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  • Title: Real-time observation of the spin-state mixing process of a micellized radical pair in weak magnetic fields by nanosecond fast field switching.
    Author: Miura T, Murai H.
    Journal: J Phys Chem A; 2008 Mar 27; 112(12):2526-32. PubMed ID: 18307324.
    Abstract:
    The singlet-triplet spin-state mixing process of a singlet-born radical pair confined in a sodium dodecyl sulfate (SDS) micelle was studied by observing the nanosecond switched external magnetic field (SEMF) effect on the transient absorption signals. A long-lived singlet radical pair is generated by the photoinduced bond cleavage reaction of tetraphenylhydrazine in an SDS micelle. Application of off-on type SEMF results in the increase of the free radical yield contrary to the decrease produced by an applied static magnetic field. The S-T mixing process in low magnetic field was observed by means of a delay-shift SEMF experiment. Observed incoherent mixing processes are explained in terms of the interplay between coherent hyperfine interaction and fast dephasing processes caused by the fluctuation of electron-spin interactions. Singlet-triplet and triplet-triplet dephasing rate constants are determined independently to be 2 x 10(8) and 0.2 x 10(8) s(-)1, respectively, by a simulation based on a modified single-site Liouville equation. This is the first direct observation of the incoherent spin-state mixing process at magnetic fields comparable to the hyperfine interactions of the radical pair.
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