Pressure-Stabilized MnSb2 with Complex Incommensurate Magnetic Order

Marcasite-type compounds have been proposed as promising hosts of exotic magnetic quantum states, yet experimental realizations in stoichiometric, disorder-free systems remain limited. Here, we report the high-pressure stabilization and magnetic characterization of MnSb ₂ , a marcasite-type compound that is thermodynamically metastable under ambient pressure. Single crystals were synthesized using a cubic multi-anvil press, and powder and single-crystal X-ray diffraction confirm the orthorhombic Pnnm structure. These crystals are stable at ambient pressure for a long time up to between 450–500 K. Heat-capacity measurements reveal phase transitions at approximately 220 K and 118 K. Neutron diffraction uncovers an unconventional magnetic ground state below 220 K. Magnetic powder neutron diffraction refinements reveal possible multiple magnetic configurations that provide comparably acceptable fits to the experimental data. While most solutions are consistent with a spin-density-wave (SDW) description, helical models systematically yield inferior agreement factors. Across a broad range of models, the Mn ordered moment reaches a maximum value of approximately 2 µ _B and remains predominantly collinear, with minimal canting along the c -axis. At 200 K, the magnetic propagation vector is q = (0, 0.3975, 0.3783); upon cooling, the b component increases toward 0.5, reflecting a temperature-dependent evolution of the modulation. The need for modification of the magnetic model between high and low temperatures further highlights the complex and strongly temperature-dependent nature of the magnetic order in this system. These results establish MnSb ₂ as a pressure-stabilized marcasite magnet with a highly tunable, complex magnetic ground state and a compelling stoichiometric platform for exploring unconventional magnetic behavior, including potential altermagnetism.