Contrasting Spin Excitations in Octahedral and Square-Planar n=8 Ruddlesden-Popper Nickelates

利用Ni L3边共振非弹性X射线散射(RIXS),本研究对比了八面体Ruddlesden-Popper(RP)相Nd9Ni8O25(非超导)及其还原后的平面相Nd9Ni8O18(具有约5 K的超导关联)中的低能自旋激发。结果显示,八面体相呈现自旋密度波(SDW)基态,有序波矢为(1/4,1/4),其低能谱由沿(0,π)和(π,π)方向的弱色散paramagnon主导;而平面相则在(1/3,0)处出现弹性峰,磁激发无色散且能量约65 meV。偏振RIXS进一步确认了两种相中磁激发的不同特性。这些发现系统揭示了两个结构家族在基态和自旋激发上的根本差异,为理解镍酸盐超导电性的机制提供了关键信息。

Controlling the Band Filling and the Band Width in Nickelate Superconductors

本研究采用高压合成与静水高压输运技术,系统调控双层镍酸盐La₃Ni₂O₇家族中的能带宽度和能带填充,以探究其对超导电性及非超导态性质的影响。通过将La部分替换为较小的Nd(增大NiO₆八面体倾斜、减小带宽),超导相所需压力显著升高;而同时引入Sr进行空穴掺杂则反转此趋势,使超导起始压力降低。在非超导态中,观察到多达三种特征电阻异常,其随压力演化,可能分别对应与超导相互竞争的电荷密度波和自旋密度波有序态。综合对比不同成分样品的相图,表明带宽和填充的独立控制是揭示该体系非常规超导机理及其竞争序的关键。

Cooperation between Electron-Phonon Coupling and Electronic Interaction in Bilayer Nickelates La₃Ni₂O₇

The recent observation of high-𝑇𝑐 superconductivity in the bilayer nickelate La3⁢Ni2⁢O7 under pressure has garnered significant interest. While researches have predominantly focused on the role of electron-electron interactions in the superconducting mechanism, the impact of electron-phonon coupling (EPC) has remained elusive and unexplored. In this Letter, we perform first-principles calculations to study the phonon spectrum and electron-phonon coupling within La3⁢Ni2⁢O7 under pressure and explore the interplay between EPC and electronic interactions on the superconductivity by employing functional renormalization group (FRG) approach. Our calculations reveal that EPC alone is insufficient to trigger superconductivity in La3⁢Ni2⁢O7 under pressure. We identify unique out-of-plane and in-plane breathing phonon modes which selectively couple with the Ni 𝑑𝑧2 and 𝑑𝑥2−𝑦2 orbitals, showcasing an orbital-selective EPC. Within the bilayer two-orbital model, it is revealed that solely electronic interactions foster 𝑠±-wave pairing characterized by notable frustration in the band space, leading to a relatively low transition temperature. Remarkably, we find that the out-of-plane EPC can act in concert with electronic interactions to promote the interlayer pairing in the 𝑑𝑧2 orbital, partially releasing the pairing frustration and thus elevating 𝑇𝑐. In contrast, the inclusion of in-plane EPC only marginally affects the superconductivity, distinct from the cuprates. Potential experimental implications in La3⁢Ni2⁢O7 are also discussed.

Correlated Electronic Structure and Density-Wave Gap in Trilayer Nickelate La₄Ni₃O₁₀

The discovery of pressurized superconductivity at 80 K in La3Ni2O7 officially brings nickelates into the family of high-temperature superconductors, which gives rise to not only new insights but also mysteries in the strongly correlated superconductivity. More recently, the sibling compound La4Ni3O10 was also shown to be superconducting below about 25 K under pressure, further boosting the popularity of nickelates in the Ruddlesden-Popper phase. In this study, combining high-resolution angle-resolved photoemission spectroscopy and ab initio calculation, we systematically investigate the electronic structures of La4Ni3O10 at ambient pressure. We reveal a high resemblance of La4Ni3O10 with La3Ni2O7 in the orbital-dependent fermiology and electronic structure, suggesting a similar electronic correlation between the two compounds. The temperature-dependent measurements imply an orbital-dependent energy gap related to the density-wave transition in La4Ni3O10. By comparing the theoretical pressure-dependent electronic structure, clues about the superconducting high-pressure phase can be deduced from the ambient measurements, providing crucial information for deciphering the unconventional superconductivity in nickelates.

Correlation between superfluid density and transition temperature in infinite-layer nickelate superconductor Nd₁₋ₓSrₓNiO₂

该研究利用扫描超导量子干涉显微镜对无限层镍基超导体Nd₀.₈Sr₀.₂NiO₂薄膜进行局域磁化率与磁通成像,以揭示零温超流密度与超导转变温度之间的关联。由于样品存在微米尺度的不均匀性,研究通过空间统计分析发现:当局部T_c高于8K时,T_c与ρ_s0呈线性关系;而当T_c低于8K时,二者呈亚线性依赖(近似T_c∝ρ_s0^{1/2})。这一整体关系与过掺杂铜氧化物超导体中的观测结果高度相似,暗示了无限层镍基超导体与铜氧化物超导体在超导机制上可能存在密切的内在联系。

Correlation-Driven Orbital-Selective Fermiology and Superconductivity in the Bilayer Nickelate La₃Ni₂O₇

该研究基于双层两轨道Hubbard模型,采用时间依赖变分原理团簇微扰理论(TDVP-CPT)与大尺度密度矩阵重正化群(DMRG)方法,系统探究了La₃Ni₂O₇中电子关联对费米面拓扑与超导配对对称性的影响。TDVP-CPT在包含多达16个物理位点的团簇上计算发现,电子关联驱动了显著的轨道选择性低能谱重构:d_{z²}轨道的谱权重逐渐耗尽,γ能带下沉至费米能级以下,而α和β能带则出现赝隙,最终在强耦合下形成以d_{x²-y²}轨道为主的费米弧。DMRG计算进一步揭示,主导的超导配对关联与该费米面重构一致演化,从弱耦合下的d_{z²}轨道主导的层间自旋单态配对转变为强耦合下的d_{x²-y²}轨道主导的配对,但始终保持s±波对称性。研究表明,γ费米面的消失非但不抑制超导电性,反而标志着关联驱动的配对通道转变,其关键中介机制包括层间反铁磁涨落、Hund耦合与轨道间杂化。

Correlation-renormalized spin-fluctuation pairing and the stabilization of s± superconductivity in pressurized La₃Ni₂O₇

该研究针对加压La₃Ni₂O₇中超导配对对称性尚未定论的问题,采用四轨道Wannier哈密顿量,将单格点双轨道动力学平均场理论(DMFT)的自能引入随机相近似(RPA),构建自能重整化粒子-空穴气泡以替代裸气泡,保持相同的局域Slater-Kanamori相互作用顶点。普通RPA计算显示主导配对属于B₂g的dxy通道,而一旦包含DMFT自能,配对层级发生反转:A₁g符号改变的s±态成为主导,B₁g dx²-y²通道次之,原先的B₂g不稳定性被强烈抑制。口袋对分解和轨道分辨磁化率表明,该反转源于d3z²-r²轨道的选择性重整化,它滤除了有利于dxy配对的γ口袋散射过程,同时保留了有利于s±的分布性口袋间散射。进一步利用双Bethe-Salpeter方程结合局域DMFT顶点计算静态自旋磁化率,得到宽广的有限动量磁响应且在Γ点附近较弱,从两粒子层面强化了s±态的自旋涨落背景。结果表明,在La₃Ni₂O₇中强关联效应并非次要修正,恰当处理关联重整化的准粒子对于准确预测超导配对对称性至关重要。

Counterintuitive inverse superconducting transition beyond 4He-cooling limit

本文报道了在Eu基无限层镍酸盐(EuxNd1-xNiO₂和EuxPr1-xNiO₂)中实现的超过液氦冷却极限的逆超导转变。通过磁场调控,在过掺杂和欠掺杂区域均观察到超导零电阻态被限制在较低临界温度(Tc-inv约2.6–5.4 K)与较高正常Tc之间,升温或增加电流密度可从电阻态驱动进入超导态,并在更高温度和电流下再次消失。系统变温输运测量表明,这一Kelvin区间的逆超导转变源于温度变化引起的Eu²⁺4f⁷相关补偿有效磁场与上临界场的交替主导,并得到了磁场下约300 mK处超导重现所形成的温度诱导重入超导现象的支持。该工作建立了磁相互作用重构的高温超导体系作为探索逆转热退相干范式的量子现象的平台,也为量子相变器件的反向设计开拓了应用场景。

Decoding Superconductivity in La₃Ni₂O₇-δ Thin Films via Ozone-Driven Structure and Oxidation Tuning

该研究通过扫描透射电子显微镜结合电子能量损失谱,对外延生长的La₃Ni₂O₇₋δ薄膜进行了详细结构分析。薄膜采用脉冲激光沉积法在SrLaAlO₄衬底上制备,经不同臭氧退火处理后表现出显著差异的超导特性。研究发现,超导相的稳定与氧化学计量均匀性、外延应变以及特定堆叠结构基序(如双层和多型体)密切相关。通过关联堆叠多型体的丰富形貌与输运行为,建立了理解双层镍酸盐薄膜中亚稳态超导相的理论框架。结果揭示了氧含量、晶格应变和结构有序性在实现环境压力超导中的关键作用,为设计新型镍基超导材料提供了明确途径。

Delafossites as an unexpected competing phase to infinite-layer oxides

通过高通量第一性原理模拟,该研究系统比较了delafossite(D1)、有序岩盐变体(D2)及无限层(IL)氧化物在ABO₂化学计量下的热力学稳定性,并构建了涵盖2346种元素组合的相图。结果表明,对于镍酸盐、钯酸盐和铂酸盐,delafossite结构的稳定性与无限层相相当甚至更优,且这两种相与钙钛矿相之间存在竞争关系。电子结构分析显示,delafossite化合物具有反转的阳离子顺序,费米面以d_{z^2}轨道贡献为主,显著区别于无限层相的d_{x^2-y^2}特征。在所有候选体系中,La-Ni组合是稳定无限层结构的热力学最优选择。此外,通过Ca、Sr、Ba进行空穴掺杂可系统提高三种过渡金属家族中无限层相的相对稳定性。这些结果揭示了合成无衬底体相无限层氧化物的根本挑战,并为实验探索新型超导化合物提供了指导。