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

Schnadt, J; Bruhwiler, PA; Patthey, L; O'Shea, JN; Sodergren, S; Odelius, M; Ahuja, R; Karis, O; Bassler, M and Persson, Petter LU , et al. (2002) In Nature 418(6898). p.620-623
Abstract
The ultrafast timescale of electron transfer processes is crucial to their role in many biological systems and technological devices. In dye-sensitized solar cells(1-4), the electron transfer from photoexcited dye molecules to nanostructured semiconductor substrates needs to be sufficiently fast to compete effectively against loss processes and thus achieve high solar energy conversion efficiencies(4). Time-resolved laser techniques indicate an upper limit of 20 to 100 femtoseconds(5-9) 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 redistribution(10,11) and intramolecular thermalization of excited states(12-14) occur. Here we use... (More)
The ultrafast timescale of electron transfer processes is crucial to their role in many biological systems and technological devices. In dye-sensitized solar cells(1-4), the electron transfer from photoexcited dye molecules to nanostructured semiconductor substrates needs to be sufficiently fast to compete effectively against loss processes and thus achieve high solar energy conversion efficiencies(4). Time-resolved laser techniques indicate an upper limit of 20 to 100 femtoseconds(5-9) 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 redistribution(10,11) and intramolecular thermalization of excited states(12-14) 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 resolution(15,16), 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 processes(17). (Less)
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publication status
published
subject
in
Nature
volume
418
issue
6898
pages
620 - 623
publisher
Nature Publishing Group
external identifiers
  • wos:000177305600037
  • pmid:12167856
  • scopus:18544367520
ISSN
0028-0836
DOI
10.1038/nature00952
language
English
LU publication?
yes
id
fde907ac-801a-41fb-a961-2da1d365bc6e (old id 332634)
date added to LUP
2007-11-12 15:49:29
date last changed
2017-12-10 03:56:21
@article{fde907ac-801a-41fb-a961-2da1d365bc6e,
  abstract     = {The ultrafast timescale of electron transfer processes is crucial to their role in many biological systems and technological devices. In dye-sensitized solar cells(1-4), the electron transfer from photoexcited dye molecules to nanostructured semiconductor substrates needs to be sufficiently fast to compete effectively against loss processes and thus achieve high solar energy conversion efficiencies(4). Time-resolved laser techniques indicate an upper limit of 20 to 100 femtoseconds(5-9) 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 redistribution(10,11) and intramolecular thermalization of excited states(12-14) 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 resolution(15,16), 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 processes(17).},
  author       = {Schnadt, J and Bruhwiler, PA and Patthey, L and O'Shea, JN and Sodergren, S and Odelius, M and Ahuja, R and Karis, O and Bassler, M and Persson, Petter and Siegbahn, H and Lunell, S and Mårtensson, Nils},
  issn         = {0028-0836},
  language     = {eng},
  number       = {6898},
  pages        = {620--623},
  publisher    = {Nature Publishing Group},
  series       = {Nature},
  title        = {Experimental evidence for sub-3-fs charge transfer from an aromatic adsorbate to a semiconductor},
  url          = {http://dx.doi.org/10.1038/nature00952},
  volume       = {418},
  year         = {2002},
}