“…Molecular wires, as the fundamental units in molecular electronics, hold promise for overcoming the existing challenges associated with conventional silicon-based electronics in terms of device miniaturization and tuning the charge transport quantum mechanically. The vast diversity and structural freedom of organic-based molecules have spurred increasing interest in probing and manipulating charge transport through single molecules. , Molecular analogs have been developed to mimic the behavior of conventional electronic devices, such as diodes, , transistors, , sensors, , photoswitches, − and thermoelectric units. − More importantly, owing to quantum mechanically dominated charge transport in single molecules, new transport phenomena that are absent in macroscopic semiconductor devices have been unfolded, including but not limited to quantum interference − and chirality induced spin selectivity. − Nonetheless, one of the major roadblocks toward developing applicable molecular electronics is the inherent low conductivity of organic molecules. , The commonly investigated molecules acting as conducting elements in a circuit are molecules with highly conjugated π-building blocks. Charge transport through a single molecule has been extensively explored using the single-molecule junction platforms that are capable of covalently connecting a molecule to two electrodes. − To date, most of the studied conjugated molecules have been shown to conduct electrons in an off-resonant, coherent regime.…”