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The influence of spin-orbit coupling (SOC) on the physical properties of the5d2 system Sr2MgOsO6 is probed via a combination of magnetometry, specific heatmeasurements, elastic and inelastic neutron scattering, and density functionaltheory calculations. Although a significant degree of frustration is expected,we find that Sr2MgOsO6 orders in a type I antiferromagnetic structure at theremarkably high temperature of 108 K. The measurements presented allow for thefirst accurate quantification of the size of the magnetic moment in a 5d2system of 0.60(2) muB - a significantly reduced moment from the expected valuefor such a system. Furthermore, significant anisotropy is identified via a spinexcitation gap, and we confirm by first principles calculations that SOC notonly provides the magnetocrystalline anisotropy, but also plays a crucial rolein determining both the ground state magnetic order and the size of the localmoment in this compound. Through comparison to Sr2ScOsO6, it is demonstratedthat SOC-induced anisotropy has the ability to relieve frustration in 5d2systems relative to their 5d3 counterparts, providing an explanation of thehigh TN found in Sr2MgOsO6.

Spin-orbit coupling control of anisotropy, ground state and frustration in 5d2 Sr2MgOsO6