-
The bilayer nickelate La3Ni2O7, a member of the Ruddlesden–Popper series, has recently garnered significant attention due to its superconductivity under high pressure (above 14 GPa) with a transition temperature of approximately 80 K [1]. Its unique bilayer structure results in an electronic configuration significantly distinct from those observed in cuprates and infinite-layer nickelates. Consequently, understanding its correlated electronic structure and superconducting mechanism has emerged as a topic of major scientific importance. Recent experimental observations have further identified the coexistence of charge and spin density wave orders in La3Ni2O7, suggesting a complex interplay among various competing electronic phases and superconductivity.
In this work, we investigate the charge order in La3Ni2O7 using a low-energy effective model that explicitly includes the Ni-eg orbitals. By employing a combined density functional theory and dynamical mean-field theory (DFT+DMFT) framework, we systematically explore the impact of the nearest-neighbor Coulomb interaction V on charge ordering and electronic correlation effects, with nonlocal interactions treated at the Hartree approximation level. Our computational methodology features a newly developed tensor-network impurity solver utilizing a natural-orbital basis and complex-time evolution, facilitating effcient and precise evaluations of the Green’s function on the real-frequency axis.
Our analysis reveals that for interaction strengths below a critical value (V ≤ Vc1 ≈ 0.46 eV), the system maintains sublattice symmetry, resulting in minimal changes to the spectral function. Several high-energy fine structures identified within the Hubbard bands correspond to remnants of atomic multiplet excitations, allowing extraction of effective Hubbard parameters. When V > Vc1, the sublattice symmetry breaks, and the system transitions into a charge-ordered state. Spectral features evolve systematically with increasing charge order, providing a clear benchmark to quantitatively assess the degree of charge disproportionation against experimental data. The quasiparticle weight Z exhibits a nonmonotonic behavior with increasing V , reaching a minimum near V ≈ 0.60 eV in the more populated sublattice as it approaches half-filling. Upon further increasing the interaction beyond Vc2 ≈ 0.63 eV, the system becomes fully charge polarized, characterized by one sublattice becoming nearly empty and the other approaching three-quarter filling.
These findings underscore the critical role of nonlocal Coulomb interactions in driving charge disproportionation and tuning electronic correlations, thereby offering fresh insights into the low-energy ordering phenomena of bilayer nickelates. -
[1] Sun H L, Huo M W, Hu X W, Li J Y, Liu Z J, Han Y F, Tang L Y, Mao Z Q, Yang P T, Wang B S, Cheng J G, Yao D X, Zhang G M, Wang M 2023 Nature 621 493
[2] Wang M, Wen H H, Wu T, Yao D X, Xiang T 2024 Chin. Phys. Lett. 41 077402
[3] Lee P A, Nagaosa N, Wen X G 2006 Rev. Mod. Phys. 78 17
[4] Keimer B, Kivelson S A, Norman M R, Uchida S, Zaanen J 2015 Nature 518 179
[5] Botana A S, Norman M R 2020 Phys. Rev. X 10 011024
[6] Luo Z H, Hu X W, Wang M, Wu W, Yao D X 2023 Phys. Rev. Lett. 131 126001
[7] Zhang Y, Lin L F, Moreo A, Dagotto E 2023 Phys. Rev. B 108 L180510
[8] Christiansson V, Petocchi F, Werner P 2023 Phys. Rev. Lett. 131 206501
[9] Oh H, Zhang Y H 2023 Phys. Rev. B 108 174511
[10] LaBollita H, Pardo V, Norman M R, Botana A S 2024 arXiv:2309.17279 [cond-mat.str-el]
[11] Lechermann F, Gondolf J, Bötzel S, Eremin I M 2023 Phys. Rev. B 108 L201121
[12] Qu X Z, Qu D W, Chen J L, Wu C J, Yang F, Li W, Su G 2024 Phys. Rev. Lett. 132 036502
[13] Shilenko D A, Leonov I V 2023 Phys. Rev. B 108 125105
[14] Wu W, Luo Z H, Yao D X, Wang M 2024 Sci. China Phys. Mech. Astron 67 117402
[15] Yang Y F, Zhang G M, Zhang F C 2023 Phys. Rev. B 108 L201108
[16] Cao Y Y, Yang Y F 2024 Phys. Rev. B 109 L081105
[17] Gu Y H, Le C C, Yang Z S, Wu X X, Hu J P 2023 arXiv:2306.07275 [cond-mat.supr-con]
[18] Liu Y B, Mei J W, Ye F, Chen W Q, Yang F 2023 Phys. Rev. Lett. 131 236002
[19] Shen Y, Qin M P, Zhang G M 2023 Chin. Phys. Lett. 40 127401
[20] Yang Q G, Wang D, Wang Q H 2023 Phys. Rev. B 108 L140505
[21] Zhang Y, Lin L F, Moreo A, Maier T A, Dagotto E 2024 Nat. Commun. 15 2470
[22] Lu C, Pan Z M, Yang F, Wu C J 2024 Phys. Rev. Lett. 132 146002
[23] Fan Z, Zhang J F, Zhan B, Lv D S, Jiang X Y, Normand B, Xiang T 2024 Phys. Rev. B 110 024514
[24] Jiang K, Wang Z Q, Zhang F C 2024 Chin. Phys. Lett. 41 017402
[25] Xia C L, Liu H Q, Zhou S J, Chen H H 2025 Nat. Commun. 16 1054
[26] Wang Y X, Zhang Y, Jiang K 2025 Chin. Phys. B 34 047105
[27] Yang Y F 2025 Chin. Phys. Lett. 42 017301
[28] Xue J R, Wang F 2024 Chin. Phys. Lett. 41 057403
[29] Ghiringhelli G, Le Tacon M, Minola M, BlancoCanosa S, Mazzoli C, Brookes N, De Luca G, Frano A, Hawthorn D, He F Z, Loew T, Moretti Sala M, Peets D, Salluzzo M, Schierle E, Sutarto R, Sawatzky G, Weschke E, Keimer B, Braicovich L 2012 Science 337 821
[30] Krieger G, Martinelli L, Zeng S, Chow L E, Kummer K, Arpaia R, Moretti Sala M, Brookes N B, Ariando A, Viart N, Salluzzo M, Ghiringhelli G, Preziosi D 2022 Phys. Rev. Lett. 129 027002
[31] Tam C C, Choi J, Ding X, Agrestini S, Nag A, Wu M, Huang B, Luo H Q, Gao P, GarcíaFernández M, Qiao L, Zhou K J 2022 Nat. Mater. 21 1116
[32] Rossi M, Osada M, Choi J, Agrestini S, Jost D, Lee Y, Lu H, Wang B Y, Lee K, Nag A, Chuang Y D, Kuo C T, Lee S J, Moritz B, Devereaux T P, Shen Z X, Lee J S, Zhou K J, Hwang H Y, Lee W S 2022 Nat. Phys. 18 869
[33] Taniguchi S, Nishikawa T, Yasui Y, Kobayashi Y, Takeda J, Shamoto S i, Sato M 1995 J. Phys. Soc. Jpn. 64 1644
[34] Seo D K, Liang W, Whangbo M H, Zhang Z, Greenblatt M 1996 Inorg. Chem. 35 6396
[35] Wu G, Neumeier J J, Hundley M F 2001 Phys. Rev. B 63 245120
[36] Liu Z J, Sun H L, Huo M W, Ma X Y, Ji Y, Yi E K, Li L S, Liu H, Yu J, Zhang Z Y, Chen Z Q, Liang F X, Dong H L, Guo H J, Zhong D Y, Shen B, Li S L, Wang M 2023 Sci. China Phys. Mech. Astron. 66 217411
[37] Liu Z, Huo M W, Li J, Li Q, Liu Y C, Dai Y M, Zhou X X, Hao J H, Lu Y, Wang M, Wen H H 2024 Nat. Commun. 15 7570
[38] Shen Y 2024 Acta Phys.Sin. 73 197104（in Chinese） [沈瑶 2024 物理学报 73 197104]
[39] Zhao D, Zhou Y B, Huo M W, Wang Y, Nie L P, Yang Y, Ying J J, Wang M, Wu T, Chen X H 2025 Sci. Bull. 70 1239
[40] Kakoi M, Oi T, Ohshita Y, Yashima M, Kuroki K, Kato T, Takahashi H, Ishiwata S, Adachi Y, Hatada N, Uda T, Mukuda H 2024 J. Phys. Soc. Jpn. 93 053702
[41] Chen K W, Liu X Q, Jiao J C, Zou M Y, Jiang C Y, Li X, Luo Y X, Wu Q, Zhang N Y, Guo Y F, Shu L 2024 Phys. Rev. Lett. 132 256503
[42] Chen X Y, Choi J, Jiang Z C, Mei J, Jiang K, Li J, Agrestini S, García-Fernández M, Sun H L, Huang X, Shen D W, Wang M, Hu J P, Lu Y, Zhou K J, Feng D L 2024 Nat. Commun. 15 9597
[43] Wang G, Wang N N, Shen X L, Hou J, Ma L, Shi L F, Ren Z A, Gu Y D, Ma H M, Yang P T, Liu Z Y, Guo H Z, Sun J P, Zhang G M, Calder S, Yan J Q, Wang B S, Uwatoko Y, Cheng J G 2024 Phys. Rev. X 14 011040
[44] Zhang Y N, Su D J, Huang Y N, Shan Z Y, Sun H L, Huo M W, Ye K X, Zhang J W, Yang Z H, Xu Y K, Su Y, Li R, Smidman M, Wang M, Jiao L, Yuan H Q 2024 Nat. Phys. 20 1269
[45] Wang Y X, Jiang K, Wang Z Q, Zhang F C, Hu J P 2024 Phys. Rev. B 110 205122
[46] Yi X W, Meng Y, Li J W, Liao Z W, Li W, You J Y, Gu B, Su G 2024 Phys. Rev. B 110 L140508
[47] Chen X J, Jiang P H, Li J, Zhong Z C, Lu Y 2025 Phys. Rev. B 111 014515
[48] Schollwöck U 2005 Rev. Mod. Phys. 77 259
[49] Haegeman J, Cirac J I, Osborne T J, Pižorn I, Verschelde H, Verstraete F 2011 Phys. Rev. Lett. 107 070601
[50] Haegeman J, Mariën M, Osborne T J, Verstraete F 2014 J. Math. Phys. 55 021902
[51] Lu Y, Höppner M, Gunnarsson O, Haverkort M W 2014 Phys. Rev. B 90 085102
[52] Lu Y, Cao X D, Hansmann P, Haverkort M W 2019 Phys. Rev. B 100 115134
[53] Cao X D, Lu Y, Hansmann P, Haverkort M W 2021 Phys. Rev. B 104 115119
[54] Cao X D, Lu Y, Stoudenmire E M, Parcollet O 2024 Phys. Rev. B 109 235110
[55] Kresse G, Furthmüller J 1996 Comput. Mater. Sci. 6 15
[56] Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865
[57] Mostofi A A, Yates J R, Lee Y S, Souza I, Vanderbilt D, Marzari N 2008 Comput. Phys. Commun. 178 685
[58] Marzari N, Vanderbilt D 1997 Phys. Rev. B 56 12847
[59] Souza I, Marzari N, Vanderbilt D 2001 Phys. Rev. B 65 035109
[60] Aryasetiawan F, Imada M, Georges A, Kotliar G, Biermann S, Lichtenstein A I 2004 Phys. Rev. B 70 195104
[61] Mravlje J, Aichhorn M, Miyake T, Haule K, Kotliar G, Georges A 2011 Phys. Rev. Lett. 106 096401
[62] Kugler F B, Zingl M, Strand H U R, Lee S S B, von Delft J, Georges A 2020 Phys. Rev. Lett. 124 016401
[63] Georges A, Medici L d, Mravlje J 2013 Annu. Rev. Condens. Matter Phys. 4 137
Metrics
- Abstract views: 41
- PDF Downloads: 2
- Cited By: 0
下载:
