Controlling magnetic exchange and anisotropy by non-magnetic ligand substitution in layered MPX3 (M = Ni, Mn; X = S, Se)

Abstract

Recent discoveries in two-dimensional (2D) magnetism have intensified the investigation of van der Waals (vdW) magnetic materials and further improved our ability to tune their magnetic properties. Tunable magnetism has been widely studied in antiferromagnetic metal thiophosphates MPX3. Substitution of metal ions M has been adopted as an important technique to engineer the magnetism in MPX3. In this work, we have studied the previously unexplored chalcogen X substitutions in MPX3 (M = Mn/Ni; X = S/Se). We synthesized the single crystals of MnPS3-xSex (0 < x < 3) and NiPS3-xSex (0 < x < 1.3) and investigated the systematic evolution of the magnetism with varying x. Our study reveals the effective tuning of magnetic interactions and anisotropies in both MnPS3 and NiPS3 upon Se substitution. Such efficient engineering of the magnetism provides a suitable platform to understand the low-dimensional magnetism and develop future magnetic devices.

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• Magnetic Anisotropy in Two-dimensional van der Waals Magnetic Materials and Their Heterostructures: Importance, Mechanisms, and Opportunities
• Giant spin Nernst effect in a two-dimensional antiferromagnet due to magnetoelastic coupling-induced gaps and interband transitions between magnon-like bands
• Understanding and tuning magnetism in layered Ising-type antiferromagnet FePSe3 for potential 2D magnet
• Identifying band structure changes of FePS3 across the antiferromagnetic phase transition
• Correlation-driven topological transition in Janus VSiGeP2As2
• Giant Magneto-Optical Schäfer-Hubert Effect in Two-Dimensional van der Waals Antiferromagnets \textit{M}PS${}_3$ (\textit{M}=Mn, Fe, Ni)
• Field-induced spin polarization in lightly Cr-substituted layered antiferromagnet NiPS3
• Spin model for the Honeycomb $\mathrm{NiP}{\mathrm{S}}_3$
• Higher-order Topological States in Chiral Split Magnons of Honeycomb Altermagnets
• Deconstruction of the anisotropic magnetic interactions from spin-entangled optical excitations in van der Waals antiferromagnets
• Topological phase diagram of Pb1-xSnxSe1-yTey
• Quantum Fluctuations in the van der Walls material $\mathrm{NiP}{\mathrm{S}}_3$
• Chalcogen Doping Effect on the Insulator-to-Metal Transition in GdPS
• Thermally-induced mimicry of quantum cluster excitations and implications for the magnetic transition in FePSe${}_3$
• Probing the band structure of the strongly correlated antiferromagnet NiPS3 across its phase transition
• AMaRaNTA: Automated First-Principles Exchange Parameters In 2D Magnets
• Strain Modulated Electronic and Optical Properties of Laterally Stitched MoSi2N4/XSi2N4 (X=W, Ti) 2D Heterostructures