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Here we report crystallographic and magnetic studies on high quality samplesof the magnetically frustrated S = 1/2 kagome antiferromagnet vesignieite,BaCu3V2O8(OD)2. Powder neutron diffraction data collected from samples obtainedby a new hydrothermal synthetic route reveal a previously unobserved trigonalP3121 structure, similar to the isoelectronic mineral SrCu3V2O8(OH)2. Therefined structure is consistent with orbital frustration of the eg d-orbitalsin a sublattice of the Cu2+ kagome network due to a dynamic Jahn-Teller effect,which persists below the magnetic transition at TN = 9K and makes the materialan interesting candidate for exploring concomitant spin and orbitalfrustration. A combination of crystallographic strain analysis andmagnetisation measurements indicate strong magnetostructural coupling which mayexplain the varied magnetic behaviour between samples of vesignieite in theliterature. The revised orbital structure is similar to that found involborthite, rather than the quantum spin liquid herbertsmithite, and providesa convincing argument for the differing magnetic properties found in thesefrustrated magnets.

Orbital frustration in the S = 1/2 kagome magnet vesignieite, BaCu3V2O8(OD)2