Low-Temperature Synthesis of Magnetic Pyrochlores (R₂Mn₂O₇, R = Y, Ho–Lu) at Ambient Pressure and Potential for High-Entropy Oxide Synthesis

Abstract

Rare-earth manganese pyrochlores (R2Mn2O7) are frustrated magnetic materials, which previously have only been accessed using expensive high-pressure and high-temperature synthesis. In the present work, we demonstrate a convenient synthetic approach to synthesize R2Mn2O7 pyrochlores at ambient pressure. A series of pyrochlores (R = Y, Ho–Lu) were prepared by a simple and cost-effective molten salt method using NaCl and KCl as the flux. Moreover, phase-selectivity was demonstrated for yttrium manganese oxides (YMnO3 and Y2Mn2O7) by a simple variation of synthesis temperature and precursors-to-chlorides ratio. The synthetic procedure does not require high pressures or temperatures nor oxygen flow. All synthesized pyrochlores demonstrated ferromagnetic behavior at low temperature, and the magnetic properties were in good agreement with those of high-pressure-synthesized materials. The versatility of the method was confirmed by the preparation of a mixed-rare earth Y0.4Er0.4Tm0.4Yb0.4Lu0.4Mn2O7 solid solutiona compositionally complex high-entropy oxide.

Tuneable Short-Range Antiferromagnetic Correlation in Fe-Containing Entropy Stabilized Oxides

“…Although complex magnetic behaviors have been reported in HEOs , such as perovskites, pyrochlores, spinels, zirconates, and Ruddlesden–Popper oxides, so far, only some of them were able to offer magnetic details, such as long-range magnetic order or magnetic phase competition, for example. For a rock salt-type (Co, Cu, Mg, Ni, and Zn)O structure, an antiferromagnetic (AFM) order has been predicted from modeling experiments, which could be confirmed by magnetic susceptibility as well as neutron diffraction below a critical temperature of ∼120 K. , Moreover, the short-range spin ordering in its glassy magnetization state can be tuned by ∼65% by changing the Cu amount from 11 to 27% .…”