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Abstract Realization of large effective phonon magnetic moment in monolayer MoS2has 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 MoS2. 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 4dand Fe 3dstates emerges, producing an orbital-phonon hybridized mode at 283 cm−1. Our magnetic field dependent measurements demonstrate that this new mode carries 2.8 effective phonon magnetic moment, which is comparable to that of the undoped MoS2. Moreover, even though a long-range magnetic order is absent in Fe-doped MoS2, 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.
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Dilute Magnetic Impurity-Induced Effective Phonon Magnetic Moment in Fe-doped Monolayer MoS$_2$
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 $$\mu_B$$ 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.
more »
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- PAR ID:
- 10646149
- Publisher / Repository:
- Zenodo
- Date Published:
- Subject(s) / Keyword(s):
- circularly polarized phonon Fe-doped MoS2 helicity-resolved magneto-Raman spectroscopy dilute magnetic semiconductor orbital-phonon coupling
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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