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Register a new userSpin stripe order in a square planar trilayer nickelate
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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. Here we report single crystal neutron diffraction measurements (both polarized and unpolarized) that establish that the ground state is indeed magnetic. The ordering is modeled as antiferromagnetic spin stripes that are commensurate with the charge stripes, the magnetic ordering occurring in individual trilayers that are essentially uncorrelated along the crystallographic c-axis. Comparison of the charge and spin stripe order parameters reveals that, in contrast to single-layer nickelates such as La2-xSrxNiO4 as well as related quasi-2D oxides including manganites, cobaltates, and cuprates, these orders uniquely appear simultaneously, thus demonstrating a stronger coupling between spin and charge than in these related low-dimensional correlated oxides.
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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 ability to probe symmetry breaking transitions on their natural time scales is one of the key challenges in nonequilibrium physics. Stripe ordering represents an intriguing type of broken symmetry, where complex interactions result in atomic-scale lines of charge and spin density. Although phonon anomalies and periodic distortions attest the importance of electron-phonon coupling in the formation of stripe phases, a direct time-domain view of vibrational symmetry breaking is lacking. We report experiments that track the transient multi-THz response of the model stripe compound La$_{1.75}$Sr$_{0.25}$NiO$_{4}$, yielding novel insight into its electronic and structural dynamics following an ultrafast optical quench. We find that although electronic carriers are immediately delocalized, the crystal symmetry remains initially frozen - as witnessed by time-delayed suppression of zone-folded Ni-O bending modes acting as a fingerprint of lattice symmetry. Longitudinal and transverse vibrations react with different speeds, indicating a strong directionality and an important role of polar interactions. The hidden complexity of electronic and structural coupling during stripe melting and formation, captured here within a single terahertz spectrum, opens new paths to understanding symmetry breaking dynamics in solids.
Strongly correlated electrons in layered perovskite structures have been the birthplace of high-temperature superconductivity, spin liquid, and quantum criticality. Specifically, the cuprate materials with layered structures made of corner sharing square planar CuO$_4$ units have been intensely studied due to their Mott insulating grounds state which leads to high-temperature superconductivity upon doping. Identifying new compounds with similar lattice and electronic structures has become a challenge in solid state chemistry. Here, we report the hydrothermal crystal growth of a new copper tellurite sulfate Cu$_3$(TeO$_4$)(SO$_4$)$cdot$H$_2$O, a promising alternative to layered perovskites. The orthorhombic phase (space group $Pnma$) is made of corrugated layers of corner-sharing CuO$_4$ square-planar units that are edge-shared with TeO$_4$ units. The layers are linked by slabs of corner-sharing CuO$_4$ and SO$_4$. Using both the bond valence sum analysis and magnetization data, we find purely Cu$^{2+}$ ions within the layers, but a mixed valence of Cu$^{2+}$/Cu${^+}$ between the layers. Cu$_3$(TeO$_4$)(SO$_4$)$cdot$H$_2$O undergoes an antiferromagnetic transition at $T_N$=67 K marked by a peak in the magnetic susceptibility. Upon further cooling, a spin-canting transition occurs at $T^{star}$=12 K evidenced by a kink in the heat capacity. The spin-canting transition is explained based on a $J_1$-$J_2$ model of magnetic interactions, which is consistent with the slightly different in-plane super-exchange paths. We present Cu$_3$(TeO$_4$)(SO$_4$)$cdot$H$_2$O as a promising platform for the future doping and strain experiments that could tune the Mott insulating ground state into superconducting or spin liquid states.
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.
We report the physical properties and electronic structure calculations of a layered chromium oxypnictide, Sr$_2$Cr$_3$As$_2$O$_2$, which crystallizes in a Sr$_2$Mn$_3$As$_2$O$_2$-type structure containing both CrO$_2$ planes and Cr$_2$As$_2$ layers. The newly synthesized material exhibits a metallic conduction with a dominant electron-magnon scattering. Magnetic and specific-heat measurements indicate at least two intrinsic magnetic transitions below room temperature. One is an antiferromagnetic transition at 291 K, probably associated with a spin ordering in the Cr$_2$As$_2$ layers. Another transition is broad, occurring at around 38 K, and possibly due to a short-range spin order in the CrO$_2$ planes. Our first-principles calculations indicate predominant two-dimensional antiferromagnetic exchange couplings, and suggest a KG-type (i.e. K$_2$NiF$_4$ type for CrO$_2$ planes and G type for Cr$_2$As$_2$ layers) magnetic structure, with reduced moments for both Cr sublattices. The corresponding electronic states near the Fermi energy are mostly contributed from Cr-3$d$ orbitals which weakly (modestly) hybridize with the O-2$p$ (As-4$p$) orbitals in the CrO$_2$ (Cr$_2$As$_2$) layers. The bare bandstructure density of states at the Fermi level is only $sim$1/4 of the experimental value derived from the low-temperature specific-heat data, consistent with the remarkable electron-magnon coupling. The title compound is argued to be a possible candidate to host superconductivity.
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