Multidimensional Characterization of Single‐Molecule Dynamics in a Plasmonic Nanocavity

Abstract Nanoscale manipulation and characterization of individual molecules is necessary to understand the intricacies molecular structure, which governs phenomena such as reaction mechanisms, catalysis, local effective temperatures, surface interactions, charge transport. Here we utilize Raman enhancement between two nanostructured electrodes in combination with direct transport measurements allow for simultaneous electrical, optical, mechanical properties a single molecule. This multi‐dimensional information yields repeatable, self‐consistent, verification single‐molecule resolution, allows detailed analysis structural configurational changes molecule situ. These experimental results are supported by machine‐learning based statistical spectral calculations provide insight into correlation its charge‐transport properties.