摘要:SummaryThe manipulation of molecule-electrode interaction is essential for the fabrication of molecular devices and determines the connectivity from electrodes to molecular components. Although the connectivity of molecular devices could be controlled by molecular design to place anchor groups in different positions of molecule backbones, the reversible switching of such connectivities remains challenging. Here, we develop an electric-field-induced strategy to switch the connectivity of single-molecule junctions reversibly, leading to the manipulation of different connectivities in the same molecular backbone. Our results offer a new concept of single-molecule manipulation and provide a feasible strategy to regulate molecule-electrode interaction.Graphical AbstractDisplay OmittedHighlights•A strategy toin-situswitch the connectivity of single-molecule junctions•A concept to manipulate the molecule-electrode interaction•A molecular switch triggered by the varying of electric field•Experiments were combined with calculations to probe the switching mechanismMolecular Electrochemistry; Quantum Electronics; Electronic Materials