Abstract

We address the distinction between resonance Raman scattering and fluorescence as the excitation source is continuously tuned through resonance. The experiments are performed in iodine vapor using a cw laser, whose intensity is electrooptically modulated in the 0.1-50-MHz frequency range. A lock-in amplifier is used to detect both the in-phase and out-of-phase response of the emission. The modulated signal is found to be the sum of two components. One component varies with angular modulation frequency ω, as (1 + ω²τ²)^-1/2, where τ is the lifetime of the excited state. The other is found to be flat within the range of modulation frequency used in the experiment. Since the results of the modulation experiment are the Fourier transform of the response to pulsed excitation, the first component corresponds to exponential decay with the fluorescence lifetime and the second corresponds to a prompt response. A density matrix calculation shows that the prompt response would be absent if the absorption were independent of laser frequency. It exists as a result of the finite inhomogeneous linewidth and the laser detuning from the center of the transition. The amplitude of the delayed and prompt components is a function of laser frequency. This gives a full description of the dynamical response to the emission to linear excitation as the laser is tuned continuously through resonance. The response of the sample to nonlinear excitation is also discussed.

© 1985 Optical Society of America