The
limitation on the spintronic applications of van der Waals
layered transition-metal dichalcogenide semiconductors is ascribed
to the intrinsic nonmagnetic feature. Recent studies have proved that
substitutional doping is an effective route to alter the magnetic
properties of two-dimensional transition-metal dichalcogenides (TMDs).
However, highly valid and repeatable substitutional doping of TMDs
remains to be developed. Herein, we report group VIII magnetic transition
metal-doped molybdenum diselenide (MoSe2) single crystals via a one-pot mixed-salt-intermediated chemical vapor deposition
method with high controllability and reproducibility. The high-angle
annular dark-field scanning transmission electron microscopy studies
further confirm that the sites of Fe are indeed substitutionally incorporated
into the MoSe2 monolayer. The Fe-doped MoSe2 monolayer with a concentration from 0.93% to 6.10% could be obtained
by controlling the ratios of FeCl3/Na2MoO4. Moreover, this strategy can be extended to create Co(Ni)-doped
MoSe2 monolayers. The magnetic hysteresis (M–H) measurements demonstrate that group VIII magnetic transition-metal-doped
MoSe2 samples exhibit room-temperature ferromagnetism.
Additionally, the Fe-doped MoSe2 field effect transistor
shows n-type semiconductor characteristics, indicating the obtainment
of a room-temperature dilute magnetic semiconductor. Our approach
is universal in magnetic transition-metal substitutional doping of
TMDs, and it inspires further research interest in the study of related
spintronic and magnetoelectric applications.