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本研究利用高亮度同步辐射X射线衍射对双层镍酸盐La₃Ni₂O₇的高质量单晶进行精确结构分析，通过大动态范围探测器成功解析了之前被忽略的弱衍射信号，这些信号的强度比主Bragg反射弱近四个数量级。这些观测证据表明，晶体中存在滑移镜面对称性破缺，导致其呈现极性结构（空间群Ima2），而非先前普遍采用的中心对称模型（Fmmm）。进一步的结构精修揭示了两个不等价镍位点，其Ni–O键长差异显著，结合键价和计算，表明镍位点电荷呈现棋盘状有序分布，并与氧八面体倾斜协同作用赋予晶体极性。该电荷有序相的结构与双层锰氧化物中的极化态类似。本研究确立了常压下La₃Ni₂O₇的极化电荷有序态，指出其与压力诱导的超导电性存在竞争关系，为理解双层镍酸盐中相竞争机制和压力超导起源提供了关键结构基础。

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We report the discovery of a novel form of Ruddlesden–Popper (RP) nickelate that stands as the first example of long-range, coherent polymorphism in this class of inorganic solids. Rather than the well-known, uniform stacking of perovskite blocks ubiquitously found in RP phases, this newly discovered polymorph of the bilayer RP phase La3Ni2O7 adopts a novel stacking sequence in which single-layer and trilayer blocks of NiO6 octahedra alternate in a “1313” sequence. Crystals of this new polymorph are described in space group Cmmm, although we note evidence for a competing Imam variant. Transport measurements at ambient pressure reveal metallic character with evidence of a charge density wave transition with an onset at T ≈ 134 K. The discovery of such polymorphism could reverberate to the expansive range of science and applications that rely on RP materials, particularly the recently reported signatures of superconductivity in bilayer La3Ni2O7 with Tc as high as 80 K above 14 GPa.

该研究采用涨落交换（FLEX）近似方法，系统分析了常压下La₃Ni₂O₇薄膜超导体在弱关联体系中的两站点两轨道模型，重点研究了空穴掺杂对超导特性的影响。通过对费米面拓扑结构的详细分析，发现当由d_{z²}反键轨道构成的δ口袋在Γ点附近形成时，δ口袋与γ口袋的嵌套以及α与β口袋之间的嵌套，在相应波矢处共同增强了s±波配对。研究进一步提出，这种由费米面嵌套驱动的自旋涨落诱导配对的增强机制，可能为提升超导转变温度提供可行途径。该工作为理解常压镍基薄膜超导体的配对机制及探索更高性能超导材料提供了理论指导。