Abstract
Time-dependent spectra of light emitted after two-photon excitation with nonresonant intermediate state are studied by the perturbation method. Two components are distinguished: a slow one ${I}_{s}$ connected with the excited-state population, and a fast one ${I}_{f}$ connected with the double-quantum optical coherence. For large detuning of the two-photon frequency from the excited-ground-state energy separation, the fluorescent light is found to be ${I}_{s}\ensuremath{-}|{I}_{f}|$, and the Raman-scattered light is ${I}_{f}$. The influence of statistics of light, laser linewidth, spectral bandwidth of the detector, and transfer of coherence from the ground to the excited state are also taken into consideration.
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