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清华大学/中山大学/南京大学Nature: La3Ni2O7-δ中氧空位和自掺杂配体空穴的可视化

  • 2026-06-07 17:33:38
清华大学/中山大学/南京大学Nature: La3Ni2O7-δ中氧空位和自掺杂配体空穴的可视化
2024年6月5日，Nature在线发表了清华大学王亚愚教授、中山大学王猛教授、南京大学卢毅教授和中科院物理所陈震教授课题组的研究论文，题目为《Visualization of oxygen vacancies and self-doped ligand holes in La3Ni2O7-δ》，论文的第一作者为Zehao Dong、Mengwu Huo和Jie Li。

二十多年来，作为铜氧化物的类似物，镍氧化物一直是高温超导的候选材料。第一种镍氧化物超导体，空穴掺杂的无限层RNiO2（R表示稀土元素），在环境条件下达到约20 K的转变温度（Tc），在压力下达到31 K。最近在转变温度约为80 K的高压下发现了La3Ni2O7-δ的超导性，这引发了广泛的实验和理论研究。关于配对机制的几个关键问题仍有待回答，例如最相关原子轨道和原子缺陷的作用。

在此研究中，作者开发了一种新的、能量过滤的、多层电子叠层（MEP）技术，并辅以电子能量损失谱（EELS），从而来解决这些关键问题。氧空位可以直接可视化，并发现其主要占据内部顶端位置，这被认为对超导性至关重要。研究精确确定了纳米级化学计量及其与氧K边光谱的相关性，这揭示了样品中氧含量和电子结构的显著不均匀性。光谱结果还表明，化学计量的La3Ni2O7具有很强的电荷转移特性，空穴从Ni位点自掺杂到O位点。

配体空穴主要位于内顶端O和平面O上，而外顶端O上的密度可忽略不计。随着O空位浓度的增加，两个位点上的配体空穴同时湮灭。这使得La3Ni2O7-δ在Zaanen-Sawatzky-Allen方案中更接近电荷转移机制，而超导无限层镍氧化物则处于相反的Mott-Hubbard机制。观测结果将有助于进一步发展和理解超导镍氧化物材料。这项研究中用于量化原子缺陷的成像技术也可以广泛应用于材料科学和凝聚态物理。

图1 MEP的实验装置和确定O含量的模拟
图2 La3Ni2O7-δ中氧空位的实验可视化与统计
图3 La3Ni2O7-δ的O K边EELS和空位分布
图4 原子分辨EELS和每个晶胞内配体空穴的分布

图5 基于DFT+U计算的O-p轨道分辨能带结构和EELS

【论文链接】
Dong, Z., Huo, M., Li, J. et al. Visualization of oxygen vacancies and self-doped ligand holes in La3Ni2O7-δ. Nature, 2024. https://doi.org/10.1038/s41586-024-07482-1

【其他相关文献】

[1] Sun, H., Huo, M., Hu, X. et al. Signatures of superconductivity near 80 K in a nickelate under high pressure. Nature, 2023, 621, 493–498. https://doi.org/10.1038/s41586-023-06408-7
[2] Luo, Z., Hu, X., Wang, M. et al. Bilayer two-orbital model of La3Ni2O7 under pressure. Phys. Rev. Lett., 2023, 131, 126001. https://doi.org/10.1103/PhysRevLett.131.126001
[3] Christiansson, V., Petocchi, F. & Werner, P. Correlated electronic structure of La3Ni2O7 under pressure. Phys. Rev. Lett., 2023, 131, 206501. https://doi.org/10.1103/PhysRevLett.131.206501
[4] Sakakibara, H., Kitamine, N., Ochi, M. et al. Possible high Tc superconductivity in La3Ni2O7 under high pressure through manifestation of a nearly-half-filled bilayer hubbard model. Phys. Rev. Lett., 2024, 132, 106002. https://doi.org/10.1103/PhysRevLett.132.106002
[5] Lu, C., Pan, Z., Yang, F. et al. Interlayer-coupling-driven high-temperature superconductivity in La3Ni2O7 under pressure. Phys. Rev. Lett., 2024, 132, 146002. https://doi.org/10.1103/PhysRevLett.132.146002
[6] Jiang, R., Hou, J., Fan, Z. et al. Pressure driven fractionalization of ionic spins results in cupratelike high-Tc superconductivity in La3Ni2O7. Phys. Rev. Lett., 2024, 132, 126503. https://doi.org/10.1103/PhysRevLett.132.126503
中科院物理所周兴江/赵林团队Nat. Phys.: 仅有空穴口袋的铁基超导体中节点s±配对对称性
中科院物理所周兴江团队Nat. Phys.: 三层铜氧化物中高温超导临界温度的电子起源
中山大学/清华大学王猛/张广铭团队Nature: 高压下镍氧化物在80 K附近的超导特征
电子科技大学乔梁团队Nature: 氢在镍氧化物超导中的关键作用
中科院物理所/中山大学Nat. Commun.: 双层镍氧化物La3Ni2O7中轨道依赖的电子关联性
康奈尔大学Nat. Mater.: 解析无限层镍氧化物薄膜的极性界面
(纯计算)维也纳工业大学Nat. Commun.: 压力下无限层镍氧化物中无掺杂的非常规超导性
(纯计算)田纳西大学Nat. Commun.: 压力下双层超导体La3Ni2O7的结构相变、s±波配对和磁条序
(纯计算)日本鸟取大学Phys. Rev. Lett.: 高压下La3Ni2O7中可能存在的高Tc超导性

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  1. CONNECT:[ UseTime:0.000983s ] mysql:host=127.0.0.1;port=3306;dbname=b460;charset=utf8mb4
  2. SHOW FULL COLUMNS FROM `fenlei` [ RunTime:0.000926s ]
  3. SELECT * FROM `fenlei` WHERE `fid` = 0 [ RunTime:0.000276s ]
  4. SELECT * FROM `fenlei` WHERE `fid` = 63 [ RunTime:0.000221s ]
  5. SHOW FULL COLUMNS FROM `set` [ RunTime:0.000426s ]
  6. SELECT * FROM `set` [ RunTime:0.000193s ]
  7. SHOW FULL COLUMNS FROM `article` [ RunTime:0.000546s ]
  8. SELECT * FROM `article` WHERE `id` = 573953 LIMIT 1 [ RunTime:0.010526s ]
  9. UPDATE `article` SET `lasttime` = 1783096733 WHERE `id` = 573953 [ RunTime:0.007614s ]
  10. SELECT * FROM `fenlei` WHERE `id` = 65 LIMIT 1 [ RunTime:0.000275s ]
  11. SELECT * FROM `article` WHERE `id` < 573953 ORDER BY `id` DESC LIMIT 1 [ RunTime:0.000495s ]
  12. SELECT * FROM `article` WHERE `id` > 573953 ORDER BY `id` ASC LIMIT 1 [ RunTime:0.001946s ]
  13. SELECT * FROM `article` WHERE `id` < 573953 ORDER BY `id` DESC LIMIT 10 [ RunTime:0.000672s ]
  14. SELECT * FROM `article` WHERE `id` < 573953 ORDER BY `id` DESC LIMIT 10,10 [ RunTime:0.001615s ]
  15. SELECT * FROM `article` WHERE `id` < 573953 ORDER BY `id` DESC LIMIT 20,10 [ RunTime:0.012126s ]
0.104056s