Quantum Transport of Single-Molecule Junctions when Theory and Experiment Meet.*

Molecular electronic transport experiments performed via Mechanically Controllable Break Junctions (MCBJ) or Scanning Tunneling Microscope on the BJ approach (STM-BJ) don’t provide direct information about the bonding of the molecule at the electrodes. However, to unmask the geometrical configuration acquired by the molecules between the electrodes, a combination of atomistic simulations, ab initio calculations, and electronic transport experiments is required.

We modeled the quantum transport of benzene, toluene, cyclohexane, and helicenes molecules over gold electrodes via Molecular Dynamics and DFT. We compared them with our experimental results, showing that this model has a high agreement.  Our model offers plausible scenarios of the experiment.  In summary, this triple comparative reveals clearly the relation between their characteristic electronic transport and the dynamic bonding of the molecule single between the electrodes. Additionally, we shed light on the nature of electrodes and their geometries.