Raman response in superconducting multiorbital systems with application to nickelates

本研究利用电子拉曼散射方法,系统分析了超导多轨道系统的拉曼响应,并以镍酸盐为应用对象。针对三种模型——包含d_{x^2-y^2}和d_{z^2}轨道的单层与双层两轨道模型,以及仅含d_{x^2-y^2}轨道的双层单轨道模型——分别考虑了d波、s±波和s波等多种配对对称性,计算了不同拉曼对称性(A1g、B1g、B2g)下的响应特征。在两轨道模型中,采用了全多轨道方法,同时计入轨道内和轨道间散射,并与将各能带拉曼响应简单相加的加性近似进行了对比。研究发现,不同配对对称性和模型结构在拉曼谱中产生独特的指纹特征,全多轨道计算揭示了加性近似可能忽略的轨道间混合效应。这些结果有助于厘清镍酸盐超导的最小模型,判断其超导能隙的大小与对称性,并为其他多轨道超导体(如铁基超导体)的拉曼实验分析提供了通用的理论框架。

Recent progress in nickelate superconductors

This review summarizes recent advances in nickelate superconductors, covering infinite-layer, bilayer, and trilayer systems, their superconducting properti

Regulating oxygen content and superconductivity in La₃Ni₂O₇₊δ

本研究通过系统调控La₃Ni₂O₇₊δ系列样品的氧含量,合成了不同相组成的材料,包括纯双层相、双层与单层-双层杂化相混合相以及含三层交生的主双层相。高压输运测量表明,这些相分别对应不同的超导转变温度(T_c),其中双层相呈现约80 K的超导电性,杂化相和三层交生相的T_c较低。氧含量不仅影响相纯度,还直接调控双层超导电性的上临界场(H_c2),纯双层相具有更高的H_c2。通过建立T_c和H_c2随氧含量变化的相图,本研究实现了对Ruddlesden-Popper镍酸盐氧含量的精确控制,为理解其高压超导机制提供了关键实验依据。

Reply to "Threefold error in the reported zero-field cooled magnetic moment of single crystal La₂SmNi₂O₇ (arXiv: 2602.23240)"

针对Korolev和Talantsev对Li等人《Nature》论文中超导相分数计算的批评,本文作者逐一回应:首先,经实验确认低温尾巴的弱上升源于背景,且未观察到顺磁迈斯纳效应,因此场冷数据可用于计算超导相分数;其次,退磁效应必须基于实际测量磁矩随超导相分数f的变化,而Korolev等错误地将退磁场视为常数,导致其公式低估f约三分之二(因子接近1/3),解释了其计算结果仅为报道值(约62.1%)约三分之一的原因;最后,样品的多种表征(能谱、X射线衍射、核四极共振、扫描透射电镜等)证实为均匀高质量块体单晶,不存在多个离散超导区域。因此,Li等人《Nature》论文中超导相分数的计算方法并未被Korolev等的分析推翻。

Resolving the electronic ground state of La₃Ni₂O₇₋δ films

The recent discovery of a superconductivity signature in La3Ni2O7-δ under a pressure of 14 GPa, with a superconducting transition temperature of around 80 K, has attracted considerable attention. An important aspect of investigating electronic structures is discerning the extent to which the electronic ground state of La3Ni2O7-δ resembles the parent state of the cuprate superconductor, a charge transfer insulator with long-range antiferromagnetism. Through X-ray absorption spectroscopy, we reveal the influence of oxygen ligands on the electronic ground states of the Ni ions, displaying a charge transfer nature akin to cuprate but with distinct orbital configurations. Additionally, in La3Ni2O7-δ films, we detect a superlattice reflection (1/4, 1/4, L) at the Ni L absorption edge using resonant X-ray scattering measurements. Further examination of the resonance profile indicates that the reflection originates from the Ni d orbitals. By evaluating the reflection’s azimuthal angle dependence, we confirm the presence of collinear antiferromagnetic spin ordering and charge-like anisotropy ordered with the same periodicity. Our findings reveal a microscopic relationship between these two components in the temperature dependence of the scattering intensity of the reflection. This investigation enriches our understanding of high-temperature superconductivity in La3Ni2O7-δ under high pressure.

Role of interstitial s orbital in a model of infinite-layer nickelates

本研究采用行列式量子蒙特卡罗方法,在三轨道Emery模型基础上加入具有三维色散的间隙$s$轨道,模拟无限层镍酸盐的低能电子结构。大规模计算发现:强关联效应显著缩小了间隙$s$轨道产生的电子口袋,但在20%空穴掺杂下口袋仍存续,大小与ARPES实验观测相当;$d_{x^2-y^2}$轨道色散受到强烈重正化,沿$k_z$方向的弱色散与实验一致。此外,与常规三轨道模型相比,引入$s$轨道后系统的短程反铁磁关联明显增强。这些结果揭示了强关联和多轨道效应在决定无限层镍酸盐低能电子态和自旋关联中的关键作用,表明必须在实际多轨道框架中处理相互作用驱动的多体物理。

Selective suppression of electronic orders via interlayer coupling in superconducting bilayer nickelate thin films

本文通过结合臭氧退火与等价稀土A位替代,在双层镍酸盐薄膜中有效施加c轴单轴压力并调控层间耦合,研究了自旋密度波(SDW)与类电荷各向异性序同超导的相互作用。共振弹性X射线散射显示,优化超导时SDW转变温度由150 K降至70 K,SDW虽被削弱但仍存在,而类电荷各向异性序在超导态被完全消除。极化分辨O K边X射线吸收谱与电子结构计算表明,A位替代引起的c轴压缩及臭氧退火填补层间氧空位,均增强层间Ni-O-Ni杂化,重构费米面并抑制SDW波矢附近的磁涨落,从而削弱SDW不稳定性。该结果说明两种电子序受不同能量尺度支配,并与自旋-无自旋条纹基态一致,为理解双层镍酸盐中密度波形成及其与超导的关系提供了新线索。

Separating the Density Wave Phase from Zero-Resistance Superconductivity in La₄Ni₃O₁₀

作者研究了三层Ruddlesden-Popper镍酸盐La4Ni3O10的高质量单晶,利用金刚石压腔显式调控非静水压分量,并结合高压电输运与同步辐射X射线衍射,区分面外主导压缩和增强的面内双轴压缩。增强的面内双轴压缩在17.2和18.9 GPa即可诱导均匀、可重复的零电阻超导态,所需压力较此前报道降低约60%;同时低压缩下的密度波相被完全抑制并与超导态分离,作者据此认为,这一结果排除了密度波序参量的软量子临界涨落作为该体系配对胶的可能性。相反,面外主导压缩仅缓慢抑制密度波,直至34 GPa仍未实现零电阻,超导迹象呈丝状且不均匀。高压XRD显示常压单斜相在高压下转变为四方相,而增强面内压缩时中间出现正交相。作者据此认为,面内双轴压缩是调控镍酸盐超导的有效手段,并统一了双层与三层Ruddlesden-Popper结构的压力尺度,且与受应变薄膜结果相联系。

Shear-stress-constrained superconductivity in Ruddlesden-Popper nickelates

Ruddlesden-Popper镍氧化物在块材高压和薄膜外延约束条件下均表现出超导电性,但高度依赖于样品质量、氧含量、缺陷和应力状态。本文提出,亚稳态RP晶格仅在Ni-O框架的局部约束变形处于一个有界的剪切应变窗口内时才进入超导态;该变形控制着八面体旋转、层间Ni-O-Ni键角以及Ni dz²与dx²-y²轨道间的耦合。这一剪切应力约束超导电性(SSCS)框架统一解释了此前观察到的压力阈值、可逆性、空间不均匀性、压力介质依赖性、薄膜-衬底敏感性以及可重复性难题。SSCS场景并不替代键角、键长、轨道占据、氧化学计量或载流子密度等传统因素的作用,而是指明这些因素协同稳定超导态所需的力学与对称性条件。镍氧化物超导体表现出的脆性与异质性并非外在复杂性,而是超导态本身的核心诊断特征。该视角为改善可重复性提供了具体实验路径,并将压缩块材、外延薄膜、化学替代样品及杂化RP结构中的物理机制统一在同一概念框架内。

Signature of Superconductivity in Pressurized La₄Ni₃O₁₀

The discovery of high-temperature superconductivity near 80 K in bilayer nickelate La3Ni2O7 under high pressures has renewed the exploration of superconducting nickelate in bulk materials. The extension of superconductivity in other nickelates in a broader family is also essential. Here, we report the experimental observation of superconducting signature in trilayer nickelate La4Ni3O10 under high pressures. By using a modified sol-gel method and post-annealing treatment under high oxygen pressure, we successfully obtained polycrystalline La4Ni3O10 samples with different transport behaviors at ambient pressure. Then we performed high-pressure electrical resistance measurements on these samples in a diamond-anvil-cell apparatus. Surprisingly, the signature of possible superconducting transition with a maximum transition temperature (T c) of about 20 K under high pressures is observed, as evidenced by a clear drop of resistance and the suppression of resistance drops under magnetic fields. Although the resistance drop is sample-dependent and relatively small, it appears in all of our measured samples. We argue that the observed superconducting signal is most likely to originate from the main phase of La4Ni3O10. Our findings will motivate the exploration of superconductivity in a broader family of nickelates and shed light on the understanding of the underlying mechanisms of high-T c superconductivity in nickelates.