Successive magnetic transitions and multiferroicity in layered honeycomb BiCrTeO$_{6}$

Abstract

Low-dimensional magnetic systems based on honeycomb lattices provide a promising platform for exploring exotic quantum phenomena that emerge from the intricate interplay of competing spin, orbital, lattice, and dipolar degrees of freedom. Here, we present a comprehensive study of the layered honeycomb lattice antiferromagnet BiCrTeO$_6$ using magnetization, specific heat, muon spin--relaxation ($\mu$SR) spectroscopy, dielectric, pyrocurrent, and high-resolution synchrotron X-ray diffraction (SXRD) measurements. Our results reveal an array of intriguing and strongly correlated phenomena, including two successive antiferromagnetic transitions at $T_{\rm N1}\approx16$ K and $T_{\rm N2}\approx11$ K, a pronounced magnetodielectric coupling effect, and ferroelectric order at $T_{\rm N2}$. Consequently, this compound emerges as a new spin-driven multiferroic system. The SXRD analysis reveals a magnetoelastic-coupling-induced structural phase transition at $T_{\rm N2}$, characterized by a symmetry lowering from P$\bar{3}$1c (163) to P31c (159), which likely triggers the onset of ferroelectricity. In addition to its low-temperature multiferroic behavior, the system exhibits dielectric relaxor characteristics at higher temperatures within the paramagnetic region ($T<50$ K), which is intrinsically linked to the antisite disorder of Cr and Te atoms.