Abstract

We report an optimized chemical vapor transport method to grow single crystals of (Mn1−xNix)2P2S6 where x = 0, 0.3, 0.5, 0.7, and 1. Single crystals up to 4 mm × 3 mm × 200 μm were obtained by this method. As-grown crystals are characterized by means of scanning electron microscopy and powder X-ray diffraction measurements. The structural characterization shows that all crystals crystallize in monoclinic symmetry with the space group C2/m (No. 12). We have further investigated the magnetic properties of this series of single crystals. The magnetic measurements of the all as-grown single crystals show long-range antiferromagnetic order along all principal crystallographic axes. Overall, the Néel temperature TN is non-monotonous; with increasing Ni2+ doping, the temperature of the antiferromagnetic phase transition first decreases from 80 K for pristine Mn2P2S6 (x = 0) up to x = 0.5 and then increases again to 155 K for pure Ni2P2S6 (x = 1). The magnetic anisotropy switches from out-of-plane to in-plane as a function of composition in (Mn1−xNix)2P2S6 series. Transport studies under hydrostatic pressure on the parent compound Mn2P2S6 evidence an insulator-metal transition at an applied critical pressure of ~22 GPa.

Highlights

  • In recent years, research of functional two-dimensional (2D) materials has stimulated activities aimed at the synthesis of new materials and studies of their functionalities.This class has drawn a great deal of interest and attention because of its unique electronic [1,2,3], magnetic [4,5,6,7,8], and optical properties [9,10,11,12] to the bulk counterpart.Layered van der Waals materials dominate among the current 2D materials

  • The transition metal phosphorus trichalcogenides (TM2 P2 Ch6 TM = transition metal; Ch = chalcogen) family belongs to the layered van der Waals materials class [22]

  • An X-ray diffraction (XRD) pattern of a polycrystalline sample was obtained by grinding as-grown single crystals

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Summary

Introduction

Research of functional two-dimensional (2D) materials has stimulated activities aimed at the synthesis of new materials and studies of their functionalities. The transition metal phosphorus trichalcogenides (TM2 P2 Ch6 TM = transition metal; Ch = chalcogen) family belongs to the layered van der Waals materials class [22] All of these materials have very similar crystal structures, a monoclinic unit cell with the space group of C2/m but different magnetic properties depending on the underlying 3d transition metal [23]. The main difference between these two pristine compounds and the key ingredient in the TM2 P2 Ch6 family is the underlying anisotropy that dictates the long-range magnetic order down to the monolayer, which eventually depends on the 3d transition metal ions [33,34,35,36] This anisotropy of the system can be tuned systematically by several methods, for example, with chemical substitution or with applied pressure.

Experimental Methods and Crystal Growth
Characterization
Interlayer spacing d calculated function of of Ni
Magnetic Properties
Magnetization and Transport
Evolution of TNofand
Transport Properties
Conclusions
P2 S6optimized
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