Function-determining Excited-State Dynamics in Transition-Metal Complex-Based Photodrugs in a Cellular Environment
Final Report Abstract
The project "Function-determining photoinduced processes in transition metal complexes as photoactivatable agents in a cellular environment" aimed to develop experimental-theoretical methods to characterize the properties of excited states in transition metal complexes. In particular, the focus was on the investigation of these complexes in living cells in the context of light-activated tumor therapy (PDT). The methodology included resonance Raman spectroscopy, time-resolved spectroscopy and transient absorption measurements. One focus was on the photophysical properties of Ru(II) polypyridyl complexes in solutions that are relevant for PDT. A correlation was found between the lifetime of non-emissive states and cytotoxicity in cell cultures. Furthermore, the influence of thiophene substituents on the spectroscopic properties of the complexes was investigated. A detailed analysis of the relaxation after photoexcitation by femtosecond time-resolved transient absorption and resonance Raman spectroscopy provides insights into the nature of the excited states and the functiondetermining length of the oligothiophene ligands, which influences the phototoxicity of the complexes in cell cultures. Methodologically, the project delivered innovations in the investigation of light-induced processes in small molecules in living human cells. In addition to the model system Astaxa-nthinin living cells, the dynamics of the electronically excited states of a PDT-active Ru(II) complex in living human cells were finally investigated. Thus, the project not only investigated structure-dynamics-function correlations in selected light-activated drugs but also made important methodological contributions to a better understanding of the photophysical processes of transition metal complexes in a cellular environment.
Publications
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Predictive Strength of Photophysical Measurements for in Vitro Photobiological Activity in a Series of Ru(II) Polypyridyl Complexes Derived from π-Extended Ligands. Inorganic Chemistry, 58(5), 3156-3166.
Reichardt, Christian; Monro, Susan; Sobotta, Fabian H.; Colón, Katsuya L.; Sainuddin, Tariq; Stephenson, Mat; Sampson, Eric; Roque, John; Yin, Huimin; Brendel, Johannes C.; Cameron, Colin G.; McFarland, Sherri & Dietzek, Benjamin
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Intracellular Photophysics of an Osmium Complex bearing an Oligothiophene Extended Ligand. Chemistry – A European Journal, 26(65), 14844-14851.
Schneider, Kilian R. A.; Chettri, Avinash; Cole, Houston D.; Reglinski, Katharina; Brückmann, Jannik; Roque, John A.; Stumper, Anne; Nauroozi, Djawed; Schmid, Sylvia; Lagerholm, Christoffer B.; Rau, Sven; Bäuerle, Peter; Eggeling, Christian; Cameron, Colin G.; McFarland, Sherri A. & Dietzek, Benjamin
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PC 2D-COS: A Principal Component Base Approach to Two-Dimensional Correlation Spectroscopy. Applied Spectroscopy, 74(4), 460-472.
Hniopek, Julian; Schmitt, Michael; Popp, Jürgen & Bocklitz, Thomas
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WE-ASCA: The Weighted-Effect ASCA for Analyzing Unbalanced Multifactorial Designs—A Raman Spectra-Based Example. Molecules, 26(1), 66.
Ali, Nairveen; Jansen, Jeroen; van den Doel, André; Tinnevelt, Gerjen Herman & Bocklitz, Thomas
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It Takes Three to Tango: The Length of the Oligothiophene Chain Determines the Nature of the Long‐Lived Excited State and the Resulting Photocytotoxicity of a Ruthenium(II) Photodrug. ChemPhotoChem, 5(5), 421-425.
Chettri, Avinash; Roque, John A.; Schneider, Kilian R. A.; Cole, Houston D.; Cameron, Colin G.; McFarland, Sherri A. & Dietzek, Benjamin
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Kinetic-Model-Free Analysis of Transient Absorption Spectra Enabled by 2D Correlation Analysis. The Journal of Physical Chemistry Letters, 12(17), 4148-4153.
Hniopek, Julian; Müller, Carolin; Bocklitz, Thomas; Schmitt, Michael; Dietzek, Benjamin & Popp, Jürgen
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Monitoring excited-state relaxation in a molecular marker in live cells–a case study on astaxanthin. Chemical Communications, 57(52), 6392-6395.
Yang, Tingxiang; Chettri, Avinash; Radwan, Basseem; Matuszyk, Ewelina; Baranska, Malgorzata & Dietzek, Benjamin
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String-Attached Oligothiophene Substituents Determine the Fate of Excited States in Ruthenium Complexes for Photodynamic Therapy. The Journal of Physical Chemistry A, 125(32), 6985-6994.
Chettri, Avinash; Schneider, Kilian R. A.; Cole, Houston D.; Roque, John A.; Cameron, Colin G.; McFarland, Sherri A. & Dietzek, Benjamin
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Interaction with a Biomolecule Facilitates the Formation of the Function-Determining Long-Lived Triplet State in a Ruthenium Complex for Photodynamic Therapy. The Journal of Physical Chemistry A, 126(8), 1336-1344.
Chettri, Avinash; Cole, Houston D.; Roque, III John A.; Schneider, Kilian R. A.; Yang, Tingxiang; Cameron, Colin G.; McFarland, Sherri A. & Dietzek-Ivanšić, Benjamin
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Using Biological Photophysics to Map the Excited‐State Topology of Molecular Photosensitizers for Photodynamic Therapy. Angewandte Chemie International Edition, 62(17).
Chettri, Avinash; Yang, Tingxiang; Cole, Houston D.; Shi, Ge; Cameron, Colin G.; McFarland, Sherri A. & Dietzek‐Ivanšić, Benjamin
