Lookup NU author(s): Dr Thomas Penfold
This work is licensed under a Creative Commons Attribution-NonCommercial 4.0 International License (CC BY-NC 4.0).
Fe(II) complexes have long been assumed unsuitable as photosensitisers because of their low-lying non-emissive metal centred (MC) states, which inhibit electron transfer. Herein, we describe the excited state relaxation of a novel Fe(II) complex that incor- porates N-heterocyclic carbene ligands designed to destabilise the MC states. Using rst principles quantum nuclear wavepacket simulations we achieve a detailed under- standing of the photoexcited decay mechanism, demonstrating that it is dominated by an ultrafast intersystem crossing from 1MLCT-3MLCT proceeded by slower kinetics associated with the conversion into the 3MC states. The slowest component of the 3MLCT decay, important in the context of photosensitisers, are much longer than re- lated Fe(II) complexes because the population transfer to the 3MC states occurs in a region of the potential where the energy gap between the 3MLCT and 3MC states is large, making the population transfer inecient.
Author(s): Pápai M, Vankó G, Rozgonyi T, Penfold T
Publication type: Article
Publication status: Published
Journal: Journal of Physical Chemistry Letters
Online publication date: 11/05/2016
Acceptance date: 11/05/2016
Date deposited: 13/05/2016
ISSN (electronic): 1948-7185
Publisher: American Chemical Society
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