Joe Paddison

Magnetism and disorder

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Orbital dimers drive spin-glass formation

P M M Thygesen, J A M Paddison, R Zhang, K A Beyer, K W Chapman, H Y Playford, M G Tucker, D A Keen, M A Hayward, and A L Goodwin, Orbital Dimer Model for the Spin-Glass State in Y2Mo2O7, Phys Rev Lett 118, 067201 (2017)

Left: In our model of Y2Mo2O7, local displacements of Jahn-Teller active Mo4+ ions (blue arrows) follow a two-in, two-out “ice rule”, and are correlated with oxide displacements (red arrows), generating disorder in magnetic interactions. Right: The frustrated geometry of the pyrochlore Mo lattice suppresses ordering of Mo-Mo orbital dimers (short Mo-Mo bonds).

The formation of a spin glass usually requires both structural disorder and frustrated magnetic interactions. Consequently, the origin of spin-glass behaviour in Y2Mo2O7 − in which magnetic Mo4+ ions occupy a frustrated pyrochlore lattice with minimal compositional disorder − has been a longstanding question. Here, we use neutron and X-ray pair-distribution function (PDF) analysis to develop a disorder model that resolves apparent incompatibilities between previously-reported PDF, EXAFS and NMR studies and provides a new and physical mechanism for spin-glass formation. We show that Mo4+ ions displace according to a local “2-in/2-out” rule on each Mo4 tetrahedron, driven by orbital dimerisation of Jahn-Teller active Mo4+ ions. Long-range orbital order is prevented by the macroscopic degeneracy of dimer coverings permitted by the pyrochlore lattice. Cooperative O2− displacements yield a distribution of Mo−O−Mo angles, which in turn introduces disorder into magnetic interactions. Our study demonstrates experimentally how frustration of atomic displacements can assume the role of compositional disorder in driving a spin-glass transition.

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