Nature research paper: Orbital-resolved observation of singlet fission
Our results let us return to the questions concerning the mechanism of the primary step raised at the beginning. In the coherent mechanism,TT would be instantaneously populated. This stands in contrast to our observation. The bitriplet is formed after the optical excitation by the 100 fs decay of the singlet exciton.
Our observations show the nature of the electronic states and reveal the significant CT character of the singlet exciton. They do not show the nuclear rearrangement that follows the perturbation by optical excitation and SF. The nuclei will relax in both steps. Specific vibrational modes will be launched that shuttle the wave packet to lower energies.
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