Controlling magnetic exchange and anisotropy by nonmagnetic ligand substitution in layered <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:mi>M</mml:mi><mml:mi mathvariant="normal">P</mml:mi><mml:msub><mml:mi>X</mml:mi><mml:mn>3</mml:mn></mml:msub></mml:mrow></mml:math> (<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:mi>M</mml:mi><mml:mo>=</mml:mo><mml:mi>Ni</mml:mi></mml:mrow></mml:math>, Mn; <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:mi>X</mml:mi><mml:mo>=</mml:mo><mml:mi mathvariant="normal">S</mml:mi></mml:mrow></mml:math>, Se)
Rabindra Basnet, Kamila M. Kotur, Miłosz Rybak, Cory Stephenson, S.M. Bishop, Carmine Autieri, Magdalena Birowska, Jin Hu
Abstract
Recent discoveries in two-dimensional magnetism have intensified the investigation of van der Waals magnetic materials and further improved our ability to tune their magnetic properties. Tunable magnetism has been widely studied in antiferromagnetic metal thiophosphates $M\mathrm{P}{X}_{3}$. Substitution of metal ions $M$ has been adopted as an important technique to engineer the magnetism in $M\mathrm{P}{X}_{3}$. In this work, we have studied the previously unexplored chalcogen $X$ substitutions in $M\mathrm{P}{X}_{3}$ ($M=\mathrm{Mn}$/Ni; $X=\mathrm{S}$/Se). We synthesized the single crystals of $\mathrm{MnP}{\mathrm{S}}_{3\ensuremath{-}x}{\mathrm{Se}}_{x}$ $(0\ensuremath{\le}x\ensuremath{\le}3)$ and $\mathrm{NiP}{\mathrm{S}}_{3\ensuremath{-}x}{\mathrm{Se}}_{x}$ $(0\ensuremath{\le}x\ensuremath{\le}1.3)$ and investigated the systematic evolution of the magnetism with varying $x$. Our study reveals the effective tuning of magnetic interactions and anisotropies in both ${\mathrm{MnPS}}_{3}$ and ${\mathrm{NiPS}}_{3}$ upon Se substitution. Such efficient engineering of the magnetism provides a suitable platform to understand the low-dimensional magnetism and develop future magnetic devices.