Journal Title
Title of Journal: Res Chem Intermed
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Abbravation: Research on Chemical Intermediates
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Publisher
Springer Netherlands
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Authors: Nobuyuki Ichinose Masahide Hagiri Junichiro Kinugasa Nobuyuki Shichi Toshihiro Nakayama
Publish Date: 2012/07/05
Volume: 39, Issue: 1, Pages: 425-435
Abstract
A chargetransfer CT complex of NOBF4 and hexamethoxybenzene HMB which gives out HMB•+ as a “fluorescent radical cation probe” upon oneelectron oxidation has been designed to explore the excited state dynamics of contact radical ion pairs by laserinduced fluorescence and femtosecond transient absorption spectroscopic techniques The acetonitrile solution of the CT complex showed weak fluorescence with a similar spectrum to that observed for free excited HMB radical cation HMB•+ suggesting the formation of HMB•+ upon the onephotonic excitation of the CT complex The laserpower dependence of the fluorescence intensity supported the onephotonic excitation event We have also observed a shortlived transient species but no longlived species by femtosecond laser flash photolysis of the CT complex The lifetime 65 ps was in good accordance with its fluorescence quantum yield 25 × 10−5 and was able to assign the transient species to the fluorescent state an excited radical ion pair HMB •+/NO• All the events were completed within the inner sphere and the short lifetime of the transient species could be attributed to rapid backelectron transfer It is concluded that the excited radical cation character in the excited state of the CT complex originates from the radical ion character in the CT complex in the ground state and that a relatively long lifetime of HMB•+ facilitates its observation even in the contact ion pair
Keywords:
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