Distinguishing Electronic Band Structure of Single-layer and Bilayer Ruddlesden-Popper Nickelates Probed by in-situ High Pressure X-ray Absorption Near-edge Spectroscopy
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| Main Authors: | , , , , , , , , , , |
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| Format: | Preprint |
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2024
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| _version_ | 1866917795753623552 |
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| author | Li, Mingtao Wang, Yiming Pei, Cuiying Zhang, Mingxin Li, Nana Guan, Jiayi Amboage, Monica Adama, N-Diaye Kong, Qingyu Qi, Yanpeng Yang, Wenge |
| author_facet | Li, Mingtao Wang, Yiming Pei, Cuiying Zhang, Mingxin Li, Nana Guan, Jiayi Amboage, Monica Adama, N-Diaye Kong, Qingyu Qi, Yanpeng Yang, Wenge |
| contents | We report a comprehensive study of electronic band structure for single-layer (SL) and bilayer (BL) RP-nickelates probed by in-situ HP X-ray absorption near edge spectroscopy (XANES). At ambient pressure (AP), the energy splitting delta_E of d_3z^2-r^2 and d_x^2-y^2 bands are directly observed in La3Ni2O7 (BL-La327) but not in La2NiO4 (SL-La214) above E_F, underlining the critical role of inner apical O atoms. A combination of DFT-based electronic band structure and projected density of states (PDOS) calculations with simulated XANES enables us to explain the observed main XANES features labelled by a, A, B', B and C when considering the orbital hybridizations, crystal field splitting (CFS) and core-hole screening of different 3d configurations for SL-La214 and BL-La327 nickelates. At high pressure (HP), the delta_E values of pre-edge peak form a dome-like evolution above 7.7 GPa with the maximum locating at around 20 GPa for metallic BL-La327. Analysis of its integrated area and FWHM provides strong evidence that the bonding d_3z^2-r^2 band crosses E_F above about 7.7 GPa for the metallic BL-La327. Growth of integrated area of pre-edge peak and C peak further evidences pressure-induced hole doping effect. Meanwhile, the pressure dependent FWHM of pre-edge peak implies a nonmonotonic evolution of orbital-selective electronic correlation above 7.7 GPa with extrema emerging at about 20 GPa. Moreover, we estimate the relative hole doping level using the energy shift of pre-edge peak, yielding 0.074 hole per Ni site or equivalently 1.1*10^21 cm^-3 at 20 GPa for the metallic BL-La327, which is comparable to cuprates. Our results have timely examined the electronic band structures as obtained from theoretical calculations, emphasizing the essential role of both d_3z^2-r^2 and d_x^2-y^2 bands as well as the electronic correlation in superconducting pairing for pressurized La3Ni2O7. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2410_04230 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Distinguishing Electronic Band Structure of Single-layer and Bilayer Ruddlesden-Popper Nickelates Probed by in-situ High Pressure X-ray Absorption Near-edge Spectroscopy Li, Mingtao Wang, Yiming Pei, Cuiying Zhang, Mingxin Li, Nana Guan, Jiayi Amboage, Monica Adama, N-Diaye Kong, Qingyu Qi, Yanpeng Yang, Wenge Superconductivity Strongly Correlated Electrons We report a comprehensive study of electronic band structure for single-layer (SL) and bilayer (BL) RP-nickelates probed by in-situ HP X-ray absorption near edge spectroscopy (XANES). At ambient pressure (AP), the energy splitting delta_E of d_3z^2-r^2 and d_x^2-y^2 bands are directly observed in La3Ni2O7 (BL-La327) but not in La2NiO4 (SL-La214) above E_F, underlining the critical role of inner apical O atoms. A combination of DFT-based electronic band structure and projected density of states (PDOS) calculations with simulated XANES enables us to explain the observed main XANES features labelled by a, A, B', B and C when considering the orbital hybridizations, crystal field splitting (CFS) and core-hole screening of different 3d configurations for SL-La214 and BL-La327 nickelates. At high pressure (HP), the delta_E values of pre-edge peak form a dome-like evolution above 7.7 GPa with the maximum locating at around 20 GPa for metallic BL-La327. Analysis of its integrated area and FWHM provides strong evidence that the bonding d_3z^2-r^2 band crosses E_F above about 7.7 GPa for the metallic BL-La327. Growth of integrated area of pre-edge peak and C peak further evidences pressure-induced hole doping effect. Meanwhile, the pressure dependent FWHM of pre-edge peak implies a nonmonotonic evolution of orbital-selective electronic correlation above 7.7 GPa with extrema emerging at about 20 GPa. Moreover, we estimate the relative hole doping level using the energy shift of pre-edge peak, yielding 0.074 hole per Ni site or equivalently 1.1*10^21 cm^-3 at 20 GPa for the metallic BL-La327, which is comparable to cuprates. Our results have timely examined the electronic band structures as obtained from theoretical calculations, emphasizing the essential role of both d_3z^2-r^2 and d_x^2-y^2 bands as well as the electronic correlation in superconducting pairing for pressurized La3Ni2O7. |
| title | Distinguishing Electronic Band Structure of Single-layer and Bilayer Ruddlesden-Popper Nickelates Probed by in-situ High Pressure X-ray Absorption Near-edge Spectroscopy |
| topic | Superconductivity Strongly Correlated Electrons |
| url | https://arxiv.org/abs/2410.04230 |