Abstract:
:Magnetic field effect studies of alkylcobalamin photolysis provide evidence for the formation of a reactive radical pair that is born in the singlet spin state. The radical pair recombination process that is responsible for the magnetic field dependence of the continuous-wave (CW) quantum yield is limited to the diffusive radical pair. Although the geminate radical pair of adenosylcob(III)alamin also undergoes magnetic field dependent recombination (A.M. Chagovetz and C. B. Grissom, J. Am. Chem. soc. 115, 12152-12157, 1993), this process does not account for the magnetic field dependence of the CW quantum yield that is only observed in viscous solvents. Glycerol and ethylene glycol increase the microviscosity of the solution and thereby increase the lifetime of the spin-correlated diffusive radical pair. This enables magnetic field dependent recombination among spin-correlated diffusive radical pairs in the solvent cage. Magnetic field dependent recombination is not observed in the presence of nonviscosigenic alcohols such as isopropanol, thereby indicating the importance of the increased microviscosity of the medium. Paramagnetic radical scavengers that trap alkyl radicals that escape the solvent cage do not diminish the magnetic field effect on the CW quantum yield, thereby ruling out radical pair recombination among randomly diffusing radical pairs, as well as excluding the involvement of solvent-derived radicals. Magnetic field dependent recombination among alkylcobalamin radical pairs has been simulated by a semi-classical model of radical pair dynamics and recombination. These calculations support the existence of a singlet radical pair precursor.
journal_name
Photochem Photobioljournal_title
Photochemistry and photobiologyauthors
Natarajan E,Grissom CBdoi
10.1111/j.1751-1097.1996.tb02460.xsubject
Has Abstractpub_date
1996-08-01 00:00:00pages
286-95issue
2eissn
0031-8655issn
1751-1097journal_volume
64pub_type
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