Magnetic dopant-induced effective phonon magnetic moment in Fe-doped monolayer MoS₂

Monolayer MoS₂ offers a platform to explore magnetism in nonmagnetic materials through strong coupling between circularly polarized phonons and electronic orbital transitions. Using magneto-Raman spectroscopy, we show that Fe substitution at Mo sites induces spin polarization in the conduction bands and creates a localized Fe-induced electronic band beneath the conduction band. This leads to a new orbital transition between Mo 4d and Fe 3d states, forming an orbital–phonon hybridized mode at 283 cm⁻¹. Under magnetic field, this new mode exhibits Zeeman splitting corresponding to an effective phonon magnetic moment of 2.8 μ_B. Meanwhile, the original orbital-phonon hybridized mode from pristine monolayer MoS₂ at 265 cm⁻¹ is still present in Fe-doped MoS₂. Our results demonstrate that dilute magnetic impurities serve as a feasible approach of creating and manipulating phonon-induced magnetic properties in 2D TMDCs.