laser spectroscopy; electron transfer; photochemistry; coordination chemistry
Larsen Christopher B., Wenger Oliver S. (2018), Circular Photoinduced Electron Transfer in a Donor-Acceptor- Acceptor Triad, in Angew. Chem. Int. Ed.
, 57, 841-845.
Schmidt Hauke C., Larsen Christopher B., Wenger Oliver S. (2018), Electron Transfer around a Molecular Corner, in Angew. Chem. Int. Ed.
, 57, 10.1002/an.
Nomrowski Julia, Wenger Oliver S. (2018), Exploiting Potential Inversion for Photoinduced Multielectron Transfer and Accumulation of Redox Equivalents in a Molecular Heptad, in J. Am. Chem. Soc.
, 140, 10.1021/ja.
Kuss-Petermann Martin, Wenger Oliver S. (2017), Exceptionally Long-Lived Photodriven Multi-Electron Storage without Sacrificial Reagents, in Chem. Eur. J.
, 23, 10808-10814.
Kuss-Petermann Martin, Orazietti Margherita, Neuburger Markus, Hamm Peter, Wenger Oliver S. (2017), Intramolecular Light-Driven Accumulation of Reduction Equivalents by Proton-Coupled Electron Transfer, in J. Am. Chem. Soc.
, 139, 5225-5232.
Pannwitz Andrea, Wenger Oliver S. (2017), Photoinduced Electron Transfer Coupled to Donor Deprotonation and Acceptor Protonation in a Molecular Triad Mimicking Photosystem II, in J. Am. Chem. Soc.
, 139, 13308-13311.
Kuss-Petermann Martin, Wenger Oliver S. (2017), Pump-Pump-Probe Spectroscopy of a Molecular Triad Monitoring Detrimental Processes for Photoinduced Charge Accumulation, in Helv. Chim. Acta
, 100, e1600283.
Schmidt Hauke C., Spulber Mariana, Neuburger Markus, Palivan Cornelia G., Meuwly Markus, Wenger Oliver S. (2016), Charge Transfer Pathways in Three Isomers of Naphthalene-Bridged Organic Mixed Valence Compounds, in J. Org. Chem.
, 81, 595-602.
Orazietti Margherita, Kuss-Petermann Martin, Hamm Peter, Wenger Oliver S. (2016), Electron Accumulation in a Molecular Pentad, in Angew. Chem. Int. Ed.
, 55, 9407-9410.
Kuss-Petermann Martin, Wenger Oliver S. (2016), Electron Transfer Rate Maxima at Large Donor−Acceptor Distances, in J. Am. Chem. Soc.
, 138, 1349-1358.
Kuss-Petermann Martin, Wenger Oliver S. (2016), Increasing Electron Transfer Rates with Increasing Donor-Acceptor Distance, in Angew. Chem. Int. Ed.
, 55, 815-819.
Bonn Annabell G., Yushchenko Oleksandr, Vauthey Eric, Wenger Oliver S. (2016), Photoinduced Electron Transfer in an Anthraquinone-[Ru(bpy)3]2+-Oligotriarylamine-[Ru(bpy)3]2+- Anthraquinone Pentad, in Inorg. Chem.
, 55, 2894-2899.
Pannwitz Andrea, Wenger Oliver S. (2016), Proton coupled electron transfer from the excited state of a ruthenium(II) pyridylimidazole complex, in Phys. Chem. Chem. Phys.
, 18, 11374-11382.
Kuss-Petermann Martin, Wenger Oliver S. (2016), Reaction Rate Maxima at Large Distances between Reactants, in Chimia
, 70, 177-181.
Kuss-Petermann Martin, Wenger Oliver S. (2016), Unusual Distance Dependences of Electron Transfer Rates, in Phys. Chem. Chem. Phys.
, 18, 18657-18664.
Bonn Annabell G., Wenger Oliver S. (2015), Charge Transfer Emission in Oligotriarylamine−Triarylborane Compounds, in J. Org. Chem.
, 80, 4097-4107.
Chen Jing, Kuss-Petermann Martin, Wenger Oliver S. (2015), Dependence of Reaction Rates for Bidirectional PCET on the Electron Donor−Electron Acceptor Distance in Phenol−[Ru(2,2′-Bipyridine)3]2+ Dyads, in J. Phys. Chem. B
, 119, 2263-2273.
Chen Jing, Wenger Oliver S. (2015), Fluoride binding to an organoboron wire controls photoinduced electron transfer, in Chem. Sci.
, 6, 3582-3592.
Bonn Annabell G., Wenger Oliver S. (2015), Photoinduced Charge Accumulation by Metal Ion-Coupled Electron Transfer, in Phys. Chem. Chem. Phys.
, 17, 24001-24010.
Bonn Annabell G., Wenger Oliver S. (2015), Photoinduced Charge Accumulation in Molecular Systems, in Chimia
, 69, 17-21.
Nomrowski Julia, Wenger Oliver S. (2015), Photoinduced PCET in Ruthenium−Phenol Systems: Thermodynamic Equivalence of Uni- and Bidirectional Reactions, in Inorg. Chem.
, 54, 3680-3687.
Heinz Luisa G., Yushchenko Oleksandr, Neuburger Markus, Vauthey Eric, Wenger Oliver S. (2015), Tetramethoxybenzene is a Good Building Block for Molecular Wires: Insights from Photoinduced Electron Transfer, in J. Phys. Chem. A
, 119, 5676-5684.
Jahnke Ann Christin, Proppe Jonny, Spulber Mariana, Palivan Cornelia G., Herrmann Carmen, Wenger Oliver S. (2014), Charge Delocalization in an Organic Mixed Valent Bithiophene Is Greater Than in a Structurally Analogous Biselenophene, in J. Phys. Chem. A
, 118, 11293-11303.
Chen Jing, Kuss-Petermann Martin, Wenger Oliver S. (2014), Distance Dependence of Bidirectional Concerted Proton–Electron Transfer in Phenol-[Ru(2,2'-bipyridine)3]2+ Dyads, in Chem. Eur. J.
, 20, 4098-4104.
Jahnke Ann Christin, Spulber Mariana, Neuburger Markus, Palivan Cornelia G., Wenger Oliver S. (2014), Electronic coupling mediated by furan, thiophene, selenophene and tellurophene in a homologous series of organic mixed valence compounds, in Chem. Commun.
, 50, 10883-10886.
Bronner Catherine, Wenger Oliver S. (2014), Long-range proton-coupled electron transfer in phenol–[Ru(2,2'-bipyrazine)3]2+ dyads, in Phys. Chem. Chem. Phys.
, 16, 3617-3622.
Bonn Annabell G., Neuburger Markus, Wenger Oliver S. (2014), Photoinduced Electron Transfer in Rhenium(I)−Oligotriarylamine Molecules, in Inorg. Chem.
, 53, 11075-11085.
Kuss-Petermann Martin, Wenger Oliver S. (2013), Mechanistic Diversity in Proton-Coupled Electron Transfer between Thiophenols and Photoexcited [Ru(2,2′-Bipyrazine)3]2+, in J. Phys. Chem. Lett.
, 4, 2535-2539.
Biological systems readily perform photoinduced proton-coupled multi-electron transfer reactions in fuel-forming processes, but no man-made system can even approximate their performance. Activation of small inert molecules such as H2O, CO2, or N2 to chemically more useful molecules (e. g., H2, HCOOH, or NH3) seems possible only via concerted transfer of multiple protons and electrons. Furthermore, these reactions usually require significant energy input. Solar light would be a particularly clean and abundant energy source for this purpose. The proposed research aims at understanding light-driven transfers of electrons and protons at the most fundamental level. This research is therefore directly relevant in the context of artificial photosynthesis, but the generation of fuels from solar light is not the primary goal of this 36-month project. The priority is on understanding some important fundamental aspects of light-to-chemical energy conversion in artificial model systems that will be synthesized specifically for this purpose. Toward this end, three lines of research with different focal points will be pursued.Sub-project 1 addresses the question over how many molecular units an electron can be delocalized in a given “molecular wire”. This research is important in order to be able to transport charge carriers over long distances. For artificial photosynthesis it will be necessary to achieve efficient spatial separation between electrons and holes. It is proposed to focus on oligo-selenophenes and oligo-tellurophenes which represent poorly explored classes of materials (Scheme 1a), particularly when compared to oligo-thiophenes which have already found use in numerous applications.Sub-project 2 focuses on the coupling of proton transfer to photoinduced electron transfer (Scheme 1b). An important goal is to elucidate under what circumstances the photoinduced transfer of an electron and a proton can occur in a concerted manner, and under what conditions the two particles preferably transfer in a stepwise (consecutive) fashion. This is important for example because photo-reduction of CO2 only appears thermodynamically feasible when occurring in concert with proton transfer. Another important goal of sub-project 2 is to explore the possibility of photoinduced long-range electron/proton transfers which formally correspond to hydrogen-atom transfer (HAT) reactions. Dyads and triads specifically designed for this purpose will be synthesized and investigated electrochemically and by transient absorption spectroscopy.In sub-project 3 molecular triads comprised of a donor (D), a sensitizer (S), and an acceptor (A) will be synthesized and investigated. In such triads long-lived charge-separated states of the type D+-S-A- are commonly accessible after photoexcitation. However, these simple charge-separated states are of limited use for further (secondary) chemistry because many of the most interesting chemical transformations require multiple electrons or holes. Therefore, sub-project 3 aims at the photo-generation of doubly charge-separated states of the type D2+-S-A2- (Scheme 1c) through stepwise two-photon excitation, similar to the photon upconversion processes explored by the applicant in the course of his Ph. D. research. In parallel, a molecular pentad offering the possibility for photoinduced two-electron reduction coupled to twofold protonation of an anthraquinone moiety will be synthesized. The three lines of research are to be pursued by 3 individual coworkers, and all of them will follow the “make-and-measure” philosophy of the applicant’s group, i. e., synthetic work will be complemented by electrochemical and optical spectroscopic experiments.