Manipulations of Electronic and Spin States in Co-Quantum Dot/WS₂ Heterostructure on a Metal-Dielectric Composite Substrate by Controlling Interfacial Carriers

Charge and spin are two intrinsic attributes of carriers governing almost all of the physical processes and operation principles in materials. Here, we demonstrate the manipulation of electronic and spin states in designed Co-quantum dot/WS₂ (Co-QDs/WS₂) heterostructures by employing a metal–dielectric composite substrate and via scanning tunneling microscope. By repeatedly scanning under a unipolar bias, switching the bias polarity, or applying a pulse through nonmagnetic or magnetic tips, the Co-QDs morphologies exhibit a regular and reproducible transformation between bright and dark dots. First-principles calculations reveal that these tunable characters are attributed to the variation of density of states and the transition of magnetic anisotropy energy induced by carrier accumulation. It also suggests that the metal–dielectric composite substrate is successful in creating the interfacial potential for carrier accumulation and realizes the electrically controllable modulations. These results will promote the exploration of electron–matter interactions in quantum systems and provide an innovative way to facilitate the development of spintronics.