Ab-Initio Study of Magnetically Intercalated Platinum Diselenide: The Impact of Platinum Vacancies

We study the magnetic properties of platinum diselenide (PtSe(2)) intercalated with Ti, V, Cr, and Mn, using first-principle density functional theory (DFT) calculations and Monte Carlo (MC) simulations. First, we present the equilibrium position of intercalants in [Formula: see text] obtained from the DFT calculations. Next, we present the magnetic groundstates for each of the intercalants in [Formula: see text] along with their critical temperature. We show that Ti intercalants result in an in-plane AFM and out-of-plane FM groundstate, whereas Mn intercalant results in in-plane FM and out-of-plane AFM. V intercalants result in an FM groundstate both in the in-plane and the out-of-plane direction, whereas Cr results in an AFM groundstate both in the in-plane and the out-of-plane direction. We find a critical temperature of <0.01 K, 111 K, 133 K, and 68 K for Ti, V, Cr, and Mn intercalants at a 7.5% intercalation, respectively. In the presence of Pt vacancies, we obtain critical temperatures of 63 K, 32 K, 221 K, and 45 K for Ti, V, Cr, and Mn-intercalated [Formula: see text] , respectively. We show that Pt vacancies can change the magnetic groundstate as well as the critical temperature of intercalated [Formula: see text] , suggesting that the magnetic groundstate in intercalated [Formula: see text] can be controlled via defect engineering.