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The magnetic ground state in the double perovskite system Sr2-xCaxCoOsO6changes from an antiferromagnet (x = 0), to a spin glass (x = 1), to aferrimagnet (x = 2) as the Ca content increases. This crossover is driven bychemical pressure effects that control the relative strength of magneticexchange interactions. The synthesis, crystal structure, and magnetism ofSrCaCoOsO6 and Ca2CoOsO6 are investigated and compared with Sr2CoOsO6. Bothcompounds 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 angleevolves from 158.0(3) degrees in SrCaCoOsO6 to 150.54(9) degrees in Ca2CoOsO6as the smaller Ca2+ ion replaces Sr2+. While this change may seem minor it hasa profound effect on the magnetism, changing the magnetic ground state fromantiferromagnetic in Sr2CoOsO6 (TN1 = 108 K, TN2 = 70 K), to a spin glass inSrCaCoOsO6 (Tf1 = 32 K, Tf2 = 13 K), to ferrimagnetic in Ca2CoOsO6 (TC = 145K). In the first two compounds the observation of two transitions is consistentwith weak coupling between the Co and Os sublattices.

Effects of chemical pressure on the magnetic ground states of the osmate double perovskites SrCaCoOsO6 and Ca2CoOsO6