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  1. Article ; Online: Intramolecular Energy Transfer Competing with Light-Driven Intermolecular Proton Transfer in an Iron(II)-NHC Complex? A Query into the Role of Photobasic Ligands and MLCT States.

    Nair, Shruthi S / Bysewski, Oliver A / Klosterhalfen, Niklas / Sittig, Maria / Winter, Andreas / Schubert, Ulrich S / Dietzek-Ivanšić, Benjamin

    ACS omega

    2024  Volume 9, Issue 11, Page(s) 13427–13439

    Abstract: Inorganic photoacids and photobases comprising of photoactive transition metal complexes (TMCs) offer the ability to modulate proton transfer reactions through light irradiation, while utilizing the excellent optical properties of the latter. This ... ...

    Abstract Inorganic photoacids and photobases comprising of photoactive transition metal complexes (TMCs) offer the ability to modulate proton transfer reactions through light irradiation, while utilizing the excellent optical properties of the latter. This provides a powerful tool for precise control over chemical reactions and processes, with implications for both fundamental science and practical applications. In this contribution, we present a novel molecular architecture amending an Fe-NHC complex with a pendant quinoline, as a prototypical photobase, as a representative earth-abundant TMC based inorganic photobase. We characterize the excited-state properties and proton-transfer dynamics using steady-state absorption and emission spectroscopy as well as pump wavelength dependent transient absorption spectroscopy in various protic solvents. The kinetics and thermodynamics of proton transfer in the quinoline moiety are influenced by both the presence of the metal center and the choice of the solvent. Furthermore, we see indications of intramolecular energy transfer from the quinoline to the MLCT state as a limiting factor for panchromatic photobasicity of the complex.
    Language English
    Publishing date 2024-03-07
    Publishing country United States
    Document type Journal Article
    ISSN 2470-1343
    ISSN (online) 2470-1343
    DOI 10.1021/acsomega.3c06196
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  2. Article ; Online: Excitation Energy-Dependent Branching Dynamics Determines Photostability of Iron(II)-Mesoionic Carbene Complexes.

    Nair, Shruthi S / Bysewski, Oliver A / Kupfer, Stephan / Wächtler, Maria / Winter, Andreas / Schubert, Ulrich S / Dietzek, Benjamin

    Inorganic chemistry

    2021  Volume 60, Issue 12, Page(s) 9157–9173

    Abstract: Photoactive metal complexes containing earth-abundant transition metals recently gained interest as photosensitizers in light-driven chemistry. In contrast to the traditionally employed ruthenium or iridium complexes, iron complexes developed to be ... ...

    Abstract Photoactive metal complexes containing earth-abundant transition metals recently gained interest as photosensitizers in light-driven chemistry. In contrast to the traditionally employed ruthenium or iridium complexes, iron complexes developed to be promising candidates despite the fact that using iron complexes as photosensitizers poses an inherent challenge associated with the low-lying metal-centered states, which are responsible for ultrafast deactivation of the charge-transfer states. Nonetheless, recent developments of strongly σ-donating carbene ligands yielded highly promising systems, in which destabilized metal-centered states resulted in prolonged lifetimes of charge-transfer excited states. In this context, we introduce a series of novel homoleptic Fe-triazolylidene mesoionic carbene complexes. The excited-state properties of the complexes were investigated by time-resolved femtosecond transient absorption spectroscopy and quantum chemical calculations. Pump wavelength-dependent transient absorption reveals the presence of distinct excited-state relaxation pathways. We relate the excitation-wavelength-dependent branching of the excited-state dynamics into various reaction channels to solvent-dependent photodissociation following the population of dissociative metal centered states upon excitation at 400 nm.
    Language English
    Publishing date 2021-06-03
    Publishing country United States
    Document type Journal Article
    ZDB-ID 1484438-2
    ISSN 1520-510X ; 0020-1669
    ISSN (online) 1520-510X
    ISSN 0020-1669
    DOI 10.1021/acs.inorgchem.1c01166
    Database MEDical Literature Analysis and Retrieval System OnLINE

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