van der Waals supramolecular transistors

van der Waals (vdW) interactions play a crucial role in various fields, including self-assembly and electronic devices. However, precisely manipulating intermolecular vdW interactions at the single-molecule level to develop supramolecular transistors remains a central challenge. In this study, we report a supramolecular transistor via electrochemical manipulation of a single molecule to a vdW dimer in nickel bis(dithiolene) (NBTE) junctions using the electrochemical scanning tunneling microscopy break-junction technique. Conductance measurements reveal that NBTE remains monomeric under positive potential but forms negatively charged vdW dimers under negative potential. This single-electron redox-driven transition triggers a ∼700-fold increase in conductance and shifts the transport path from in-plane to cross-plane. Theoretical calculations confirm that the dimer is stabilized predominantly by vdW interactions, further enhanced by electric fields, thereby enabling fine regulation of the transistor's conductance. This work demonstrates the first single-electron supramolecular transistor dictated by intermolecular vdW forces, offering a promising strategy for low-power vdW electronics.