Electronic Correlations in Fe x Ni y PS 3 Van der Waals Materials: Insights from Angle-Resolved Photoelectron Spectroscopy and DFT.

Recently layered antiferromagnetic materials with different magnetic orderings attract increased attention. It was found that these properties can be preserved down to the monolayer limit opening large perspectives for their applications in (opto)spintronics and sensing, however, lacking the experimental results on electronic structure studies. Here the results of angle-resolved photoelectron spectroscopy (ARPES) studies accompanied by DFT calculations for FeNiPS layered van der Waals (vdW) alloys are presented, addressing the effects of electronic correlations in these materials. It is demonstrated that in the case of FePS the top of the valence band is formed by the hybrid Fe 3d-S 3p states and is of pure S 3p character for NiPS, respectively, whereas for the mixed Fe-Ni-based vdW alloy the electronic structure is a sum of contributions from the parent compounds. The obtained results give a clear understanding of the nature of the insulating state in studied MPX materials and pave the way on their applications in different areas.