Theory of photoinduced phase dynamics in organic charge-transfer complexes

In the quasi-one-dimensional mixed-stack organic charge-transfer complex, TTF-CA, photoirradiation is known to trigger transitions between the neutral and ionic phases. Here we use a one-dimensional extended Peierls–Hubbard model with alternating potentials and calculate the mean-field dynamics of charge density coupled with that of lattice displacements. We show qualitative differences between the photoinduced ionic-to-neutral and neutral-to-ionic transitions, which are consistent with recent experimental findings. That is, the ionic-to-neutral transition proceeds cooperatively, characterized by threshold behavior, while the neutral-to-ionic transition proceeds uncooperatively, characterized by linear behavior. The threshold absorption in the former depends on the strength or the duration of the pulse. The coherence during the transition dynamics is also different between the two transitions. In the ionic-to-neutral transition, a clear interference effect is observed as a function of the interval when the pulse is spilt into two.