The configuration effect on the exciton dynamics of zinc chlorin aggregates

Excitonic energy transfer among the zinc chlorin molecules is significant for the photovoltaic process because of their high sensitivities to harvesting sunlight. Zinc chlorin monomers and dimers can be synthesized experimentally, and they can form various self-assembled structures. Using the realistic parameters of zinc chlorin molecules, we assume that 20 molecules with J-, H- or J-H aggregation are arranged in a line and we investigate their dipole configuration effect on exciton dynamics. The expectation value approximation of operators is applied to derive the equations of motion of multi-exciton states. The temporal evolution of multi-exciton states is analyzed in the scheme of density matrix theory. Our simulations show that the inter-molecular coupling results in an exciton band and the wave-packet progressing excited by the resonant laser pulse exhibits attractive or repulsive behavior at the exciton level due to the dipole configuration effect. In the defined J-H coupling, the coherent wave-packet cannot overcome the configuration barrier to the no-excited part. The exciton dynamics revealed here might be helpful to better understand the energy transfer process in organic photovoltaic devices.

Automated summary

This study investigates the excitonic energy transfer among zinc chlorin molecules arranged in different aggregation modes. Through density matrix theory analysis, it is found that inter-molecular coupling leads to the formation of an exciton band. Furthermore, the dipole configuration effect results in attractive or repulsive behavior of the wave-packet excited by resonant laser pulse at the exciton level.