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We analyze electronically excited nuclear wave functions and their coherencewhen subjecting a molecule to the action of natural, pulsed incoherentsolar-like light, and to that of ultrashort coherent light assumed to have thesame center frequencies and spectral bandwidths. Specifically, we compute thespatio-temporal dependence of the excited wave packets and their electroniccoherence for these two types of light sources, on different electronicpotential energy surfaces. The resultant excited state wave functions are shownto be qualitatively different, reflecting the light source from which theyoriginated. In addition, electronic coherence is found to decay significantlyfaster for incoherent light than for coherent ultrafast excitation, for bothcontinuum and bound wave packets. These results confirm that the dynamicsobserved in studies using ultrashort coherent pulses are not relevant tonaturally occurring solar-induced processes such as photosynthesis and vision.

The Nature of Quantum States Created by One Photon Absorption: Pulsed Coherent vs. Pulsed Incoherent Light