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  4. Beyond Vibrationally Mediated Electron Transfer: Coherent Phenomena Induced by Ultrafast Charge Separation
 
research article

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

Huber, Robert
•
Dworak, Lars
•
Moser, Jacques E.  
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2016
Journal of Physical Chemistry C

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.

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Type
research article
DOI
10.1021/acs.jpcc.6b02012
Web of Science ID

WOS:000375521700013

Author(s)
Huber, Robert
Dworak, Lars
Moser, Jacques E.  
Grätzel, Michael  
Wachtveitl, Josef
Date Issued

2016

Publisher

American Chemical Society

Published in
Journal of Physical Chemistry C
Volume

120

Start page

8534

End page

8539

Editorial or Peer reviewed

REVIEWED

Written at

OTHER

EPFL units
GR-MO  
LPI  
Available on Infoscience
April 23, 2016
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/125852
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