Objective
The main goal of the Project is to reveal the crucial factors which control the mechanism of excited-state ET reactions - either conventional sudden electron jump from an electron donor to an acceptor (after preliminary reorganization of the reactants and media according to the Marcus theory) or gradual shift of electron density (correlated with the changes of nuclear co-ordinates of reactants and medium) yielding exciplexes as transients. The dynamics of the formation of primary products - exciplexes and geminate radical ion pairs, their interconversions as well as their transformation into the triplet state will be studied by time-resolved fluorescence and absorption spectroscopy (fs, ps, and ns) and by magnetic field effects for various organic compounds. The effects of the driving force of ET (-0.3 < deltaGet < 0.2eV) medium polarity and reactants structure on the competition of these two mechanisms will be compared. This should indicate factors which control the competition of this novel transient exciplex formation mechanism with alternative electron jump mechanism.
Joint application of time resolved emission and absorption spectroscopy and magnetic field effect is expected to provide direct, detailed and complete information on the competition of the mechanisms of direct formation of contact (CRIP) and solvent separated ion pairs (SSRIP) in encounter complexes and of their delayed formation through transient exciplexes. Magnetic field effect can be used efficiently to discriminate between prompt and gradual ET (weak and strong coupling) even in the cases when exciplexes cannot be detected by emission spectroscopy and to evaluate the relative contributions of each mechanism to the total quenching process from the amplitude of the magnetic field effect.
Three types of results are planned to be reached.
Qualitative confirmation of the transient exciplex mechanism in wide range of representative systems. Time-resolved spectroscopic investigation (fs, ps, and ns) and magnetic field effect will provide direct kinetic data on the formation of radical ions either from transient exciplexes or at direct interaction of excited molecules with electron donor or acceptor.
Quantitative confirmation of the transient exciplex mechanism by comparison of directly measured rate constants of exciplex and radical ions formation and decay with apparent quenching rate constants and radical ions quantum yields obtained in steady-state experiments in the region of kinetic control
(deltaGet > -0.3eV).
The development of quantitative theory of ET following the mechanism of correlated electronic and nuclear reorganization on the base of the dependences of exciplex formation equilibrium and rate constants, lifetimes, rate constants and activation parameters of exciplex dissociation into radical ions and conversion into triplet states on -Get, solvent polarity. These dependences will be obtained from experimental data on temperature effect on the yields and rates of exciplexes and radical ions and compared with simple theoretical models.
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Programme(s)
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Topic(s)
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Funding Scheme
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Coordinator
SW7 2AZ London
United Kingdom
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