Time-dependent single molecule spectral lines

A general conceptual problem of time-dependent single molecule spectra is discussed theoretically in the framework of recently developed intensity-time-frequency correlation spectroscopy. It is shown that the new method is closely related to a "gedanken" three-pulse photon echo experiment done on an ensemble of identical molecules interacting with statistically identical microscopic environments. The correlation function is an integral transform (under certain conditions a Fourier transform) of the echo amplitude as a function of the delay between the first and the second pulses. [S0163-1829(99)10907-X].