Asmara Teguh Citra, Green Robert J, Suter Andreas, Wei Yuan, Zhang Wenliang, Knez Daniel, Harris Grant, Tseng Yi, Yu Tianlun, Betto Davide, Garcia-Fernandez Mirian, Agrestini Stefano, Klein Yannick Maximilian, Kumar Neeraj, Galdino Carlos William, Salman Zaher, Prokscha Thomas, Medarde Marisa, Müller Elisabeth, Soh Yona, Brookes Nicholas B, Zhou Ke-Jin, Radovic Milan, Schmitt Thorsten
PSI Center for Photon Science, Paul Scherrer Institute, Forschungsstrasse 111, Villigen PSI, CH-5232, Switzerland.
European X-Ray Free-Electron Laser Facility GmbH, Holzkoppel 4, 22869, Schenefeld, Germany.
Adv Mater. 2024 Sep;36(38):e2310668. doi: 10.1002/adma.202310668. Epub 2024 Aug 5.
Strongly-correlated transition-metal oxides are widely known for their various exotic phenomena. This is exemplified by rare-earth nickelates such as LaNiO, which possess intimate interconnections between their electronic, spin, and lattice degrees of freedom. Their properties can be further enhanced by pairing them in hybrid heterostructures, which can lead to hidden phases and emergent phenomena. An important example is the LaNiO/LaTiO superlattice, where an interlayer electron transfer has been observed from LaTiO into LaNiO leading to a high-spin state. However, macroscopic emergence of magnetic order associated with this high-spin state has so far not been observed. Here, by using muon spin rotation, x-ray absorption, and resonant inelastic x-ray scattering, direct evidence of an emergent antiferromagnetic order with high magnon energy and exchange interactions at the LaNiO/LaTiO interface is presented. As the magnetism is purely interfacial, a single LaNiO/LaTiO interface can essentially behave as an atomically thin strongly-correlated quasi-2D antiferromagnet, potentially allowing its technological utilization in advanced spintronic devices. Furthermore, its strong quasi-2D magnetic correlations, orbitally-polarized planar ligand holes, and layered superlattice design make its electronic, magnetic, and lattice configurations resemble the precursor states of superconducting cuprates and nickelates, but with an S→1 spin state instead.
强关联过渡金属氧化物因其各种奇异现象而广为人知。稀土镍酸盐如LaNiO就是一个例子,它在电子、自旋和晶格自由度之间存在紧密的相互联系。通过将它们配对形成混合异质结构,可以进一步增强其性能,这可能导致隐藏相和新出现的现象。一个重要的例子是LaNiO/LaTiO超晶格,在其中观察到了从LaTiO到LaNiO的层间电子转移,从而导致高自旋态。然而,迄今为止尚未观察到与这种高自旋态相关的磁有序的宏观出现。在这里,通过使用μ子自旋旋转、x射线吸收和共振非弹性x射线散射,给出了在LaNiO/LaTiO界面出现具有高磁振子能量和交换相互作用的反铁磁有序的直接证据。由于磁性纯粹是界面性的,单个LaNiO/LaTiO界面本质上可以表现为原子级薄的强关联准二维反铁磁体,这可能使其在先进的自旋电子器件中得到技术应用。此外,其强准二维磁关联、轨道极化的平面配体空穴和层状超晶格设计使其电子、磁和晶格构型类似于超导铜酸盐和镍酸盐的前驱体状态,但自旋态为S→1。