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Register a new userGiant orbital polarization of Ni$^{2+}$ in square planar environment
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Understanding the electronic behavior of Ni$^{2+}$ in a square planar environment of oxygen is the key to unravel the origin of the recently discovered superconductivity in the hole doped nickelate Nd$_{0.8}$Sr$_{0.2}$NiO$_2$. To identify the major similarities/dissimilarities between nickelate and cuprate superconductivity, the study of the electronic structure of Ni$^{2+}$ and Cu$^{2+}$ in an identical square planar environment is essential. In order to address these questions, we investigate the electronic structure of Sr$_2$CuO$_3$ and Ni doped Sr$_2$CuO$_3$ single crystals containing (Cu/Ni)O$_4$ square planar units. Our polarization dependent X-ray absorption spectroscopy experiments for Ni in Sr$_2$Cu$_{0.9}$Ni$_{0.1}$O$_3$ have revealed very large orbital polarization, which is a characteristic feature of high $T_c$ cuprate. This arises due to the low spin $S$=0 configuration with two holes in Ni 3$d_{x^2-y^2}$ orbitals - in contrast to the expected high spin $S$=1 state from Hunds first rule. The presence of such $S$=0 Ni$^{2+}$ in hole doped nickelate would be analogous to the Zhang Rice singlet. However, the Mott Hubbard insulating nature of the NiO$_4$ unit would point towards a different electronic phase space of nickelates, compared to high $T_c$ cuprates.
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High temperature cuprate superconductivity remains a defining problem in condensed matter physics. Among myriad approaches to addressing this problem has been the study of alternative transition metal oxides with similar structures and 3d electron count that are suggested as proxies for cuprate physics. None of these analogs has been superconducting, and few are even metallic. Here, we report that the low-valent, quasi-two-dimensional trilayer compound, Pr4Ni3O8 avoids a charge-stripe ordered phase previously reported for La4Ni3O8, leading to a metallic ground state. By combining x-ray absorption spectroscopy and density functional theory calculations, we further find that metallic Pr4Ni3O8 exhibits a low-spin configuration and significant orbital polarization of the unoccupied eg states with pronounced dx2-y2 character near the Fermi energy, both hallmarks of the cuprate superconductors. Belonging to a regime of 3d electron count found for hole-doped cuprates, Pr4Ni3O8 thus represents one of the closest analogies to cuprates yet reported and a singularly promising candidate for high-Tc superconductivity if appropriately doped.
The electronic states near the Fermi level of recently discovered superconductor Ba$_2$CuO$_{4-delta}$ consist primarily of the Cu $d_{x^2-y^2}$ and $d_{3z^2-r^2}$ orbitals. We investigate the electronic correlation effect and the orbital polarization of an effective two-orbital Hubbard model mimicking the low-energy physics of Ba$_2$CuO$_{4-delta}$ in the hole-rich regime by utilizing the dynamical mean-field theory with the Lanczos method as the impurity solver. We find that the hole-overdoped Ba$_2$CuO$_{4-delta}$ with $3d^8$ (Cu$^{3+}$) is in the orbital-selective Mott phase (OSMP) at half-filling, and the typical two-orbital feature remains in Ba$_2$CuO$_{4-delta}$ when the electron filling approaches $n_esim 2.5$, which closely approximates to the experimental hole doping for the emergence of the high-$T_c$ superconductivity. We also obtain that the orbital polarization is very stable in the OSMP, and the multiorbital correlation can drive orbital polarization transitions. These results indicate that in hole-overdoped Ba$_2$CuO$_{4-delta}$ the OSMP physics and orbital polarization, local magnetic moment, and spin or orbital fluctuations still exist. We propose that our present results are also applicable to Sr$_2$CuO$_{4-delta}$ and other two-orbital cuprates, demanding an unconventional multiorbital superconducting scenario in hole-overdoped high-$T_c$ cuprates.
Using polarized neutron diffraction and x-ray resonant magnetic scattering (XRMS) techniques, multiple phase transitions were revealed in an underdoped, non-superconducting Eu(Fe$_{1-x}$Ir$_{x}$)$_{2}$As$_{2}$ ($mathit{x}$ = 0.06) single crystal. Compared with the parent compound EuFe$_{2}$As$_{2}$, the tetragonal-to-orthorhombic structural phase transition and the antiferromagnetic order of the Fe$^{2+}$ moments are significantly suppressed to $mathit{T_{S}}$ = 111 (2) K and $mathit{T_{N,Fe}}$= 85 (2) K by 6% Ir doping, respectively. In addition, the Eu$^{2+}$ spins order within the $mathit{ab}$ plane in the A-type antiferromagnetic structure similar to the parent compound. However, the order temperature is evidently suppressed to $mathit{T_{N,Eu}}$= 16.0 (5) K by Ir doping. Most strikingly, the XRMS measurements at the Ir $mathit{L_{3}}$ edge demonstrates that the Ir 5$mathit{d}$ states are also magnetically polarized, with the same propagation vector as the magnetic order of Fe. With $mathit{T_{N,Ir}}$ = 12.0 (5) K, they feature a much lower onset temperature compared with $mathit{T_{N,Fe}}$. Our observation suggests that the magnetism of the Eu sublattice has a considerable effect on the magnetic nature of the 5$mathit{d}$ Ir dopant atoms and there exists a possible interplay between the localized Eu$^{2+}$ moments and the conduction $mathit{d}$-electrons on the FeAs layers.
In strongly correlated multi-orbital systems, various ordered phases appear. In particular, the orbital order in iron-based superconductors attracts much attention since it is considered to be the origin of the nematic state. In order to clarify the essential condition for realizing orbital orders, we study simple two-orbital ($d_{xz}$, $d_{yz}$) Hubbard model. We find that the orbital order, which corresponds to the nematic order, appears due to the vertex corrections even in the two-orbital model. Thus, $d_{xy}$ orbital is not essential to realize the nematic orbital order. The obtained orbital order depends on the orbital dependence and the topology of fermi surfaces. We also find that another type of orbital order, which is rotated $45^circ$, appears in the heavily hole-doped case.
How superconductivity interacts with charge or nematic order is one of the great unresolved issues at the center of research in quantum materials. Ba$_{1-x}$Sr$_{x}$Ni$_{2}$As$_{2}$ (BSNA) is a charge ordered pnictide superconductor recently shown to exhibit a six-fold enhancement of superconductivity due to nematic fluctuations near a quantum phase transition (at $x_c=0.7$). The superconductivity is, however, anomalous, with the resistive transition for $0.4 < x< x_c$ occurring at a higher temperature than the specific heat anomaly. Using x-ray scattering, we discovered a new charge density wave (CDW) in BSNA in this composition range. The CDW is commensurate with a period of two lattice parameters, and is distinct from the two CDWs previously reported in this material. We argue that the anomalous transport behavior arises from heterogeneous superconductivity nucleating at antiphase domain walls in this CDW. We also present new data on the incommensurate CDW, previously identified as being unidirectional, showing that is a rotationally symmetric, 4$Q$ state with $C_4$ symmetry. Our study establishes BSNA as a rare material containing three distinct CDWs, and an exciting testbed for studying coupling between CDW, nematic, and SC orders.
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