通过第一性原理密度泛函理论计算，系统研究了双层Ruddlesden-Popper型镍酸盐La₃Ni₂O₇薄膜中四价元素替代的电子掺杂效应。研究发现，与铜氧化物不同，铈（Ce）掺杂难以有效向低能带引入电子载流子，而锆（Zr）、铪（Hf）和钍（Th）可作为高效电子掺杂剂。这些元素替代能显著增大Ni-dz²轨道间的层间跳跃积分t⊥，可能增强层间超交换耦合J⊥，进而潜在提高超导转变温度Tc。利用约束随机相位近似评估了相互作用参数，发现电子掺杂使得低能轨道（包括Ni-dx²-y²和dz²及其杂化氧轨道）的占据增加，并改变了层内与层间轨道的电子填充比例。结构分析显示，掺杂剂离子半径的差异导致Ni-O键长变化，其中Zr和Hf引起晶格收缩，而Th掺杂效果最强。结果表明，Zr、Hf、Th是实现La₃Ni₂O₇电子掺杂的候选材料，为澄清该体系中电子配对机制的争议提供了新途径。
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通过结合密度泛函理论和动力学平均场理论，研究了无限层镍酸盐LaNiO₂在电子掺杂和空穴掺杂下电子结构、磁性与关联效应的演化。结果显示，由于稀土5d态的存在，Ni-d_{x²-y²}带的自掺杂效应呈现显著不对称：空穴掺杂强烈抑制自掺杂，而电子掺杂虽增大稀土5d电子口袋尺寸，却未有效空穴掺杂Ni-d_{x²-y²}带。这一差异直接影响磁性响应——空穴掺杂迅速压制反铁磁序，电子掺杂则使反铁磁态保持为基态。尽管存在这些差异，两种掺杂下的电子关联均由Ni-d_{x²-y²}轨道主导，表明单带描述在电子和空穴掺杂区均可能适用。
预测超导转变温度（Tc）仍面临挑战。本研究提出可解释且结构、化学感知的高斯过程模型 GP-Tc，通过图元直方图编码局部键合环境，并结合地球移动距离构建有效核，实现带不确定度的 Tc 预测。分析表明，仅需相邻原子间电子亲和势差分布、原子间距及少量元素特征即可预测不同超导家族的 Tc，揭示电子亲和势差是连接局域键合与宏观超导性的关键化学参数，且机制无关。该模型复现了无限层镍酸盐 Nd0.8Sr0.2NiO2 的实验 Tc 范围，并预测化学计量 PtPb3Bi 的超导性，实验证实 Tc≈3 K。此外，GP-Tc 通过网页接口开放，并识别出 SrNiO2 与 K(PRh)2 等高优先级候选材料。
研究人员利用臭氧辅助原子层外延技术，在NdAlO3衬底上生长了La2PrNi2O7薄膜，引入了高达-2.14%的极端压缩应变，实现了起始临界温度达60 K、零电阻温度33 K和20 K处抗磁转变的高温超导性，磁输运测量确认其为准二维超导态。对比应变片与高压块材的相图发现，尽管两者都通过抑制自旋密度波驱动超导，但晶格响应存在分歧：薄膜在其c轴参数窗口显著发散，而面内参数与块材一致。关键的是，霍尔测量揭示了电子性质的二分性，最佳超导薄膜呈现负霍尔系数的类电子特征，与高压块材和非超导拉伸正系数的类空穴特征截然对立。这表明应变与压力策略均能有效调控潜在关联调制，超越特定费米面拓扑的限制，从而驱动超导性。这项工作建立了一个研究镍酸盐多轨道物理的宏观平台，为探索高温超导机制提供了新维度。
High-temperature superconductivity was discovered in the pressurized nickelate La3Ni2O7 which has a unique bilayer structure and mixed valence state of nickel. The properties at ambient pressure contain crucial information of the fundamental interactions and bosons mediating superconducting pairing. Here, using X-ray absorption spectroscopy and resonant inelastic X-ray scattering, we identified that Ni 3 $${d}_{{x}^{2}-{y}^{2}}$$, Ni 3 $${d}_{{z}^{2}}$$, and ligand oxygen 2p orbitals dominate the low-energy physics with a small charge-transfer energy. Well-defined optical-like magnetic excitations soften into quasi-static spin-density-wave ordering, evidencing the strong electronic correlation and rich magnetic properties. Based on an effective Heisenberg spin model, we extract a much stronger inter-layer effective magnetic superexchange than the intra-layer ones and propose two viable magnetic structures. Our findings emphasize that the Ni 3 $${d}_{{z}^{2}}$$orbital bonding within the bilayer induces novel electronic and magnetic excitations, setting the stage for further exploration of La3Ni2O7 superconductor.
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Trilayer Ruddlesden-Popper phase La4Ni3O10 has been observed with Tc of ∼30 K at high pressure in a recent experiment, which further expanded the family of nickelate superconductors. In this study, we explored the effects of electronic correlations in La4Ni3O10 using density functional theory plus dynamical mean-field theory at ambient and high pressures. Our derived spectral functions and Fermi surface of the ambient pressure phase are nicely consistent with the experimental results by angle-resolved photoemission spectroscopy, which emphasized the importance of electronic correlations in La4Ni3O10. We also found the electronic correlations in pressurized La4Ni3O10 are both orbital-dependent and layer-dependent due to the presence of Hund’s rule coupling. There is a competition between the Hund’s rule coupling and the crystal-field splitting, and therefore, the Ni–O layers with weaker crystal-field splitting energy would have stronger electronic correlations.