Magnetic field and temperature dependencies shed light on the recombination kinetics of a transition metal donor/acceptor system

T. Von Feilitzsch; P. Härter; O. Schiemann; M. E. Michel-Beyerle; U. E. Steiner; P. Gilch

doi:10.1021/ja0547174

Magnetic field and temperature dependencies shed light on the recombination kinetics of a transition metal donor/acceptor system

T. Von Feilitzsch, P. Härter, O. Schiemann, M. E. Michel-Beyerle, U. E. Steiner, P. Gilch

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Abstract

The radical pair recombination of an intramolecular electron-transfer system containing a transition metal moiety has been addressed by femtosecond spectroscopy. The radical pair is formed by ultrafast electron transfer (90 fs) from a ferrocene residue to a photoexcited Nile blue moiety. Its recombination proceeds on the picosecond time scale in a multiexponential fashion. The kinetic pattern is a manifestation of spin processes competing with electron transfer. Magnetic field effects on these kinetics allow one to disentangle the two contributions, Their temperature dependencies yield the activation parameters of the two processes. The discussion focuses on the mechanism of electron spin relaxation. Strong evidence for the Orbach/Kivelson mechanism will be given.

Original language	English
Pages (from-to)	15228-15235
Number of pages	8
Journal	Journal of the American Chemical Society
Volume	127
Issue number	43
DOIs	https://doi.org/10.1021/ja0547174
State	Published - 2 Nov 2005

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title = "Magnetic field and temperature dependencies shed light on the recombination kinetics of a transition metal donor/acceptor system",

abstract = "The radical pair recombination of an intramolecular electron-transfer system containing a transition metal moiety has been addressed by femtosecond spectroscopy. The radical pair is formed by ultrafast electron transfer (90 fs) from a ferrocene residue to a photoexcited Nile blue moiety. Its recombination proceeds on the picosecond time scale in a multiexponential fashion. The kinetic pattern is a manifestation of spin processes competing with electron transfer. Magnetic field effects on these kinetics allow one to disentangle the two contributions, Their temperature dependencies yield the activation parameters of the two processes. The discussion focuses on the mechanism of electron spin relaxation. Strong evidence for the Orbach/Kivelson mechanism will be given.",

author = "{Von Feilitzsch}, T. and P. H{\"a}rter and O. Schiemann and Michel-Beyerle, {M. E.} and Steiner, {U. E.} and P. Gilch",

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T1 - Magnetic field and temperature dependencies shed light on the recombination kinetics of a transition metal donor/acceptor system

AU - Von Feilitzsch, T.

AU - Härter, P.

AU - Schiemann, O.

AU - Michel-Beyerle, M. E.

AU - Steiner, U. E.

AU - Gilch, P.

PY - 2005/11/2

Y1 - 2005/11/2

N2 - The radical pair recombination of an intramolecular electron-transfer system containing a transition metal moiety has been addressed by femtosecond spectroscopy. The radical pair is formed by ultrafast electron transfer (90 fs) from a ferrocene residue to a photoexcited Nile blue moiety. Its recombination proceeds on the picosecond time scale in a multiexponential fashion. The kinetic pattern is a manifestation of spin processes competing with electron transfer. Magnetic field effects on these kinetics allow one to disentangle the two contributions, Their temperature dependencies yield the activation parameters of the two processes. The discussion focuses on the mechanism of electron spin relaxation. Strong evidence for the Orbach/Kivelson mechanism will be given.

AB - The radical pair recombination of an intramolecular electron-transfer system containing a transition metal moiety has been addressed by femtosecond spectroscopy. The radical pair is formed by ultrafast electron transfer (90 fs) from a ferrocene residue to a photoexcited Nile blue moiety. Its recombination proceeds on the picosecond time scale in a multiexponential fashion. The kinetic pattern is a manifestation of spin processes competing with electron transfer. Magnetic field effects on these kinetics allow one to disentangle the two contributions, Their temperature dependencies yield the activation parameters of the two processes. The discussion focuses on the mechanism of electron spin relaxation. Strong evidence for the Orbach/Kivelson mechanism will be given.

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M3 - Article

AN - SCOPUS:27544491198

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VL - 127

SP - 15228

EP - 15235

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 43

ER -

Magnetic field and temperature dependencies shed light on the recombination kinetics of a transition metal donor/acceptor system

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