This review comprehensively presents the fifty-year journey of surface-enhanced Raman spectroscopy (SERS), covering its discovery, pivotal phases, innovative methods, and key inspirations from the pioneers and trailblazers.

A cascade chemical reaction is selectively activated through oriented external electric field at the single-molecule scale.

We applied a combination of mechanically controllable break junction (MCBJ) and in situ surface enhanced Raman spectroscopy (SERS) methods to investigate the long-standing single-molecule conductance discrepancy of prototypical benzene-1,4-dithiol (BDT) junctions. Single-molecule conductance characterization, together with configuration analysis of the molecular junction, suggested that disulfide-mediated dimerization of BDT contributed to the low conductance feature, which was further verified by the detection of S–S bond formation through in situ SERS characterization. Control experiments demonstrated that the disulfide-mediated dimerization could be tuned via the chemical inhibitor. Our findings suggest that a combined electrical and SERS method is capable of probing chemical reactions at the single-molecule level.

The cross-plane charge transport is demonstrated in single-molecule two-dimensional van der Waals heterojunctions.