Superconductivity onset above 60 K in ambient-pressure nickelate films

本研究采用巨大氧化原子层外延法,在极端非平衡条件下于SrLaAlO4衬底上生长(La,Pr)3Ni2O7薄膜,实现了常压下约63 K的超导起始转变温度,零电阻温度达约37 K,抗磁信号起始约23 K。该方法通过高温和原位充分氧化克服了亚稳态超导相的结构不稳定性,X射线衍射和扫描透射电镜证实薄膜具有大范围晶态纯度。输运测量显示正常态电阻温度幂律指数α从低起始转变温度样品的费米液体行为(α≈2)向高起始转变温度样品的奇异金属行为(α≈1)系统演化,直接将增强的超导性与非费米液体行为关联。互电感技术绘制的涡旋熔化相图揭示二维熔化极限被抑制至近零,层间耦合强度显著强于铋系铜氧化物。这些结果表明镍酸盐是常压下具有强层间耦合的奇异金属高温超导体。

superconductor insulator transition

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Superconductor-insulator transitions in infinite-layer nickelates controlled via operando monitored reduction

该研究通过开发原位监测还原(OMR)方法,实现了对无限层镍酸盐超导体中Ni 3d轨道电子占据从约3d⁷到3d⁹的超宽范围连续调控,从而可控地驱动超导体-绝缘体转变(SIT)。结合同步辐射X射线吸收谱和扫描透射电镜对氧原子的分析,精确标定了电子占据态,并进一步利用离子液体门控和磁场调制SIT。Nernst效应测量显示,与铜氧化物不同,配对在电阻开始下降时即已启动,而迈斯纳效应仅在零电阻态才出现,标志着全局相位相干性的建立。角度依赖的磁输运研究表明,转变温度区间内超导呈现二维与三维特征的混合,表明所观察的SIT偏离了经典二维模型。这些结果在氧含量-磁场-温度参数空间内为理解无限层镍酸盐中结构与电子相变的相互作用提供了独特视角。

superfluid density

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Suppressed density wave and emergent negative magnetoresistance in Tb-doped La₃Ni₂O₇

The suppression of density wave in bilayer nickelate La3⁢Ni2⁢O7 under pressure has been identified as a critical factor enabling pressure-induced high-temperature superconductivity. However, this density wave state exhibits remarkable stability against most alternative tuning methods except the high-pressure technique. Herein through systematic investigations of Tb doping effects on electrical transport and magnetic properties, we observe a gradual suppression of density wave transition temperature with the increasing Tb concentration, accompanied by the emergence of negative magnetoresistance persisting up to 14 T. Magnetic susceptibility measurements further reveal the formation of a doping-induced spin-glass state, which likely accounts for the observed negative magnetoresistance phenomenon. This work establishes an effective chemical doping approach to manipulate the density wave state and correlated quantum state in La3⁢Ni2⁢O7, offering new insights into the mechanism of high-temperature superconductivity and potential pathways toward achieving ambient-pressure superconductivity in bulk nickelate crystals.

Symmetry analysis

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Symmetry-Based Microscopic Theory of the Unconventional Pairing Mechanism in La₅Ni₃O₁₁

本文基于对称性唯象方法,结合电荷自洽密度泛函理论与动力学平均场理论,系统研究了杂化镍酸盐La₅Ni₃O₁₁的低温物理与非常规配对机制。研究发现,单层子系统处于莫特绝缘态,超导电性主要源于双层子系统中Ni-e_g轨道。该体系呈现双能隙超导特征,主导配对来自d_{z²}轨道间的层间耦合,次要配对来自d_{x²-y²}轨道内的层内耦合。与高压下La₃Ni₂O₇相比,La₅Ni₃O₁₁中超导转变温度T_c的降低可归因于层间配对贡献的减弱,这直接反映在跃迁参数比值|t_{\perp}^z/t_{\parallel}^{x}|的减小上。该统一图像为理解双层NiO₂面内超导配对机制及γ口袋的作用提供了微观理论框架。

synchrotron X-ray diffraction

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t linear resistivity

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The evolution of pairing correlation with 3d_{z^{2}} electron filling in a bilayer two-orbital model for La₃Ni₂O₇

通过密度矩阵重正化群方法,该工作在一维最小几何结构上系统研究了加压双层镍氧化物La₃Ni₂O₇中有效双层双轨道模型的超导配对关联随Ni 3d_{z²}轨道填充的演化。通过调节轨道化学势差异,将3d_{z²}轨道从1/12掺杂连续调控至近半填充,发现超导关联在半填充附近被显著抑制,表明该轨道的巡游性有利于配对。此外,在电荷涨落较大的区域配对关联增强,暗示电荷序与超导之间存在竞争。这些结果支持了既有的理论图像:层间反铁磁超交换提供配对胶水,而巡游的3d_{z²}轨道通过杂化将配对传递并建立长程相干性。研究明确了3d_{z²}轨道巡游性对超导的关键作用,为理解该体系中非常规配对机制提供了重要依据。