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Theoretical treatments of ultrafast electron transfer from adsorbed dye molecule to semiconductor nanocrystalline surface
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10.1063/1.2359445
/content/aip/journal/jcp/125/15/10.1063/1.2359445
http://aip.metastore.ingenta.com/content/aip/journal/jcp/125/15/10.1063/1.2359445

Figures

Image of FIG. 1.
FIG. 1.

Scheme of the pump-probe observation of ET process from to by monitoring the stimulated emission from to the ground state .

Image of FIG. 2.
FIG. 2.

Energy level scheme for .

Image of FIG. 3.
FIG. 3.

Effect of vibrational relaxation on photoinduced ET.

Image of FIG. 4.
FIG. 4.

Experimentally observed absorption spectra of DTB-Pe molecule (blue line) and the theoretical fitting (black line) with parameters given in Table I. (a) The result in toluene and (b) the result of DTB-Pe on surface. The 0-0 transition energies are is in the toluene solution and on surface.

Image of FIG. 5.
FIG. 5.

(a) The induced absorption spectra constructed from the theory. At time , the induced absorption is from the reactant state to higher neutral states , while at time , contributions from both reactant state and product state appear. (b) In the work of Burfeindt et al. (Ref. 25), the induced absorption at is attributed to the reactant induced absorption, while at they conclude that the induced absorption from the product state is observed.

Image of FIG. 6.
FIG. 6.

The theoretical calculation of the time trace of transient absorption (TRABS) for a one-mode system. The energy gap is and the vibrational mode is . The solid curve is the reactant TRABS, and the dashed curve is the product TRABS. The probing frequency is set at respective peak positions of the induced absorption spectra of both reactant and product states. For discussion see text.

Image of FIG. 7.
FIG. 7.

The experimental observation of the reactant TRABS and product TRABS, done by Zimmermann et al. (Ref. 11). For discussion see text.

Image of FIG. 8.
FIG. 8.

TRABS time trace constructed theoretically for the one-mode model system. Here the frequency of the mode is changed to . For discussion see text.

Image of FIG. 9.
FIG. 9.

The TRABS dynamics observed at to the red side of the respective peak positions of the induced absorption spectra of both reactant and product state. For discussion see text.

Image of FIG. 10.
FIG. 10.

The TRABS dynamics of the model system when the energy gap between reactant and product is increased to . The other conditions are the same as in Fig. 6. For discussion see text.

Image of FIG. 11.
FIG. 11.

The TRABS dynamics of the model system when the energy gap between reactant and product is increased to . The other conditions are the same as in Fig. 6. For discussion see text.

Tables

Generic image for table
Table I.

The parameters of the vibrational modes used in the fitting of the absorption spectra of DTB-Pe molecule in toluene solution and on surface. The value is the Huang-Rhys factor, or the (vibronic) coupling constant.

Generic image for table
Table II.

The energy gaps of the transitions.

Generic image for table
Table III.

The coupling constant between different electronic potential surfaces and the inhomogeneity in calculating the transient absorption spectra.

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/content/aip/journal/jcp/125/15/10.1063/1.2359445
2006-10-18
2014-04-24
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Theoretical treatments of ultrafast electron transfer from adsorbed dye molecule to semiconductor nanocrystalline surface
http://aip.metastore.ingenta.com/content/aip/journal/jcp/125/15/10.1063/1.2359445
10.1063/1.2359445
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