Infinite-layer nickelates as Ni-e$$g$$ Hund’s metals
Abstract
The recent and exciting discovery of superconductivity in the hole-doped infinite-layer nickelate Nd1-$$δ$$Sr$$δ$$NiO2 draws strong attention to correlated quantum materials. From a theoretical viewpoint, this class of unconventional superconducting materials provides an opportunity to unveil a physics hidden in correlated quantum materials. Here we study the temperature and doping dependence of the local spectrum as well as the charge, spin and orbital susceptibilities from first principles. By using ab initio LQSGW+DMFT methodology, we show that onsite Hund’s coupling in Ni-$$d$$ orbitals gives rise to multiple signatures of Hund’s metallic phase in Ni-e$$g$$ orbitals. The proposed picture of the nickelates as an e$$g$$ (two orbital) Hund’s metal differs from the picture of the Fe-based superconductors as a five orbital Hund’s metal as well as the picture of the cuprates as doped charge transfer insulators. Our finding uncovers a new class of the Hund’s metals and has potential implications for the broad range of correlated two orbital systems away from half-filling.
- Authors:
-
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Korea Advanced Institute Science and Technology (KAIST), Daejeon (Korea, Republic of)
- Brookhaven National Laboratory (BNL), Upton, NY (United States); Rutgers University, Newark, NJ (United States)
- Brookhaven National Laboratory (BNL), Upton, NY (United States); Korea Institute for Advanced Study (KIAS), Seoul (Korea, Republic of)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Research Foundation of Korea (NRF)
- OSTI Identifier:
- 2007529
- Report Number(s):
- BNL-224868-2023-JAAM
Journal ID: ISSN 2397-4648
- Grant/Contract Number:
- SC0012704; AC02-05CH11231; 2018R1A2B2005204; 2018M3D1A1058754
- Resource Type:
- Accepted Manuscript
- Journal Name:
- npj Quantum Materials
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2397-4648
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Electronic properties and materials; Superconducting properties and materials
Citation Formats
Kang, Byungkyun, Melnick, Corey, Semon, Patrick, Ryee, Siheon, Han, Myung Joon, Kotliar, Gabriel, and Choi, Sangkook. Infinite-layer nickelates as Ni-e$g$ Hund’s metals. United States: N. p., 2023.
Web. doi:10.1038/s41535-023-00568-5.
Kang, Byungkyun, Melnick, Corey, Semon, Patrick, Ryee, Siheon, Han, Myung Joon, Kotliar, Gabriel, & Choi, Sangkook. Infinite-layer nickelates as Ni-e$g$ Hund’s metals. United States. https://doi.org/10.1038/s41535-023-00568-5
Kang, Byungkyun, Melnick, Corey, Semon, Patrick, Ryee, Siheon, Han, Myung Joon, Kotliar, Gabriel, and Choi, Sangkook. Wed .
"Infinite-layer nickelates as Ni-e$g$ Hund’s metals". United States. https://doi.org/10.1038/s41535-023-00568-5. https://www.osti.gov/servlets/purl/2007529.
@article{osti_2007529,
title = {Infinite-layer nickelates as Ni-e$g$ Hund’s metals},
author = {Kang, Byungkyun and Melnick, Corey and Semon, Patrick and Ryee, Siheon and Han, Myung Joon and Kotliar, Gabriel and Choi, Sangkook},
abstractNote = {The recent and exciting discovery of superconductivity in the hole-doped infinite-layer nickelate Nd1-$δ$Sr$δ$NiO2 draws strong attention to correlated quantum materials. From a theoretical viewpoint, this class of unconventional superconducting materials provides an opportunity to unveil a physics hidden in correlated quantum materials. Here we study the temperature and doping dependence of the local spectrum as well as the charge, spin and orbital susceptibilities from first principles. By using ab initio LQSGW+DMFT methodology, we show that onsite Hund’s coupling in Ni-$d$ orbitals gives rise to multiple signatures of Hund’s metallic phase in Ni-e$g$ orbitals. The proposed picture of the nickelates as an e$g$ (two orbital) Hund’s metal differs from the picture of the Fe-based superconductors as a five orbital Hund’s metal as well as the picture of the cuprates as doped charge transfer insulators. Our finding uncovers a new class of the Hund’s metals and has potential implications for the broad range of correlated two orbital systems away from half-filling.},
doi = {10.1038/s41535-023-00568-5},
journal = {npj Quantum Materials},
number = 1,
volume = 8,
place = {United States},
year = {Wed Jul 12 00:00:00 EDT 2023},
month = {Wed Jul 12 00:00:00 EDT 2023}
}
Works referenced in this record:
Nickelate superconductors—a renaissance of the one-band Hubbard model
journal, August 2020
- Kitatani, Motoharu; Si, Liang; Janson, Oleg
- npj Quantum Materials, Vol. 5, Issue 1
Linearized self-consistent quasiparticle GW method: Application to semiconductors and simple metals
journal, October 2017
- Kutepov, A. L.; Oudovenko, V. S.; Kotliar, G.
- Computer Physics Communications, Vol. 219
A substantial hybridization between correlated Ni-d orbital and itinerant electrons in infinite-layer nickelates
journal, May 2020
- Gu, Yuhao; Zhu, Sichen; Wang, Xiaoxuan
- Communications Physics, Vol. 3, Issue 1
Multitier self-consistent
journal, September 2017
- Nilsson, F.; Boehnke, L.; Werner, P.
- Physical Review Materials, Vol. 1, Issue 4
Correlated electronic structure of colossal thermopower : An ARPES and ab initio study
journal, May 2020
- Chikina, A.; Ma, J. -Z.; Brito, W. H.
- Physical Review Research, Vol. 2, Issue 2
Orbital-selective superconductivity in a two-band model of infinite-layer nickelates
journal, September 2020
- Adhikary, Priyo; Bandyopadhyay, Subhadeep; Das, Tanmoy
- Physical Review B, Vol. 102, Issue 10
Self-doped Mott insulator for parent compounds of nickelate superconductors
journal, January 2020
- Zhang, Guang-Ming; Yang, Yi-feng; Zhang, Fu-Chun
- Physical Review B, Vol. 101, Issue 2
Band gaps and electronic structure of transition-metal compounds
journal, July 1985
- Zaanen, J.; Sawatzky, G. A.; Allen, J. W.
- Physical Review Letters, Vol. 55, Issue 4
Hubbard model in infinite dimensions: A quantum Monte Carlo study
journal, July 1992
- Jarrell, M.
- Physical Review Letters, Vol. 69, Issue 1
Type-II model in superconducting nickelate
journal, May 2020
- Zhang, Ya-Hui; Vishwanath, Ashvin
- Physical Review Research, Vol. 2, Issue 2
Frequency-dependent local interactions and low-energy effective models from electronic structure calculations
journal, November 2004
- Aryasetiawan, F.; Imada, M.; Georges, A.
- Physical Review B, Vol. 70, Issue 19
Dynamical Mean-Field Theory Plus Numerical Renormalization-Group Study of Spin-Orbital Separation in a Three-Band Hund Metal
journal, September 2015
- Stadler, K. M.; Yin, Z. P.; von Delft, J.
- Physical Review Letters, Vol. 115, Issue 13
Orbital and spin character of doped carriers in infinite-layer nickelates
journal, December 2021
- Rossi, M.; Lu, H.; Nag, A.
- Physical Review B, Vol. 104, Issue 22
Hundness versus Mottness in a three-band Hubbard–Hund model: On the origin of strong correlations in Hund metals
journal, June 2019
- Stadler, K. M.; Kotliar, G.; Weichselbaum, A.
- Annals of Physics, Vol. 405
Hole superconductivity in infinite-layer nickelates
journal, November 2019
- Hirsch, J. E.; Marsiglio, F.
- Physica C: Superconductivity and its Applications, Vol. 566
Correlated fermions on a lattice in high dimensions
journal, December 1989
- M�ller-Hartmann, E.
- Zeitschrift f�r Physik B Condensed Matter, Vol. 74, Issue 4
A new construction of thermodynamic mean-field theories of itinerant fermions: application to the Falicov-Kimball model
journal, June 1991
- Janiš, V.
- Zeitschrift für Physik B Condensed Matter, Vol. 83, Issue 2
Sodium Hydride as a Powerful Reducing Agent for Topotactic Oxide Deintercalation: Synthesis and Characterization of the Nickel(I) Oxide LaNiO 2
journal, September 1999
- Hayward, M. A.; Green, M. A.; Rosseinsky, M. J.
- Journal of the American Chemical Society, Vol. 121, Issue 38
Model Construction and a Possibility of Cupratelike Pairing in a New Nickelate Superconductor
journal, August 2020
- Sakakibara, Hirofumi; Usui, Hidetomo; Suzuki, Katsuhiro
- Physical Review Letters, Vol. 125, Issue 7
Iron-Based Layered Superconductor La[O 1- x F x ]FeAs ( x = 0.05−0.12) with T c = 26 K
journal, March 2008
- Kamihara, Yoichi; Watanabe, Takumi; Hirano, Masahiro
- Journal of the American Chemical Society, Vol. 130, Issue 11
Lifshitz transition and frustration of magnetic moments in infinite-layer upon hole doping
journal, June 2020
- Leonov, I.; Skornyakov, S. L.; Savrasov, S. Y.
- Physical Review B, Vol. 101, Issue 24
Ab initio many-body correlations in the electronic structure of
journal, April 2020
- Olevano, Valerio; Bernardini, Fabio; Blase, Xavier
- Physical Review B, Vol. 101, Issue 16
Charge Disproportionation, Mixed Valence, and Janus Effect in Multiorbital Systems: A Tale of Two Insulators
journal, May 2019
- Isidori, Aldo; Berović, Maja; Fanfarillo, Laura
- Physical Review Letters, Vol. 122, Issue 18
Superconductivity seen in a non-magnetic nickel oxide
journal, August 2019
- Sawatzky, George A.
- Nature, Vol. 572, Issue 7771
Effective Hamiltonian for nickelate oxides
journal, February 2020
- Zhang, Hu; Jin, Lipeng; Wang, Shanmin
- Physical Review Research, Vol. 2, Issue 1
Janus-Faced Influence of Hund’s Rule Coupling in Strongly Correlated Materials
journal, December 2011
- de’ Medici, Luca; Mravlje, Jernej; Georges, Antoine
- Physical Review Letters, Vol. 107, Issue 25
Thermopower and Entropy: Lessons from
journal, July 2016
- Mravlje, Jernej; Georges, Antoine
- Physical Review Letters, Vol. 117, Issue 3
Breakdown of the scaling relation of anomalous Hall effect in Kondo lattice ferromagnet USbTe
journal, February 2023
- Siddiquee, Hasan; Broyles, Christopher; Kotta, Erica
- Nature Communications, Vol. 14, Issue 1
Formation of a two-dimensional single-component correlated electron system and band engineering in the nickelate superconductor
journal, November 2019
- Nomura, Yusuke; Hirayama, Motoaki; Tadano, Terumasa
- Physical Review B, Vol. 100, Issue 20
Hund-Heisenberg model in superconducting infinite-layer nickelates
journal, December 2020
- Chang, Jun; Zhao, Jize; Ding, Yang
- The European Physical Journal B, Vol. 93, Issue 12
Magnetic penetration depth and in superconducting nickelates
journal, February 2020
- Bernardini, F.; Olevano, V.; Cano, A.
- Physical Review Research, Vol. 2, Issue 1
Signatures of Mottness and Hundness in archetypal correlated metals
journal, June 2019
- Deng, Xiaoyu; Stadler, Katharina M.; Haule, Kristjan
- Nature Communications, Vol. 10, Issue 1
Synthesis of the infinite layer Ni(I) phase NdNiO2+x by low temperature reduction of NdNiO3 with sodium hydride
journal, June 2003
- Hayward, M. A.; Rosseinsky, M. J.
- Solid State Sciences, Vol. 5, Issue 6
Nonlocal Coulomb interaction and spin-freezing crossover as a route to valence-skipping charge order
journal, March 2020
- Ryee, Siheon; Sémon, Patrick; Han, Myung Joon
- npj Quantum Materials, Vol. 5, Issue 1
Thermodynamics and correlation functions of the Falicov-Kimball model in large dimensions
journal, September 1989
- Brandt, U.; Mielsch, C.
- Zeitschrift f�r Physik B Condensed Matter, Vol. 75, Issue 3
Orbital differentiation in Hund metals
journal, September 2019
- Kugler, Fabian B.; Lee, Seung-Sup B.; Weichselbaum, Andreas
- Physical Review B, Vol. 100, Issue 11
Coherence–incoherence crossover in the normal state of iron oxypnictides and importance of Hund's rule coupling
journal, February 2009
- Haule, K.; Kotliar, G.
- New Journal of Physics, Vol. 11, Issue 2
Discussion of the paper by de Boer and Verwey
journal, August 1937
- Mott, N. F.; Peierls, R.
- Proceedings of the Physical Society, Vol. 49, Issue 4S
Electronic structure of the parent compound of superconducting infinite-layer nickelates
journal, January 2020
- Hepting, M.; Li, D.; Jia, C. J.
- Nature Materials, Vol. 19, Issue 4
The Basis of the Electron Theory of Metals, with Special Reference to the Transition Metals
journal, July 1949
- Mott, N. F.
- Proceedings of the Physical Society. Section A, Vol. 62, Issue 7
Electronic structure of Pu and Am metals by self-consistent relativistic method
journal, April 2012
- Kutepov, Andrey; Haule, Kristjan; Savrasov, Sergey Y.
- Physical Review B, Vol. 85, Issue 15
Hund Physics Landscape of Two-Orbital Systems
journal, May 2021
- Ryee, Siheon; Han, Myung Joon; Choi, Sangkook
- Physical Review Letters, Vol. 126, Issue 20
First-principles treatment of Mott insulators: linearized QSGW+DMFT approach
journal, July 2016
- Choi, Sangkook; Kutepov, Andrey; Haule, Kristjan
- npj Quantum Materials, Vol. 1, Issue 1
Fluctuation-frustrated flat band instabilities in
journal, September 2020
- Choi, Mi-Young; Pickett, Warren E.; Lee, Kwan-Woo
- Physical Review Research, Vol. 2, Issue 3
Phase Diagram and Superconducting Dome of Infinite-Layer Thin Films
journal, October 2020
- Zeng, Shengwei; Tang, Chi Sin; Yin, Xinmao
- Physical Review Letters, Vol. 125, Issue 14
Extended dynamical mean-field theory and method
journal, August 2002
- Sun, Ping; Kotliar, Gabriel
- Physical Review B, Vol. 66, Issue 8
Hund’s Induced Fermi-Liquid Instabilities and Enhanced Quasiparticle Interactions
journal, April 2017
- de’ Medici, Luca
- Physical Review Letters, Vol. 118, Issue 16
Critical Nature of the Ni Spin State in Doped
journal, May 2020
- Jiang, Mi; Berciu, Mona; Sawatzky, George A.
- Physical Review Letters, Vol. 124, Issue 20
Hubbard model in infinite dimensions
journal, March 1992
- Georges, Antoine; Kotliar, Gabriel
- Physical Review B, Vol. 45, Issue 12
High-Spin to Low-Spin and Orbital Polarization Transitions in Multiorbital Mott Systems
journal, September 2007
- Werner, Philipp; Millis, Andrew J.
- Physical Review Letters, Vol. 99, Issue 12
Selective Mott Physics as a Key to Iron Superconductors
journal, April 2014
- de’ Medici, Luca; Giovannetti, Gianluca; Capone, Massimo
- Physical Review Letters, Vol. 112, Issue 17
Superconducting Dome in Infinite Layer Films
journal, July 2020
- Li, Danfeng; Wang, Bai Yang; Lee, Kyuho
- Physical Review Letters, Vol. 125, Issue 2
Robust -wave superconductivity of infinite-layer nickelates
journal, February 2020
- Wu, Xianxin; Di Sante, Domenico; Schwemmer, Tilman
- Physical Review B, Vol. 101, Issue 6
Orbital selectivity in Hund's metals: The iron chalcogenides
journal, January 2013
- Lanatà, Nicola; Strand, Hugo U. R.; Giovannetti, Gianluca
- Physical Review B, Vol. 87, Issue 4
Superconductivity from Emerging Magnetic Moments
journal, December 2015
- Hoshino, Shintaro; Werner, Philipp
- Physical Review Letters, Vol. 115, Issue 24
Possible highT c superconductivity in the Ba?La?Cu?O system
journal, June 1986
- Bednorz, J. G.; M�ller, K. A.
- Zeitschrift f�r Physik B Condensed Matter, Vol. 64, Issue 2
Nickelate superconductors: Multiorbital nature and spin freezing
journal, January 2020
- Werner, Philipp; Hoshino, Shintaro
- Physical Review B, Vol. 101, Issue 4
ComDMFT: A massively parallel computer package for the electronic structure of correlated-electron systems
journal, November 2019
- Choi, Sangkook; Semon, Patrick; Kang, Byungkyun
- Computer Physics Communications, Vol. 244
From quantum matter to high-temperature superconductivity in copper oxides
journal, February 2015
- Keimer, B.; Kivelson, S. A.; Norman, M. R.
- Nature, Vol. 518, Issue 7538
Improved conductivity of infinite-layer LaNiO2 thin films by metal organic decomposition
journal, December 2013
- Ikeda, Ai; Manabe, Takaaki; Naito, Michio
- Physica C: Superconductivity, Vol. 495
Iron-Based Layered Superconductor: LaOFeP
journal, August 2006
- Kamihara, Yoichi; Hiramatsu, Hidenori; Hirano, Masahiro
- Journal of the American Chemical Society, Vol. 128, Issue 31
Kinetic frustration and the nature of the magnetic and paramagnetic states in iron pnictides and iron chalcogenides
journal, September 2011
- Yin, Z. P.; Haule, K.; Kotliar, G.
- Nature Materials, Vol. 10, Issue 12
Impact of f-d Kondo cloud on superconductivity of nickelates
journal, March 2023
- Kang, Byungkyun; Kim, Hyunsoo; Zhu, Qiang
- Cell Reports Physical Science, Vol. 4, Issue 3
High‐Pressure Synthesis of A 2 NiO 2 Ag 2 Se 2 (A=Sr, Ba) with a High‐Spin Ni 2+ in Square‐Planar Coordination
journal, December 2018
- Matsumoto, Yuki; Yamamoto, Takafumi; Nakano, Kousuke
- Angewandte Chemie International Edition, Vol. 58, Issue 3
Two-band model for magnetism and superconductivity in nickelates
journal, December 2019
- Hu, Lun-Hui; Wu, Congjun
- Physical Review Research, Vol. 1, Issue 3
Hund’s coupling and its key role in tuning multiorbital correlations
journal, May 2011
- de’ Medici, Luca
- Physical Review B, Vol. 83, Issue 20
Electronic structure of rare-earth infinite-layer
journal, November 2019
- Jiang, Peiheng; Si, Liang; Liao, Zhaoliang
- Physical Review B, Vol. 100, Issue 20
Superconductivity in an infinite-layer nickelate
journal, August 2019
- Li, Danfeng; Lee, Kyuho; Wang, Bai Yang
- Nature, Vol. 572, Issue 7771
Hund-Enhanced Electronic Compressibility in FeSe and its Correlation with
journal, November 2018
- Villar Arribi, Pablo; de’ Medici, Luca
- Physical Review Letters, Vol. 121, Issue 19
Infinite-layer : is not
journal, October 2004
- Lee, K. -W.; Pickett, W. E.
- Physical Review B, Vol. 70, Issue 16
Correlated Lattice Fermions in Dimensions
journal, January 1989
- Metzner, Walter; Vollhardt, Dieter
- Physical Review Letters, Vol. 62, Issue 3
Late transition metal oxides with infinite-layer structure: Nickelates versus cuprates
journal, February 2020
- Lechermann, Frank
- Physical Review B, Vol. 101, Issue 8
First-Principles Approach to the Electronic Structure of Strongly Correlated Systems: Combining the Approximation and Dynamical Mean-Field Theory
journal, February 2003
- Biermann, S.; Aryasetiawan, F.; Georges, A.
- Physical Review Letters, Vol. 90, Issue 8
Dynamical mean-field theory of strongly correlated fermion systems and the limit of infinite dimensions
journal, January 1996
- Georges, Antoine; Kotliar, Gabriel; Krauth, Werner
- Reviews of Modern Physics, Vol. 68, Issue 1
Mott-Hubbard transition in infinite dimensions
journal, August 1992
- Rozenberg, M. J.; Zhang, X. Y.; Kotliar, G.
- Physical Review Letters, Vol. 69, Issue 8
Strong Correlations from Hund’s Coupling
journal, April 2013
- Georges, Antoine; Medici, Luca de'; Mravlje, Jernej
- Annual Review of Condensed Matter Physics, Vol. 4, Issue 1
Doping evolution of the Mott–Hubbard landscape in infinite-layer nickelates
journal, January 2021
- Goodge, Berit H.; Li, Danfeng; Lee, Kyuho
- Proceedings of the National Academy of Sciences, Vol. 118, Issue 2
Coherence-Incoherence Crossover and the Mass-Renormalization Puzzles in
journal, March 2011
- Mravlje, Jernej; Aichhorn, Markus; Miyake, Takashi
- Physical Review Letters, Vol. 106, Issue 9
Strongly correlated doped hole carriers in the superconducting nickelates: Their location, local many-body state, and low-energy effective Hamiltonian
journal, May 2021
- Lang, Zi-Jian; Jiang, Ruoshi; Ku, Wei
- Physical Review B, Vol. 103, Issue 18
Induced magnetic two-dimensionality by hole doping in the superconducting infinite-layer nickelate
journal, February 2020
- Ryee, Siheon; Yoon, Hongkee; Kim, Taek Jung
- Physical Review B, Vol. 101, Issue 6
Doping a Mott insulator: Physics of high-temperature superconductivity
journal, January 2006
- Lee, Patrick A.; Nagaosa, Naoto; Wen, Xiao-Gang
- Reviews of Modern Physics, Vol. 78, Issue 1
Hund's metal physics: From to
journal, October 2020
- Wang, Y.; Kang, C. -J.; Miao, H.
- Physical Review B, Vol. 102, Issue 16
Numerical solution of the d =∞ Hubbard model: Evidence for a Mott transition
journal, August 1992
- Georges, Antoine; Krauth, Werner
- Physical Review Letters, Vol. 69, Issue 8
Lattice-shifted nematic quantum critical point in FeSe1−xSx
journal, April 2021
- Chibani, S.; Farina, D.; Massat, P.
- npj Quantum Materials, Vol. 6, Issue 1
Direct observation of infinite NiO 2 planes in LaNiO 2 films
journal, May 2016
- Ikeda, Ai; Krockenberger, Yoshiharu; Irie, Hiroshi
- Applied Physics Express, Vol. 9, Issue 6
Strong correlations make high-temperature superconductors robust against disorder
journal, July 2008
- Garg, Arti; Randeria, Mohit; Trivedi, Nandini
- Nature Physics, Vol. 4, Issue 10
Orbital selective Kondo effect in heavy fermion superconductor UTe2
journal, June 2022
- Kang, Byungkyun; Choi, Sangkook; Kim, Hyunsoo
- npj Quantum Materials, Vol. 7, Issue 1
Spin Freezing Transition and Non-Fermi-Liquid Self-Energy in a Three-Orbital Model
journal, October 2008
- Werner, Philipp; Gull, Emanuel; Troyer, Matthias
- Physical Review Letters, Vol. 101, Issue 16
Orbital differentiation and the role of orbital ordering in the magnetic state of Fe superconductors
journal, November 2012
- Bascones, E.; Valenzuela, B.; Calderón, M. J.
- Physical Review B, Vol. 86, Issue 17