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The recent epitaxial growth of 1T-phase of PtSe2 monolayer (ML) has opened apossibility for its novel applications, in particular for spintronics device.However, in contrast to 2H-phase of transition-metal dichalcogenides (TMDs),the absence of spin splitting in the PtSe2 ML may limit the functionality forspintronics application. Through fully-relativistic density-functional theorycalculations, we show that large spin splitting can be induced in the PtSe2 MLby introducing a substitutional halogen impurity. Depending on the atomicnumber (Z) of the halogen dopants, we observe an enhancement of the spinsplitting in the localized impurity states (LIS), which is due to the increasedcontribution of the p-d orbitals coupling. More importantly, we identify verylarge Rashba splitting in the LIS near Fermi level around the Gamma pointcharacterized by hexagonal warping of the Fermi surface. We show that theRashba splitting can be controlled by adjusting the doping concentration.Therefore, this work paves a possible way to induce the significant Rashbasplitting in the two-dimensional TMDs, which is useful for spintronic devicesoperating at room temperature.

Strong Rashba effect in the localized impurity states of halogen-doped monolayer PtSe2