Dilute magnetic impurity-induced effective phonon magnetic moment in Fe-doped monolayer MoS₂

Abstract Realization of large effective phonon magnetic moment in monolayer MoS 2 has established an important route for exploring intriguing magnetic phenomena in a nonmagnetic material. The sizable coupling between the orbital transition and the circularly polarized phonon results in the large effective phonon magnetic moment. In this work, using magneto-Raman spectroscopy, we investigate substitutional doping of magnetic atoms as a tuning knob of the electronic and phononic properties of MoS 2 . We show that Fe-doping polarizes the spin of the conduction bands and introduces a localized Fe band underneath the conduction band. As a result, an additional orbital transition between the Mo 4 d and Fe 3 d states emerges, producing an orbital-phonon hybridized mode at 283 cm −1 . Our magnetic field dependent measurements demonstrate that this new mode carries 2.8 <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" overflow="scroll"> <mml:mrow> <mml:msub> <mml:mi>μ</mml:mi> <mml:mrow> <mml:mrow> <mml:mi mathvariant="normal">B</mml:mi> </mml:mrow> </mml:mrow> </mml:msub> </mml:mrow> </mml:math> effective phonon magnetic moment, which is comparable to that of the undoped MoS 2 . Moreover, even though a long-range magnetic order is absent in Fe-doped MoS 2 , the local magnetic moment of Fe modifies the nature of the spin fluctuation, producing monotonically increasing quasielastic scattering spectral weight as temperature decreases. Our results highlight two-dimensional dilute magnetic semiconductors synthesized by substitutional doping as a promising material platform to manipulate the phonon magnetic moment through orbital-phonon coupling.