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The ability to tune exchange (magnetic) interactions between 3d transition metals in perovskite structures has proven to be a powerful route to discovery of novel properties. Here we demonstrate that the introduction of 3d-5d exchange pathways in double perovskites enables additional tunability, a result of the large spatial extent of 5d wave functions. Using x-ray probes of magnetism and structure at high pressure, we show that compression of Sr2FeOsO6 drives an unexpected continuous change in the sign of Fe-Os exchange interactions and a transition from antiferromagnetic to ferrimagnetic order. We analyze the relevant electron-electron interactions, shedding light into fundamental differences with the more thoroughly studied 3d-3d systems

physical review. b, condensed matter and materials physics

Fragility of ferromagnetic double exchange interactions and pressure tuning of magnetism in<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mn>3</mml:mn><mml:mi>d</mml:mi><mml:mtext>−</mml:mtext><mml:mn>5</mml:mn><mml:mi>d</mml:mi></mml:math>double perovskite<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:msub><mml:mi mathvariant="normal">Sr</mml:mi><mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">FeOsO</mml:mi><mml:mn>6</mml:mn></mml:msub></mml:…

Fragility of ferromagnetic double exchange interactions and pressure tuning of magnetism in3d−5ddouble perovskiteSr2FeOsO6