Abstract

The multiferroic nature of the honeycomb-lattice $\mathrm{M}{\mathrm{n}}_{2}{\mathrm{V}}_{2}{\mathrm{O}}_{7}$ was investigated through detailed temperature, high-pressure, and magnetic-field-dependent measurements. A first-order martensiticlike structural phase transition with the thermal hysteresis associated with magnetic, heat-capacity, and dielectric anomalies was observed between ${T}_{Mh}$ (303 K) and ${T}_{Mc}$ (291 K). External pressure up to 15.41 kbar suppresses the thermal hysteresis in the magnetization data, indicating that the high-temperature \ensuremath{\beta}-phase persists down to the lower temperature under 15.41 kbar. Furthermore, isothermal capacitance-stress hysteresis loops along with crystallographic Aizu notation of $2/mF\overline{1}$ supports a martensitic phase transition driving ferroelastic ordering near or below room temperature. At low temperature, a long-range antiferromagnetic ordering was observed at ${T}_{N}\ensuremath{\sim}17\phantom{\rule{0.16em}{0ex}}\mathrm{K}$. With increasing the external pressure up to 15.41 kbar, 100% enhancement of ${T}_{N}$ was observed and a metamagnetic transition at 5 K was enhanced near 3 T. High-field magnetization study up to 60 T induces multiple metamagnetic transitions below ${T}_{N}$. Below ${T}_{N}$, a magnetostriction induced magnetoelectric coupling was observed and further supported by the temperature-dependent x-ray studies. Taking these comprehensive research findings into account, we established that $\mathrm{M}{\mathrm{n}}_{2}{\mathrm{V}}_{2}{\mathrm{O}}_{7}$ is a unique multifunctional material with the coexistence of ferroelastic and antiferromagnetic orderings and with weak magnetoelectric coupling.

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