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

TL;DR

This study explores how substituting non-magnetic selenium in layered MPX3 compounds allows precise control over magnetic interactions and anisotropy, advancing the development of tunable 2D magnetic materials.

Contribution

It introduces the first systematic investigation of chalcogen substitution in MPX3, demonstrating effective tuning of magnetic properties in MnPS3-xSex and NiPS3-xSex.

Findings

Magnetic interactions are effectively tuned by Se substitution.

Magnetic anisotropy can be controlled through ligand substitution.

Systematic evolution of magnetism with varying Se content was observed.

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.