Magnetodielectric detection of magnetic quadrupole order in Ba(TiO)Cu4(PO4)4 with Cu4O12 square cupolas

K. Kimura (), P. Babkevich, M. Sera, M. Toyoda, K. Yamauchi, G. S. Tucker, J. Martius, T. Fennell, P. Manuel, D. D. Khalyavin, R. D. Johnson, T. Nakano, Y. Nozue, H. M. Rønnow and T. Kimura
Additional contact information
K. Kimura: Graduate School of Engineering Science, Osaka University
P. Babkevich: Laboratory for Quantum Magnetism, Institute of Physics, École Polytechnique Fédérale de Lausanne (EPFL)
M. Sera: Graduate School of Engineering Science, Osaka University
M. Toyoda: Tokyo Institute of Technology
K. Yamauchi: ISIR-SANKEN, Osaka University
G. S. Tucker: Laboratory for Quantum Magnetism, Institute of Physics, École Polytechnique Fédérale de Lausanne (EPFL)
J. Martius: Laboratory for Quantum Magnetism, Institute of Physics, École Polytechnique Fédérale de Lausanne (EPFL)
T. Fennell: Laboratory for Neutron Scattering and Imaging, Paul Scherrer Institut
P. Manuel: ISIS facility, STFC Rutherford Appleton Laboratory, Chilton
D. D. Khalyavin: ISIS facility, STFC Rutherford Appleton Laboratory, Chilton
R. D. Johnson: ISIS facility, STFC Rutherford Appleton Laboratory, Chilton
T. Nakano: Graduate School of Science, Osaka University
Y. Nozue: Graduate School of Science, Osaka University
H. M. Rønnow: Laboratory for Quantum Magnetism, Institute of Physics, École Polytechnique Fédérale de Lausanne (EPFL)
T. Kimura: Graduate School of Engineering Science, Osaka University

Nature Communications, 2016, vol. 7, issue 1, 1-7

Abstract: 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)Cu4(PO4)4. The present result serves as a useful guide for exploring and designing new ME-active materials based on vortex-like spin arrangements.

Date: 2016
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DOI: 10.1038/ncomms13039

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