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Wave packet propagation succeeding electron transfer (ET) from alizarin dyemolecules into the nanocrystalline TiO2 semiconductor has been studied byultrafast transient absorption spectroscopy. Due to the ultrafast time scale ofthe ET reaction of about 6 fs the system shows substantial differences tomolecular ET systems. We show that the ET process is not mediated by molecularvibrations and therefore classical ET theories lose their applicability. Herethe ET reaction itself prepares a vibrational wave packet and not theelectromagnetic excitation by the laser pulse. Furthermore, the generation ofphonons during polaron formation in the TiO2 lattice is observed in real timefor this system. The presented investigations enable an unambiguous assignmentof the involved photoinduced mechanisms and can contribute to a correspondingextension of molecular ET theories to ultrafast ET systems like alizarin/TiO2.

Beyond Vibrationally Mediated Electron Transfer: Coherent Phenomena Induced by Ultrafast Charge Separation