Journal
ADVANCED SCIENCE
Volume 7, Issue 24, Pages -Publisher
WILEY
DOI: 10.1002/advs.202001174
Keywords
2D ferromagnets; dilute magnetic semiconductors; room-temperature ferromagnetism; tungsten disulfide; vanadium doping
Categories
Funding
- Air Force Office of Scientific Research (AFOSR) [FA9550-18-1-0072]
- NSF-IUCRC Center for Atomically Thin Multifunctional Coatings (ATOMIC)
- Two-Dimensional Crystal Consortium (2DCC-MIP), a National Science Foundation Materials Innovation Platform [DMR-1539916]
- U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-FG02-07ER46438]
- VISCOSTONE USA [1253113200]
- NSF [DMR EPM 2006231]
- NSF I/UCRC on Multi-functional Integrated System Technology (MIST) Center [IIP-1439644, IIP-1439680, IIP-1738752, IIP-1939009, IIP-1939050, IIP-1939012]
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Dilute magnetic semiconductors (DMS), achieved through substitutional doping of spin-polarized transition metals into semiconducting systems, enable experimental modulation of spin dynamics in ways that hold great promise for novel magneto-electric or magneto-optical devices, especially for two-dimensional (2D) systems such as transition metal dichalcogenides that accentuate interactions and activate valley degrees of freedom. Practical applications of 2D magnetism will likely require room-temperature operation, air stability, and (for magnetic semiconductors) the ability to achieve optimal doping levels without dopant aggregation. Here, room-temperature ferromagnetic order obtained in semiconducting vanadium-doped tungsten disulfide monolayers produced by a reliable single-step film sulfidation method across an exceptionally wide range of vanadium concentrations, up to 12 at% with minimal dopant aggregation, is described. These monolayers develop p-type transport as a function of vanadium incorporation and rapidly reach ambipolarity. Ferromagnetism peaks at an intermediate vanadium concentration of similar to 2 at% and decreases for higher concentrations, which is consistent with quenching due to orbital hybridization at closer vanadium-vanadium spacings, as supported by transmission electron microscopy, magnetometry, and first-principles calculations. Room-temperature 2D-DMS provide a new component to expand the functional scope of van der Waals heterostructures and bring semiconducting magnetic 2D heterostructures into the realm of practical application.
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