| CONDENSED MATTER: ELECTRONIC STRUCTURE, ELECTRICAL, MAGNETIC, AND OPTICAL PROPERTIES |
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Contrasting Magnetism in Isovalent Layered LaSr$_{3}$NiRuO$_{4}$H$_{4}$ and LaSrNiRuO$_{4}$ due to Distinct Spin-Orbital States |
| Xuan Wen1, Ke Yang1, Hua Wu1,2** |
1Laboratory for Computational Physical Sciences (MOE), State Key Laboratory of Surface Physics, and Department of Physics, Fudan University, Shanghai 200433
2Collaborative Innovation Center of Advanced Microstructures, Nanjing 210093
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| Cite this article: |
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Xuan Wen, Ke Yang, Hua Wu 2019 Chin. Phys. Lett. 36 077501 |
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Abstract The recently synthesized first $4d$ transition-metal oxide-hydride LaSr$_{3}$NiRuO$_{4}$H$_{4}$ with the unusual high H:O ratio surprisingly displays no magnetic order down to 1.8 K. This is in sharp contrast to the similar unusual low-valent Ni$^{+}$-Ru$^{2+}$ layered oxide LaSrNiRuO$_{4}$ which has a rather high ferromagnetic (FM) ordering Curie temperature $T_{\rm C}\sim 250$ K. Using density functional calculations with the aid of crystal field level diagrams and superexchange pictures, we find that the contrasting magnetism is due to the distinct spin-orbital states of the Ru$^{2+}$ ions (in addition to the common Ni$^{+}$ $S=1/2$ state but with a different orbital state): the Ru$^{2+}$ $S=0$ state in LaSr$_{3}$NiRuO$_{4}$H$_{4}$, but the Ru$^{2+}$ $S=1$ state in LaSrNiRuO$_{4}$. The Ru$^{2+}$ $S=0$ state has the $(xy)^2(xz,yz)^4$ occupation due to the RuH$_4$O$_2$ octahedral coordination, and then the nonmagnetic Ru$^{2+}$ ions dilute the $S=1/2$ Ni$^+$ sublattice which consequently has a very weak antiferromagnetic superexchange and thus accounts for the presence of no magnetic order down to 1.8 K in LaSr$_{3}$NiRuO$_{4}$H$_{4}$. In strong contrast, the Ru$^{2+}$ $S=1$ state in LaSrNiRuO$_{4}$ has the $(3z^2-r^2)^2(xz,yz)^3(xy)^1$ occupation due to the planar square RuO$_4$ coordination, and then the multi-orbital FM superexchange between the $S=1/2$ Ni$^+$ and $S=1$ Ru$^{2+}$ ions gives rise to the high $T_{\rm C}$ in LaSrNiRuO$_{4}$. This work highlights the importance of spin-orbital states in determining the distinct magnetism.
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Received: 14 May 2019
Published: 20 June 2019
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| PACS: |
75.25.Dk
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(Orbital, charge, and other orders, including coupling of these orders)
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71.70.-d
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(Level splitting and interactions)
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71.20.-b
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(Electron density of states and band structure of crystalline solids)
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| Fund: Supported by the National Natural Science Foundation of China under Grant Nos 11674064 and 11474059, and the National Key Research and Development Program of China under Grant No 2016YFA0300700. |
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