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Register a new userOrbital control of noncollinear magnetic order in nickelate heterostructures
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We have used resonant x-ray diffraction to develop a detailed description of antiferromagnetic ordering in epitaxial superlattices based on two-unit-cell thick layers of the strongly correlated metal LaNiO3. We also report reference experiments on thin films of PrNiO3 and NdNiO3. The resulting data indicate a spiral state whose polarization plane can be controlled by adjusting the Ni d-orbital occupation via two independent mechanisms: epitaxial strain and quantum confinement of the valence electrons. The data are discussed in the light of recent theoretical predictions.
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Oxygen vacancies play a crucial role in the control of the electronic, magnetic, ionic, and transport properties of functional oxide perovskites. Rare earth nickelates (RENiO$_{3-x}$) have emerged over the years as a rich platform to study the interplay between the lattice, the electronic structure, and ordered magnetism. In this study, we investigate the evolution of the electronic and magnetic structure in thin films of RENiO$_{3-x}$, using a combination of X-ray absorption spectroscopy and imaging, resonant X-ray scattering, and extended multiplet ligand field theory modeling. We find that oxygen vacancies modify the electronic configuration within the Ni-O orbital manifolds, leading to a dramatic evolution of long-range electronic transport pathways despite the absence of nanoscale phase separation. Remarkably, magnetism is robust to substantial levels of carrier doping, and only a moderate weakening of the $(1/4, 1/4, 1/4)_{pc}$ antiferromagnetic order parameter is observed, whereas the magnetic transition temperature is largely unchanged. Only at a certain point long-range magnetism is abruptly erased without an accompanying structural transition. We propose the progressive disruption of the 3D magnetic superexchange pathways upon introduction of point defects as the mechanism behind the sudden collapse of magnetic order in oxygen-deficient nickelates. Our work demonstrates that, unlike most other oxides, ordered magnetism in RENiO$_{3-x}$ is mostly insensitive to carrier doping. The sudden collapse of ordered magnetism upon oxygen removal may provide a new mechanism for solid-state magneto-ionic switching and new applications in antiferromagnetic spintronics.
Magnetic ordering phenomena have a profound influence on the macroscopic properties of correlated-electron materials, but their realistic prediction remains a formidable challenge. An archetypical example is the ternary nickel oxide system RNiO3 (R = rare earth), where the period-four magnetic order with proposals of collinear and non-collinear structures and the amplitude of magnetic moments on different Ni sublattices have been subjects of debate for decades. Here we introduce an elementary model system - NdNiO3 slabs embedded in a non-magnetic NdGaO3 matrix - and use polarized resonant x-ray scattering (RXS) to show that both collinear and non-collinear magnetic structures can be realized, depending on the slab thickness. The crossover between both spin structures is correctly predicted by density functional theory and can be qualitatively understood in a low-energy spin model. We further demonstrate that the amplitude ratio of magnetic moments in neighboring NiO6 octahedra can be accurately determined by RXS in combination with a correlated double cluster model. Targeted synthesis of model systems with controlled thickness and synergistic application of polarized RXS and ab-initio theory thus provide new perspectives for research on complex magnetism, in analogy to two-dimensional materials created by exfoliation.
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.
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.
Resonant inelastic x-ray scattering is used to investigate the electronic origin of orbital polarization in nickelate heterostructures taking $mathrm{LaTiO_3-LaNiO_3-3x(LaAlO_3)}$, a system with exceptionally large polarization, as a model system. We find that heterostructuring generates only minor changes in the Ni $3d$ orbital energy levels, contradicting the often-invoked picture in which changes in orbital energy levels generate orbital polarization. Instead, O $K$-edge x-ray absorption spectroscopy demonstrates that orbital polarization is caused by an anisotropic reconstruction of the oxygen ligand hole states. This provides an explanation for the limited success of theoretical predictions based on tuning orbital energy levels and implies that future theories should focus on anisotropic hybridization as the most effective means to drive large changes in electronic structure and realize novel emergent phenomena.
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