Magnetic Structural Unit with Convex Geometry: a Building Block Hosting an Exchange-striction-driven Magnetoelectric Coupling

Abstract

We perform a combined experimental and theoretical study of a magnetic-field ($B$) induced evolution of magnetic and ferroelectric properties in an antiferromagnetic material Pb(TiO)Cu${}_4$(PO${}_4$)${}_4$, whose structure is characterized by a staggered array of Cu${}_4$O${}_{12}$ magnetic units with convex geometry known as square cupola. Our experiments show a $B$-induced phase transition from a previously reported low-$B$ linear magnetoelectric phase to a new high-$B$ magnetoelectric phase, which accompanies a 90${}^{\circ }$ flop of electric polarization and gigantic magnetodielectric effect. Moreover, we observe a $B$-induced sign reversal of ferroelectric polarization in the high-$B$ phase. Our model and first-principles calculations reveal that the observed complex magnetoelectric behavior is well explained in terms of a $B$-dependent electric polarization generated in each Cu${}_4$O${}_{12}$ unit by the so-called exchange striction mechanism. The present study demonstrates that the materials design based on the magnetic structural unit with convex geometry deserves to be explored for developing strong magnetoelectric couplings.

arXiv comment13 pages, 9 figures

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Cited by in corpus (6)

• 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 structure in square cupola compound Ba(TiO)Cu${}_4$(PO${}_4$)${}_4$: a ${}^{31}$P NMR Study
• Spin-1/2 $XXZ$ Heisenberg cupolae: magnetization process and related enhanced magnetocaloric effect
• Optical Hall response in spin-orbit coupled metals: Comparative study of magnetic cluster monopole, quadrupole, and toroidal orders
• High-field phase diagram of the chiral-lattice antiferromagnet Sr(TiO)Cu4(PO4)4