“…The first single-molecule optical detection experiment was achieved by absorption using a doublemodulation technique, but had to be carried out at cryogenic conditions, under which the absorption cross-section of the zero-phonon line is 10 6 times larger. 21 Indirect detection schemes combined with modulation techniques have been developed for absorption-based detection, [22][23][24][25] 4 including ground-state depletion microscopy 15,26 and photothermal microscopy. 11,13,14,16,[27][28][29][30] However, most studies using these methods have reported single-wavelength imaging without yielding spectroscopic information.…”