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Monolayer transition metal dichalcogenides (TMDs) with strong spin-orbitcoupling combined with broken inversion symmetry, leading to a coupling of spinand valley degrees of freedom, make these materials highly interesting forpotential spintronics and valleytronic applications. However, engineering thespin-orbit coupling (SOC) at room temperature as demand after devicefabrication is still a great challenge for their practical applications. Herewe reversibly engineer the spin-orbit coupling of monolayer MoS2 by laserirradiation under controlled gas environments, where the spin-orbit splittinghas been effectively regulated within 120 meV to 200 meV. Furthermore, thephotoluminescence (PL) intensity of B exciton can be invertible manipulationover 2 orders of magnitude. We attribute the engineering of spin-orbitsplitting to the reduction of binding energy combined with bandrenormalization, originating from the enhanced absorption coefficient ofmonolayer MoS2 under inert gases and subsequent the significantly boostedcarrier concentrations. Reflectance contrast spectra during the engineeringstage provide unambiguous proof to support our interpretation. Our approachoffers a new avenue to actively control the SOC strength in TMDs materials atroom temperature and paves the way for designing innovative spintronicsdevices.

Reversible engineering the spin-orbit coupling of monolayer MoS2 via laser irradiation under controlled gas atmospheres