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The control of photophysical properties of iron complexes and especially oftheir excited states decay is a great challenge in the search for sustainablealternatives to noble metals in photochemical applications. Herein we reportthe synthesis and investigations of the photophysics of mer and fac ironcomplexes bearing bidentate pyridyl-NHC ligands, coordinating the Fe with threeligand-field enhancing carbene bonds. Ultrafast transient absorptionspectroscopy reveals two distinct excited state populations for both mer andfac forms, ascribed to the populations of the T1 and the T2 states,respectively, which decay to the ground state via parallel pathways. We find3-4 ps and 15-20 ps excited state lifetimes, with respective amplitudesdepending on the isomer. The longer lifetime exceeds the one reported for ironcomplexes with tridentate ligands analogues involving four iron-carbene bonds.By combining experimental and computational results, a mechanism based on thedifferential trapping of the triplet states in spin-crossover regions isproposed for the first time to explain the impact of the fac/mer isomerism onthe overall excited-state lifetimes. Our results clearly highlight the impactof bidentate Pyridyl-NHC ligands on the photophysics of iron complexes,especially the paramount role of fac/mer isomerism in modulating the overalldecay process, which can be potentially exploited in the design of newFe(II)-based photoactive compound.

Impact of the fac/mer isomerism on the excited states dynamics of pyridyl-carbene Fe(II) complexes