek, Jens
- Scientific Reports, Vol. 7, Issue 1
Mott Transition and Magnetism in Rare Earth Nickelates and its Fingerprint on the X-ray Scattering
journal, September 2017
- Haule, Kristjan; Pascut, Gheorghe L.
- Scientific Reports, Vol. 7, Issue 1
Finite-temperature phase diagram of (111) nickelate bilayers
journal, September 2018
- Janson, Oleg; Held, Karsten
- Physical Review B, Vol. 98, Issue 11
Observation of an antiferromagnetic quantum critical point in high-purity LaNiO$_3$
text, January 2020
- Liu, Changjiang; Humbert, Vincent F. C.; Bretz-Sullivan, Terence
- arXiv
Site-Selective Probe of Magnetic Excitations in Rare-Earth Nickelates Using Resonant Inelastic X-ray Scattering
text, January 2018
- Lu, Y.; Betto, D.; Fürsich, K.
- Karlsruhe