The discovery of superconductivity in Sr-doped NdNiO$_{2}$ is a crucial breakthrough in the long pursuit for nickel oxide materials with electronic and magnetic properties similar to those of the cuprates. NdNiO$_2$ is the infinite-layer member of a family of square-planar nickelates with general chemical formula R$_{n+1}$Ni$_n$O$_{2n+2}$ (R = La, Pr, Nd, $n= 2, 3, ... \infty$). In this letter, we investigate superconductivity in the trilayer member of this series (R$_4$Ni$_3$O$_8$) using a combination of first-principles and $t-J$ model calculations. R$_4$Ni$_3$O$_8$ compounds resemble cuprates more than RNiO$_2$ materials in that only Ni-$d_{x^{2}-y^{2}}$ bands cross the Fermi level, they exhibit a largely reduced charge transfer energy, and as a consequence superexchange interactions are significantly enhanced. We find that the superconducting instability in doped R$_4$Ni$_3$O$_8$ compounds is considerably stronger with a maximum gap about four times larger than that in Sr$_{0.2}$Nd$_{0.8}$NiO$_2$.
Mode-selective phonon effects on magnetism and superconductivity in trilayer nickelates
Universität Würzburg（维尔茨堡大学）；Nagoya University（名古屋大学）；Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所北京凝聚态物理国家研究中心）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）；Hefei National Laboratory, and New Cornerstone Science Laboratory（合肥国家实验室和新基石科学实验室）；Institute of Theoretical Physics, Chinese Academy of Sciences（中国科学院理论物理研究所）
The recent discovery of superconductivity in hole-doped planar nickelates R1-xSrNiO2 (R=Pr,Nd) raises the foundational question of how the electronic structure and electronic correlations of these Ni1+ compounds compare to those of the Cu2+ cuprate superconductors. Here, we present an Angle-Resolved Photoemission Spectroscopy (ARPES) study of the trilayer nickelate Pr4Ni3O8, revealing an electronic structure and Fermi surface very similar to that of the hole-doped cuprates but with a few critical differences. Specifically, the main portions of the Fermi surface are extremely similar to that of…
Trilayer nickelates, which exhibit a high degree of orbital polarization combined with an electron count (d8.67) corresponding to overdoped cuprates, have been identified as a promising candidate platform for achieving high-Tc superconductivity. One such material, La4Ni3O8, undergoes a semiconductor-insulator transition at ~105 K, which was recently shown to arise from the formation of charge stripes. However, an outstanding issue has been the origin of an anomaly in the magnetic susceptibility at the transition and whether it signifies formation of spin stripes akin to single layer nickelates…
Magnetic Correlations and Pairing Tendencies of the Hybrid Stacking Nickelate Superlattice La$_7$Ni$_5$O$_{17}$ (La$_3$Ni$_2$O$_7$/La$_4$Ni$_3$O$_{10}$) under Pressure
Low-valent nickelates R$_{n+1}$Ni$_n$O$_{2n+2}$ (R = rare earth) containing Ni$^{1+}$ (d$^{9}$) with a quasi-two-dimensional (quasi-2D) square planar coordination geometry possess structural and electronic properties that are similar to those of high-Tc cuprates, including superconductivity itself in the doped infinite layer ($n = \infty$) RNiO$_2$ system. Within this R$_{n+1}$Ni$_n$O$_{2n+2}$ nickelate family, the crystallographic isomorphs Pr$_4$Ni$_3$O$_8$ and La$_4$Ni$_3$O$_8$ exhibit singularly different ground states: Pr$_4$Ni$_3$O$_8$ is metallic and La$_4$Ni$_3$O$_8$ is a charge- and s…
Multiorbital character of the density wave in trilayer nickelate superconductors
Max-Planck-Institute for Solid State Research（马克斯·普朗克固体研究所）；Facultad de Ciencias Exactas, Ingeniería y Agrimensura and Instituto de Física Rosario (UNR-CONICET)（罗萨里奥大学精确科学、工程与测量学院及罗萨里奥物理研究所（UNR-CONICET））；RIKEN Interdisciplinary Theoretical and Mathematical Sciences (iTHEMS)（理化学研究所跨学科理论与数学科学中心 (iTHEMS)）
The discovery of superconductivity in a $d^{9-δ}$ nickelate has inspired disparate theoretical perspectives regarding the essential physics of this class of materials. A key issue is the magnitude of the magnetic superexchange, which relates to whether cuprate-like high-temperature nickelate superconductivity could be realized. We address this question using Ni L-edge and O K-edge spectroscopy of the reduced trilayer nickelate $d^{9-1/3}$ La4Ni3O8 and associated theoretical modeling. A magnon energy scale of ~80 meV resulting from a nearest-neighbor magnetic exchange of $J = 69(4)4$ meV is obs…
The recent discovery of the superconductivity in the doped infinite layer nickelates $R$NiO$_2$ ($R$=La, Pr, Nd) is of great interest since the nickelates are isostructural to doped (Ca,Sr)CuO$_2$ having superconducting transition temperature ($T_{\rm c}$) of about 110 K. Verifying the commonalities and differences between these oxides will certainly give a new insight into the mechanism of high $T_{\rm c}$ superconductivity in correlated electron systems. In this paper, we review experimental and theoretical works on this new superconductor and discuss the future perspectives for the "nickel …
Multiorbital Anisotropy and Magnetic Excitations in Trilayer Nickelate Pr$_4$Ni$_3$O$_{10}$
Harvard University（哈佛大学）；Brookhaven National Laboratory（布鲁克海文国家实验室）；Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory（SLAC国家加速器实验室斯坦福材料与能源科学研究所）；European Synchrotron Radiation Facility（欧洲同步辐射装置）；Argonne National Laboratory（阿贡国家实验室）
Expanding the trilayer Ruddlesden-Popper nickelate family: Synthesis and characterization of Sm$_4$Ni$_3$O$_{10-δ}$ single crystals
National Laboratory of Solid State Microstructures and Department of Physics, Center for Superconducting Physics and Materials, Collaborative Innovation Center of Advanced Microstructures, Nanjing University（南京大学固体微结构物理国家重点实验室、物理系、超导物理与材料中心、先进微结构协同创新中心）
The discovery of superconducting nickelates reignited hope for elucidating the high-$T_{\textrm{c}}$ superconductivity mechanism in the isostructural cuprates. While in the cuprates, the superconducting gap opens up on a single-band of the quasi-2D Fermi surface, the nickelates are known to have 3D nature of electronic structure with multi-band. This raises a serious question about the role of 2D nature for the high-$T_{\textrm{c}}$ superconductivity. Here, employing dynamical mean field theory combined with GW method, we found the Kondo effect driven by the strong correlation of Nd-4$f$ and N…
We report the crystal structures and physical properties of trilayer nickelates Nd$_4$Ni$_3$O$_{10}$ and Nd$_4$Ni$_3$O$_8$. Measurements of magnetization and electrical resistivity display contrasting behaviors in the two compounds. Nd$_4$Ni$_3$O$_{10}$ shows a paramagnetic metallic behavior with a metal to metal phase transition($T^{\ast}$) at about 162 K, as revealed by both magnetic susceptibility and resistivity. Further magnetoresistance and Hall coefficient results show a negative magnetoresistance at low temperatures and the carrier type of Nd$_4$Ni$_3$O$_{10}$ is dominated by hole-type…
We analyze the electronic structure of different surface terminations for infinite-layer nickelates. Surface NiO$_2$ layers are found to be buckled, in contrast to planar bulk layers. While the rare-earth terminated surface fermiology is similar to the bulk limit of the nickelates, the NiO$_2$ terminated surface band structure is significantly altered, originating from the effect of absence of rare-earth atoms on the crystal field splitting. Contrary to the bulk Fermi surfaces, there are two Ni-$3d$ Fermi pockets, giving rise to enhanced spectral weight around the $\bar{\text{M}}$ point in the…
Electronic structure and magnetic tendencies of trilayer La$_4$Ni$_3$O$_{10}$ under pressure: structural transition, molecular orbitals, and layer differentiation
Recently Li et al (2019 Nature 572 624) discovered a new type of oxide superconductor Nd0.8Sr0.2NiO2 with T$_c$ = 14 K. To classify superconductivity in this infinite-layer nickelate experimental upper critical field, B$_{c2}$(T), and the self-field critical current densities, J$_c$(sf,T), reported by Li et al (2019 Nature 572 624), are analysed in assumption of s-, d-, and p-wave pairing symmetries and single- and multiple-band superconductivity. Based on deduced the ground-state superconducting energy gap, $Δ$(0), the London penetration depth, $λ$(0), the relative jump in electronic specific…
The recent observation of superconductivity in infinite-layer nickelate Nd$_{0.8}$Sr$_{0.2}$NiO$_{2}$ has received considerable attention. Despite the many efforts to understand the superconductivity in infinite-layer nickelates, a consensus on the underlying mechanism for the superconductivity has yet to be reached, partly owing to the challenges with the material synthesis. Here, we report the successful growth of superconducting infinite-layer Nd$_{0.8}$Sr$_{0.2}$NiO$_{2}$ films by pulsed-laser deposition and soft chemical reduction. The details on growth process will be discussed.
The recent discovery of superconductivity in infinite-layer nickelate films has aroused great interest since it provides a new platform to explore the mechanism of high-temperature superconductivity. However, superconductivity only appears in the thin film form and synthesizing superconducting nickelate films is extremely challenging, limiting the in-depth studies on this compound. Here, we explore the critical parameters in the growth of high quality nickelate films using molecular beam epitaxy (MBE). We found that stoichiometry is crucial in optimizing the crystalline structure and realizing…
Multiple Magnetic Transitions in the Trilayer Nickelate Pr$_4$Ni$_3$O$_{10}$ Revealed by Muon-Spin Rotation
PSI Center for Neutron and Muon Sciences CNM（瑞士保罗谢勒研究所中子与缪子科学中心）；Department of Physics, University of Zurich（苏黎世大学物理系）；Key Laboratory of Advanced Functional Materials, Ministry of Education, College of Materials Science and Engineering, Beijing University of Technology（北京工业大学材料科学与工程学院先进功能材料教育部重点实验室）；TU Dortmund University, Department of Physics（多特蒙德工业大学物理系）
Low-valence nickelates $-$ including infinite-layer (IL) and trilayer (TL) compounds $-$ are longstanding candidates for mimicking the high-temperature superconductivity of cuprates. A recent breakthrough in the field came with the discovery of superconductivity in hole-doped IL nickelates. Yet, the degree of similarity between low-valence nickelates and cuprates is the subject of a profound debate for which soft x-ray spectroscopy experiments at the Ni $L$- and O $K$-edge provided critical input. In this review, we will discuss the essential elements of the electronic structure of low-valance…
Employing first-principles density functional theory calculations and Wannierization of the low energy band structure, we analyze the electronic structure of undoped, infinite-layer nickelate compounds, NdNiO$_2$, PrNiO$_2$ and LaNiO$_2$. Our study reveals important role of non-zero $f$-ness of Nd and Pr atoms, as opposed to $f^{0}$ occupancy of La. The non-zero $f$-ness becomes effective in lowering the energy of the rare-earth 5$d$ hybridized axial orbital, thereby enhancing the electron pockets and influencing the Fermi surface topology. The Fermi surface topology of NdNiO$_2$ and PrNiO$_2$…
Intertwined Charge and Spin Density Waves in Trilayer Nickelate La$_4$Ni$_3$O$_{10}$ Revealed by $^{139}$La NQR
Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；Beijing National Laboratory for Condensed Matter Physics（北京凝聚态物理国家研究中心）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）；State Key Laboratory of Crystal Materials, Institute of Crystal Materials, Shandong University（山东大学晶体材料研究所晶体材料国家重点实验室）；State Key Laboratory of Quantum Functional Materials, School of Physical Science and Technology, ShanghaiTech University（上海科技大学物质科学与技术学院量子功能材料国家重点实验室）；School of Physics and Astronomy, Beijing Normal University（北京师范大学物理与天文学院）；Key Laboratory of Multiscale Spin Physics, Ministry of Education, Beijing Normal University（北京师范大学多尺度自旋物理教育部重点实验室）
We use scanning tunneling microscopy to investigate Bi2Sr2Ca2Cu3O10+δ trilayer cuprates from the optimally doped to overdoped regime. We find that the two distinct superconducting gaps from the inner and outer CuO2 planes both decrease rapidly with doping, in sharp contrast to the nearly constant Tc. Spectroscopic imaging reveals the absence of quasiparticle interference in the antinodal region of overdoped samples, showing an opposite trend to that in single- and double-layer compounds. We propose that the existence of two types of inequivalent CuO2 planes and the intricate interaction betwee…
