Experimental evidence for sub-3-fs charge transfer from an aromatic adsorbate to a semiconductor

Joachim Schnadt, Paul A. Brühwiler (), Luc Patthey, James N. O'Shea, Sven Södergren, Michael Odelius, Rajeev Ahuja, Olof Karis, Margit Bässler, Petter Persson, Hans Siegbahn, S. Lunell and Nils Mårtensson
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Joachim Schnadt: Uppsala University
Paul A. Brühwiler: Uppsala University
Luc Patthey: Swiss Light Source, Paul-Scherrer-Institut
James N. O'Shea: Uppsala University
Sven Södergren: Uppsala University
Michael Odelius: Uppsala University
Rajeev Ahuja: Uppsala University
Olof Karis: Uppsala University
Margit Bässler: MAX-Lab, University of Lund
Petter Persson: Uppsala University
Hans Siegbahn: Uppsala University
S. Lunell: Uppsala University
Nils Mårtensson: Uppsala University

Nature, 2002, vol. 418, issue 6898, 620-623

Abstract: Abstract The ultrafast timescale of electron transfer processes is crucial to their role in many biological systems and technological devices. In dye-sensitized solar cells1,2,3,4, the electron transfer from photo-excited dye molecules to nanostructured semiconductor substrates needs to be sufficiently fast to compete effectively against loss processes and thus achieve high solar energy conversion efficiencies4. Time-resolved laser techniques indicate an upper limit of 20 to 100 femtoseconds5,6,7,8,9 for the time needed to inject an electron from a dye into a semiconductor, which corresponds to the timescale on which competing processes such as charge redistribution10,11 and intramolecular thermalization of excited states12,13,14 occur. Here we use resonant photoemission spectroscopy, which has previously been used to monitor electron transfer in simple systems with an order-of-magnitude improvement in time resolution15,16, to show that electron transfer from an aromatic adsorbate to a TiO2 semiconductor surface can occur in less than 3 fs. These results directly confirm that electronic coupling of the aromatic molecule to its substrate is sufficiently strong to suppress competing processes17.

Date: 2002
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DOI: 10.1038/nature00952

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