Abstract

Abstract Among van der Waals layered ferromagnets, monolayer vanadium diselenide (VSe 2 ) stands out due to its robust ferromagnetism. However, the exfoliation of monolayer VSe 2 is challenging, not least because the monolayer flake is extremely unstable in air. Using an electrochemical exfoliation approach with organic cations as the intercalants, monolayer 1T‐VSe 2 flakes are successfully obtained from the bulk crystal at high yield. Thiol molecules are further introduced onto the VSe 2 surface to passivate the exfoliated flakes, which improves the air stability of the flakes for subsequent characterizations. Room‐temperature ferromagnetism is confirmed on the exfoliated 2D VSe 2 flakes using a superconducting quantum interference device (SQUID), X‐ray magnetic circular dichroism (XMCD), and magnetic force microscopy (MFM), where the monolayer flake displays the strongest ferromagnetic properties. Se vacancies, which can be ubiquitous in such materials, also contribute to the ferromagnetism of VSe 2 , although density functional theory (DFT) calculations show that such effect can be minimized by physisorbed oxygen molecules or covalently bound thiol molecules.