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    Iron(II) Coordination Complexes with Panchromatic Absorption and Nanosecond Charge-Transfer Excited State Lifetimes

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    Date
    2019-11-18
    Author
    Braun, Jason
    Lozada, Issiah
    Kolodziej, Charles
    Burda, Clemens
    Newman, Kelly M E
    van Lierop, Johan
    Davis, Rebecca L
    Herbert, David E
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    Abstract
    Replacing current benchmark rare-element photosensitizers with ones based on abundant and low-cost metals such as iron would help facilitate the large-scale implementation of solar energy conversion. To do so, the ability to extend the lifetimes of photogenerated excited states of iron complexes is critical. Here, we present a sensitizer design in which iron(ii) centres are supported by frameworks containing benzannulated phenanthridine and quinoline heterocycles paired with amido donors. These complexes exhibit panchromatic absorption and nanosecond charge-transfer excited state lifetimes, enabled by the combination of vacant, energetically accessible heterocycle-based acceptor orbitals and occupied molecular orbitals destabilized by strong mixing between amido nitrogen atoms and iron. This finding shows how ligand design can extend metal-to-ligand charge-transfer-type excited state lifetimes of iron(ii) complexes into the nanosecond regime and expand the range of potential applications for iron-based photosensitizers.
    URI
    http://hdl.handle.net/1993/36069
    DOI
    10.1038/s41557-019-0357-z
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    • Faculty of Science Scholarly Works [209]
    • University of Manitoba Scholarship [1981]

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