Coherent nonlinear dynamics of photoinduced cooperative phenomena at 0 K is studied by numerical calculations on a model of molecular crystals. We found that the photoinduced nucleation process is triggered only when a certain amount of excitation energy is supplied in a narrow part of the system; i.e., there exists the smallest size of the cluster of excited molecules which makes the nucleation possible. As a result, the portion of the cooperatively converted molecules is nonlinearly dependent on the photoexcitation strength, which has been observed in various materials.

• Received 21 August 2007

DOI:https://doi.org/10.1103/PhysRevLett.100.116403