Synthesis of Group VIII Magnetic Transition-Metal-Doped Monolayer MoSe₂

Abstract

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.

Liquid Phase Edge Epitaxy of Transition-Metal Dichalcogenide Monolayers

“…Other magnetic element doped monolayers have been obtained and some with significant M−H loops at low temperatures, such as Fe/MoSe 2 (Figure S25). 43,44 ■ CONCLUSIONS Overall, we have developed an edge-contact LPEE for the growth of high-quality monolayers, monolayer alloys, and magnetic-element doped monolayers of transition-metal dichalcogenides. In situ optical imaging directly supports the edge epitaxy mechanism.…”

“…Other magnetic element doped monolayers have been obtained and some with significant M – H loops at low temperatures, such as Fe/MoSe 2 (Figure S25). , …”

Defect engineering of two-dimensional materials for advanced energy conversion and storage

“…96,97 Recently, great scientific attention has been focused on the heteroatom doping of monolayer TMDs for property optimization, such as the doping with transition metals ( e.g. , Fe, 98 Co, 99 Ni, 100 and Re 101 ) or non-metal elements ( e.g. , N, 102 O, 103 and P 104 ).…”

“…67,94,95 Owing to their different electronegativity and atomic sizes compared to a carbon atom, the geometrical configuration and electronic structure of graphene are redistributed upon the heteroatom doping, thereby improving the electrochemical performances. 96,97 Recently, great scientific attention has been focused on the heteroatom doping of monolayer TMDs for property optimization, such as the doping with transition metals (e.g., Fe, 98 Co, 99 Ni, 100 and Re 101 ) or non-metal elements (e.g., N, 102 O, 103 and P 104 ). For example, Li et al prepared Co-doped 1T-MoS 2 monolayers with a remarkably distorted structure in which Co-S bonds formed on the basal plane.…”

Liquid-precursor-intermediated synthesis of atomically thin transition metal dichalcogenides

“…Except for V atoms, other magnetic atoms such as Fe, Co, and Ni can also dope the 2D TMDs and modulate the ferromagnetic properties of the materials. 87…”