M. Wu et al., PHOTOCHEMISTRY AND FLUORESCENCE EMISSION DYNAMICS OF SINGLE MOLECULESIN SOLUTION - B-PHYCOERYTHRIN, Journal of physical chemistry, 100(43), 1996, pp. 17406-17409
We report the first detailed studies of the photochemistry of single m
olecules in aqueous solution. Photolysis of single B-phycoerythrin (B-
PE) molecules, a highly fluorescent phycobiliprotein containing 34 bil
in chromophores, is observed as an abrupt cessation of the fluorescenc
e emission from individual molecules as they flow through a similar to
40 pL probe volume. These measurements demonstrate that B-PE is photo
lyzed in a single photochemical step. The observation of abrupt photob
leaching of single molecules could not be made in a bulk measurement b
ecause the signal would be averaged over many molecules to yield a con
tinuous decay. Photon pair correlation measurements of the fluorescenc
e detected from single B-PE molecules demonstrate that the molecule be
haves as a single quantum system, not as a collection of 34 independen
t chromophores.