We continue to explore the rich photophysics of TATA+, a metal-free photosensitizer recently used in complex multielectron photoredox catalytic reactions. Upon excitation of the dye in acetonitrile solution (left), a triplet excited state (3TATA+*) is populated upon intersystem crossing (ISC) with a time constant of 8.9 ns. From there, in addition to the spin-forbidden repopulation of either S0 or S1 (reverse ISC resulting in delayed fluorescence), a diffusion-controlled intermolecular symmetry-breaking charge separation (SB-CS) channel is at play. In this pathway, two excited molecules in the triplet state undergo an electron transfer, resulting in the symmetry-broken pair TATA•/TATA•2+ (with a lifetime of 19 µs) as confirmed by spectral references obtained from electrochemical reductions (right).
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Eric Vauthey
Physical Chemistry Department - Sciences II - University of Geneva
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