Magnetodielectric detection of magnetic quadrupole order in Ba(TiO)Cu${}_4$(PO${}_4$)${}_4$ with Cu${}_4$O${}_{12}$ square cupolas

Abstract

In vortex-like spin arrangements, multiple spins can combine into emergent multipole moments. Such multipole moments have broken space-inversion and time-reversal symmetries, and can therefore exhibit linear magnetoelectric (ME) activity. Three types of such multipole moments are known: toroidal, monopole, and quadrupole moments. So far, however, the ME-activity of these multipole moments has only been established experimentally for the toroidal moment. Here, we propose a magnetic square cupola cluster, in which four corner-sharing square-coordinated metal-ligand fragments form a noncoplanar buckled structure, as a promising structural unit that carries an ME-active multipole moment. We substantiate this idea by observing clear magnetodielectric signals associated with an antiferroic ME-active magnetic quadrupole order in the real material Ba(TiO)Cu${}_4$(PO${}_4$)${}_4$. The present result serves as a useful guide for exploring and designing new ME-active materials based on vortex-like spin arrangements.

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References in corpus (3)

• Spin current and magneto-electric effect in non-collinear magnets
• Role of the Dzyaloshinskii-Moriya interaction in multiferroic perovskites
• Magnetoelectric MnPS3 thiophosphate as a new candidate for ferrotoroidicity

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