Molecular eigenstates lifetimes

Here we describe the development of the coherent-control toolbox with gas-phase iodine molecules [37 1, 48]. The gas-phase molecules are isolated from each other, so that they have long coherence lifetime, serving as an ideal platform to observe and control quantum coherence. First, we describe our experiments to observe and control the temporal evolution of the WP interference. Second, the eigenstate picture of the WP interference is presented. Finally, we demonstrate the application of WPI to ultrafast molecular computing. 

In the derivation we have neglected the possibility of overlapping molecular resonances (i.e. we have assumed that there are not couples of eigenstates so close in energy that they can emit identical photons). Furthermore, a width Fp has been attributed to the excited state l p), which accounts for its finite lifetime due to spontaneous emission or other decay mechanisms. The first term in Eq. (17) is dominant when Eg + huj Ep, i.e. for resonant Raman (RR) scattering. 

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