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Abstract

Transition metal dichalcogenide (TMD) monolayers offer an innovative platform for encoding and manipulating information through the valley degree of freedom. While unique valley-related physical phenomena have been reported so far, practical applications still require advanced control over the valley polarization efficiency and the valley Zeeman effect. Recently, the introduction of spin-polarized metal atoms as substitutional defects was reported to break the time-reversal symmetry in TMD monolayers, consequently inducing a room-temperature ferromagnetic ordering and enhancing the valley-dependent optical responses. Here, we report valley asymmetries for vanadium-doped WS$_2$ monolayers. With a given magnetic polarization, one valley exhibits larger Zeeman slope and degree of circular polarization than the other valley. Additionally, the overall degree of circular polarization in the doped samples is approximately twice that of the pristine WS$_2$ monolayer. Density functional theory calculations in the doped structure show that different energy shifts in conduction band edges due to spin-dependent hybridization lead to different exciton energies between valleys, which is consistent with the experimental observations. Our results pave the way for valleytronic technologies based on defect-engineered two-dimensional materials.

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