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Electron transfer in porphyrin—quinone cyclophanes studied on the pico- and femto-second time scale

✍ Scribed by W. Frey; R. Klann; F. Laermer; T. Elsaesser; E. Baumann; M. Futscher; H.A. Staab


Publisher
Elsevier Science
Year
1992
Tongue
English
Weight
429 KB
Volume
190
Category
Article
ISSN
0009-2614

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✦ Synopsis


Electron transfer in porphyrin-quinone cyclophanes is investigated by fluorescence and absorption spectroscopy with pico-and femto-second pulses. In nonpolar solvents, the S~ state of the porphyrin shows a lifetime from 300 ps up to several nanoseconds, depending upon the number of quinones and upon their electron affinity. Comparative measurements in polar solvents demonstrate very fast electron transfer on a time scale between 1 and 10 ps. The results are analyzed with the aid of quantum-chemical calculations which give the energy of the charge transfer states and the relevant coupling strengths. For nonpolar solvents, theory suggests fluctuation-induced charge separation and/or direct radiationless internal conversion from the porphyrin Sl to the ground state. In polar solution, the molecules exist in a tilted configuration with strong electronic coupling and charge transfer states well below the Sl level, resulting in fast electron transfer and subsequent charge recombination within 10-40 ps.