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It is worth noting that such spectral trajectories cannot be obtained when a large ensemble of molecules is in resonance. 1 Physical Principles and Methods of Single-Molecule Spectroscopy in Solids Figure 11. Schematic of the temporal behavior of photon emission from a single molecule showing bunching on the scale of the triplet lifetime (upper half) and antibunching on the scale of the inverse of the Rabi frequency (lower half). 23 200 photons IIIIIIIIIIIIIIIIIIIIIIIIJIIIIIII 1- P x” erally uncorrelated, thus the behavior of an ensemble-averaged quantity such as a spectral hole would only be a broadening and smearing of the line.
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The three noise terms in the denominator of Eq. 4 represent shot noise contributions from the emitted fluorescence, background, and dark signals, respectively. For a detailed discussion of the collection efficiency for a single molecule taking into account the dipole radiation pattern, total internal reflection, and the molecular orientation, see Ref. 60. Assuming the collection efficiency D is maximized, Eq. 4 shows that there are several physical parameters which must be chosen carefully in order to maximize the SNR.