Nonadiabatic simulation of singlet fission dynamics in tetracene clusters: The topology of quantum coherence in a global view.

The delocalization of excitonic states and the interstate quantum coherence are of great importance in understanding fundamental mechanisms in exciton dynamics such as singlet fission. The accurate theoretical description on this key component requires dynamic simulations to be performed at the molecular level in a nonadiabatic framework. Here, we apply the recently developed nonadiabatic active state trajectory method to simulate fission dynamics in tetracene clusters of up to 10 monomers. It is shown that a global view of the topology of quantum coherence in terms of molecular details such as packing configurations, spatial delocalization of states, and the topology of coherent regime plays an important role in modulating fission dynamics, which suggests a new focus for nonadiabatic control of exciton dynamics and provides valuable dynamical information and physical insights for artificial design. [ABSTRACT FROM AUTHOR]