Determining structural transformations of single molecules (SMs) is an important fundamental scientific endeavor. Optical spectroscopies are the dominant tools used to unravel the physical and chemical features of individual molecules and have substantially contributed to surface science and biotechnology. In particular, Raman spectroscopy can identify reaction intermediates and reveal underlying reaction mechanisms; however, SM Raman experiments are subject to intrinsically weak signal intensities and considerable signal attenuation within the spectral dispersion systems of the spectrometer. Here, to monitor the structural transformation of an SM on the millisecond time scale, a plasmonic nanocavity substrate has been used to enable Raman vibrational and fluorescence spectral signals to be simultaneously collected and correlated, which thus allows a detection of photo-induced bond cleavage between the xanthene and phenyl group of a single rhodamine B isothiocyanate molecule in real time. This technique provides a novel method for investigating light-matter interactions and chemical reactions at the SM level.
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