Photochemistry and Photophysics of Coordination Compounds

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250 M.T. Indelli et al. chemical lesion in DNA. Investigations of photoinitiated repair of duplexes containing a single thymine dimer lesion were carried out with visible light (400 nm) using both nontethered and tethered complexes (Fig. 17). The quantum yield for photorepair with a Rh(III)-tethered complex is substantially (about ca. 30 fold) reduced compared to the noncovalently bound complex. Since the repair efficiency does not appear to be very sensitive to the distance between intercalated rhodium complex and the thymine dimer, the authors suggest that the observed disparity likely results from differences in π-stacking. In addition, evidences that the repair efficiency diminished with disruption of the intervening π-stack confirm that the DNA helix mediates this long-range oxidative repair reaction. 5 Conclusion A large number of rhodium(III) polypyridine complexes and their cyclometalated analogues have been investigated from the viewpoint of photochemistry, photophysics and of their possible applications. As mononuclear species, Rh(III) polypyridine complexes display interesting photophysical properties, with lowest excited states of LC type for tris bis-chelated species, and increasing role of MC states for mixed-ligand halopolypyridine species. In Rh(III) cyclometalated complexes, the covalent character of the C – Rh bonds makes the excited state classification less clearcut, with strong mixing of LC, MLCT, and LLCT character. Many polynuclear and supramolecular systems containing Rh(III) polypyridine and related units have been synthesized and studied, taking advantage of the favorable properties of these units as good electron acceptors and strong photo-oxidants. In particular, Ru(II)-Rh(IIII) dyads have been actively investigated for the study of photoinduced electron transfer, with specific interest in driving force, distance, and bridging ligand effects. A limited number of supramolecular systems of higher nuclearity have also been produced. Among these, of particular interest are trinuclear species containing rhodium dihalo polypyridine units, which can act as two-electron storage components thanks to their Rh(III)/Rh(I) redox behavior. Finally, a large amount of work has been devoted to the use of Rh(III) polypyridine complexes as intercalators for DNA. In this role, they have shown a very versatile behavior, being used for direct strand photocleavage marking the site of intercalation, to induce long-distance photochemical damage or dimer repair, or to act as electron acceptors in long-range electron transfer processes. Acknowledgements Financial support from MUR (PRIN 2006) is gratefully acknowledged.
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