Abstract
The metal-molecule interface, particularly the molecular adsorption site, plays a decisive role in the efficiency and durability of organic electronics and the characteristic variability of molecular electronics. However, precise molecular-scale handling of the metal-molecule interface remains to be achieved, owing to technical limitations. Here, we developed a hybrid spectro-electrical technique that enables detailed in situ characterization of the metal-molecule interface at room temperature with single-molecule resolution. This non-destructive technique combines surface-enhanced Raman spectroscopy and current-voltage measurements to obtain correlated structural and electronic details of a single 1, 4-benzenedithiol molecule suspended between two Au electrodes. Significantly, this technique was found to be sensitive to the molecular adsorption site, thus providing an important step toward the reliable integration of millions of individual molecular components into working devices.