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

Journal Article · · 2D Materials
 [1];  [2];  [2];  [3];  [1];  [4];  [2];  [5];  [5];  [5];  [4];  [3];  [1];  [6];  [1]
  1. Auburn University, AL (United States)
  2. Texas Tech University, Lubbock, TX (United States)
  3. Stevens Institute of Technology, Hoboken, NJ (United States)
  4. Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  5. University of Northern Iowa, Cedar Falls, IA (United States)
  6. Texas Tech Univ., Lubbock, TX (United States)
Realization of large effective phonon magnetic moment in monolayer MoS2 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 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 4d and Fe 3d 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 $$\mu_{\mathrm{B}}$$ 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.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
SC0012704
OSTI ID:
2997750
Report Number(s):
BNL--229030-2025-JAAM
Journal Information:
2D Materials, Journal Name: 2D Materials Journal Issue: 4 Vol. 12; ISSN 2053-1583
Publisher:
IOP PublishingCopyright Statement
Country of Publication:
United States
Language:
English

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