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Primary processes in photophysics and photochemistry of a potential light-activated anti-cancer dirhodium complex

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Abstract

Photophysics and photochemistry of a potential light-activated cytotoxic dirhodium complex [Rh2(µ-O2CCH3)2(bpy)(dppz)](O2CCH3)2, where bpy = 2,2′-bipyridine, dppz = dipyrido[3,2-a:2′,3′-c]phenazine (Complex 1 or Rh2) in aqueous solutions was studied by means of stationary photolysis and time-resolved methods in time range from hundreds of femtoseconds to microseconds. According to the literature, Complex 1 demonstrates both oxygen-dependent (due to singlet oxygen formation) and oxygen-independent cytotoxicity. Photoexchange of an acetate ligand to a water molecule was the only observed photochemical reaction, which rate was increased by oxygen removal from solutions. Photoexcitation of Complex 1 results in the formation of the lowest triplet electronic excited state, which lifetime is less than 10 ns. This time is too short for diffusion-controlled quenching of the triplet state by dissolved oxygen resulting in 1O2 formation. We proposed that singlet oxygen is produced by photoexcitation of weakly bound van der Waals complexes [Rh2…O2], which are formed in solutions. If this is true, no oxygen-independent light-induced cytotoxicity of Complex 1 exists. Residual cytotoxicity deaerated solutions are caused by the remaining [Rh2…O2] complexes.

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The Supporting Information file contains NMR data and some raw data of ultrafast TA experiment as well as exact formulae for SADS extraction from the global fit results.

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Acknowledgements

The financial support of the Russian Science Foundation (Grant No. 22-23-00248) is gratefully acknowledged. Sergei V. Chekalin acknowledges funding by the research project FFUU-2022-0004 of the Institute of Spectroscopy of the Russian Academy of Sciences.

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Authors and Affiliations

  1. Voevodsky Institute of Chemical Kinetics and Combustion, Siberian Branch of the Russian Academy of Sciences, Novosibirsk, Russian Federation

    Veronica V. Semionova, Ivan P. Pozdnyakov, Vjacheslav P. Grivin & Evgeni M. Glebov

  2. Novosibirsk State University, Novosibirsk, Russian Federation

    Ilia V. Eltsov & Evgeni M. Glebov

  3. Nikolaev Institute of Inorganic Chemistry, Siberian Branch of the Russian Academy of Sciences, Novosibirsk, Russian Federation

    Danila B. Vasilchenko & Evgeniya V. Polyakova

  4. Institute of Spectroscopy, Russian Academy of Sciences, Troitsk, Moscow, Russian Federation

    Alexei A. Melnikov & Sergei V. Chekalin

  5. Key Laboratory of Environmental Biotechnology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Bei**g, China

    Lei Wang

  6. Department of Physics, High School of Economy, Moscow, Russian Federation

    Alexei A. Melnikov

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  1. Veronica V. Semionova
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Semionova, V.V., Pozdnyakov, I.P., Grivin, V.P. et al. Primary processes in photophysics and photochemistry of a potential light-activated anti-cancer dirhodium complex. Photochem Photobiol Sci 23, 153–162 (2024). https://doi.org/10.1007/s43630-023-00509-y

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