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

Wave packet propagation succeeding electron transfer (ET) from alizarin dye molecules into the nanocrystalline TiO2 semiconductor has been studied by ultrafast transient absorption spectroscopy. Because of the ultrafast time scale of the ET reaction of about 6 fs, the system shows substantial differences to molecular ET systems. We show that the ET process is not mediated by molecular vibrations, and therefore classical ET theories lose their applicability. Here the ET reaction itself prepares a vibrational wave packet and not the electromagnetic excitation by the laser pulse. Furthermore, the generation of phonons during polaron formation in the TiO2 lattice is observed in real time for this system. The presented investigations enable an unambiguous assignment of the involved photoinduced mechanisms and can contribute to a corresponding extension of molecular ET theories to ultrafast ET systems like alizarin/TiO2.


Published in:
The Journal of Physical Chemistry C, 120, 8534-8539
Year:
2016
Publisher:
Washington, American Chemical Society
ISSN:
1932-7455
Laboratories:




 Record created 2016-04-23, last modified 2018-03-18

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