$A$-cation control of magnetoelectric quadrupole order in $A$(TiO)Cu${}_4$(PO${}_4$)${}_4$ ($A$ = Ba, Sr, and Pb)

Abstract

Ferroic magnetic quadrupole order exhibiting macroscopic magnetoelectric activity is discovered in the novel compound $A$(TiO)Cu${}_4$(PO${}_4$)${}_4$ with $A$ = Pb, which is in contrast with antiferroic quadrupole order observed in the isostructural compounds with $A$ = Ba and Sr. Unlike the famous lone-pair stereochemical activity which often triggers ferroelectricity as in PbTiO${}_3$, the Pb${}^{2+}$ cation in Pb(TiO)Cu${}_4$(PO${}_4$)${}_4$ is stereochemically inactive but dramatically alters specific magnetic interactions and consequently switches the quadrupole order from antiferroic to ferroic. Our first-principles calculations uncover a positive correlation between the degree of $A$-O bond covalency and a stability of the ferroic quadrupole order.

arXiv comment7 pages, 4 figures

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Cited by in corpus (11)

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• Symmetry analysis with spin crystallographic groups: Disentangling effects free of spin-orbit coupling in emergent electromagnetism
• Frustration of square cupola in Sr(TiO)Cu${}_4$(PO${}_4$)${}_4$
• Capacitive detection of magnetostriction, dielectric constant, and magneto-caloric effects in pulsed magnetic fields
• Magnetoelectric behavior from cluster multipoles in square cupolas: Study of Sr(TiO)Cu${}_4$(PO${}_4$)${}_4$ in comparison with Ba and Pb isostructurals
• Magnetic Structural Unit with Convex Geometry: a Building Block Hosting an Exchange-striction-driven Magnetoelectric Coupling
• Magnetic structure in square cupola compound Ba(TiO)Cu${}_4$(PO${}_4$)${}_4$: a ${}^{31}$P NMR Study
• The spin-1/2 coupled tetramer system Ba(TiO)Cu${}_4$(PO${}_4$)${}_4$ probed by magnetization, specific heat, and ${}^{31}$P-NMR
• High-field phase diagram of the chiral-lattice antiferromagnet Sr(TiO)Cu4(PO4)4
• Spin dynamics in the square-lattice cupola system Ba(TiO)Cu${}_4$(PO${}_4$)${}_4$
• Microscopic Magnetism of A(TiO)Cu4(PO4)4 (A = Ba, Pb, Sr): 31P and 63,65Cu NMR Study