Abstract
A new oxide, LaMn3Ni2Mn2O12, was prepared by high-pressure and high-temperature synthesis methods. The compound crystallizes in an AA'3B2B'2O12-type A-site and B-site ordered quadruple perovskite structure. The charge combination is confirmed to be LaMn3+3Ni2+2Mn4+2O12, where La and Mn3+ are 1:3 ordered at the A and A' sites and the Ni2+ and Mn4+ are also distributed at the B and B' sites in an orderly fashion in a rocksalt-type manner, respectively. A G-type antiferromagnetic ordering originating from the A'-site Mn3+ sublattice is found to occur at TN ≈ 46 K. Subsequently, the spin coupling between the B-site Ni2+ and B'-site Mn4+ sublattices leads to an orthogonally ordered spin alignment with a net ferromagnetic component near TC ≈ 34 K. First-principles calculations demonstrate that the A'-site Mn3+ spins play a crucial role in determining the spin structure of the B and B' sites. This LaMn3Ni2Mn2O12 provides a rare example that shows orthogonal spin ordering in the B and B' sites assisted by ordered A-site magnetic ions in perovskite systems.
Original language | English |
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Pages (from-to) | 8988-8996 |
Number of pages | 9 |
Journal | Chemistry of Materials |
Volume | 28 |
Issue number | 24 |
DOIs | |
State | Published - Dec 27 2016 |
Funding
The authors thank G. B. Li for his useful discussion. This work was supported by the 973 Project of the Ministry of Science and Technology of China (Grants 2014CB921500 and 2016YFA0300701), the National Natural Science Foundation of China (Grant 11574378), and the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant XDB07030300). J.A.A. is grateful for the financial support of Spanish MINECO Project MAT2013-41099-R. The work at ORNL HFIR (H.C. and C.d.C.) was sponsored by the Scientific User Facilities Division, Office of Science, Basic Energy Sciences, U.S. Department of Energy.