The nickelate Pr4Ni3O8 features quasi-two-dimensional layers consisting of three stacked square-planar NiO2 planes, in a similar way to the well-known cuprate superconductors. The mixed-valent nature of Ni and its metallic properties makes it a candidate for potentially unconventional superconductivity. We have synthesized Pr4Ni3O8 by topotactic reduction of Pr4Ni3O10 in 10 percent hydrogen gas, and report on measurements of powder-neutron diffraction, magnetization and muon-spin rotation (uSR). We find that Pr4Ni3O8 shows complicated spin-glass behavior with a distinct magnetic memory effect in the temperature range from 2 to 300 K and a freezing temperature T_s ~ 68 K. Moreover, the analysis of uSR spectra indicates two magnetic processes characterized by remarkably different relaxation rates: a slowly-relaxing signal, resulting from paramagnetic fluctuations of Pr/Ni ions, and a fast-relaxing signal, whose relaxation rate increases substantially below ~ 70 K which can be ascribed to the presence of short-range correlated regions. We conclude that the complex spin-freezing process in Pr4Ni3O8 is governed by these multiple magnetic interactions. It is possible that the complex magnetism in Pr4Ni3O8 is detrimental to the occurrence of superconductivity.
Motivated by the recent discovery of superconductivity in infinite-layer nickelate thin films, we report on a synthesis and magnetization study on bulk samples of the parent compounds ${R}$NiO$_{2}$ (${R}$=La, Pr, Nd). The frequency-dependent peaks of the AC magnetic susceptibility, along with remarkable memory effects, characterize spin-glass states. Furthermore, various phenomenological parameters via different spin glass models show strong similarity within these three compounds as well as with other rare-earth metal nickelates. The universal spin-glass behaviour distinguishes the nickelate…
Time-reversal symmetry breaking superconductivity with electronic glass in nickelate (La, Pr, Sm)3Ni2O7 films
Peking University（北京大学）；Southern University of Science and Technology（南方科技大学）；Renmin University of China（中国人民大学）；ShanghaiTech University（上海科技大学）；Boston College（波士顿学院）；Tsinghua University（清华大学）
In strongly correlated materials, lattice, charge, spin and orbital degrees of freedom interact with each other, leading to emergent physical properties such as superconductivity, colossal magnetic resistance and metal-insulator transition. Quasi-2D square planar nickelates, Rn+1NinO2n+2 (R=rare earth, n=2, 3...), are of significant interest and long sought for cuprate analogue due to the 3d9 electronic configuration of Ni+, the same as the active ion Cu2+ in the high-Tc superconducting cuprates. The field has attracted intense attention since 2019 due to the discovery of superconductivity in …
We report a comprehensive study of magnetic correlations in LaNiO$_{2}$, a parent compound of the recently discovered family of infinite-layer (IL) nickelate superconductors, using multiple experimental and theoretical methods. Our specific heat, muon-spin rotation ($μ$SR), and magnetic susceptibility measurements on polycrystalline LaNiO$_{2}$ show that long-range magnetic order remains absent down to 2 K. Nevertheless, we detect residual entropy in the low-temperature specific heat, which is compatible with a model fit that includes paramagnon excitations. The $μ$SR and low-field static and …
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…
Doping dependence of local moments in infinite layer nickelates
Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory（斯坦福材料与能源科学研究所，SLAC国家加速器实验室）；Stanford University（斯坦福大学）；PSI Center for Neutron and Muon Sciences（瑞士保罗谢勒研究所中子与μ子科学中心）；Northwestern University（西北大学）；Laboratoire de Physique des Solides, Université Paris-Saclay, CNRS UMR 8502（巴黎萨克雷大学固体物理实验室，CNRS UMR 8502）；Department of Applied Physics, Stanford University（斯坦福大学应用物理系）
Universal orbital and magnetic structures in infinite-layer nickelates
Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory（斯坦福材料能源科学研究所，SLAC国家加速器实验室）；Department of Physics, Stanford University（斯坦福大学物理系）；School of Applied and Engineering Physics, Cornell University（康奈尔大学应用工程物理学院）；Kavli Institute at Cornell for Nanoscale Technology, Cornell University（康奈尔大学纳米技术卡弗里研究所）；Diamond Light Source（钻石光源）；Department of Materials Science and Engineering, Stanford University（斯坦福大学材料科学与工程系）
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…
Luttinger Liquid Behavior in a Single-Layer Nickelate La1.4Sr0.6NiO4
Tsinghua University（清华大学）；Yale University（耶鲁大学）；University of Oxford（牛津大学）；Diamond Light Source（钻石光源）；SLAC National Accelerator Laboratory（斯坦福直线加速器中心）；Shanghai Advanced Research Institute, Chinese Academy of Sciences（中国科学院上海高等研究院）；University of Science and Technology of China（中国科学技术大学）；ShanghaiTech University（上海科技大学）
To understand the superconductivity recently discovered in Nd$_{0.8}$Sr$_{0.2}$NiO$_2$, we carried out LDA+DMFT (local density approximation plus dynamical mean-field theory) and magnetic force response calculations. The on-site correlation in Ni-$3d$ orbitals causes notable changes in the electronic structure. The calculated temperature-dependent susceptibility exhibits the Curie-Weiss behavior, indicating the localized character of its moment. From the low-frequency behavior of self-energy, we conclude that the undoped phase of this nickelate is Fermi-liquid-like contrary to cuprates. Intere…
Magnetism and superconductivity are closely entangled, elucidating the magnetic interactions in nickelate superconductors is at the heart of understanding the pairing mechanism. Our first-principles and spin-wave theory calculations highlight that NdNiO$_2$ is in the vicinity of a transition between a quasi-two-dimensional (2D) antiferromagnetic (AFM) state and a three-dimensional (3D) C-AFM state. Both states could accurately reproduce the experimentally measured magnetic excitation spectra, which was previously explained in terms of a 2D model. We further reveal that hole doping stabilizes a…
Ultrafast Magneto-Pressure Spectroscopy and Control of Correlated Phases in a Trilayer Nickelate
Ames National Laboratory, U.S. Department of Energy（艾姆斯国家实验室）；Department of Physics and Astronomy, Iowa State University（爱荷华州立大学物理与天文学系）；Materials Science Division, Argonne National Laboratory（阿贡国家实验室材料科学部）；School of Physics, Southeast University（东南大学物理学院）；Department of Physics, University of Alabama at Birmingham（阿拉巴马大学伯明翰分校物理系）
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…
Three-Dimensional Electronic Structures in Superconducting Ruddlesden-Popper Bilayer Nickelate Films
Southern University of Science and Technology（南方科技大学）；Quantum Science Center of Guangdong-Hong Kong-Macao Greater Bay Area（粤港澳大湾区量子科学中心）；University of Science and Technology of China（中国科学技术大学）；Shanghai Jiao Tong University（上海交通大学）；Tsinghua University（清华大学）
Electronic structure, quasiparticle renormalizations, and magnetic correlations in the alternating single-layer bilayer nickelate La$_5$Ni$_3$O$_{11}$
M. N. Mikheev Institute of Metal Physics, Russian Academy of Sciences（俄罗斯科学院 M.N. 米赫耶夫金属物理研究所）；Institute of Physics and Technology, Ural Federal University（乌拉尔联邦大学物理与技术研究所）
{\it Ab initio} prediction of $d_{x^2-y^2}$-wave superconductivity in infinite-layer nickelates
National Taiwan University（台湾大学）；National Center for Theoretical Sciences（国家理论科学中心）；Institute of Atomic and Molecular Sciences, Academia Sinica（中央研究院原子与分子科学研究所）
We report structural and physical properties of a new quasi-one-dimensional Cr-based compound, KCr$_{3}$As$_{3}$, which is prepared by potassium deintercalation from the superconductive K$_{2}$Cr$_{3}$As$_{3}$. KCr$_{3}$As$_{3}$ adopts the TlFe$_{3}$Te$_{3}$-type structure with space group $P6_{3}$/$m$ (No. 176). The high-temperature magnetic susceptibility obeys the Curie-Weiss law with an effective magnetic moment of 0.68 $μ_{\mathrm{B}}$/Cr. Below 56 K the susceptibility deviates from the high-temperature Curie-Weiss behavior, coinciding with the rapid increase in resistivity, which suggest…
Origin of Spin Stripes in Bilayer Nickelate La$_3$Ni$_2$O$_7$
The Chinese University of Hong Kong（香港中文大学）；Johns Hopkins University（约翰斯·霍普金斯大学）；Stanford University（斯坦福大学）；SLAC National Accelerator Laboratory（斯坦福直线加速器中心）
Electronic structure and magnetic correlations in the epitaxially strained bilayer nickelate La$_3$Ni$_2$O$_{7}$
M. N. Mikheev Institute of Metal Physics, Russian Academy of Sciences（俄罗斯科学院 M.N. 米凯耶夫金属物理研究所）；Institute of Physics and Technology, Ural Federal University（乌拉尔联邦大学物理与技术学院）
Recently, superconductivity at about 9-15K was discovered in Nd$_{1-x}$Sr$_x$NiO$_2$ infinite-layer thin films, which has stimulated enormous interests in related rare-earth nickelates. Usually, the first step to synthesize this 112 phase is to fabricate the RNiO$_3$ phase, however, it was reported that the 113 phase is very difficult to be synthesized successfully due to the formation of unusual Ni$^{3+}$ oxidation state. And the difficulty of preparation is enhanced as the ionic radius of rare-earth element decreases. In this work, we report the synthesis and investigation on multiple physic…
Quantum critical origin of strange-metals at the end of a pseudogap phase in infinite-layer nickelates
École Polytechnique, Institut Polytechnique de Paris（巴黎综合理工学院，巴黎理工学院）；Université de Sherbrooke（舍布鲁克大学）；Nanjing University（南京大学）；National High Magnetic Field Laboratory（国家高磁场实验室）
A unified theory of thin film and bulk bilayer nickelates
School of Physics, Hangzhou Normal University（杭州师范大学物理学院）；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）
We report a microscopic model wherein the unconventional superconductivity emerges from an incoherent `Cooper-pair glass' state. Driven by the pair-pair interaction, a new type of quasi-Bose phase transition is at work. The interaction leads to the unconventional coupling of the quasiparticles to excited pair states, or `super-quasiparticles', with a non-retarded energy-dependent gap. The model describes quantitatively the quasiparticle excitation spectra of both cuprates and pnictides, including the universal `peak-dip-hump' signatures, and for the pseudogap phase above $T_c$. The results sho…
