The Crystal Structure and Magnetic Behavior of Quinary Osmate and Ruthenate Double Perovskites la ABB ′o6 (A = Ca, Sr; B = Co, Ni; B ′ = Ru, Os)

Ryan Morrow, Michael A. McGuire, Jiaqiang Yan, Patrick M. Woodward

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20 Scopus citations

Abstract

Six LaABB′O6 (A = Ca, Sr; B = Co, Ni; B′ = Ru, Os) double perovskites were synthesized, several for the first time, and their crystal structures and magnetic behavior were characterized with neutron powder diffraction and direct-current and alternating-current magnetometry. All six compounds crystallize with P21/n space group symmetry, resulting from a-a-c+ octahedral tilting and complete rock salt ordering of transition-metal ions. Despite the electronic configurations of the transition-metal ions, either d8-d3 or d7-d3, not one of the six compounds shows ferromagnetism as predicted by the Goodenough-Kanamori rules. LaSrNiOsO6, LaSrNiRuO6, and LaCaNiRuO6 display long-range antiferromagnetic order, while LaCaNiOsO6, LaCaCoOsO6, and LaSrCoOsO6 exhibit spin-glass behavior. These compounds are compared to the previously studied LaCaCoRuO6 and LaSrCoRuO6, both of which order antiferromagnetically. The observed variations in magnetic properties can be attributed largely to the response of competing superexchange pathways due to changes in B-O-B′ bond angles, differences in the radial extent of the 4d (B′ = Ru) and 5d (B′ = Os) orbitals, and filling of the t2g orbitals of the 3d ion.

Original languageEnglish
Pages (from-to)2989-3001
Number of pages13
JournalInorganic Chemistry
Volume57
Issue number6
DOIs
StatePublished - Mar 19 2018

Funding

Support for this research was provided the Center for Emergent Materials an NSF Materials Research Science and Engineering Center (DMR-1420451). A portion of this research was performed at Oak Ridge National Laboratory’s Spallation Neutron Source, which is sponsored by the U.S. Department of Energy, Office of Basic Energy Sciences. M.A.M. acknowledges support from the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. R.M. acknowledges support from the Alexander von Humboldt Foundation. The authors thank A. Huq and P. Whitfield for assistance with the neutron powder diffraction experiments.

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