Photoaddition of two guanine bases to single Ru-TAP complexes. Computational studies and ultrafast spectroscopies to elucidate the pH dependence of primary processes

The Journal of Physical Chemistry. B
Lionel MarcélisAndrée Kirsch-De Mesmaeker

Abstract

The covalent photoadduct (PA) between [Ru(TAP)3](2+) (TAP = 1,4,5,8-tetraazaphenanthrene) and guanosine monophosphate (GMP) opened the way to interesting photobiological applications. In this context, the PA's capability upon illumination to give rise to the addition of a second guanine base is especially interesting. The origins of these intriguing properties are for the first time thoroughly investigated by an experimental and theoretical approach. The PA's spectroscopic and redox data combined with TDDFT results corroborated with resonance Raman data show that the properties of this PA (pKa around 7) depend on the solution pH. Theoretical results indicate that the acid form PA.H(+) when excited should relax to MLCT (metal-to-ligand charge transfer) excited states, in contrast to the basic form PA whose excited state should have LLCT/ILCT (ligand-to-ligand charge transfer/intra ligand charge transfer) characteristics. Ultrafast excitation of PA.H(+) at pH 5.9 produces continuous dynamic processes in a few hundred picoseconds involving coupled proton-electron transfers responsible for luminescence quenching. Long-lived species of a few microseconds capable of reacting with GMP are produced at that pH, in agreement with the for...Continue Reading

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Jun 19, 2013·Philosophical Transactions. Series A, Mathematical, Physical, and Engineering Sciences·Lionel MarcélisAndrée Kirsch-De Mesmaeker

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Citations

May 5, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Sofia KajoujCécile Moucheron
Nov 1, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Bjørn C PoulsenThorfinnur Gunnlaugsson
Nov 28, 2017·Chemical Society Reviews·Fergus E PoyntonThorfinnur Gunnlaugsson
Feb 22, 2017·Inorganic Chemistry·Ludovic Troian-GautierMichel Luhmer
May 17, 2018·Journal of the American Chemical Society·Christopher S BurkeTia E Keyes
Nov 23, 2021·Journal of the American Chemical Society·Fabian DrögeJim A Thomas

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