Abstract

Ultrafast relaxation dynamics of the photoexcited one-dimensional molecular chain coupled with the phonon field is theoretically investigated. The time evolution of the system is formulated by the time-dependent variational method with a coherent state trial function. The temporal changes of the exciton coherence size and the energy relaxation strongly depend on the exciton transfer, the exciton–phonon coupling strength, and the phonon bandwidth. The calculated time-resolved spontaneous emission spectrum well reflects the temporal change of the exciton coherence: The intensity and the peak position represent the coherence size and the energy dissipation. A cooperative spontaneous emission, super-radiance, periodically appears as long as the exciton coherence maintains over the entire system as a result of in-phase oscillation of phonon modes.

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