Transfer of Vibrational Coherence Through Incoherent Energy Transfer Process in F\"{o}rster Limi

We study transfer of coherent nuclear oscillations between an excitation energy donor and an acceptor in a simple dimeric electronic system coupled to an unstructured thermodynamic bath and some pronounced vibrational intramolecular mode. Our focus is on the non-linear optical response of such a system, i.e. we study both excited state energy transfer and the compensation of the so-called ground state bleach signal. The response function formalism enables us to investigate a heterodimer with monomers coupled strongly to the bath and by a weak resonance coupling to each other (F\"{o}rster rate limit). Our work is motivated by recent observation of various vibrational signatures in 2D coherent spectra of energy transferring systems including large structures with a fast energy diffusion. We find that the vibrational coherence can be transferred from donor to acceptor molecules provided the transfer rate is sufficiently fast. The ground state bleach signal of the acceptor molecules does not show any oscillatory signatures, and oscillations in ground state bleaching signal of the donor prevail with the amplitude which is not decreasing with the relaxation rate.Comment: 11 pages, 9 figure

Ultrafast Charge Transfer Visualized by Two-Dimensional Electronic Spectroscopy

Two-dimensional electronic spectroscopy (2D-ES) is used to investigate ultrafast excited-state dynamics in a lutetium bisphthalocyanine dimer. Following optical excitation, a chain of electron and hole transfer steps gives rise to characteristic cross-peak dynamics in the electronic 2D spectra. The combination of density matrix propagation and quantum chemical calculations results in a molecular view of the charge transfer dynamics and highlights the role of the counter-ion in providing an energetic perturbation which promotes charge transfer across the complex

Ultrafast Charge Transfer Visualized by Two-Dimensional Electronic Spectroscopy

Two-dimensional electronic spectroscopy (2D-ES) is used to investigate ultrafast excited-state dynamics in a lutetium bisphthalocyanine dimer. Following optical excitation, a chain of electron and hole transfer steps gives rise to characteristic cross-peak dynamics in the electronic 2D spectra. The combination of density matrix propagation and quantum chemical calculations results in a molecular view of the charge transfer dynamics and highlights the role of the counter-ion in providing an energetic perturbation which promotes charge transfer across the complex