Project Summary: Dilute magnetic semiconductors, achieved through substitutional doping of magnetic atoms into semiconducting systems, enable experimental modulation of spin dynamics for novel magneto-electric or magneto-optical devices, especially in 2D 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 the ability to achieve optimal doping levels without dopant aggregation. 2DCC-MIP theorists collaborated closely with a highly interdisciplinary team of experimentalists both within and beyond the MIP to obtain evidence for room-temperature ferromagnetic order in vanadium-doped tungsten disulfide monolayers synthesized by a reliable single-step method with minimal dopant aggregation. First-principles calculations suggest that quenches due to orbital hybridization occurs at closer vanadium–vanadium spacings; this prediction is supported by transmission electron microscopy and magnetometry. These insights and discoveries help bring semiconducting 2D magnetic heterostructures closer to practical application.
Published in Adv. Sci. 2020, 7, 2001174
2DCC Role: First-principles theory of dopant energetics and mechanisms of magnetism, electron microscopy and collaborative synthesis.