Abstract
Octahedral distortion in ABO3 perovskite materials is ubiquitous because of the ionic size mismatch between A and B cations, leading to various kinds of crystal symmetry. However, such a distortion always results in centrosymmetric structures except for the covalent bond formation because of the second-order Jahn–Teller (SOJT) effect that occurs with d0 or lone-pair cations. Here, we report that an unusual combination of the layered A-site cation ordering and B-site rock salt ordering in NaYNiWO6 prepared under high-pressure and high-temperature conditions results not only in a polar (P21) structure, as revealed by the neutron diffraction analysis, but exhibits multiferroic properties below the magnetic ordering of Ni2+ ions (TN = 21 K). Analysis of the neutron diffraction data at 20 K reveals an incommensurate sinusoidal spin ordering with the propagation vector, ki = (0.471(2), 0, 0.491(4)), and a commensurate collinear spin structure with kc = (0.5, 0, 0.5) below 18 K. X-ray diffraction data confirm the polar structure in Dy, Ho, and Yb compounds. All four compounds exhibit a switchable change in electric polarization (ΔP) at the magnetic ordering temperatures, demonstrating coupling between ferroelectricity and magnetism.
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