A systematic study of TMOn (TM = V, Cr, Mn, and Fe; n = 3 and 6) clusters embedded in PtS2 monolayer

Doping-based magnetism engineering is an effective approach to make new multifunctional two-dimensional (2D) materials from the non-magnetic counterparts. In this work, doping with TMOn clusters (TM = V, Cr, Mn, and Fe; n = 3 and 6) is proposed to induce feature-rich electronic and magnetic properties in PtS2 monolayer. Pristine monolayer is a non-magnetic semiconductor with indirect energy gap of 1.81(2.67) eV as obtained from PBE(HSE06)-based calculations. PtS3-type multivacancies magnetize significantly the monolayer, induce the emergence of the half-metallicity. In this case, a total magnetic moment of 1.90 µB is obtained and magnetic properties are produced mainly by atoms around the vacancy sites. Meanwhile, PtS2 monolayer is metallized by creating PtS6-type multivacancies without magnetization. Depending on the type of TMOn cluster, feature-rich either diluted magnetic semiconductor or half-metallic natures are induced, which are regulated mainly by the incorporated clusters. Except for FeO6 cluster, TM atom and O atoms exhibit the antiparallel spin orientation, such that total magnetic moments between 1.00 and 4.00 µB are obtained. Meanwhile, the parallel spin ordering gives a large total magnetic moment of 5.99 µB for FeO6-doped monolayer. Furthermore, the Bader charge analysis indicates that all the clusters attract charge from the host monolayer that is mainly due to the electronegative O atoms. Our results may introduce the cluster doping as an efficient way to create new spintronic 2D materials from a non-magnetic PtS2 monolayer.