Pressure-induced polymorphism and piezochromism in Mn2FeSbO6

Abstract

In the last decade, major efforts have been devoted to searching for polar magnets due to their vast potential applications in spintronic devices. However, the polar magnets are rare because of conflicting electronic configuration requirements of ferromagnetism and electric polarization. Double-perovskite oxides with a polar structure containing transition metal elements represent excellent candidates for the polar magnet design. Herein, the crystal structure evolution of Mn2FeSbO6 (MFSO) was investigated at pressures reaching ∼50 GPa by in situ synchrotron X-ray diffraction (XRD), Raman scattering, and ab initio calculation techniques. The XRD results reveal ilmenite- to perovskite-type phase transition at around 35 GPa. An additional intermediate phase, observed in the range of 31–36 GPa by Raman spectroscopy, but not the XRD technique, is proposed to represent the polar LiNbO3 phase. It is argued that this phase emerged due to the heating effect of the Raman-excitation laser. The LiNbO3-type MFSO compounds, displaying an intrinsic dipole ordering, represent a promising candidate for multiferroic materials. The detected phase transitions were found to be reversible although a significant hysteresis was noticeable between compression and decompression runs. Moreover, a pressure-induced piezochromism, signifying a bandgap change, was discovered by the direct visual observations and corroborated by ab initio calculations. The present study benefits an efficient high-pressure synthesis of polar magnetic double-perovskite oxides in the future.