Universal electronic structure of multi-layered nickelates via oxygen-centered planar orbitals
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| Format: | Preprint |
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2025
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| author | Au-Yeung, Christine C. Chen, X. Smit, S. Bluschke, M. Zimmermann, V. Michiardi, M. Moen, P. C. Kraan, J. Pang, C. S. B. Suen, C. T. Zhdanovich, S. Zonno, M. Gorovikov, S. Liu, Y. Levy, G. Elfimov, I. S. Berciu, M. Sawatzky, G. A. Mitchell, J. F. Damascelli, A. |
| author_facet | Au-Yeung, Christine C. Chen, X. Smit, S. Bluschke, M. Zimmermann, V. Michiardi, M. Moen, P. C. Kraan, J. Pang, C. S. B. Suen, C. T. Zhdanovich, S. Zonno, M. Gorovikov, S. Liu, Y. Levy, G. Elfimov, I. S. Berciu, M. Sawatzky, G. A. Mitchell, J. F. Damascelli, A. |
| contents | Superconductivity has been demonstrated in the family of multi-layered nickelates La$_3$Ni$_2$O$_7$ and La$_4$Ni$_3$O$_{10}$. Key questions remain open regarding the low-energy electronic states that support superconductivity in these compounds. Here we take advantage of the natural polymorphism between bilayer (2222) and alternating monolayer-trilayer (1313) stacking sequences that arises in bulk La$_3$Ni$_2$O$_7$ crystals, and by employing angle-resolved photoemission spectroscopy (ARPES) we identify a universal low-energy electronic structure in this family of materials. We observe the fingerprint of a doping-dependent spin-density wave (SDW) instability -- strong and coherent enough to reconstruct the Fermi surface, both by gapping out regions of the low-energy electronic structure as well as translating the $β$ pocket by a vector $Q_{tβ}$ consistent with the results of previous neutron and x-ray scattering experiments. Using an effective tight-binding model, we simulate the spectral weight distribution observed in our ARPES dichroism experiments and establish that the low-energy electronic phenomenology is dominated by oxygen-centered planar orbitals, which evolve from the $d_{3x^2-r^2}$ and $d_{3y^2-r^2}$ symmetry characteristic of 3-spin polarons (3SP) to the familiar $d_{x^2-y^2}$ Zhang-Rice singlets (ZRS) that support high-temperature superconductivity in cuprates. By inclusion of magnetic moments on plaquettes of oxygen orbitals in our model, we show that ZRS-like states mediate the SDW. Combined with the observation that oxygen annealing is required to induce superconductivity in both thin films and bulk La$_3$Ni$_2$O$_7$, this demonstrates that the ZRS population dictates whether the ground state favors density-wave order or superconductivity -- with hole doping suppressing the former and stabilizing the latter, as in the cuprates. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2502_20450 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Universal electronic structure of multi-layered nickelates via oxygen-centered planar orbitals Au-Yeung, Christine C. Chen, X. Smit, S. Bluschke, M. Zimmermann, V. Michiardi, M. Moen, P. C. Kraan, J. Pang, C. S. B. Suen, C. T. Zhdanovich, S. Zonno, M. Gorovikov, S. Liu, Y. Levy, G. Elfimov, I. S. Berciu, M. Sawatzky, G. A. Mitchell, J. F. Damascelli, A. Superconductivity Superconductivity has been demonstrated in the family of multi-layered nickelates La$_3$Ni$_2$O$_7$ and La$_4$Ni$_3$O$_{10}$. Key questions remain open regarding the low-energy electronic states that support superconductivity in these compounds. Here we take advantage of the natural polymorphism between bilayer (2222) and alternating monolayer-trilayer (1313) stacking sequences that arises in bulk La$_3$Ni$_2$O$_7$ crystals, and by employing angle-resolved photoemission spectroscopy (ARPES) we identify a universal low-energy electronic structure in this family of materials. We observe the fingerprint of a doping-dependent spin-density wave (SDW) instability -- strong and coherent enough to reconstruct the Fermi surface, both by gapping out regions of the low-energy electronic structure as well as translating the $β$ pocket by a vector $Q_{tβ}$ consistent with the results of previous neutron and x-ray scattering experiments. Using an effective tight-binding model, we simulate the spectral weight distribution observed in our ARPES dichroism experiments and establish that the low-energy electronic phenomenology is dominated by oxygen-centered planar orbitals, which evolve from the $d_{3x^2-r^2}$ and $d_{3y^2-r^2}$ symmetry characteristic of 3-spin polarons (3SP) to the familiar $d_{x^2-y^2}$ Zhang-Rice singlets (ZRS) that support high-temperature superconductivity in cuprates. By inclusion of magnetic moments on plaquettes of oxygen orbitals in our model, we show that ZRS-like states mediate the SDW. Combined with the observation that oxygen annealing is required to induce superconductivity in both thin films and bulk La$_3$Ni$_2$O$_7$, this demonstrates that the ZRS population dictates whether the ground state favors density-wave order or superconductivity -- with hole doping suppressing the former and stabilizing the latter, as in the cuprates. |
| title | Universal electronic structure of multi-layered nickelates via oxygen-centered planar orbitals |
| topic | Superconductivity |
| url | https://arxiv.org/abs/2502.20450 |