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Very recently, a new superconductor with Tc = 80 K has been reported in nickelate (La3Ni2O7) at around 15–40 GPa conditions (Nature, 621, 493, 2023), which is the second type of unconventional superconductor, besides cuprates, with Tc above liquid nitrogen temperature. However, the phase diagram plotted in this report was mostly based on the transport measurement under low-temperature and high-pressure conditions, and the assumed corresponding X-ray diffraction (XRD) results were carried out at room temperature. This encouraged us to carry out in situ high-pressure and low-temperature synchrotron XRD experiments to determine which phase is responsible for the high Tc state. In addition to the phase transition from the orthorhombic Amam structure to the orthorhombic Fmmm structure, a tetragonal phase with the space group of I4/mmm was discovered when the sample was compressed to around 19 GPa at 40 K where the superconductivity takes place in La3Ni2O7. The calculations based on this tetragonal structure reveal that the electronic states that approached the Fermi energy were mainly dominated by the eg orbitals (3dz2 and 3dx2–y2) of Ni atoms, which are located in the oxygen octahedral crystal field. The correlation between Tc and this structural evolution, especially Ni–O octahedra regularity and the in-plane Ni–O–Ni bonding angles, is analyzed. This work sheds new light to identify what is the most likely phase responsible for superconductivity in double-layered nickelate.

139 La-NMR/NQR measurements of La 3 Ni 2 O 7-δ (δ∼0.0 and δ∼0.08), and La 4 Ni 3 O 10 have been performed. 139 La-NMR and transport and magnetic studies have also been carried out for Tl(La 2 Sr 2 )Ni 2 O 9 . Anomalous temperature ( T ) dependence of the longitudinal relaxation rates 1/ T 1 has been found at temperatures T A ∼(140–150 K) for all the systems. In Tl(La 2 Sr 2 )Ni 2 O 9 , there exists a transition to a magnetically ordered state at T ∼20 K. The large broadening of the NMR spectra observed for Tl(La 2 Sr 2 )Ni 2 O 9 below 20 K indicates that the system is in the charge ordered state in the temperature region between 20 K and T A with localized magnetic moments at Ni sites. The NQR intensity of La 4 Ni 3 O 10 begins to decrease rapidly with decreasing T at T A ∼140 K and almost disappears at T ∼120 K (wipeout). By arguing results of the present experimental studies, we propose that in all the systems with NiO 2 planes studied here exhibit similar type transitions to the charge ordered states at temperatures T A , all of which are in the narrow T region around 140 K. It has also been found that all the systems exhibit resistivity anomalies in the T region of (450–550) K, which suggests that they have a tendency of similar type changes or transitions of their electronic states at the temperatures, too.

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研究人员采用脉冲激光沉积结合氢化钙拓扑还原法，成功制备了一系列无限层结构 Nd₁₋ₓEuₓNiO₂ 薄膜，掺杂范围扩展至 x=0–0.7。电输运测量揭示在 0.2≤x≤0.5 区间存在一个超导穹顶，其掺杂宽度大于分子束外延制备的样品，与化学溶液法相当。其中 x=0.3 的薄膜表现出最优超导转变温度约 31 K，显著高于其他真空外延技术所得数值，表明脉冲激光沉积是制备高质量、高转变温度该类镍氧化物超导薄膜的有效途径。磁输运实验在欠掺杂和过掺杂区域均观测到强健的磁场增强与重入超导行为，这归因于 Eu²⁺ 局域磁矩在外场下的极化产生内部交换场，部分补偿外场所致；仅靠 Jaccarino-Peter 效应不足以完全解释该现象，暗示存在其他机制。在刚高于起始超导转变温度的低温区，霍尔电阻呈现非线性特征，且未伴随明显的磁滞，这可能源于磁性杂质散射。这些结果突出了磁性稀土 Eu²⁺ 离子在赋予无限层镍氧化物奇异物理属性中的关键作用。

The ambient-pressure superconductivity in La3⁢Ni2⁢O7 thin films via compressive epitaxial strain provides a highly accessible platform for diverse characterization techniques, facilitating the studies of high-temperature superconductivity. Here, we systematically map the phase diagram and reveal the superconducting dome with an electron-hole crossover in compressively strained La3−𝑥⁢Sr𝑥⁢Ni2⁢O7−𝛿 thin films by simultaneously tuning Sr doping and oxygen content. The maximum transition temperature (𝑇𝑐) coincides with an anomalous sign change in the Hall coefficient (𝑅𝐻), reminiscent of electron-doped cuprates, which may signal a Fermi surface reconstruction. Beyond the superconducting dome, a ln⁡1/𝑇 insulating regime and a 𝑇-linear resistivity regime are also resolved, resembling behaviors observed in cuprates and infinite-layer nickelates. This work reveals a dome-shaped relationship between 𝑇𝑐 and 𝑅𝐻 and establishes a key framework for understanding unconventional superconductivity in nickelate systems.

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2023年，双层镍氧化物La₃Ni₂O₇在约14 GPa高压下被发现超导，临界温度近80 K，其结构与高温铜氧化物相似，随后又发现了三层La₄Ni₃O₁₀的超导性。这两种化合物属于Ruddlesden–Popper相，由NiO₂方晶格层与LaO岩盐层交替堆叠构成。当前研究主要沿三个方向展开：扩展化合物化学多样性、通过元素替代提升超导转变温度、以及阐明超导配对机制。然而，关键实验必须在高压下进行，这给机理研究带来困难，因此开发在更低压力甚至常压下表现超导的镍氧化物具有重要意义。本文综述了这些体系的现有知识，重点介绍已较为成熟的样品合成与表征方法，并简要概述其电子性质，旨在为后续材料探索和物理机制理解提供基础。

本研究系统构建了多层方形平面镍酸盐Nd_{n+1}Ni_nO_{2n+2}（n=4–8）的超导相图，发现n=4至7的化合物呈现超导转变迹象，起始临界温度最高达12.9 K（n=6），n=8仅显示微弱超导关联。通过降低层数n，超导各向异性因钕位4f电子效应发生反转——电子结构趋近铜酸盐特性，且磁涨落在超导区及过掺杂非超导区持续存在。值得注意的是，该超导区与化学掺杂无限层镍酸盐重叠，揭示了不同结构实现在方形平面镍酸盐中的共性与差异。这一工作确立了通过原子精度层状设计合成新型镍基超导体的通用模板。

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该研究针对生长在SrLaAlO4(001)衬底上的双层镍酸盐薄膜（包括La2PrNi2O7和La2SmNi2O7），解释其电阻测量中常见的零电阻不完整和两步超导转变。作者通过圆形电极器件测量转变的方位角依赖，发现两步特征与衬底台阶-平台取向直接相关：电流平行台阶边缘时呈单步转变，垂直时两步转变最明显；ADF-STEM还在台阶处直接观察到结构破坏区。作者据此把薄膜建模为较高转变温度的完整区和较低转变温度的台阶弱链接区，并用简单模型与有限元模拟复现实验特征；结构破坏区横向尺寸约1–5 nm，与Ginzburg-Landau面内相干长度约2–3 nm相当，支持Josephson型弱链接图像。输运测量进一步显示转变甚至超导是否出现强烈依赖平均平台宽度：约920和540 nm的样品可达零电阻，约250 nm者未达零电阻，约120 nm者超导缺失。该工作将台阶诱导弱链接识别为双层镍酸盐薄膜两步转变的微观起源，为理解各向异性与逾渗输运及低临界电流提供框架。