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Ultrafast Photoinduced Electron Transfer at Electrodes: The General Case of a Heterogeneous Electron-Transfer Reaction

MPG-Autoren
http://pubman.mpdl.mpg.de/cone/persons/resource/persons22242

Willig,  Frank
Theory, Fritz Haber Institute, Max Planck Society;

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Zitation

Gundlach, L., & Willig, F. (2012). Ultrafast Photoinduced Electron Transfer at Electrodes: The General Case of a Heterogeneous Electron-Transfer Reaction. ChemPhysChem, 13(12), 2877-2881. doi:10.1002/cphc.201200151.


Zitierlink: http://hdl.handle.net/11858/00-001M-0000-0010-76D2-8
Zusammenfassung
The general case of a heterogeneous electron-transfer reaction is realized by ultrafast electron transfer from a light-absorbing molecule to a wide continuum of electronic acceptor states, realizing the so-called wide band limit. Experimental data obtained for perylene dye/TiO2 systems confirm the predictions of fully quantum mechanical model calculations of the dynamics. The energy distribution of the injected electron shows an energy loss due to excitations of high-energy (quantum) vibrational modes in the ionized perylene moiety. The electrontransfer mechanism is non-adiabatic and the reaction is ultrafast, for example, with a time constant of 9 fs for the COOH anchor-bridge group. The underlying strong coupling of the electronic states to high-energy vibrational modes is a characteristic feature of sensitizer molecules.