Variation between Antiferromagnetism and Ferrimagnetism in NiPS3 by Electron Doping

Abstract

How to electrically control magnetic properties of a magnetic material is promising towards spintronic applications, where the investigation of carrier doping effects on antiferromagnetic (AFM) materials remains challenging due to their zero net magnetization. In this work, we found electron doping dependent variation of magnetic orders of a two-dimensional (2D) AFM insulator NiPS3, where doping concentration is tuned by intercalating various organic cations into the van der Waals gaps of NiPS3 without introduction of defects and impurity phases. The doped NiPS3 shows an AFM-ferrimagnetic (FIM) transition at doping level of 0.2-0.5 electrons/cell and a FIM-AFM transition at doping level of ≥0.6 electrons/cell. We propose that the found phenomenon is due to competition between Stoner exchange dominated inter-chain ferromagnetic order and super-exchange dominated inter-chain AFM order at different doping level. Our studies provide a viable way to exploit correlation between electronic structures and magnetic properties of 2D magnetic materials for realization of magnetoelectric effect.

Charge compensation in a layered van der Waals NiPS3 host through various cationic intercalations

“…Interestingly, a similar reaction between TBA + and NiPS 3 was performed by Mi et al, demonstrating an interlayer distance of only 11.46 Å. 13 This may be an effect of different amounts of intercalation, leading to the assumption that this is a stepwise process, which is supported by the work of Chen et al 19 They investigated the reaction between FePS 3 and 1,10-phenanthroline aer certain intercalation intervals with ex situ XRD, and also observed different stages resulting from changes in the intercalant orientation. Changes in oxidation This journal is © The Royal Society of Chemistry 2024 states and the local structure upon EMIM intercalation were monitored with operando Ni K-edge XAS, and ex situ P and S Kedge XAS measurements, as shown in Fig.…”

“…S2 in the ESI †), is in agreement with a common observation for intercalation of organic ions into transition metal phosphorus trisul-des. 13,19,21,46 For example, tetrabutylammonium (TBA + ) intercalation into NiPS 3 was demonstrated by Choi et al with an increased c-parameter of 14.5-15.3 Å. 10 The variation is a result of various crystallographic phases with different orientations of the organic molecule between the layers.…”

“…Therefore, as an alternative, intercalation of large cations or organic molecules, leading to detectable changes in the crystal structure, is also of interest for these compounds. For example, insertion of complex ammonium cations with different organic groups such as tetrabutyl ammonium (TBA + ), tetrapropyl ammonium (TPA + ) and cetyltrimethyl ammonium (CTA + ) were demonstrated in NiPS 3 , 13,14 while MnPS 3 is known to be a host for poly(phenylene vinylene) and for pyridine. 15,16 In the family of transition metal phosphorus trisuldes, different aspects of intercalation have been comprehensively studied in NiPS 3 .…”