Effects of chemical pressure on the magnetic ground states of the osmate double perovskites SrCaCoOs6 and Ca2CoOsO6

Morrow, Ryan; Yan, Jiaqiang; McGuire, Michael A.; Freeland, John W.; Haskel, Daniel; Woodward, Patrick M.

doi:10.1103/PhysRevB.92.094435

Title: Effects of chemical pressure on the magnetic ground states of the osmate double perovskites SrCaCoOs₆ and Ca₂CoOsO₆

Journal Article · Mon Sep 21 00:00:00 EDT 2015 · Physical Review. B, Condensed Matter and Materials Physics

DOI:https://doi.org/10.1103/PhysRevB.92.094435· OSTI ID:1265814

Morrow, Ryan ^[1]; Yan, Jiaqiang ^[2]; McGuire, Michael A. ^[3]; Freeland, John W. ^[4]; Haskel, Daniel ^[4]; Woodward, Patrick M. ^[1]

The Ohio State Univ., Columbus, OH (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

The magnetic ground state in the double perovskite system Sr_2-xCa_xCoOsO₆ changes from an antiferromagnet (x=0), to a spin glass (x=1), to a ferrimagnet (x=2) as the Ca content increases. Moreover, this crossover is driven by chemical pressure effects that control the relative strength of magnetic exchange interactions. The synthesis, crystal structure, and magnetism of SrCaCoOsO₆ and Ca₂CoOsO₆ are investigated and compared with Sr₂CoOsO₆. Both compounds adopt a monoclinic crystal structure with rock-salt ordering of Co²⁺ and Os⁶⁺ and a^-a^-b⁺ octahedral tilting, but the average Co–O–Os bond angle evolves from 158.0(3) in SrCaCoOsO₆ to 150.54(9)° in Ca₂CoOsO₆ as the smaller Ca²+ ion replaces Sr²⁺. And while this change may seem minor, it has a profound effect on the magnetism, changing the magnetic ground state from antiferromagnetic in Sr₂CoOsO₆ (TN1=108K, T_N2=70K), to a spin glass in SrCaCoOsO₆ (T_f1=32K, T_f2=13K), to ferrimagnetic in Ca₂CoOsO₆ (T_C=145K). Finally, in the first two compounds the observation of two transitions is consistent with weak coupling between the Co and Os sublattices.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357

OSTI ID:: 1265814

Alternate ID(s):: OSTI ID: 1222364

Journal Information:: Physical Review. B, Condensed Matter and Materials Physics, Vol. 92, Issue 9; ISSN 1098-0121

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 32 works

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[OsF ₆ ] ^{x −} : Molecular Models for Spin-Orbit Entangled Phenomena Pedersen, Kasper S.; Woodruff, Daniel N.; Singh, Saurabh Kumar Chemistry - A European Journal, Vol. 23, Issue 47 https://doi.org/10.1002/chem.201702894	journal	July 2017
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