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Register a new userMagnetic exchange coupling in cuprate-analog $d^9$ nickelates
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Motivated by the recent discovery of superconductivity in doped NdNiO$_2$, we study the magnetic exchange interaction $J$ in layered $d^9$ nickelates from first principles. The mother compounds of the high-$T_{rm c}$ cuprates belong to the charge-transfer regime in the Zaanen-Sawatzky-Allen diagram and have $J$ larger than 100 meV. While this feature makes the cuprates very different from other transition metal oxides, it is of great interest whether layered $d^9$ nickelates can also have such a large $J$. However, one complexity is that NdNiO$_2$ is not a Mott insulator due to carrier doping from the block layer. To compare the cuprates and $d^9$ nickelates on an equal basis, we study RbCa$_2$NiO$_3$ and $A_{2}$NiO$_{2}$Br$_2$ ($A$: a cation with the valence of $2.5+$), which were recently designed theoretically by block-layer engineering. These nickelates are free from the self-doping effect and belong to the Mott-Hubbard regime. We show that these nickelates share a common thread with the high-$T_{rm c}$ cuprates in that they also have a significant exchange interaction $J$ as large as about 100 meV.
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The discovery of unconventional superconductivity in hole doped NdNiO2, similar to CaCuO2, has received enormous attention. However, different from CaCuO2, RNiO2 (R = Nd, La) has itinerant electrons in the rare-earth spacer layer. Previous studies show that the hybridization between Ni-dx2-y2 and rare-earth-d orbitals is very weak and thus RNiO2 is still a promising analog of CaCuO2. Here, we perform first-principles calculations to show that the hybridization between Ni-dx2-y2 orbital and itinerant electrons in RNiO2 is substantially stronger than previously thought. The dominant hybridization comes from an interstitial-s orbital rather than rare-earth-d orbitals, due to a large inter-cell hopping. Because of the hybridization, Ni local moment is screened by itinerant electrons and the critical U_Ni for long-range magnetic ordering is increased. Our work shows that the electronic structure of RNiO2 is distinct from CaCuO2, implying that the observed superconductivity in infinite-layer nickelates does not emerge from a doped Mott insulator.
High-Tc superconductivity in cuprates is generally believed to arise from carrier doping an antiferromagnetic Mott (AFM) insulator. Theoretical proposals and emerging experimental evidence suggest that this process leads to the formation of intriguing electronic liquid crystal phases. These phases are characterized by ordered charge and/or spin density modulations, and thought to be intimately tied to the subsequent emergence of superconductivity. The most elusive, insulating charge-stripe crystal phase is predicted to occur when a small density of holes is doped into the charge-transfer insulator state, and would provide a missing link between the undoped parent AFM phase and the mysterious, metallic pseudogap. However, due to experimental challenges, it has been difficult to observe this phase. Here, we use surface annealing to extend the accessible doping range in Bi-based cuprates and achieve the lightly-doped charge-transfer insulating state of a cuprate Bi2Sr2CaCu2O8+x. In this insulating state with a charge transfer gap at the order of ~1 eV, using spectroscopic-imaging scanning tunneling microscopy, we discover a unidirectional charge-stripe order with a commensurate 4a0 period along the Cu-O-Cu bond. Importantly, this insulating charge-stripe crystal phase develops before the onset of the pseudogap and the formation of the Fermi surface. Our work provides new insights into the microscopic origin of electronic inhomogeneity in high-Tc cuprates.
Spontaneous symmetry breaking constitutes a paradigmatic classification scheme of matter. However, broken symmetry also entails domain degeneracy that often impedes identification of novel low symmetry states. In quantum matter, this is additionally complicated by competing intertwined symmetry breaking orders. A prime example is that of unconventional superconductivity and density-wave orders in doped cuprates in which their respective symmetry relation remains a key question. Using uniaxial pressure as a domain-selective stimulus in combination with x-ray diffraction, we unambiguously reveal that the fundamental symmetry of the charge order in the prototypical cuprate La$_{1.88}$Sr$_{0.12}$CuO$_4$ is characterized by uniaxial stripes. We further demonstrate the direct competition of this stripe order with unconventional superconductivity via magnetic field tuning. The stripy nature of the charge-density-wave state established by our study is a prerequisite for the existence of a superconducting pair-density-wave -- a theoretical proposal that clarifies the interrelation of intertwined quantum phases in unconventional superconductors -- and paves the way for its high-temperature realization.
We report on a resonant soft X-ray spectroscopy study of the electronic and magnetic structure of the cuprate-manganite interface. Polarized X-ray spectroscopy measurements taken at the Cu L edge reveal up to a five-fold increase in the dichroic signal as compared to past experimental and theoretical values. Furthermore an increase in the degree of interlayer charge transfer up to 0.25e (where e is charge of an electron) per copper ion is observed leading to a profound reconstruction in the orbital scheme for these interfacial copper ions. It is inferred that these enhancement are related to an increase in TMI observed for manganite layers grown with rapidly modulated flux.
The race to obtain a higher critical temperature (Tc) in the superconducting cuprates has been virtually suspended since it was optimized under high pressure in a hole-doped trilayer cuprate. We report the anomalous increase in Tc under high pressure for the electron-doped infinite-layer cuprate Sr0.9La0.1CuO2 in the vicinity of the antiferromagnetic critical point. By the application of a pressure of 15 GPa, Tc increases to 45 K, which is the highest temperature among the electron-doped cuprates and ensures unconventional superconductivity. We describe the electronic phase diagram of Sr1-xLaxCuO2 to discuss the relation between the antiferromagnetic order and superconductivity.
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