We investigate the low temperature structural and physical properties of the trilayer nickelates R4Ni3O10 (R = La, Pr and Nd) using resistivity, thermopower, thermal conductivity, specific heat, high-resolution synchrotron powder X-ray diffraction and thermal expansion experiments. We show that all three compounds crystallize with a monoclinic symmetry, and undergo a metal-to-metal (MMT) transition at 135 K (La), 156 K (Pr) and 160 K (Nd). At MMT, the lattice parameters show distinct anomalies; however, without any lowering of the lattice symmetry. Unambiguous signatures of MMT are also seen in magnetic and thermal measurements, which suggest a strong coupling between the electronic, magnetic and structural degrees of freedom in these nickelates. Analysis of thermal expansion yields hydrostatic pressure dependence of MMT in close agreement with experiments. We show that the 9-fold coordinated Pr ions in the rocksalt (RS) layers have a crystal field (CF) split doublet ground state with possible antiferromagnetic ordering at 5 K. The Pr ions located in the perovskite block (PB) layers with 12-fold coordination, however, exhibit a non-magnetic singlet ground state. The CF ground state of Nd in both RS and PB layers is a Kramers doublet. Heat capacity of R = Nd shows a Schottky-like anomaly near35 K, and an upturn below T = 10 K suggesting the presence of short-range correlations between the Nd moments. However, no signs of long-range ordering could be found down to 2 K despite a sizeable theta_p ~ -40 K. The strongly suppressed magnetic long-range ordering in both R = Pr and Nd suggests the presence of strong magnetic frustration in these compounds. The low-temperature resistivity shows a T^0.5 dependence. No evidence for the heavy fermion behavior could be found in any of the three compounds.
The quasi-two-dimensional nickelate La4Ni3O8 (La-438) is an anion deficient n=3 Ruddlesden-Popper (R-P) phase that consists of trilayer networks of square planar Ni ions, formally assigned as Ni1+ and Ni2+ in a 2:1 ratio. While previous studies on polycrystalline samples have identified a 105 K phase transition with a pronounced electronic and magnetic response but weak lattice character, no consensus on the origin of this transition has been reached. Here we show using synchrotron x-ray diffraction on high-pO2 floating-zone grown single crystals that this transition is driven by a real space …
Density-wave order enhances the phonon thermal Hall effect in a trilayer nickelate
Wuhan National High Magnetic Field Center and School of Physics, Huazhong University of Science and Technology（华中科技大学物理学院）；State Key Laboratory of Surface Physics and Department of Physics, Fudan University（复旦大学物理系）；State Key Laboratory of Quantum Functional Materials, School of Physical Science and Technology, ShanghaiTech University（上海科技大学物理科学与技术学院）；Department of Physics, Tsinghua University（清华大学物理系）
Interplay of phonons, intertwined density waves, and induced spin density wave in trilayer nickelates Pr4-xLaxNi3O10
Indian Institute of Technology Mandi（印度理工学院曼迪分校）；Indian Institute of Science Education and Research Pune（印度科学教育研究所浦那分校）；Indian Institute of Technology Kanpur（印度理工学院坎普尔分校）
Collective spin excitations in trilayer nickelate La$_4$Ni$_3$O$_{10}$
The Chinese University of Hong Kong（香港中文大学）；State Key Laboratory of Quantum Information Technologies and Materials, The Chinese University of Hong Kong（香港中文大学量子信息技术与材料国家重点实验室）；Physik-Institut, Universität Zürich（苏黎世大学物理研究所）；European Synchrotron Radiation Facility（欧洲同步辐射装置）；Fudan University（复旦大学）
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…
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 cuprat…
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…
Comparative Raman study of Ruddlesden-Popper nickelates and the monolayer-trilayer polymorph
Max-Planck-Institute for Solid State Research（马克斯·普朗克固体的研究所）；Hefei National Laboratory（合肥国家实验室）；University of Science and Technology Beijing（北京科技大学）；University of Stuttgart（斯图加特大学）；Institute of Theoretical Physics, Chinese Academy of Sciences（中国科学院理论物理研究所）
Lattice-charge coupling in a trilayer nickelate with intertwined density wave order
Argonne National Laboratory（阿贡国家实验室）；Institute of High Energy Physics, Chinese Academy of Sciences（中国科学院高能物理研究所）；Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；Brookhaven National Laboratory（布鲁克海文国家实验室）；Center for Computational Quantum Physics, Flatiron Institute（平顿研究院计算量子物理中心）；Arizona State University（亚利桑那州立大学）；Southeast University（东南大学）；Shandong University（山东大学）；Northwestern University（西北大学）
Electronic Origin of Density Wave Orders in a Trilayer Nickelate
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所凝聚态物理国家实验室）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）；Guangdong Provincial Key Laboratory of Magnetoelectric Physics and Devices, School of Physics, Sun Yat-Sen University（中山大学物理学院广东省磁电物理与器件重点实验室）；Technical Institute of Physics and Chemistry, Chinese Academy of Sciences（中国科学院化学物理研究所）；Institute of Theoretical Physics, Chinese Academy of Sciences（中国科学院理论物理研究所）
Correlated Electronic Structure and Density-Wave Gap in Trilayer Nickelate La4Ni3O10
Tsinghua University（清华大学）；Lanzhou University（兰州大学）；Songshan Lake Materials Laboratory（松山湖材料实验室）；ShanghaiTech University（上海科技大学）；University of Oxford（牛津大学）
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…
We report nuclear magnetic resonance data in the bilayer nickelate La3Ni2O6. This material belongs to a family of low valence nickel oxides with square planar coordination of the Ni ions and is isoelectronic to the high temperature superconducting cuprates. Although the three layer nickelate compound exhibits a spin-state transition accompanied by antiferromagnetic order, the bilayer material shows no phase transition. The NMR data in the bilayer La3Ni2O6 reveal the presence of antiferromagnetic spin fluctuations down to 5K that are surprisingly similar to those present in the magnetically ord…
We investigate the crystal structure and the electronic properties of the trilayer nickelate La$_4$Ni$_3$O$_{10}$ by means of quantum mechanical calculations in the framework of the density functional theory. We find that, at low temperature, La$_4$Ni$_3$O$_{10}$ undergoes a hitherto unreported structural phase transition and transforms to a new monoclinic $P2_1/a$ phase. This phase exhibits electronic properties in agreement with recent angle-resolved photoemission spectroscopy data reported in H.\ Li \emph{et al}., Nat.\ Commun.\ \textbf{8}, 704 (2017) and should be considered in models focu…
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)）
Unveiling pressurized bulk superconductivity in a trilayer nickelate Pr4Ni3O10 single crystal
ShanghaiTech University（上海科技大学）；Songshan Lake Materials Laboratory（松山湖材料实验室）；Center for High Pressure Science and Technology Advanced Research（高压科学前沿研究中心）；Institute for Shanghai Advanced Research in Physical Sciences (SHARPS)（上海物理科学研究院）；Beijing University of Technology（北京工业大学）；Japan Synchrotron Radiation Research Institute（日本同步辐射研究机构）；University of Oxford（牛津大学）；Tsinghua University（清华大学）
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…
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）
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）
Ab initio calculations have been performed to unravel the origin of the recently found superlattice peaks in the trilayer nickelate La$_4$Ni$_3$O$_8$. These peaks arise from static charge ordering of Ni$^{2+}$/ Ni$^{1+}$ stripes oriented at 45$^{\circ}$ to the Ni-O bonds. An insulating state originates from a combination of structural distortions and magnetic order, with the gap being formed solely within the d$_{x^2-y^2}$ manifold of states. When doped, electrons or holes would go into these states, in a similar fashion to what occurs in the cuprates. Analogous calculations suggest that check…
Layer Architecture Shapes Electronic, Magnetic, and Lattice Interactions in Ruddlesden-Popper Nickelates
Brookhaven National Laboratory（布鲁克海文国家实验室）；Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory（斯坦福物质与能源科学研究所，SLAC国家加速器实验室）；The University of Tennessee, Knoxville（田纳西大学诺克斯维尔分校）；Harvard University（哈佛大学）；Argonne National Laboratory（阿贡国家实验室）；Oak Ridge National Laboratory（橡树岭国家实验室）；National Synchrotron Light Source II, Brookhaven National Laboratory（国家同步光源二期，布鲁克海文国家实验室）
Electronic structure and magnetic tendencies of trilayer La$_4$Ni$_3$O$_{10}$ under pressure: structural transition, molecular orbitals, and layer differentiation
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）
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）
Single crystals of the metallic Ruddlesden-Popper trilayer nickelates R$_4$Ni$_3$O$_{10}$ (R=La, Pr) were successfully grown using an optical-image floating zone furnace under oxygen pressure (pO$_2$) of 20 bar for La$_4$Ni$_3$O$_{10}$ and 140 bar for Pr$_4$Ni$_3$O$_{10}$. A combination of synchrotron and laboratory x-ray single crystal diffraction, high-resolution synchrotron x-ray powder diffraction and measurements of physical properties revealed that R$_4$Ni$_3$O$_{10}$ (R=La, Pr) crystallizes in the monoclinic $P$2$_1$/$a$ (Z=2) space group at room temperature, and that a metastable ortho…
Magnetic configurations and excitations in high-$T_{c}$ multilayer nickelates
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，凝聚态物理北京国家实验室）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）；Institute of Theoretical Physics, Chinese Academy of Sciences（中国科学院理论物理研究所）；New Cornerstone Science Laboratory, Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所，新基石科学实验室）
A full implementation of the $ab$ $initio$ density functional plus dynamical mean field theory (DFT+DMFT) formalism to perform total energy calculations and structural relaxations is proposed and implemented. The method is applied to the structural and metal-insulator transitions of the rare earth nickelate perovskites as a function of rare earth ion, pressure, and temperature. In contrast to previous DFT and DFT+$U$ theories, the present method accounts for the experimentally observed structure of $La$NiO$_3$ and the insulating nature of the other perovskites, and quantitatively reproduces th…
Spin-density-wave transition in monolayer-trilayer La3Ni2O7 single crystals
ShanghaiTech University（上海科技大学）；Songshan Lake Materials Laboratory（松山湖材料实验室）；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）；University of Chinese Academy of Sciences（中国科学院大学）；Center for High Pressure Science and Technology Advanced Research（高压科学先进研究发展中心）；Shanghai Key Laboratory of Material Frontiers Research in Extreme Environments (MFree)（极端环境材料前沿研究上海市重点实验室）；Institute for Shanghai Advanced Research in Physical Sciences (SHARPS)（上海高等研究院物理科学研究所）；ShanghaiTech Laboratory for Topological Physics（上海科技大学拓扑物理实验室）；Shanghai Key Laboratory of High-resolution Electron Microscopy（高分辨电子显微学上海市重点实验室）；Department of Physics, Clarendon Laboratory, University of Oxford（牛津大学克拉伦登实验室物理系）；School of Physical Sciences, Great Bay University（大湾区大学物理科学学院）
Theoretical analysis on the possibility of superconductivity in a trilayer Ruddlesden-Popper nickelate La$_4$Ni$_3$O$_{10}$ under pressure and its experimental examination: comparison with La$_3$Ni$_2$O$_7$
Dissecting superconductivity in the Ruddlesden-Popper nickelates: The role of electron correlation and interlayer magnetic exchange
Diamond Light Source（钻石光源）；National Synchrotron Radiation Laboratory and School of Nuclear Science and Technology, University of Science and Technology of China（中国科学技术大学核科学与技术学院/国家同步辐射实验室）；Guangdong Provincial Key Laboratory of Magnetoelectric Physics and Devices, School of Physics, Sun Yat-Sen University（中山大学物理学院/广东省铁电与磁器件重点实验室）；Department of Physics, University of Oxford（牛津大学物理系）；National Laboratory of Solid State Microstructures and Department of Physics, Nanjing University（南京大学固体微结构物理国家重点实验室/物理学院）；Collaborative Innovation Center of Advanced Microstructures, Nanjing University（南京大学先进微结构协同创新中心）
Magnetism of the alternating monolayer-trilayer phase of La$_3$Ni$_2$O$_7$
PSI Center for Neutron and Muon Sciences CNM（瑞士保罗谢勒研究所中子与μ子科学中心）；Max-Planck-Institute for Solid State Research（马克斯·普朗克固体研究所）；Physikalisches Institut, Universität Stuttgart（斯图加特大学第二物理研究所）
Heterostructure engineering provides an efficient way to obtain several unconventional phases of LaNiO3, which is otherwise paramagnetic, metallic in bulk form. In this work, a new class of short periodic superlattices, consisting of LaNiO3 and EuNiO3 have been grown by pulsed laser interval deposition to investigate the effect of structural symmetry mismatch on the electronic and magnetic behaviors. Synchrotron based soft and hard X-ray resonant scattering experiments have found that these heterostructures undergo simultaneous electronic and magnetic transitions. Most importantly, LaNiO3 with…
Rare-earth nickelates exhibit a metal-insulator transition accompanied by a structural distortion that breaks the symmetry between formerly equivalent Ni sites. The quantitative theoretical description of this coupled electronic-structural instability is extremely challenging. Here, we address this issue by simultaneously taking into account both structural and electronic degrees of freedom using a charge self-consistent combination of density functional theory and dynamical mean-field theory, together with screened interaction parameters obtained from the constrained random phase approximatio…
