Ultrafast Charge Transfer Visualized by Two-Dimensional Electronic Spectroscopy

Two-dimensional electronic spectroscopy (2D-ES) is used to investigate ultra fast 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.